Toughened carbon-containing glass material

Abstract

In some implementations, a carbonaceous glass material includes a surface-to-air interface and a mesophase region extending from the surface-to-air interface in a direction toward a depth within the carbonaceous glass material. The surface-to-air interface may be exposed to ambient air, and the mesophase region may include a plurality of few-layer graphene (FLG) nanosheets formed in response to rebinding and / or self-nucleation of a plurality of carbon-containing radicals implanted within the mesophase region. The FLG nanosheets have an aperiodic orientation configured to at least partially inhibit the formation or propagation of microcracks and / or micropores in the carbonaceous glass material. The glass material may also include a compressive stress layer disposed between the mesophase region of the carbon-containing glass material and the surface-to-air interface, the compressive stress layer induced by ion bombardment of the carbon-containing glass material with a plurality of ionized inert gas particles.

Description

[0001] This application is a divisional application of an application with an application date of July 23, 2021, an invention name of “Toughened Carbon-Containing Glass Material”, an international application number of PCT / US2021 / 042994 and a Chinese national application number of 202180055909.5. Technical Field

[0002] The present disclosure relates generally to glass materials, and in particular, to making, enhancing and / or strengthening glass materials having few-layer graphene (FLG) nanosheets dispersed throughout one or more portions of the glass material. Background Art

[0003] Glass is a non-crystalline solid material that can be used in a variety of fields, including, for example, windows, digital screen displays, optical instruments, and medical storage containers. Glass can contain silicon dioxide (SiO2) (also referred to as silica) as the main component material. In general, glass can be formed as follows: a mixture of dry granular silicon dioxide and other solid raw materials is heated until the mixture reaches a softened semi-solid state, and then the mixture is rapidly cooled to prevent the mixture from forming a crystalline structure. Glass is relatively fragile than other solid materials, and can be more easily scratched, cracked, and / or shattered than other solid materials. Therefore, it is necessary to have glass and glass materials that are stronger, less fragile, and less prone to cracking than conventional glass and glass materials. Summary of the invention

[0004] The systems, methods and devices of the present disclosure each have several novel aspects, no single one of which is solely responsible for the desirable attributes disclosed herein.

[0005] A novel aspect of the subject matter described in the present disclosure may be implemented as a manufacturing method. In various implementations, the method may be used to manufacture, enhance and / or strengthen a carbon-containing glass material. In some implementations, the method may include flowing hydrocarbon gas and silane into a reactor. The method may include providing an additive to the reactor, including any one or more of lithium, nickel, manganese, copper, trimethylaluminum (TMA), trimethylgallium (TMG) or sulfur. The method may include generating a non-thermal equilibrium plasma based on the excitation of hydrocarbon gas and silane by microwave energy, wherein the non-thermal equilibrium plasma includes a plurality of methyl radicals. The method may include at least using methyl radicals to ion bombard the surface of the carbon-containing glass material with an air interface, the ion bombardment being configured to generate an intermediate phase region within the carbon-containing glass material. The method may include forming a plurality of few-layer graphene (FLG) nanosheets in an intermediate phase region of the carbon-containing glass material at different concentration levels based on the recombination or self-nucleation of a plurality of methyl radicals. The plurality of FLG nanosheets may be dispersed throughout the mesophase region in a non-periodic orientation that may at least partially inhibit the formation or propagation of cracks and / or surface defects in the carbon-containing glass material. The method may include doping one or more surfaces of at least some of the FLG nanosheets formed in the mesophase region with an additive. The method may include embedding the additive between adjacent graphene layers within at least some of the FLG nanosheets formed in the mesophase region of the carbon-containing glass material.

[0006] In various implementations, the carbon-containing glass material may include any one or more of silicate glass, soda-lime glass, alkali-aluminosilicate glass, or borosilicate glass. In some implementations, the alkali-aluminosilicate glass is composed of about 57% to 60% SiO2, about 10% to 25% Al2O3, and about 10% alkaline earth metal. Silane may be a liquid precursor or silane gas with silane. In one implementation, the FLG nanosheets formed in the mesophase region have a combined weight of less than 2% of the carbon-containing glass material. In some cases, the additive may include an alkali metal (such as lithium, sodium, potassium, calcium, fluorine, or bromine), a transition metal (such as copper or iron), or any combination thereof. In other cases, the additive may include lithium, nickel, manganese, copper, trimethylaluminum (TMA), trimethylgallium (TMG), sulfur, or any combination thereof.

[0007] The mesophase region may extend from the surface of the carbon-containing glass material to a depth of about one micron in the carbon-containing glass material. In some implementations, the upper portion of the mesophase region adjacent to the surface and air interface has a relatively high concentration of FLG nanosheets, and the lower portion of the mesophase region away from the surface and air interface has a relatively low concentration of FLG nanosheets. In some aspects, the FLG nanosheets in the upper portion of the mesophase region have a size of about 20 nanometers (nm), and the FLG nanosheets in the lower portion of the mesophase region have a size of about 2 nm. In some implementations, the size of the FLG nanosheets in the gradient portion of the mesophase region between the upper and lower portions of the mesophase region gradually decreases in the direction toward the depth of the mesophase region. In some aspects, the FLG nanosheets in the lower portion of the mesophase region are uniformly distributed in the plane of the lower portion of the mesophase region. In addition, or in an alternative example, the density of a plurality of FLG nanosheets may gradually decrease along the direction extending from the surface and air interface to the depth of the mesophase region.

[0008] In various implementations, the additive may be configured to self-heal cracks formed in the carbon-containing glass material after the additive is exposed to ambient air. For example, the additive may be oxidized when exposed to reactants present in ambient air (such as gaseous oxygen, O2 and / or moisture (H2O), and the resulting oxidized additive may extend into cracks and / or surface defects formed in the carbon-containing glass material. In some aspects, the oxidized additive may also coat the surface of the cracks and / or surface defects formed in the carbon-containing glass material. In some cases, the additive may be embedded between adjacent graphene layers of the FLG nanosheet during a post-processing operation. The post-processing operation may include isothermal treatment in a vacuum or in an inert atmosphere.

[0009] Another novel aspect of the subject matter described in the present disclosure may be implemented as a manufacturing method. In various implementations, the method may be used to manufacture, enhance and / or strengthen a carbon-containing glass material. In some implementations, the method may include supplying a non-thermal equilibrium plasma including a plurality of positively charged gas particles and a plurality of ionized inert gas particles into a reaction chamber. The method may include accelerating at least a plurality of positively charged gas particles through the reaction chamber based on applying an external potential to the non-thermal equilibrium plasma. The method may include bombarding the surface and air interface of the carbon-containing glass material with accelerated positively charged gas particles and ionized inert gas particles. The method may include forming an intermediate phase region in the carbon-containing glass material in response to the bombardment of the accelerated positively charged gas particles and ionized inert gas particles. The intermediate phase region, which may extend from the surface and air interface along a direction orthogonal to the surface and air interface to a depth of about one micron in the carbon-containing glass material, may have a plurality of microcracks or micropores formed therein by bombardment. In some cases, the microcracks or micropores may have a size between about 5 nanometers (nm) and 10 nm. The method may include forming a compressive stress layer in a carbon-containing glass material in response to bombardment of at least ionized noble gas particles. The compressive stress layer may be disposed between an interphase region of the carbon-containing glass material and a surface-air interface. The carbon-containing glass material may include a silicate glass, a soda-lime glass, an alkali-aluminosilicate glass, a borosilicate glass, or any combination thereof. In one implementation, the alkali-aluminosilicate glass is composed of about 57% to 60% SiO2, about 10% to 25% Al2O3, and about 10% alkaline earth metals.

[0010] In some cases, the non-thermal equilibrium plasma can include an intrinsic potential. In some aspects, the intrinsic potential of the non-thermal equilibrium plasma can be sufficient to allow at least some positively charged gas particles and / or ionized noble gas particles to penetrate the surface of the glass material and the air interface without applying an external potential to the reaction chamber.

[0011] The method may also include implanting a plurality of carbon-based free radicals separated from a non-thermal equilibrium plasma into a mesophase region of a carbon-containing glass material, while bombarding the surface and air interface with accelerated positively charged gas particles and ionized inert gas particles. The method may include forming a plurality of few-layer graphene (FLG) nanosheets in a mesophase region of a carbon-containing glass material based on the recombination and / or self-nucleation of a plurality of implanted carbon-based free radicals. Carbon-based free radicals may be implanted in the mesophase region at one or more different incident angles. In some aspects, the upper portion of the mesophase region adjacent to the surface and air interface may have a relatively high concentration of FLG nanosheets, and the lower portion of the mesophase region away from the surface and air interface may have a relatively low concentration of FLG nanosheets. In addition, the FLG nanosheets in the upper portion of the mesophase region may have a size of about 20 nanometers (nm), and the FLG nanosheets in the lower portion of the mesophase region may have a size of about 2 nm. In one implementation, the size of the FLG nanosheets formed in the mesophase region gradient portion between the upper and lower portions of the mesophase region gradually decreases in the direction of the depth toward the mesophase region. In some aspects, the FLG nanosheets in the lower portion of the mesophase region can be uniformly distributed in the plane of the lower portion of the mesophase region.

[0012] In some implementations, the method may further include embedding an additive between adjacent graphene layers within the FLG nanosheets formed in the mesophase region. In some cases, the additive may include an alkali metal (such as lithium, sodium, potassium, calcium, fluorine, or bromine), a transition metal (such as copper or iron), or any combination thereof. In other cases, the additive may include lithium, nickel, manganese, copper, trimethylaluminum (TMA), trimethylgallium (TMG), sulfur, or any combination thereof. In one implementation, the first portion of the additive embedded in the FLG nanosheets formed in the upper portion of the mesophase region has a molar fraction of about 50%, and the second portion of the additive embedded in the FLG nanosheets formed in the lower portion of the mesophase region has a molar fraction of about 2%. Other portions of the additive implanted in the region between the upper and lower portions of the mesophase region may have a molar fraction that gradually decreases in the direction of the depth toward the mesophase region.

[0013] The additive may be configured to self-heal cracks formed in the carbon-containing glass material upon exposure of the additive to reactants present in ambient air, such as gaseous oxygen, O2, and / or moisture (H2O). For example, the additive may oxidize upon exposure to such reactants in ambient air, and the resulting oxidized additive may extend into cracks and / or surface defects formed in the carbon-containing glass material. In some aspects, the oxidized additive may also coat the surface of cracks and / or surface defects formed in the carbon-containing glass material.

[0014] Another novel aspect of the subject matter described in the present disclosure can be achieved via a carbon-containing glass material. In some implementations, the carbon-containing glass material can include a surface-air interface and an intermediate phase region. The intermediate phase region can extend from the surface-air interface, along a direction orthogonal to the surface-air interface, to a depth of about one micron within the carbon-containing glass material. The intermediate phase region can include a plurality of few-layer graphene (FLG) nanosheets formed in response to the recombination and / or self-nucleation of a plurality of carbon-containing free radicals implanted within the intermediate phase region. The plurality of FLG nanosheets can have a non-periodic orientation that is configured to at least partially inhibit the formation or propagation of cracks and / or surface defects in the carbon-containing glass material.

[0015] In some implementations, the FLG nanosheets formed in the upper portion of the mesophase region adjacent to the surface-air interface may have a size of about 20 nanometers (nm), and the FLG nanosheets formed in the lower portion of the mesophase region away from the surface-air interface may have a size of about 2 nm. In some aspects, the density of the FLG nanosheets formed in the mesophase region gradually decreases along the direction extending from the surface-air interface to the depth of the mesophase region. In some cases, the mesophase region may have a fracture toughness of less than 50 gigapascals (GPa). In addition, or in an alternative example, the FLG nanosheets formed in the mesophase region of the glass material may be configured to induce a compressive stress (CS) greater than 150 megapascals (MPa) in the mesophase region. In some aspects, each FLG nanosheet formed in the mesophase region includes between 3 and 5 graphene layers stacked on top of each other and has a combined weight of less than 2% of the carbon-containing glass material.

[0016] In various implementations, the mesophase region may also include additives embedded between adjacent graphene layers within the FLG nanosheets formed in the mesophase region. In some cases, the additive may include an alkali metal (such as lithium, sodium, potassium, calcium, fluorine, or bromine), a transition metal (such as copper or iron), or any combination thereof. In other cases, the additive may include lithium, nickel, manganese, copper, trimethylaluminum (TMA), trimethylgallium (TMG), sulfur, or any combination thereof. The additive may be configured to self-repair cracks formed in the carbon-containing glass material after the additive is exposed to ambient air. For example, the additive may be oxidized when exposed to ambient air, and the resulting oxidized additive may extend to cracks and / or surface defects formed in the carbon-containing glass material. In some aspects, the oxidized additive may also coat the surface of cracks and / or surface defects formed in the carbon-containing glass material.

[0017] In some implementations, the carbon-containing glass material may also include a compressive stress layer formed below the surface and air interface. In one implementation, the compressive stress layer may be formed by bombarding the surface and air interface of the carbon-containing glass material with a plurality of ionized inert gas particles. The ionized inert gas particles may penetrate the surface and air interface of the carbon-containing glass material and form microcracks or micropores in one or more portions of the mesophase region. In some cases, the microcracks or micropores may have a size between about 5 nanometers (nm) and 10 nm. BRIEF DESCRIPTION OF THE DRAWINGS

[0018] Details of one or more implementations of the subject matter described in the present disclosure are set forth in the accompanying drawings and the following detailed description. Other features, aspects, and advantages will become apparent from the detailed description, drawings, and claims. Note that the relative dimensions of the following figures may not be drawn to scale.

[0019] Figure 1 An example carbon-containing glass material is shown according to some implementations.

[0020] Figure 2 According to some implementations, Figure 1 Example FLG nanosheets that can be formed in a carbon-containing glass material.

[0021] Figure 3A Describes a method that can be used according to some implementations Figure 1 Example toughening mechanisms in carbon-containing glassy materials.

[0022] Figure 3B Describes a method that can be used according to some implementations Figure 1 Another example toughening mechanism in carbon-containing glassy materials.

[0023] Figure 3C Describes a method that can be used according to some implementations Figure 1 Another example toughening mechanism in carbon-containing glassy materials.

[0024] Figure 4 Example carbon-containing glass materials having more than one mesophase region are shown according to some implementations.

[0025] Figure 5 Describes some implementations Figure 1 Part of a carbon-containing glass material.

[0026] Figure 6 An example reactor that may be used to manufacture, enhance, and / or strengthen carbon-containing glass materials according to some implementations is shown.

[0027] Figure 7Another example reactor that may be used to manufacture, enhance, and / or strengthen carbon-containing glass materials according to some other implementations is shown.

[0028] Fig. 8A A flow chart illustrating example operations for strengthening a carbon-containing glass material is shown, according to some implementations.

[0029] Figure 8B A flow chart illustrating another example operation for strengthening a carbon-containing glass material is shown, according to some implementations.

[0030] Figure 8C A flow chart illustrating another example operation for strengthening a carbon-containing glass material is shown, according to some implementations.

[0031] Fig.9A and Fig. 9B A flow chart illustrating example operations for forming a carbon-containing glass material is shown, according to some other implementations.

[0032] Fig.10 A flow chart illustrating another example operation for forming a carbon-containing glass material is shown, according to some other implementations.

[0033] Like reference numbers and names in the various drawings indicate like elements. DETAILED DESCRIPTION

[0034] Aspects of the present disclosure are provided in the following description and related drawings for various examples, which are provided for illustrative purposes. Alternative aspects may be designed without departing from the scope of the present disclosure. In addition, well-known elements of the present disclosure will not be described in detail or will be omitted to avoid making the relevant details of the present disclosure difficult to understand.

[0035] The toughness of a material may indicate the ability of the material to withstand an applied force without undergoing mechanical fracture, and may depend at least in part on the compressive strength, tensile strength, and fracture toughness of the material. The compressive strength of a material may indicate the ability of the material to withstand an applied force, which may be measured in Pascals (Pa). The ultimate tensile strength (UTS) of a material may indicate the maximum stress that the material can withstand when stretched or pulled before mechanical failure (such as before breaking into pieces). The fracture toughness of a material indicates the inherent ability of the material to resist fracture and / or cracking.

[0036] Glass and glass-containing materials are also susceptible to cracking caused by external forces, such as cracking caused by an object striking the glass. For example, when an external force equal to or greater than a certain fracture energy is applied to the glass material, the external force may cause cracks to form in the glass-containing material and / or may cause pre-existing cracks to propagate and propagate throughout the glass material. In addition, when the glass material is subjected to compressive or tensile stresses, pre-existing defects in the glass material, such as scratches and surface blemishes, may exacerbate the applied compressive and / or tensile stresses, which in turn may cause relatively high stress concentrations to occur at or near the pre-existing defects. Portions of the glass material associated with relatively high stress concentrations may be more susceptible to crack formation and propagation than other portions of the glass material.

[0037] Conventional glass has a tensile strength of about 7 megapascals (MPa), and has a theoretical maximum tensile strength of about 17 gigapascals (GPa), several orders of magnitude higher than its typical tensile strength. The relatively high value of the theoretical maximum tensile strength of glass can be attributed to the strong chemical bonds between silicon and oxygen in silicon oxide (SiO2) molecules, which form the basis of many glass materials. However, flaws and surface defects (such as microcracks, cracks, and scratches) introduced into glass materials during conventional manufacturing techniques typically reduce the measured tensile strength of glass materials from the theoretical maximum tensile strength to a typical tensile strength of about 7 MPa.

[0038] Applicants have determined that during conventional manufacturing methods, the introduction of impurities into glass can result in relatively high brittleness of the glass. These impurities, which are typically introduced into glass as a strengthening mechanism, may reduce the compressive strength, tensile strength, and / or fracture toughness of the glass material. For example, when heating the glass, the unmelted or undissolved portion of such impurities may cause one or more laminated layers to form on or within the glass material, which in turn may produce internal stresses within the glass material, reducing the overall strength of the glass material. The unmelted or undissolved portion of these impurities may also inadvertently provide nucleation and growth sites for crack formation and / or propagation throughout the glass. In addition, conventional thermal and chemical strengthening methods may expose the molten glass to moisture, dust, and other particles in the ambient air, thereby exposing the glass to other impurities, which may further reduce the compressive strength, tensile strength, and / or fracture toughness of the glass material.

[0039] According to various implementations of the subject matter disclosed herein, the surface and air interface of the glass material can be bombarded with carbon-based free radicals, ionized inert gas particles, additives, positively charged particles, or any combination thereof. The glass material can be bombarded with ionized inert gas particles and / or positively charged particles, which can penetrate the surface and air interface of the glass material and generate microcracks and / or micropores in the mesophase region of the glass material. Carbon-based free radicals can be implanted into the microcracks and / or micropores generated in the mesophase region by bombardment. In some aspects, carbon-based free radicals can also be implanted in other parts of the glass material. The implanted carbon-based free radicals can recombine and / or self-nucleate to form multiple FLG nanosheets in the entire mesophase region. The FLG nanosheets can be dispersed throughout the mesophase region in a random or non-periodic orientation, thereby inhibiting the formation and / or propagation of cracks in the glass material. In some aspects, one or more surfaces of the FLG nanosheets formed in the mesophase region can be doped with additives.

[0040] The additive may be embedded between adjacent graphene layers of the FLG nanosheets, which are dispersed throughout the mesophase region. Subsequently, when the glass material generates one or more cracks in response to an external force applied to the glass material, the additive portion embedded in the FLG nanosheets at or near the one or more cracks may be exposed to ambient air. The chemical reaction between the exposed additive and the ambient air may produce a metal oxide, which extends into one or more cracks formed in the glass material and / or coats the surface of the cracks. The extension of the metal oxide into the cracks and the metal oxide coating formed on the exposed surface of the cracks may prevent or at least inhibit the further propagation of the cracks in the glass material. In this way, the technology disclosed herein can be used to manufacture, enhance and / or strengthen glass and glass materials without introducing undesirable impurities, which may reduce the compressive strength, tensile strength and / or fracture toughness of the glass or glass material.

[0041] Figure 1 A carbon-containing glass material 100 that can be manufactured, enhanced, and / or strengthened according to one or more aspects of the subject matter disclosed herein is shown. The carbon-containing glass material 100 can be any suitable type of glass, glass-containing material, or carbon-containing glass material. In some implementations, the glass material 100 can be or include an alkali-aluminosilicate glass having a composition of about 57%-60% SiO2, about 10%-25% Al2O3, and about 10% alkaline earth metals. In some aspects, the glass material 100 can have a carbon content of 9.8×10 -6 / K thermal expansion rate. In other implementations, the glass material 100 may be or may include (but is not limited to) borosilicate glass, silicate glass, or soda-lime glass. In some cases, the glass material 100 may be chemically strengthened using one or more conventional glass strengthening methods before applying the various glass strengthening techniques disclosed herein. For example, the glass material 100 may be chemically strengthened via thermal tempering, surface crystallization, and / or via application of other chemicals to the glass material 100. In other cases, the glass material 100 may be a chemically strengthened glass, such as Gorilla Glass, available from Corning, Inc. (Corning, New York). ® Glass. In some other cases, the glass material 100 can be Dragontrail glass available from AsahiGlass Co., Tokyo, Japan.

[0042] The glass material 100 includes a surface-to-air interface 110, a mesophase region 120, and a substrate region 130 as shown. The surface-to-air interface 110 may be exposed to an external environment including ambient air 102, and may provide an interface through which carbon-based free radicals, ionized noble gas particles, additives, positively charged particles, and other particles or mixtures may penetrate and / or be implanted into the glass material during the manufacture of the glass material 100. The mesophase region 120 extends from the surface-to-air interface 110, along a direction 150 orthogonal to the surface-to-air interface 110, to a depth 122 of the glass material 100, and may be configured to have an enhanced and / or strengthened glass material 100 using one or more mechanisms. In some aspects, the depth 122 of the mesophase region 120 may be about 1 micron, while in other aspects, the depth 122 of the mesophase region 120 may be between about 1 micron and 10 microns. In some implementations, a monolayer 112 of excess carbon may be deposited and / or disposed on the mesophase region 120. In some aspects, a monolayer of excess carbon can help strengthen and / or toughen the mesophase region 120 by providing a reinforcing material or substance that can be used to absorb and / or dissipate energy from impact or other sources.

[0043] In various implementations, the mesophase region 120 can be formed within the glass material 100 by bombarding the surface-air interface 110 with carbon-based free radicals, ionized noble gas particles, additives, positively charged particles, and / or other suitable particles or materials. The carbon-based free radicals can be (but are not limited to) methyl free radicals. In some implementations, the carbon-based free radicals and ionized noble gas particles can be provided by (or extracted from) a non-thermal equilibrium plasma in a reaction chamber. The non-thermal equilibrium plasma can be generated by exciting hydrocarbon gas and silane with microwave energy in a reaction chamber, for example, as described in Figure 6 and Figure 7Describe in more detail.

[0044] Ionized inert gas particles, which may be, but are not limited to, argon and / or helium, may penetrate the surface-to-air interface 110 and "soften" one or more portions of the glass material 100, such as by creating pores in the glass material 100. More specifically, the ionized inert gas particles may fragment into various atoms, molecules, and particles of the glass material 100 and create pores by replacing at least some of the fragmented atoms, molecules, and particles. The ionized inert gas particles may have different masses and / or different sizes that may increase the depth and / or concentration of ion penetration. In some cases, the pores formed by the ionized inert gas particles may form a compressive stress layer 115 between the interphase region 120 and the surface-to-air interface 110. In some implementations, the compressive stress layer 115 may be induced by ion bombarding the glass material 100 with a plurality of ionized inert gas particles (such as with respect to Figure 6 and Figure 7 Any of those particles presented and discussed).

[0045] The carbon-based free radicals may be implanted in pores and / or small cracks formed by bombarding the glass material 100 with ionized inert gas particles. After being implanted in the glass material 100, the carbon-based free radicals may recombine and self-nucleate to form a plurality of few-layer graphene (FLG) nanosheets 140 dispersed throughout the mesophase region 120. The formation of the FLG nanosheets 140 may reduce the value of the Young's modulus of the mesophase region 120, thereby increasing the fracture toughness of the glass material 100. In some aspects, the FLG nanosheets 140 may reduce the value of the Young's modulus from about 50 GPa to about 150 MPa.

[0046] The FLG nanosheets 140 may be dispersed throughout the mesophase region 120 in a random or non-periodic orientation that at least partially inhibits the formation or propagation of cracks and / or surface defects in the glass material 100. The FLG nanosheets 140 may also act as an energy reservoir that may absorb and / or dissipate external forces (such as fracture energy) occurring at or near cracks and crack tips in the glass material 100. In some implementations, the FLG nanosheets 140 formed in the upper portion 120A of the mesophase region 120 adjacent to the surface-air interface 110 may have a size of about 20 nanometers (nm), and the FLG nanosheets 140 formed in the lower portion 120B of the mesophase region 120 away from the surface-air interface 110 may have a size of about 2 nm. In some aspects, the size of the FLG nanosheets in the transition portion 120C of the mesophase region 120 between the upper portion 120A and the lower portion 120B of the mesophase region 120 gradually decreases along the direction 150 toward the depth 122 of the mesophase region 120. In some cases, the FLG nanosheets 140 formed within the mesophase region 120 can have a combined weight of less than 2% of the glass material 100.

[0047] The density of the FLG nanosheets 140 formed in the mesophase region 120 may gradually decrease along a direction 150 from the surface-air interface 110 to a depth 122 of the glass material 100. For example, the density of the FLG nanosheets 140 may decrease by about 0-5%, about 5%-10%, about 10%-15%, about 15%-20%, about 20%-25%, about 25%-30%, about 30%-35%, about 35%-40%, about 40%-45%, about 45%-50%, about 50%-55%, about 55%-60%, about 60%-65%, about 65%-70%, about 70%-75%, about 75%-80%, about 80%-85%, about 85%-90%, about 90%-95%, and 95%-100% per unit depth. In some aspects, the density per unit depth may be between about 10 nm and 50 nm. In other aspects, the depth per unit may be between about 50 nm and 100 nm.

[0048] In various implementations, the density of the FLG nanosheets 140 formed within the mesophase region 120 of the glass material 100 may be controlled and fine-tuned by adjusting one or more aspects of the method for implanting carbon-based free radicals into the glass material 100. The compressive residual stress of the mesophase region 120 may have a positive correlation with the density of the FLG nanosheets 140 formed in the mesophase region 120. Therefore, the compressive residual stress of the mesophase region 120 may be increased (or set to a relatively high value) by increasing the density of the FLG nanosheets 140 formed therein, and the compressive residual stress of the mesophase region 120 may be reduced (or set to a relatively low value) by reducing the density of the FLG nanosheets 140 formed therein. In this way, the compressive residual stress of the mesophase region 110 may be adjusted to discrete levels. For example, in some aspects, the compressive residual stress of the mesophase region 110 can be adjusted to a level between about 0 and 25 MPa, between about 25 and 50 MPa, between about 50 and 75 MPa, between about 75 and 100 MPa, between about 100 and 125 MPa, or about 125 MPa.

[0049] The additive may be any suitable material, particle, or mixture that can be implanted into the glass material 100 and configured to self-repair cracks or surface defects formed in the glass material 100. In some cases, the additive may include an alkali metal (such as lithium, sodium, potassium, calcium, fluorine, or bromine), a transition metal (such as copper or iron), or any combination thereof. In other cases, the additive may include lithium, nickel, manganese, copper, trimethylaluminum (TMA), trimethylgallium (TMG), sulfur, or any combination thereof. The additive may be implanted into one or more portions of the glass material 100 in any suitable manner. For example, in some aspects, the additive may be implanted into the glass material 100 while the carbon-based free radicals are implanted into the mesophase region 120, while in other aspects, the additive may be implanted into the glass material 100 independently of the carbon-based free radicals. In one implementation, the additive may be doped on one or more surfaces of the FLG nanosheets 140 formed in the glass material 100. After being implanted into the glass material 100, the additive may be embedded between adjacent graphene layers of the FLG nanosheets 140.

[0050] Subsequently, when the additive is exposed to ambient air, a chemical reaction between the additive and certain components in the ambient air (such as H2O and O2 molecules) may oxidize the additive. The oxidized additive may extend into and / or coat the surfaces of the cracks, cracks, and surface defects adjacent to the embedded FLG nanosheets 140. For example, when the glass material 100 generates one or more cracks in response to an external force applied to the glass material 100, the portion of the additive embedded in the FLG nanosheets 140 at or near the cracks, cracks, and surface defects may be exposed to the ambient air 102. The chemical reaction between the exposed additive and the ambient air 102 may produce a metal oxide, which extends into and / or coats the surfaces of the cracks, cracks, and surface defects formed in the glass material 100. The extension of the metal oxide into the cracks, cracks, and surface defects and the metal oxide coating on the exposed surfaces of the cracks, cracks, and surface defects may prevent or at least inhibit the further propagation of the cracks, cracks, and surface defects in the glass material 100. As such, the techniques disclosed herein may be used to manufacture, strengthen, and / or reinforce glass and glass materials without introducing undesirable impurities that may reduce the compressive strength, tensile strength, and / or fracture toughness of the glass or glass material.

[0051] In some implementations, the non-thermal equilibrium plasma may also include a plurality of positively charged particles that may be separated from carbon-based free radicals and ionized inert gas particles in the reaction chamber. An external electric field or potential may be used to accelerate the positively charged particles through the reaction chamber, thereby increasing the speed and energy at which the positively charged particles may impact the surface of the glass material 100 and the air interface 110. In this way, the accelerated particles may penetrate the glass material 100 with greater energy and further soften one or more portions of the glass material 100 that define the mesophase region 120.

[0052] In one implementation, the formation of FLG nanosheets 140 within the mesophase region 120 may be controlled in order to adjust the temporal and spatial aspects of the intrinsic strain field within the mesophase region 120. For example, carbon-based radicals implanted in the glass material 100 may recombine to form ordered 2D sp 2 FLG nanosheets having a defined density and size distribution in a region of the mesophase region 120 less than about 1 mm below the surface-air interface 110. In some aspects, the intrinsic strain field can be a 2D sp nanosheet in the reaction chamber before implanting the mesophase region 120 of the glass material 100. 2 The result of controlled self-nucleation and growth of graphene nanoparticles. 2D sp 2The controllable self-nucleation and growth of graphene nanoparticles may be a result of the presence of a supersaturated amount of energized carbon-based radicals in a non-equilibrium plasma from which the carbon-based radicals are generated.

[0053] In some other implementations, other carbon-based particles can be flowed into the reaction chamber and subsequently implanted within the mesophase region 120 of the glass material 100. These other carbon-based particles can further enhance the fracture toughness of the mesophase region 120 and / or can further inhibit crack formation and propagation throughout the glass material 100. In some aspects, these other carbon-based particles, which can be referred to as secondary carbon particles, can be implanted within the upper portion 120A of the mesophase region 120.

[0054] In some aspects, different hydrocarbon precursor supply gases (such as methane, ethanol with different C / H ratios, ethanol with different oxygen contents, etc.) can be used to generate specific plasma chemistries (such as C+, C2, CH3·, O - The plasma chemistry generates carbon-based radicals and then implants them into the mesophase region 120 of the glass material 100. In some aspects, the size of the FLG nanosheets 140 can be selected or adjusted based on the specific purpose of forming the resulting graphene. For example, the FLG nanosheets used to adjust various quantum effects of the glass material 100 can have a size of less than 5 nm, while the FLG nanosheets used to adjust the optical transmission or absorption characteristics of the glass material 100 can have a size between about 5 nm and 50 nm.

[0055] The FLG nanosheets 140 may cause the mesophase region 120 to have a different refractive index than the substrate portion 130 of the glass material 100. In one implementation, the FLG nanosheets 140 formed in the mesophase region 120 may be configured such that a change in light transmission caused by scattering at the surface and air interface 110 of the glass material 100 is less than about 0.5%.

[0056] The formation of FLG nanosheets 140 in the mesophase region 120 and the penetration of energized ions therein can cause an engineered gradient in the mesophase region 120, which exhibits a linear to Gaussian distribution. In some aspects, one or more mechanical, chemical, electrical and / or optical properties can be adjusted based on the concentration of the FLG nanosheets 140 formed in the mesophase region 120. The FLG nanosheets 140 formed in the mesophase region 120 can also enhance the fracture toughness of the glass material 100 by dissipating the fracture energy and other external forces applied to the glass material 100. In this way, the formation of FLG nanosheets 140 in the mesophase region 120 based on the technology disclosed herein can strengthen the glass material 100 without introducing undesirable impurities into the glass material 100.

[0057] Figure 2 According to some implementations, Figure 1 An example FLG nanosheet 200 may be formed in the glass material 100. The FLG nanosheet 200 may be Figure 1 An example of FLG nanosheets 140 formed in the glass material 100 of the present invention may have a curved or curled structure, wherein the carbon-carbon bonded atomic groups may bend or fold in response to an external force, pressure, or load. For example, when an external force is applied to the glass material 100, the presence of the FLG nanosheets 140 in the mesophase region 120 may cause the glass material 100 to bend, bend, and / or fold (rather than, for example, crack or break) in response to the external force. In this way, the glass and glass materials manufactured, enhanced, and / or strengthened using the techniques disclosed herein may absorb and / or dissipate energy and stress associated with external forces, pressures, and loads, thereby reducing the overall compressive stress experienced by the glass material 100.

[0058] At once Figure 2 For example, the FLG nanosheet 200 includes four graphene layers 201-204 as shown, and the graphene layers are stacked on top of each other (such as in the vertical direction or substantially in the vertical direction). In other implementations, the FLG nanosheet 200 may include other numbers of graphene layers. The number of graphene layers in the FLG nanosheet 200 may affect one or more properties of the FLG nanosheet 200. These properties may include (but are not limited to) the ability to absorb or dissipate energy, the ability to conduct electricity, and the ability to self-repair cracks formed in glass and glass materials. For example, increasing the number of graphene layers in the FLG nanosheet 200 can enhance the ability of the glass material 100 to absorb or dissipate energy, can enhance the ability of the glass material 100 to conduct electricity, and can enhance the ability of the glass material 100 to self-repair cracks and other surface defects. Therefore, for at least some implementations, Figure 1 The FLG nanosheets 140 formed in the glass material 100 may have a relatively large number of graphene layers (such as 10 or more graphene layers), for example, to maximize the ability of the glass material 100 to absorb energy, dissipate energy, conduct electricity, and self-repair cracks.

[0059] However, increasing the number of graphene layers in the FLG nanosheet 200 increases the thickness of the FLG nanosheet 200, which in turn increases the opacity of the FLG nanosheet 200. In general, opacity is a measure of the ability to block electromagnetic radiation and light. For example, an opaque material is neither transparent (such as allowing all received light to pass through the material) nor translucent (such as allowing only a portion of the received light to pass through the material), but reflects, scatters and / or absorbs all received light. In addition, when light strikes an interface between two layers, two materials, two configurations and / or two substances in a material, some light may not pass through the interface. That is, some light may be absorbed by the interface, some light may be absorbed by the interface, and some light may be scattered by the interface (and the remaining light is transmitted through the material). Therefore, when the FLG nanosheet 200 includes more than a certain number of graphene layers or exceeds a certain thickness, the opacity of the FLG nanosheet 200 may exceed a threshold value, making the glass material in which the network of FLG nanosheets 200 is formed no longer suitable for some optical applications. For example, the strengthened glass material 100 is no longer suitable for optical applications.

[0060] Applicants have determined that when glass materials such as Figure 1 When formed in a carbon-containing glass material 100 of the present invention, the FLG nanosheets 200 having 3 to 5 graphene layers achieve a desired balance between the ability of the glass material to absorb energy, dissipate energy, conduct electricity, and self-heal cracks and the optical transparency of the glass material (such as the ability to pass light with a loss amount and / or refraction amount less than a threshold amount). Applicants have also determined that the FLG nanosheets 200 formed in the mesophase region 120 of the glass material 100 have a thickness between about 1 nm and 3 nm and have lateral dimensions (such as length and width) between about 100 nm and 100 μm. In one implementation, the FLG nanosheets 200 formed in the upper portion 120A of the mesophase region 120 have a lateral dimension of about 20 nm, and the FLG nanosheets 200 formed in the lower portion 120B of the mesophase region 120 have a lateral dimension of about 2 nm.

[0061] Figure 3A An example mechanism 300A for toughening a glass material according to some implementations is depicted. The glass material includes a surface-to-air interface 302 and a mesophase region 304. The surface-to-air interface 302 (which may be Figure 1 The surface of the glass material 304 (which may be an example of a surface-air interface 110) may provide an interface through which various particles and materials may be bombarded, implanted, and / or incorporated into the glass material. Figure 1 An example of an intermediate phase region 120 of the embodiment of the present invention includes a plurality of FLG nanosheets 200 formed therein, for example, as described above with reference to Figure 1and Figure 2 As stated. Figure 3A As shown in FIG. 3 , the glass material also includes a crack 310 having a width W1 across the surface-to-air interface 302 and a depth D1 extending into the glass material. The crack 310 is also shown to include a crack tip 312 .

[0062] One of the FLG nanosheets 200 (in Figure 3A The crack 310 is "bridged" by a first end of the FLG nanosheet 200A (represented as FLG nanosheet 200A in the figure). That is, the first end of the FLG nanosheet 200A is bonded to the portion of the glass material on the right side of the crack 310, and the second end of the FLG nanosheet 200A is bonded to the portion of the glass material on the left side of the crack 310. As a result of this bridging, the FLG nanosheet 200A can absorb and / or dissipate forces, stresses, and loads applied to the portion of the glass material near the crack 310. In addition, since the crack 310 is likely to propagate in a vertical downward direction 305 in response to the tensile stress pulling the opposite sides of the crack 310 away from each other, the position and orientation of the FLG nanosheet 200A relative to the crack 310 can guide the crack 310 to propagate in a lateral direction 315, which is orthogonal to the vertical direction 305 and parallel to the surface of the glass material and the air interface 302.

[0063] In various implementations, the additive may be embedded between adjacent graphene layers of the FLG nanosheets 200 formed in the glass material (for simplicity, Figure 3A The additive is not shown in the figure). In some cases, the additive may be doped onto one or more surfaces of at least some of the FLG nanosheets 200. The additive may oxidize upon exposure to ambient air and form an oxidized material that extends into and / or coats the surface of the crack 310 formed in the glass material. In some cases, the additive may include an alkali metal (such as lithium, sodium, potassium, calcium, fluorine, or bromine), a transition metal (such as copper or iron), or any combination thereof. In other cases, the additive may include lithium, nickel, manganese, copper, trimethylaluminum (TMA), trimethylgallium (TMG), sulfur, or any combination thereof. Thus, the presence of such additives embedded within the FLG nanosheets 200 may cause the cracks 310 formed in the glass material (as well as other cracks not shown for simplicity) to self-heal.

[0064] In some implementations, the surface energy effect may cause the embedded additive to form spheres on or near the surface of the corresponding FLG nanosheet 200. In some cases, the metal spheres may have a diameter between about 1 nm and 5 nm. Upon application of an external force, the metal spheres may diffuse and create pores between the FLG nanosheets 200 (such as based on the Kirkendall effect). At least some of the pores may absorb and / or dissipate the fracture energy present at the crack tip 312, thereby preventing the crack 310 from further propagating into or across the glass material.

[0065] Figure 3B An example mechanism 300B for toughening a glass material according to other implementations is depicted. The glass material includes a surface-air interface 302 and a mesophase region 304. The surface-air interface 302 (which may be Figure 1 The surface of the glass material 304 (which may be an example of a surface-air interface 110) may provide an interface through which various particles and materials may be bombarded, implanted, and / or incorporated into the glass material. Figure 1 An example of an intermediate phase region 120 of the embodiment of the present invention includes a plurality of FLG nanosheets 200 formed therein, for example, as described above with reference to Figure 1 and Figure 2 As stated. Figure 3B As shown in FIG. 3 , the glass material further includes a crack 320 having a width W2 across the surface-to-air interface 302 and a depth D2 extending into the glass material. The crack 320 is also shown to include a crack tip 322 .

[0066] One of the FLG nanosheets 200 (in Figure 3B320) is positioned below the crack tip 322 and oriented substantially orthogonal to the depth D2 of the crack 320. When the crack 320 is subjected to an applied force that causes the crack 320 to begin to propagate along the vertical downward direction 305, the FLG nanosheet 200B located below the crack tip 322 can absorb and / or diffuse a certain amount or portion of the applied force so that the crack does not propagate further beyond the FLG nanosheet 200B. In some cases, the orthogonal orientation of the FLG nanosheet 200B relative to the crack 320 can cause the crack 320 to "branch" and form one or more microcracks at or near the crack tip 322. Compared to the crack 320, the microcracks are relatively small and have relatively low energy, and therefore may not propagate laterally beyond the FLG nanosheet 201 along the direction 315 or laterally beyond the FLG nanosheet 202 along the direction 316. More specifically, since the orientation of the FLG nanosheets 201 and 202 is orthogonal to the transverse microcracks, the transverse microcracks may not have enough energy to penetrate or break the FLG nanosheets 201 and 202. In this way, the FLG nanosheet 200B can inhibit the crack 320 (and other cracks not shown for simplicity) from vertically propagating through the glass material, and the FLG nanosheets 201 and 202 can inhibit the microcracks from propagating laterally through the glass material.

[0067] Figure 3C An example mechanism 300C for toughening a glass material according to some implementations is depicted. The glass material includes a surface-to-air interface 302 and a mesophase region 304. The surface-to-air interface 302 (which may be Figure 1 The surface of the glass material 304 (which may be an example of a surface-air interface 110) may provide an interface through which various particles and materials may be bombarded, implanted, and / or incorporated into the glass material. Figure 1 An example of an intermediate phase region 120 of the embodiment of the present invention includes a plurality of FLG nanosheets 200 formed therein, for example, as described above with reference to Figure 1 and Figure 2 As stated. Figure 3C As shown in FIG. 3 , the glass material also includes a crack 330 having a width W3 across the surface-to-air interface 302 and a depth D3 extending into the glass material. The crack 330 is also shown to include a crack tip 332 .

[0068] One of the FLG nanosheets 200 (in Figure 3CThe graphene layers in the FLG nanosheet 200C (represented as FLG nanosheet 200C) are adjacent to the crack tip 332 and oriented substantially parallel to the crack 330. When the crack 330 is subjected to an externally applied force that causes the crack 320 to begin to propagate toward the FLG nanosheet 200C along the lateral direction 315, the graphene layers within the FLG nanosheet 200C exhibit sliding movement relative to each other, thereby absorbing and / or dissipating, for example, at least some of the externally applied force, thereby inhibiting the crack 330 from further propagating through the glass material.

[0069] Figure 4 An example carbon-containing glass material 400 having more than one mesophase region is shown according to some other implementations. As shown, the glass material 400 may include a first mesophase region 420(1), a second mesophase region 420(2), and a third region 430. Each of the first mesophase region 420(1) and the second mesophase region 420(2) may include a plurality of FLG nanosheets (such as formed by recombination or self-nucleation of carbon-based free radicals implanted or bombarded into the glass material). In some implementations, each of the first mesophase region 420(1) and the second mesophase region 420(2) may be Figure 1 1 and 1. An example of an interphase region 120 of a glass material 100 of the present invention. That is, a plurality of FLG nanosheets 402, 404 may be formed in each of the first interphase region 420(1) and the second interphase region 420(2) to enhance and / or strengthen the glass material 400. In some aspects, the orientation of the FLG nanosheets 402, 404 may reduce potential surface defects or damage of the first interphase region 420(1) and the second interphase region 420(2). In some aspects, the FLG nanosheets 402, 404 within the first interphase region 420(1) and the second interphase region 420(2) may be formed in different orientations. For example, the first FLG nanosheet 402 may have a first orientation, and the second FLG nanosheet 404 may have a second orientation different from the first orientation. The first interphase region 420(1) may also include other FLG nanosheets (not shown for simplicity) having one or more orientations different from the first orientation and the second orientation.

[0070] The FLG nanosheets 402, 404 formed within various portions of the glass material 400 can form graphene networks integrated within various molecular structures of the glass material 400. The graphene networks (which in some aspects can be similar to grain boundaries observed in nanocrystalline matrix structures) can extend laterally (such as along width and length) through the glass material 400 and form a toughening or strengthening mechanism that can enhance the compressive strength, tensile strength, and fracture toughness of the glass material 400.

[0071] Figure 5A portion of a carbon-containing glass material 500 is depicted according to some other implementations. The glass material 500 (which may be Figure 1 1 ) includes a surface-air interface 510, an intermediate phase region 520, a self-healing layer 530, a crack 540 formed in the glass material 500, and a plurality of FLG nanosheets 550 formed in the glass material 500. For simplicity, the portion of the glass material 500 below the intermediate phase region 520 is Figure 5 Not shown in FIG.

[0072] As shown, the self-healing layer 530 may be disposed within the mesophase region 520 of the glass material and may extend to the surface and air interface 510 of the glass material 500. One or more additives 560 may be embedded between adjacent graphene layers 552 of at least some of the FLG nanosheets 550 formed within the glass material (for simplicity, Figure 5 552 of only one FLG nanosheet 550 is shown in FIG. 55). In some cases, the additive may include an alkali metal such as lithium, sodium, potassium, calcium, fluorine, or bromine, a transition metal such as copper or iron, or any combination thereof. In other cases, the additive may include lithium, nickel, manganese, copper, trimethylaluminum (TMA), trimethylgallium (TMG), sulfur, or any combination thereof.

[0073] As the crack 540 propagates from the surface and air interface 510 of the glass material 500 into the self-healing layer 530 in a vertical downward direction 501, the crack 540 exposes a group of FLG nanosheets 550 at or near the crack tip 542 to the ambient air. Chemical reactions between additives embedded in the group of FLG nanosheets 550 and certain components of the ambient air, such as oxygen (O2) molecules 570 and water (H2O) molecules 572, produce oxides, such as metal oxides 580 and / or metal oxide-hydroxides 582, that extend into the crack 540 and / or coat the exposed surface 541 of the crack. The diffusion of the oxides 580 and / or 582 into the crack 540 and the resulting coating on the exposed surface 541 of the crack 540 prevent or at least inhibit the crack 540 from further propagating through the glass material 500. As such, the techniques disclosed herein may be used to manufacture, strengthen, and / or reinforce the glass material 500 without introducing undesirable impurities that may reduce the compressive strength, tensile strength, and / or fracture toughness of the glass material 500 .

[0074] In some implementations, thermal or microwave energy can be applied to the glass material 500 during manufacturing (such as within a reaction chamber) to enhance diffusion of the additive 560 into the crack tip 542 , which can increase the rate of production of the metal oxide 580 and the metal oxide-hydroxide 582 .

[0075] Figure 6 An example reactor 600 that can be used to manufacture, strengthen, and / or reinforce a carbon-containing glass material is shown according to some implementations. In some cases, a glass material strengthened and / or reinforced using the techniques described herein may become more resilient to the propagation of existing cracks and / or the formation of new cracks when external forces are applied to the glass material 650. Additionally, or in the alternative, the reactor 600 can be implemented as a plasma torch.

[0076] Reactor 600 may include a microwave energy source 610, an input gas inlet 615, a reaction vessel 620, an electric potential source 630, and a metal substrate 640. Reaction vessel 620 may include a reaction chamber 622, a downstream region 624, and a collector electrode 626. Reaction chamber 622 has a length L along a direction 602 parallel to reaction chamber 622. Input gas inlet 615 is coupled between reaction vessel 620 and a process material source (not shown for simplicity) and may be used to flow or otherwise provide material 605 (such as one or more gases, liquids, particles, etc.) into reaction chamber 622. For example, in some cases, material 605 may include a variety of structured carbons such as, but not limited to, CNTs, fullerenes, and the like.

[0077] The microwave energy source 610 can generate microwave energy 612, which can excite the material 605 to generate a plasma from which carbon-based free radicals can be separated or extracted. In some cases, the microwave energy source 610 can generate pulsed microwave energy, such as described in co-owned U.S. Patent Nos. 9,767,992 and 10,314,512. In other cases, the microwave energy source 610 can generate continuous microwave energy. The microwave energy source 610 can include control circuitry that can adjust various characteristics of the microwave energy 612 based on one or more control signals (CTRL). For example, the CTRL signal can determine one or more of the pulse duration, pulse frequency, duty cycle, instantaneous power level, or average power level of the microwave energy 612. Thus, by adjusting the pulse duration, pulse frequency, duty cycle, instantaneous power level, and / or average power level of the microwave energy 612 generated to form a non-thermal equilibrium plasma in the reaction chamber 622, the reactor 600 can configure the size, number, and concentration of FLG nanosheets to be formed in the glass material 650. The ability to control the energy applied to the non-thermal equilibrium plasma allows targeted reactions to occur and promotes the distribution of FLG nanosheets and other particles throughout the glass material 650.

[0078] In some implementations, a mixture of hydrocarbon gas and silane can flow into the reaction chamber 622 via the input gas inlet 615 at a suitable flow rate. The hydrocarbon gas can be any suitable carbon-containing gas, such as (but not limited to) methane gas. Silane can be any suitable silane gas or a liquid precursor containing silane. In some aspects, silane can flow into the reaction chamber 622 at a flow rate between about 1 standard liter / minute (slm) and 10 slm / minute. In some aspects, for example, an additive can be provided to the reaction chamber 622 while the mixture flows into the reaction chamber 622. In some cases, the additive can include an alkali metal (such as lithium, sodium, potassium, calcium, fluorine or bromine), a transition metal (such as copper or iron), or any combination thereof. In other cases, the additive can include lithium, nickel, manganese, copper, trimethylaluminum (TMA), trimethylgallium (TMG), sulfur, or any combination thereof. The additive can flow into the reactor at a flow rate between about 1% and 75% of the hydrocarbon gas flow rate.

[0079] The microwave energy 612 generated by the microwave energy source 610 can be directed into a portion of the reaction chamber 622 containing a mixture of hydrocarbon gas and silane. The microwave energy 612, which can have a power level between about 300 watts (W) and 25 kilowatts (kW), can excite the mixture of hydrocarbon gas and silane to produce a non-thermal equilibrium plasma. In some aspects, the microwave energy source 610 can be a klystron or a traveling wave tube amplifier (TWTA). The non-thermal equilibrium plasma can include carbon-based free radicals (such as methyl radicals), positively charged particles, ionized inert gas particles, or any combination thereof. In various implementations, the carbon-based free radicals, positively charged particles, and / or ionized inert gas particles 660 output from the reaction chamber 622 via the collector 626 can be directed to the surface of the glass material 650 and the air interface via bombardment and / or implantation. Carbon-based radicals, positively charged particles, and / or ionized noble gas particles may bombard the glass material 650 to form, strengthen, and / or strengthen one or more portions of the glass material 650. A portion of the glass material 650 formed, strengthened, or strengthened according to the techniques disclosed herein may have increased compressive strength, increased tensile strength, and increased fracture toughness, and thus be more resilient to cracking and surface defects than conventional glass materials.

[0080] More specifically, carbon-based free radicals and ionized inert gas particles separated from the non-thermal equilibrium plasma in the reaction chamber 622 can bombard the surface and air interface of the glass material 650. The ionized inert gas particles can penetrate the surface and air interface of the glass material 650 and form microcracks, micropores, and / or surface defects in a portion of the glass material 650 below the surface and air interface. In some aspects, the microcracks, micropores, and / or surface defects formed by ion bombarding the glass material 650 can define a mesophase region of the glass material 650. The carbon-based free radicals that penetrate the surface and air interface of the glass material 650 can be implanted in the mesophase region.

[0081] In some implementations, an external electric field can be applied to the reaction chamber 622 to accelerate the positively charged particles through the reaction chamber 622 along the direction 604 toward the glass material 650, thereby increasing the speed and energy at which the positively charged particles can impact the surface and air interface of the glass material 650. For example, the potential source 630 can generate a negative electric field or potential that can accelerate the positively charged particles along the direction 604 toward the glass material 650 located on the metal substrate 640. In some aspects, the negative potential generated by the potential source 630 can be configured to extract or separate positively charged gas particles from the non-thermal equilibrium plasma based on the electrical polarity. In this way, the negative electric field or potential can allow the positively charged particles, as well as the ionized noble gas particles and carbon-based free radicals, to penetrate deeper into the mesophase region of the glass material 650.

[0082] Carbon-based free radicals implanted in the mesophase region of the glass material 650 may recombine and self-nucleate to form a plurality of FLG nanosheets. The FLG nanosheets may be dispersed throughout the mesophase region of the glass material 650 in a non-periodic orientation that at least partially inhibits crack formation or propagation in the glass material 650. In some aspects, the FLG nanosheets formed in the mesophase region may enhance the fracture toughness of the glass material 650 by reducing the value of the Young's modulus in the mesophase region, such as, but not limited to, from about 50 GPa to about 150 MPa. The FLG nanosheets formed in the mesophase region may also act as an energy reservoir that absorbs and / or dissipates external forces applied to existing cracks and / or crack tips in the glass material 650.

[0083] As discussed, the concentration and size of the FLG nanosheets formed in the glass material 650 can decrease toward the depth of the mesophase region along the direction 604. For example, in some implementations, the FLG nanosheets formed in the upper portion of the mesophase region of the glass material 650 can have a size of about 20 nanometers (nm), and the FLG nanosheets formed in the lower portion of the mesophase region of the glass material 650 can have a size of about 2 nm. In some cases, the size of the FLG nanosheets formed between the upper and lower portions of the mesophase region can be a gradually decreasing size along the direction 604.

[0084] In some implementations, one or more surfaces of the FLG nanosheets formed in the mesophase region of the glass material 650 can be doped with an additive, as discussed above. The additive, which can be embedded between adjacent graphene layers of at least some of the FLG nanosheets formed in the mesophase region of the glass material 650, can cause cracks and other surface defects in the glass material 650 to self-heal when exposed to ambient air, for example, as discussed above with reference to FIG. Figure 1 , Figure 2 , Figures 3A-3C , Figure 4 and Figure 5 Discussed.

[0085] In various implementations, the reactor 600 can be cylindrical with a diameter of up to 1 inch. In some implementations, the reactor 600 can be configured as a Gaussian reactor, while in other implementations, the reactor 600 can be configured as a non-Gaussian reactor (such as where plasma produced in a non-Gaussian reactor generally exhibits superior energy dissipation and distribution than plasma produced in a Gaussian reactor).

[0086] Figure 7 Another example reactor 700 that can be used to manufacture, enhance, and / or strengthen carbon-containing glass materials according to some other implementations is shown. In some aspects, the reactor 700 can be similar to Figure 6 The reactor 600 of FIG. 1 and may differ in other aspects from Figure 6Reactor 600. For example, reactor 700 may include microwave energy source 610, input gas inlet 615, reaction vessel 720, potential source 730, metal substrate 640, and collector electrode 626. One aspect in which reactor 700 differs from reactor 600 is that, instead of using potential source 630 to generate an electric field within one or more portions of reaction chamber 720, reactor 700 includes multiple electrodes 728 positioned on opposite sides of one or more portions of reaction chamber 720. Electrodes 728 may be configured to generate an internal electric field (e.g., based on the current and / or voltage provided by power source 732), which may accelerate, for example, multiple positively charged particles, so that the accelerated positively charged particles have a greater speed and greater energy when bombarding into glass material 650. Additionally or alternatively, the reactor 700 may also include another potential source (not shown for simplicity) positioned such that a negative potential appears across the reaction chamber 722 along the direction 704, and the negative potential induces a current 732 along the inward wall of the reaction chamber 722. The current 732 induced within the reaction chamber 722 may form a magnetic field that may attract positively charged gas particles and at least accelerate the positively charged gas particles through the reaction chamber 722 and out of the collector 626 toward the glass material 650.

[0087] In addition to applying methane gas to reactor 600 and reactor 700 to generate carbon-based free radicals, the carbon-containing precursor may also include any known carbon particles or structures, such as those disclosed in ISO / TS 80004-13:2017 (en) titled "Nanotechnology - Vocabulary - Part 13: Graphene and related two-dimensional (2D) materials."

[0088] In some aspects, the hydrocarbon gas flowing into the reactor 700 may be a short-chain hydrocarbon gas, while in other aspects, the hydrocarbon gas flowing into the reactor 700 may be a long-chain hydrocarbon gas. In some cases, the hydrocarbon gas may include methane (CH4) and / or butane (C4H 10 In various implementations, suitable carbon-based radicals may be generated from a non-thermal equilibrium plasma based on one or more of the following:

[0089] ● The input carbon-containing gas flow rate is 100 standard cubic centimeters per minute (sccm) to 5 standard liters per minute (slm);

[0090] • Lower flow rates generally provide enhanced fidelity and adjustability, and thus may help accelerate the passage of carbon-based species through reaction chambers 622 and 710, which may result in a reduced doping rate of the various additives 604 and 704;

[0091] ● Higher flow rates generally produce higher outputs but may reduce the fidelity and / or orientation of the FLG nanosheets;

[0092] ● To provide various suitable silicon source rates, silane and / or a liquid precursor containing silane, such as hexamethyldisiloxane (HMDSO) or hexamethyldisilazane (HMDSN), as well as pure silane, may be flowed into the reactors 600 and 700. In some implementations, the silicon source rate may be one of: 1-10 L / min, 11-20 L / min, 21-30 L / min, 31-40 L / min, 41-50 L / min, 51-60 L / min, 61-70 L / min, 71-80 L / min, 81-90 L / min, 91-100 L / min, 101-200 L / min, or 201-530 L / min, wherein higher flow rates may allow for additional coatings of the corresponding additive material to appear on the accelerated ionized particles 616 and 716;

[0093] ● A gaseous substance containing lithium (Li), nickel (Ni), manganese (Mn), copper (Cu), trimethylaluminum (TMA), trimethylgallium (TMG), and sulfur (S) may be flowed into the reactors 600 and 700 to provide a silicon source rate of one of: 1-10 L / min, 11-20 L / min, 21-30 L / min, 31-40 L / min, 41-50 L / min, 51-60 L / min, 61-70 L / min, 71-80 L / min, 81-90 L / min, 91-100 L / min, 101-200 L / min, or 201-530 L / min, wherein a higher flow rate may allow for a thicker additive coating on the FLG nanosheets 316A and 316B;

[0094] • Additives including silica may flow into reactors 600 and 700 and / or be dispersed in particle form at a rate of about 1%-75% of the methane gas flow rate;

[0095] • Additives may be configured to coat and / or modify the accelerated ionized particles 660;

[0096] • A preferred chemistry for the carbon-containing glass material 650 may include between about 0.1%-5% additives and between about 65%-99% silicon dioxide, with the remainder attributed to carbon-containing materials (such as FLG nanosheets);

[0097] • Reactors 600 and 700 may be tuned to achieve at least 96% optical transmittance of portions of carbon-containing glass material 650 in the visible spectrum and / or to tune the refractive index of carbon-containing glass material 650; and

[0098] • Providing uniform coloration of the carbon-containing glass material 650, given that graphene generally exhibits a neutral light transmission density.

[0099] Fig. 8A FIG. 8 is a flowchart illustrating example operations 800 for strengthening glass materials according to some implementations. In various implementations, operations 800 may be performed in a reaction chamber, such as, but not limited to, Figure 6 Reactor 600 or Figure 7 In other implementations, operation 800 may be performed in another suitable reaction chamber or chemical processing equipment. In some implementations, operation 800 may be used to implant particles into a carbon-containing glass material that includes a surface-air interface and a mesophase region that extends from the surface-air interface and along a direction perpendicular to the surface-air interface to a certain depth of the carbon-containing glass material, such as as shown in FIG. Figures 1 to 7 In some aspects, operation 800 begins at block 802, where a non-thermal equilibrium plasma is supplied to a reaction chamber, the non-thermal equilibrium plasma comprising a plurality of positively charged gas particles and a plurality of ionized inert gas particles. Operation 800 continues at block 804, where at least a plurality of positively charged gas particles are accelerated through the reaction chamber based on applying an external potential to the non-thermal equilibrium plasma. Operation 800 continues at block 806, where a surface-air interface of a carbon-containing glass material is bombarded with the accelerated positively charged gas particles and the ionized inert gas particles. Operation 800 continues at block 808, where an intermediate phase region is formed in the carbon-containing glass material in response to the bombardment of the accelerated positively charged gas particles and the ionized inert gas particles, wherein a plurality of pores are formed in the intermediate phase region and extend from the surface-air interface and along a direction normal to the surface-air interface to a certain depth of the carbon-containing glass material. Operations 800 continue at block 810 by forming a compressive stress layer in the carbon-containing glass material in response to bombardment of at least ionized noble gas particles, the compressive stress layer disposed between a mesophase region and a surface and air interface of the carbon-containing glass material.

[0100] In various implementations, the carbon-containing glass material may include silicate glass, soda-lime glass, alkali-aluminosilicate glass, borosilicate glass, or any combination thereof. In some implementations, the alkali-aluminosilicate glass is composed of about 57% to 60% SiO2, about 10% to 25% Al2O3, and about 10% alkaline earth metal.

[0101] In some implementations, the external potential can be configured to accelerate positively charged gas particles. Additionally, or in the alternative, the non-thermal equilibrium plasma can also include an intrinsic potential. In some aspects, the intrinsic potential of the non-thermal equilibrium plasma can be sufficient to implant at least some FLG nanosheets into the mesophase region without applying an external potential to the reaction chamber. In various implementations, the bombardment can form a plurality of microcracks or micropores in one or more portions of the carbon-containing glass material.

[0102] Figure 8B FIG. 8 is a flowchart illustrating an example method 820 for strengthening a glass material according to some implementations. In various implementations, operation 820 may be performed at Fig. 8A In other implementations, operation 820 may be performed after bombarding the surface and air interface with accelerated positively charged gas particles and ionized inert gas particles in block 806 of the present invention. Fig. 8A The operation 820 is performed simultaneously with forming a compressive stress layer in the frame 810 of the embodiment. For example, the operation 820 starts from the frame 822, wherein a plurality of carbon-based free radicals separated from the non-thermal equilibrium plasma are implanted into the mesophase region of the carbon-containing glass material, while bombarding the surface and the air interface with accelerated positively charged gas particles and ionized inert gas particles. The operation 820 continues at the frame 824, wherein a plurality of few-layer graphene (FLG) nanosheets are formed in the mesophase region of the carbon-containing glass material based on the recombination and / or self-nucleation of the plurality of carbon-based free radicals. In some implementations, the carbon-based free radicals can be implanted into the mesophase region at one or more different incident angles.

[0103] In various implementations, the upper portion of the mesophase region adjacent to the surface and the air interface has a relatively high concentration of FLG nanosheets, and the lower portion of the mesophase region away from the surface and the air interface has a relatively low concentration of FLG nanosheets. In some implementations, the FLG nanosheets in the upper portion of the mesophase region adjacent to the surface and the air interface have a size of about 20 nanometers (nm), and the FLG nanosheets in the lower portion of the mesophase region away from the surface and the air interface have a size of about 2 nm. The FLG nanosheets in the lower portion of the mesophase region may be uniformly distributed in the plane of the lower portion of the mesophase region. In one implementation, the size of the FLG nanosheets formed in the mesophase region gradient portion between the upper and lower portions of the mesophase region gradually decreases in the direction of the depth toward the mesophase region. In some aspects, each FLG nanosheet may include three to five layers of graphene. In other aspects, the FLG nanosheets may have a combined weight of less than 2% of the carbon-containing glass material.

[0104] Figure 8C FIG. 8 is a flowchart illustrating an example method 830 for strengthening a glass material according to some implementations. In various implementations, operation 830 may be performed at Fig. 8A In other implementations, operation 830 may be performed after bombarding the surface and air interface with accelerated positively charged gas particles and ionized inert gas particles in block 806 of the present invention. Fig. 8A The operation 830 is performed simultaneously with forming a compressive stress layer in block 810 of the embodiment. For example, operation 830 begins at block 832, where an additive is embedded between adjacent graphene layers within each FLG nanosheet. In some cases, the additive may include an alkali metal (such as lithium, sodium, potassium, calcium, fluorine, or bromine), a transition metal (such as copper or iron), or any combination thereof. In other cases, the additive may include lithium, nickel, manganese, copper, trimethylaluminum (TMA), trimethylgallium (TMG), sulfur, or any combination thereof.

[0105] In various implementations, a first portion of the additive embedded in the FLG nanosheets in the upper portion of the mesophase region has a molar fraction of about 50%, and a second portion of the additive embedded in the FLG nanosheets in the lower portion of the mesophase region has a molar fraction of about 2%. In some implementations, other portions of the additive implanted in the region between the first portion and the second portion of the mesophase region have a molar fraction that gradually decreases along a direction toward the depth of the mesophase region.

[0106] In various implementations, the additive is configured to cause the carbon-containing glass material to self-heal based on exposure of the additive to ambient air. For example, the additive may oxidize upon exposure to ambient air and form an oxidized additive (such as an oxidized metal) based on exposure to ambient air. The oxidized additive may extend into microcracks and / or micropores formed in the carbon-containing glass material. The oxidized additive may also coat the surface of microcracks and / or micropores formed in the carbon-containing glass material.

[0107] Fig.9A and Fig. 9B Flowchart showing example operations 900 for forming a carbon-containing glass material according to some implementations. In various implementations, operations 900 may be performed in a reaction chamber, such as (but not limited to) Figure 6 Reactor 600 or Figure 7 In other implementations, operation 900 may be performed in another suitable reaction chamber or chemical processing equipment. In some implementations, operation 900 may be used to implant particles into a carbon-containing glass material including a surface and an air interface, such as in Figures 1 to 7In various implementations, operation 900 begins at block 902, where hydrocarbon gas and silane are flowed into a reactor. Operation 900 continues at block 904, where an additive is provided to the reactor, including any one or more of lithium, nickel, manganese, copper, trimethylaluminum (TMA), trimethylgallium (TMG), or sulfur. Operation 900 continues at block 906, where a non-thermal equilibrium plasma is generated based on excitation of the hydrocarbon gas and silane by microwave energy, where the non-thermal equilibrium plasma includes a plurality of methyl radicals. Operation 900 continues at block 908, where an ion bombardment is performed on a surface of a carbon-containing glass material and an air interface with at least methyl radicals, where the ion bombardment is configured to generate an intermediate phase region within the carbon-containing glass material. Operation 900 continues at box 910, where a plurality of few-layer graphene (FLG) nanosheets are formed in a mesophase region of a carbon-containing glass material at different concentration levels based on recombination or self-nucleation of a plurality of methyl radicals, the plurality of FLG nanosheets being dispersed throughout the mesophase region in a non-periodic orientation, the non-periodic orientation being configured to at least partially inhibit crack and / or surface defect formation or propagation in the carbon-containing glass material. Operation 900 continues at box 912, where one or more surfaces of at least some of the FLG nanosheets are doped with an additive. Operation 900 continues at box 914, where the additive is embedded between adjacent graphene layers within at least some of the FLG nanosheets formed in the mesophase region of the carbon-containing glass material.

[0108] In various implementations, the glass material may include any one or more of silicate glass, soda lime glass, alkali aluminosilicate glass, or borosilicate glass. In some implementations, the alkali aluminosilicate glass is composed of about 57% to 60% SiO2, about 10% to 25% Al2O3, and about 10% alkaline earth metal. In some other implementations, the silane may be a liquid precursor containing silane or a silane gas. In one implementation, the FLG nanosheets formed in the mesophase region have a combined weight of less than 2% of the carbon-containing glass material.

[0109] In various implementations, the mesophase region extends from the surface-air interface to a depth of about one micron within the carbon-containing glass material. In some implementations, the density of the plurality of FLG nanosheets decreases gradually along a direction extending from the surface-air interface to the depth of the mesophase region.

[0110] In various implementations, the upper portion of the mesophase region adjacent to the surface-air interface has a relatively high concentration of FLG nanosheets, and the lower portion of the mesophase region away from the surface-air interface has a relatively low concentration of FLG nanosheets. In some implementations, the size of the FLG nanosheets in the gradient portion of the mesophase region between the upper and lower portions of the mesophase region gradually decreases in a direction toward the depth of the mesophase region. In some aspects, the FLG nanosheets in the lower portion of the mesophase region are uniformly distributed in the plane of the lower portion of the mesophase region.

[0111] In some implementations, the additive can be embedded between adjacent graphene layers of the FLG nanosheet during post-fabrication isothermal processing in a vacuum or inert atmosphere. The additive can be configured to cause the carbon-containing glass material to self-heal based on exposure of the additive to ambient air. For example, based on exposure of the additive to ambient air, the additive can oxidize and form an oxidized additive. The oxidized additive can diffuse into one or more cracks and / or surface defects in the carbon-containing glass material, and can also coat the surface of one or more cracks and / or surface defects in the carbon-containing glass material.

[0112] Fig.10 FIG. 1 is a flowchart illustrating example operations 1000 for forming a carbon-containing glass material according to some other implementations. In various implementations, operations 1000 may be performed in conjunction with Fig.9A and Fig. 9B One or more processes of the example operation 900 of are performed simultaneously. For example, the operation 1000 begins at block 1002, where the formation of microcracks and / or micropores in the carbon-containing glass material is induced before the FLG nanosheets are formed in the mesophase region. In some implementations, the microcracks and / or micropores can be formed in the glass material by bombarding the surface and air interface of the glass material with accelerated charged particles and / or ionized inert gas particles, wherein the particles can penetrate the surface and air interface and / or can impact the surface and air interface with sufficient impact force to form small cracks, microcracks or pores in the glass material without reducing the strength or fracture toughness of the glass material.

[0113] In one embodiment, the present invention provides a carbon-containing glass material, the carbon-containing glass material comprising:

[0114] Surface-air interfaces exposed to ambient air; and

[0115] a mesophase region extending from the surface-air interface in a direction toward a depth within the carbon-containing glass material, wherein:

[0116] The mesophase region includes a plurality of few-layer graphene (FLG) nanosheets formed in response to recombination and / or self-nucleation of a plurality of carbon-containing radicals implanted in the mesophase region; and

[0117] The plurality of FLG nanosheets have a non-periodic orientation configured to at least partially inhibit the formation or propagation of microcracks and / or microvoids in the carbon-containing glass material.

[0118] In one embodiment, the density of the plurality of FLG nanosheets gradually decreases along the direction extending from the surface-air interface toward the depth of the mesophase region.

[0119] In one embodiment, the carbon-containing glass material further comprises a compressive stress layer disposed between the mesophase region and the surface-air interface of the carbon-containing glass material, the compressive stress layer being induced by ion bombarding the carbon-containing glass material with a plurality of ionized inert gas particles.

[0120] In one embodiment, the ionized noble gas particles are configured to form a plurality of microcracks or micropores between the FLG nanosheets formed in the mesophase region.

[0121] In one embodiment, the microcracks or micropores have a size between about 5 nanometers (nm) and 10 nm.

[0122] In one embodiment, at least some of the microcracks or microvoids are configured to dissipate fracture energy experienced at one or more crack tips in the carbon-containing glass material.

[0123] In one embodiment, the carbon-containing glass material further comprises a monolayer of excess carbon disposed on the mesophase region.

[0124] In one embodiment, the carbon-containing glass material further includes an additive embedded between adjacent graphene layers within the FLG nanosheets formed within the mesophase region.

[0125] In one embodiment, the additive includes any one or more of lithium, sodium, potassium, calcium or other alkali metals.

[0126] In one embodiment, the additive includes any one or more of copper, iron or other transition metals.

[0127] In one embodiment, the additive is configured to cause self-healing of cracks formed in the carbon-containing glass material after the additive is exposed to the ambient air.

[0128] In one embodiment, the additive is configured to form an oxidized additive upon exposure to one or more reactants present in the ambient air.

[0129] In one embodiment, the oxidized additive is configured to expand into one or more cracks and / or surface flaws in the carbon-containing glass material.

[0130] In one embodiment, the depth of the mesophase region is about 1 micron.

[0131] In one embodiment, the plurality of FLG nanosheets are configured to induce a compressive residual stress greater than 150 megapascals (MPa) in the mesophase region.

[0132] In one embodiment, the plurality of FLG nanosheets comprise about 2% of the combined weight of the carbon-containing glass material.

[0133] In one embodiment, the FLG nanosheets formed in the upper portion of the mesophase region adjacent to the surface-air interface have a size of about 20 nanometers (nm), and the FLG nanosheets formed in the lower portion of the mesophase region away from the surface-air interface have a size of about 2 nm.

[0134] In one embodiment, each of the FLG nanosheets formed in the mesophase region includes 3 to 5 graphene layers stacked longitudinally on each other.

[0135] In one embodiment, the carbon-containing glass material has an optical transmittance of at least 96% across the visible spectrum.

[0136] In one embodiment, the mesophase region of the carbon-containing glass material has a first refractive index and other portions of the carbon-containing glass material have a second refractive index different from the first refractive index.

[0137] As used herein, a phrase referring to "at least one of" a list of items refers to any combination of those items, including single members. As an example, "at least one of a, b, or c" is intended to cover: a, b, c, ab, ac, bc, and abc. The various illustrative logics, logic blocks, modules, circuits, and algorithmic procedures described in conjunction with the implementations disclosed herein may be implemented as electronic hardware, computer software, or a combination of both. The interchangeability of hardware and software has been generally described in terms of functionality and is illustrated in the various illustrative components, blocks, modules, circuits, and processes described above. Whether such functionality is implemented in hardware or software depends on the specific application and design constraints for the overall system.

[0138] Various modifications to the implementations described in this disclosure may be apparent to those skilled in the art, and the general principles defined herein may be applied to other implementations without departing from the spirit or scope of the disclosure. Therefore, it is not intended that the claims be limited to the implementations shown herein, but rather should be consistent with the broadest scope consistent with the disclosure, the principles and novel features disclosed herein.

Claims

1. A carbon-containing glass material, comprising: Surface-air interface exposed to ambient air; as well as a mesophase region extending from the surface-air interface in a direction toward a depth within the carbon-containing glass material, wherein: The mesophase region includes a plurality of few-layer graphene (FLG) nanosheets formed in response to recombination and / or self-nucleation of a plurality of carbon-containing radicals implanted in the mesophase region; and The plurality of FLG nanosheets have a non-periodic orientation configured to at least partially inhibit the formation or propagation of microcracks and / or microvoids in the carbon-containing glass material. 2 . The carbon-containing glass material of claim 1 , wherein a density of the plurality of FLG nanosheets gradually decreases along the direction extending from the surface-air interface toward the depth of the mesophase region.

3. The carbon-containing glass material of claim 1 , further comprising a compressive stress layer disposed between the mesophase region of the carbon-containing glass material and the surface-air interface, the compressive stress layer being induced by ion bombarding the carbon-containing glass material with a plurality of ionized inert gas particles. 4 . The carbon-containing glass material of claim 3 , wherein the ionized noble gas particles are configured to form a plurality of microcracks or micropores between the FLG nanosheets formed in the mesophase region.

5. The carbon-containing glass material of claim 4, wherein the microcracks or micropores have a size between about 5 nanometers (nm) and 10 nm.

6. The carbon-containing glass material of claim 4, wherein at least some of the microcracks or microvoids are configured to dissipate fracture energy experienced at one or more crack tips in the carbon-containing glass material.

7. The carbon-containing glass material of claim 1, further comprising a monolayer of excess carbon disposed on the mesophase region.

8. The carbon-containing glass material of claim 1, further comprising an additive embedded between adjacent graphene layers within the FLG nanosheets formed in the mesophase region. 9 . The carbon-containing glass material according to claim 8 , wherein the additive comprises any one or more of lithium, sodium, potassium, calcium or other alkali metals.

10. The carbon-containing glass material of claim 8, wherein the additive comprises any one or more of copper, iron or other transition metals.

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