Method for internal filling regulation of single-walled carbon nanotube device and optoelectronic device application thereof

Abstract

This application relates to the fields of nanomaterials and optoelectronic devices, and particularly to a method for controlling the internal filling of single-walled carbon nanotube devices and its optoelectronic applications. The method includes: fabricating a single-chiral single-walled carbon nanotube device; performing interface pretreatment on the single-chiral single-walled carbon nanotube device; using a filling material to internally fill the pretreated single-chiral single-walled carbon nanotube device, followed by heat treatment to allow the filling material to migrate into the internal region of the single-walled carbon nanotube, forming an internal filling control structure. This application allows the filling material to enter the interior or interface region of the carbon nanotube without damaging the single-chiral single-walled carbon nanotube network structure and electrode contact state, constructing a stable internal filling control structure. Based on the interfacial charge transfer and band synergistic modulation effect between the filling material and the single-chiral single-walled carbon nanotube, effective control of the device's carrier transport behavior and photoelectric response characteristics is achieved.

Description

Technical Field

[0001] This application relates to the fields of nanomaterials and optoelectronic devices, and in particular to a method for controlling the internal filling of a single-walled carbon nanotube device and its optoelectronic device applications. Background Technology

[0002] In recent years, single-walled carbon nanotubes (SWCNTs) have attracted widespread attention in fields such as photodetectors, field-effect transistors, and flexible electronic devices due to their excellent one-dimensional carrier transport properties, tunable band structure, and good light absorption. In particular, single chiral semiconductor SWCNTs obtained through chiral separation can effectively eliminate the interference of metallic carbon nanotubes on device performance and are considered a key material basis for realizing high-performance carbon nanotube optoelectronic devices.

[0003] Related research mainly focuses on the following technical routes: First, device construction methods based on high-purity semiconductor or single-chiral SWCNTs, such as obtaining semiconductor single-walled carbon nanotubes with specific chirality (e.g., (6, 5)) through aqueous two-phase extraction, density gradient centrifugation, or selective oxidation to improve the on / off ratio and photoresponse performance of the device; Second, methods to regulate device performance through surface modification or external composite materials, such as introducing organic molecules, two-dimensional materials, or metal nanostructures on the surface of carbon nanotube networks to improve light absorption or carrier injection behavior; Third, photoelectric control schemes based on heterojunction structures, which enhance the separation efficiency of photogenerated carriers by forming heterojunctions between SWCNTs and other semiconductor materials.

[0004] The existing technologies have the following problems and disadvantages: (1) Limited means of device-level performance regulation. Existing research is mostly focused on the material preparation and chiral separation stages. Once the device is constructed, its performance regulation means are relatively limited, and it is difficult to effectively optimize the photoresponse characteristics of the device through post-processing. (2) Unstable interface of external modification methods. When functional materials are introduced through surface modification or external composite, the modification layer is usually located on the surface of the carbon nanotube network or the electrode interface. It is easy to desorb or degrade in subsequent testing or environmental changes, resulting in unstable device performance. (3) Poor compatibility between filling or modification processes and micro / nano device processes. Existing carbon nanotube filling or modification methods mostly rely on strong reaction or solution treatment processes, which are usually carried out in the material powder or thin film stage. It is difficult to directly apply to micro / nano devices with completed electrode construction, and it is easy to damage the carbon nanotube network structure and electrode contact state. (4) Limited improvement in photoresponsivity and specific detectivity. In existing single-chiral SWCNT optoelectronic devices, although lower dark current and better switching characteristics can be obtained, the responsivity and specific detectivity of the devices are still difficult to meet the requirements of high-sensitivity detection due to limitations in light absorption capacity and photogenerated carrier separation efficiency. (5) Lack of internal structure control schemes for single-chiral SWCNTs. Existing technologies mostly focus on the external structure or interface control of carbon nanotubes, and rarely conduct systematic design from the internal or internal interface structure of carbon nanotubes. A controllable and stable internal filling control technology scheme suitable for single-chiral SWCNT micro-nano devices has not yet been formed. Therefore, it is urgent to develop a post-processing control method that is highly compatible with the fabrication process of single-chiral single-walled carbon nanotube micro-nano devices, so as to achieve effective control of the internal or internal interface structure of carbon nanotubes without destroying the structural integrity and chiral purity of the device, thereby significantly improving the photoresponsivity, specific detectivity and long-term stability of the device. Summary of the Invention

[0005] This application provides a method for controlling the internal filling of a single-walled carbon nanotube device and its application in optoelectronic devices. By introducing a filling material after the device is fabricated, the internal and interface regions of the single-walled carbon nanotube can be controlled, thereby improving the photoelectric response performance and operational stability of the device.

[0006] To address the aforementioned technical problems, in a first aspect, embodiments of this application provide a method for controlling the internal filling of a single-walled carbon nanotube device, comprising the following steps: first, preparing a single-chiral single-walled carbon nanotube device; then, performing interface pretreatment on the single-chiral single-walled carbon nanotube device; finally, using a filling material to internally fill the pretreated single-chiral single-walled carbon nanotube device and performing heat treatment to allow the filling material to migrate into the internal region of the single-walled carbon nanotube, forming an internal filling control structure.

[0007] In some exemplary embodiments, the interface pretreatment includes cleaning and / or heat treatment; wherein the cleaning medium during the cleaning process is one or more of deionized water or organic solvents; and the heat treatment is performed under an inert atmosphere, vacuum, or protective atmosphere.

[0008] In some exemplary embodiments, the filler material is a material that can migrate to the interior and / or interface region of single-walled carbon nanotubes under heat treatment conditions and exert a regulatory effect on the electrical and optoelectronic properties of the device; the filler material includes one or more of phosphorus, arsenic, antimony, bismuth, sulfur, selenium, and tellurium. In some exemplary embodiments, during the internal filling process, the pretreated single-chiral single-walled carbon nanotube device and the filling material are placed in the same closed processing container and spaced apart along the axial direction of the closed processing container.

[0009] In some exemplary embodiments, the sealed processing container is a quartz tube; the filling material and the pretreated single chiral single-walled carbon nanotube device are placed in different regions of the quartz tube, so that the two are spatially separated, so that the filling material can migrate and fill to the device side under subsequent heat treatment conditions.

[0010] In some exemplary embodiments, the sealed processing container is heat-treated to cause the filling material to migrate under heating conditions and enter the internal cavity structure and / or interface region of the single-walled carbon nanotubes driven by concentration gradient, chemical potential difference and / or interfacial interaction, thereby forming an internal filling structure.

[0011] In some exemplary embodiments, the heat treatment is performed under vacuum, inert atmosphere or protective atmosphere conditions; the heat treatment temperature is 300~700 °C; and the heat treatment time is 30~600 min.

[0012] In some exemplary embodiments, the amount of filler material used is 1 to 50 mg.

[0013] Secondly, this application also provides a single-walled carbon nanotube device, which is prepared by the internal filling control method of the single-walled carbon nanotube device described in the above embodiments. The filling material exists stably in the interior or inner interface region of the single-walled carbon nanotube and forms an internal filling control structure.

[0014] Thirdly, embodiments of this application also provide an application of the single-walled carbon nanotube device as described in the above embodiments in photoelectric detection and field-effect transistor devices.

[0015] The technical solution provided in this application has at least the following advantages: This application provides a method for controlling the internal filling of a single-walled carbon nanotube device and its application in optoelectronic devices. The method includes the following steps: First, a single-chiral single-walled carbon nanotube device is prepared; then, the single-chiral single-walled carbon nanotube device undergoes interface pretreatment; finally, the pretreated single-chiral single-walled carbon nanotube device is internally filled with a filling material and then subjected to heat treatment to allow the filling material to migrate into the internal region of the single-walled carbon nanotube, forming an internal filling control structure.

[0016] This application provides a method for controlling the internal filling of single-walled carbon nanotube devices and its optoelectronic applications. Using pre-fabricated single-chiral single-walled carbon nanotube devices as the object, an internal filling process is introduced after device fabrication. The device is controlled by using filler materials from Group 15 and Group 16 elements, with phosphorus (P) or tellurium (Te) preferred as filler materials, to achieve control over the device's optoelectronic performance. Without disrupting the single-chiral single-walled carbon nanotube network structure and electrode contact state, the filler material is introduced into the interior or interface region of the carbon nanotubes, constructing a stable internal filling control structure. Based on the interfacial charge transfer and band synergistic modulation between the filler material and the single-chiral single-walled carbon nanotubes, effective control over the device's carrier transport behavior and photoelectric response characteristics is achieved. Compared to unfilled single-chiral single-walled carbon nanotube devices, the internally filled devices exhibit significant tunable changes in photoresponse behavior and detection characteristics. The method described in this application is mild, highly compatible with micro / nano device fabrication processes, and applicable to single-walled carbon nanotube phototransistors and related optoelectronic devices. Attached Figure Description

[0017] One or more embodiments are illustrated by way of example with reference to the accompanying drawings. These illustrations do not constitute a limitation on the embodiments, and unless otherwise stated, the figures in the drawings are not to be limited by scale.

[0018] Figure 1 This is a schematic diagram of the phosphorus (P) filling process for a (6, 5) type single-chiral single-walled carbon nanotube device provided in an embodiment of this application.

[0019] Figure 2 This is a schematic diagram of the tellurium (Te) filling process for a (6, 5) type single-chiral single-walled carbon nanotube device provided in an embodiment of this application.

[0020] Figure 3 Thermogravimetric analysis (TGA) curves of unfilled single-chiral single-walled carbon nanotubes (SWCNT), phosphorus-filled devices (SWCNT@P), and tellurium-filled devices (SWCNT@Te) provided in an embodiment of this application in the range of 30-1000 °C.

[0021] Figure 4 A comparison of the Raman spectra of unfilled SWCNT, SWCNT@P, and SWCNT@Te provided in an embodiment of this application.

[0022] Figure 5 The graph shows the responsivity (R) of the SWCNT@P device and the unfilled SWCNT device provided in an embodiment of this application as a function of wavelength.

[0023] Figure 6 The external quantum efficiency (EQE) curves of the SWCNT@P device and the unfilled SWCNT device provided in an embodiment of this application are shown as a function of wavelength.

[0024] Figure 7 The specific detectivity (D) of the SWCNT@P device compared to the unfilled SWCNT device provided in an embodiment of this application * (The curve shows the variation of wavelength.)

[0025] Figure 8 The graph shows the responsivity (R) of the SWCNT@Te device and the unfilled SWCNT device as a function of wavelength, according to an embodiment of this application.

[0026] Figure 9 The external quantum efficiency (EQE) curves of the SWCNT@Te device and the unfilled SWCNT device provided in an embodiment of this application are shown as a function of wavelength.

[0027] Figure 10 The external quantum efficiency (D) of the SWCNT@Te device provided in an embodiment of this application compared to that of an unfilled SWCNT device * (The curve shows the variation of wavelength.) Detailed Implementation

[0028] As the background technology indicates, single-chiral single-walled carbon nanotubes (SWCNTs) hold significant promise for applications in photodetectors and field-effect transistors due to their tunable bandgap and excellent optoelectronic properties. However, exposed SWCNT network devices still face challenges in practical applications, such as high interface state density, severe carrier recombination, and insufficient environmental stability, which limit their photoelectric response performance and device stability. Introducing functional filling materials into SWCNTs holds promise for modulating their carrier transport behavior and band structure, thereby improving device performance.

[0029] To address the aforementioned technical problems, this application provides a method for controlling the internal filling of a single-walled carbon nanotube device and its application in optoelectronic devices. The method includes the following steps: First, fabricating a single-chiral single-walled carbon nanotube device; then, performing interface pretreatment on the single-chiral single-walled carbon nanotube device; finally, internally filling the pretreated single-chiral single-walled carbon nanotube device with a filling material and performing heat treatment to allow the filling material to migrate into the internal region of the single-walled carbon nanotube, forming an internal filling control structure. This method, by introducing a filling material after device fabrication, achieves control over the internal and interface regions of the single-walled carbon nanotube, thereby improving the device's photoelectric response performance and operational stability.

[0030] The embodiments of this application will now be described in detail with reference to the accompanying drawings. However, those skilled in the art will understand that many technical details have been provided in the embodiments of this application to facilitate a better understanding of the application. However, the technical solutions claimed in this application can be implemented even without these technical details and various variations and modifications based on the following embodiments.

[0031] This application provides a method for controlling the internal filling of a single-walled carbon nanotube device and its optoelectronic application, including the following steps: The constructed single-chiral single-walled carbon nanotube micro / nano devices undergo interface pretreatment to remove residual surfactants or dispersants from the device surface and the inside of the channels, thus opening the internal channels of the carbon nanotubes. Subsequently, the treated devices are placed in a treatment environment containing filling material. The filling material is then heated to migrate into the interior of the single-chiral single-walled carbon nanotubes or the interface region under the drive of concentration gradient, chemical potential difference, or interfacial interaction, thereby achieving internal filling regulation.

[0032] The above method can achieve the stabilizing effect between the filling material and the single-walled carbon nanotubes without significantly affecting the network structure and electrode contact state of the single-walled carbon nanotubes, thereby improving the carrier transport behavior and photoelectric response characteristics of the device.

[0033] Specifically, a single-chiral single-walled carbon nanotube device is constructed using conventional methods in the art. The single-chiral single-walled carbon nanotubes can be obtained through chiral separation and deposited between prefabricated electrodes to form a channel network. The device substrate can be a silicon-based substrate, the gate dielectric layer can be a silicon dioxide layer, and the electrode structure can be interdigitated electrodes or other electrode structures suitable for micro / nano devices. The single-walled carbon nanotube dispersion can be deposited in the electrode channel region by methods such as drop coating, spin coating, spraying, transfer, or printing, thereby forming a single-chiral single-walled carbon nanotube conductive network.

[0034] Interface pretreatment is performed on single-chiral single-walled carbon nanotube devices to remove residual dispersants, surfactants, or other impurities from the device surface and carbon nanotube network, and to improve the device interface state. The interface pretreatment includes cleaning and / or heat treatment; wherein the cleaning medium can be deionized water, organic solvents, or combinations thereof, and the heat treatment can be performed under an inert atmosphere, vacuum, or protective atmosphere. This interface pretreatment reduces the impact of device surface residues on the subsequent filling process and improves the accessibility of the internal channels and interface regions of the single-walled carbon nanotubes to the filling material.

[0035] After the device is fabricated and the interface pretreatment is completed, a filling material is selected to fill the interior of the single-chiral single-walled carbon nanotube device. The filling material is a material that can migrate to the interior and / or interface region of the single-walled carbon nanotube under heat treatment conditions and exert a modulating effect on the electrical and optoelectronic properties of the device.

[0036] In some embodiments, the filler material is a Group 15 or Group 16 element and related materials.

[0037] In some embodiments, the filler material includes one or more of phosphorus, arsenic, antimony, bismuth, sulfur, selenium, and tellurium.

[0038] In a more preferred embodiment, the filler material is phosphorus and / or tellurium. The form of the filler material includes powder, granules, flakes, nanosheets, thin sheets, or combinations thereof. In some preferred embodiments, the phosphorus material may be in flake or nanosheet form, and the tellurium material may be in powder or granule form.

[0039] The filling process is carried out in a closed processing container, preferably in a quartz tube, with the filling material separated from the device to be processed, so as to allow the filling material to migrate and fill towards the device side under subsequent heat treatment conditions. In some preferred embodiments, the filling material and the device to be processed are placed at an axial distance along the processing container, preferably at opposite ends of the quartz tube.

[0040] The heat treatment causes the filler material to migrate into the internal region of the single-walled carbon nanotubes, forming a stable internal filling structure.

[0041] The sealed processing container is heat-treated to induce the migration of the filling material under heating conditions. Driven by concentration gradient, chemical potential difference, and / or interfacial interactions, the material enters the internal cavity structure and / or interfacial region of the single-walled carbon nanotubes, thereby forming an internal filling structure. The heat treatment can be performed under vacuum, inert atmosphere, or protective atmosphere; the heat treatment temperature is 300–700 °C, preferably 400–600 °C; the heat treatment time is 30–600 min, preferably 120–480 min. The amount of filling material can be adjusted according to the volume of the processing container, the device size, and the target filling degree, preferably 1–50 mg, more preferably 5–20 mg.

[0042] In some specific embodiments, the heat treatment may be performed at approximately 500 °C for approximately 360 min.

[0043] The filling process can be carried out under vacuum, inert atmosphere, or protective atmosphere conditions.

[0044] In some preferred embodiments, the filling process is performed in a vacuum environment.

[0045] The internal filling control method of the single-walled carbon nanotube device provided in this application will be described in detail below through specific embodiments.

[0046] refer to Figure 1 and Figure 2 This application provides an internal filling method based on (6, 5) type single-chiral single-walled carbon nanotubes (SWCNTs). In some embodiments, the single-walled carbon nanotubes are single-chiral semiconductor single-walled carbon nanotubes, preferably (6, 5) type single-walled carbon nanotubes. The filling material can be Group 15 and Group 16 elements and related materials, preferably phosphorus and / or tellurium. The following description uses phosphorus filling and tellurium filling as examples.

[0047] The following describes the phosphorus filling method.

[0048] refer to Figure 1 This embodiment provides a phosphorus filling method based on (6, 5) type SWCNTs, including the following steps: Step S1: Place the separated and purified single-walled carbon nanotube network device and the filling material together in a closed processing container, wherein the filling material and the device are separated; preferably, the sample is loaded under an inert atmosphere and the processing container is vacuumed or sealed under a protective atmosphere.

[0049] Step S2: Place the processing container in a heating device and perform heat treatment according to a preset temperature program to allow the filling material to migrate into the interior and / or inner interface region of the single-walled carbon nanotubes and complete the filling.

[0050] Step S3: After filling is completed, the sample is cooled and further post-processing can be performed to improve the stability of the filled structure and the working stability of the device, and then the phosphorus-filled SWCNT@P device is obtained.

[0051] The filling method used in this application is simple and highly controllable. The degree of phosphorus filling can be effectively controlled by adjusting the temperature program. A stable interface is formed between phosphorus and SWCNT, which is beneficial for regulating carrier transport behavior and improving the optoelectronic performance of the device.

[0052] The specific steps are as follows: ① The prepared (6, 5) type SWCNT network device and the filling material are placed in a quartz tube. The amount of the filling material can be 1 to 50 mg, preferably 5 to 20 mg.

[0053] ② Vacuum the quartz tube and seal it, or seal it under an inert / protective atmosphere.

[0054] ③ Heat to the target temperature at the set heating rate and hold for a predetermined time to allow phosphorus to migrate into the interior and / or inner interface region of the SWCNT; the filling temperature can be 300-700 ℃, preferably 400-600 ℃; the filling time can be 30-600 min, preferably 120-480 min.

[0055] ④ After cooling to room temperature, remove the sample for post-processing to obtain the SWCNT@P device.

[0056] The following describes the tellurium filling method.

[0057] refer to Figure 2 This embodiment also provides a tellurium filling method based on (6, 5) type SWCNTs. Its process flow is basically the same as that of the phosphorus filling method, except that the filling material is changed to tellurium material.

[0058] In this embodiment, the amount of phosphorus material used can be approximately 10 mg.

[0059] The specific steps are as follows: ① Reference Figure 2 This embodiment also provides a tellurium filling method based on a single chiral single-walled carbon nanotube device. The process flow is basically the same as the phosphorus filling method described above, except that the filling material is replaced with tellurium or tellurium-containing material.

[0060] ② Vacuum the quartz tube and seal it, or seal it under an inert / protective atmosphere.

[0061] ③ Heating is performed according to the set heating program, so that the tellurium material migrates into the interior or interface region of SWCNT under high temperature conditions.

[0062] ④ After cooling to room temperature, remove the sample to obtain the SWCNT@Te device.

[0063] In this embodiment, the amount of tellurium material used can be approximately 10 mg.

[0064] During tellurium filling, tellurium material can also enter the interior or interface region of the SWCNT driven by concentration gradient and chemical potential difference, thereby modulating the photoelectric response behavior of the device. In some embodiments, a post-processing step is included after filling. The post-processing step includes one or more of the following: heat treatment, atmosphere treatment, optical treatment, electrical treatment, chemical treatment, plasma treatment, or encapsulation treatment, to further stabilize the filled structure, remove residual surface adsorbates, and improve the device's operational stability. Preferably, the post-processing can be performed under vacuum, inert atmosphere, or protective atmosphere conditions.

[0065] Examples and Comparative Examples Example 1 (Phosphorus-filled) In this embodiment, a (6, 5) type SWCNT network device and 10 mg of phosphorus material are encapsulated in a quartz tube, according to... Figure 1 The filling process was performed at the indicated temperature to obtain the SWCNT@P device. A comparison of the sample states before and after filling is shown below. Figure 1 As shown in (b).

[0066] Example 2 (tellurium filling) In this embodiment, a (6, 5) type SWCNT network device and 10 mg of tellurium powder are encapsulated in a quartz tube, according to... Figure 2 The temperature program shown is used for filling to obtain the SWCNT@Te device.

[0067] Comparative Example 1 (Unfilled) This comparative example is a (6, 5) type SWCNT network device without filler processing.

[0068] The electrical and optoelectronic properties of the device after internal filling modulation are characterized to evaluate the impact of the filling treatment on the device's carrier transport behavior and photoresponse characteristics. In a preferred embodiment, when phosphorus and / or tellurium are used as the filling material, interfacial charge transfer and band modulation can occur between the filling material and the single chiral single-walled carbon nanotubes, thereby improving the device's photoresponse performance, detection performance, and operational stability. In a preferred embodiment, when phosphorus is used as the filling material, the device's photoresponsivity and specific detectivity are improved, while maintaining low dark current and good operational stability.

[0069] Thermogravimetric analysis was performed on SWCNT, SWCNT@P, and SWCNT@Te samples, and the results are as follows: Figure 3As shown in the figure, the thermogravimetric curves indicate that the filler material was successfully introduced into the SWCNT structure.

[0070] Raman spectroscopy characterization was performed on SWCNT, SWCNT@P, and SWCNT@Te samples, and the results are as follows: Figure 4 As shown, the Raman characteristic peaks of the filled sample changed compared to the unfilled sample, indicating an interaction between the filler material and SWCNTs.

[0071] The device performance tests are as follows: The photoelectric performance of the devices in Example 1 (SWCNT@P) and Comparative Example 1 was tested, and their responsivity R curves are shown below. Figure 5 As shown, the external quantum efficiency (EQE) curve is as follows: Figure 6 As shown, the specific detectivity D* curve is as follows: Figure 7 As shown in the figure. The results indicate that, in the phosphorus-filled embodiment, the device's photoresponse capability in the visible-near-infrared band is significantly enhanced.

[0072] The photoelectric performance of the devices in Example 2 (SWCNT@Te) and Comparative Example 1 was tested, and their responsivity R curves are shown below. Figure 8 As shown, the external quantum efficiency (EQE) curve is as follows: Figure 9 As shown, the specific detectivity D * Curves Figure 10 As shown in the figure. The results indicate that tellurium filling can modulate the photoelectric response behavior of the device, and its response characteristics differ from those of the unfilled device.

[0073] Table 1 compares the key optoelectronic performance parameters of the single chiral single-walled carbon nanotube devices in the embodiments and comparative examples of the present invention, including responsivity (R), external quantum efficiency (EQE), and specific detectivity (D). * ), as shown below.

[0074] Table 1. Performance Comparison of Single-Walled Carbon Nanotube Optoelectronic Devices

[0075] The experimental results above show that after phosphorus filling, the (6,5) type SWCNT device can still maintain its electrical modulation characteristics, and introduce new interface charge transfer and energy level modulation effects through the internal filling structure, thereby improving the photoelectric response performance of the device; tellurium filling can also change the response behavior of the device, providing the possibility for device performance regulation in different application scenarios.

[0076] Compared with existing technologies, the internal filling control method for single-walled carbon nanotube devices provided in this application has the following advantages: In existing research on optoelectronic devices using single-chiral single-walled carbon nanotubes, device performance is typically limited by factors such as the small intrinsic light absorption cross-section of carbon nanotubes and the high recombination efficiency of photogenerated carriers. Publicly available literature reports that photodetectors constructed based on single-chiral (e.g., (6, 5) type) SWCNTs generally have responsivity around 10. -3 ~10 -1 Within the A / W range, the specific detectivity is typically around 10. 9 ~10 11 In the Jones range, while improving responsivity, there are often problems such as increased dark current or decreased device stability.

[0077] The device-level internal filling control method proposed in this application enables internal structure control in single-chiral SWCNT micro / nano devices with completed electrode fabrication. In a preferred embodiment, when the filling material is phosphorus, the device responsivity can be improved to 2-5 times that of unfilled devices, and the specific detectivity can reach 10-1. 11 ~10 12 It achieves Jones-level performance while maintaining low dark current and stable gate voltage regulation characteristics.

[0078] Compared with external composite or material stage modification methods, this application achieves post-processing control of device performance by forming a filling control structure inside and / or in the internal interface region of single-walled carbon nanotubes. This eliminates the need to introduce an additional external functional interface layer, which is beneficial for balancing device response performance and operational stability.

[0079] Furthermore, this application also provides a single chiral single-walled carbon nanotube device, which is prepared using the internal filling control method described in the above embodiments. The device is characterized in that the filling material is stably present inside or in the internal interface region of the single chiral single-walled carbon nanotube, forming an internal filling control structure.

[0080] In addition, this application embodiment also provides a single chiral single-walled carbon nanotube field-effect transistor with photoelectric response. The field-effect transistor uses a single chiral single-walled carbon nanotube network with internal filling regulation as the channel material. Under gate voltage regulation and illumination conditions, the field-effect transistor exhibits electrical modulation characteristics and photoelectric response characteristics.

[0081] Based on the above technical solutions, this application provides a method for controlling the internal filling of a single-walled carbon nanotube device and its application in optoelectronic devices. The method includes the following steps: First, a single-chiral single-walled carbon nanotube device is prepared; then, the single-chiral single-walled carbon nanotube device undergoes interface pretreatment; finally, the pretreated single-chiral single-walled carbon nanotube device is internally filled with a filling material and then subjected to heat treatment to allow the filling material to migrate into the internal region of the single-walled carbon nanotube, forming an internal filling control structure.

[0082] This application provides a method for controlling the internal filling of single-walled carbon nanotube (SHU) devices and its optoelectronic applications. Using pre-fabricated single-chiral SHU devices as the subject, an internal filling process is introduced after device fabrication. This involves using filler materials from Group 15 and Group 16 elements, with phosphorus or tellurium being preferred, to control the device's optoelectronic performance. Without disrupting the SHU network structure or electrode contact state, the filler material is introduced into the interior or interface region of the carbon nanotubes, constructing a stable internal filling control structure. Based on the interfacial charge transfer and bandgap modulation between the filler material and the SHU, effective control over the device's carrier transport behavior and photoelectric response characteristics is achieved. Compared to unfilled SHU devices, the internally filled devices exhibit significant tunability changes in photoresponse behavior and detection characteristics. The method described in this application is mild, highly compatible with micro / nano device fabrication processes, and applicable to SHU phototransistors and related optoelectronic devices.

[0083] Those skilled in the art will understand that the above-described embodiments are specific examples of implementing this application, and in practical applications, various changes in form and detail may be made without departing from the spirit and scope of this application. Any person skilled in the art can make their own modifications and alterations without departing from the spirit and scope of this application; therefore, the scope of protection of this application should be determined by the scope defined in the claims.

Claims

1. A method for controlling the internal filling of a single-walled carbon nanotube device, characterized in that, Includes the following steps: Fabrication of single-chiral single-walled carbon nanotube devices; Interface pretreatment is performed on the single chiral single-walled carbon nanotube device; The pretreated single-chiral single-walled carbon nanotube device is internally filled with a filling material and then subjected to heat treatment to allow the filling material to migrate into the internal region of the single-walled carbon nanotube, forming an internal filling control structure.

2. The method for controlling the internal filling of a single-walled carbon nanotube device according to claim 1, characterized in that, The interface pretreatment includes cleaning and / or heat treatment; wherein, the cleaning medium during the cleaning process is one or more of deionized water or organic solvents; and the heat treatment is carried out under an inert atmosphere, vacuum or protective atmosphere.

3. The method for controlling the internal filling of a single-walled carbon nanotube device according to claim 1, characterized in that, The filling material is a material that can migrate into the interior and / or interface region of single-walled carbon nanotubes under heat treatment conditions and exert a regulatory effect on the electrical and optoelectronic properties of the device. The filler material includes one or more of phosphorus, arsenic, antimony, bismuth, sulfur, selenium, and tellurium.

4. The method for controlling the internal filling of a single-walled carbon nanotube device according to claim 1, characterized in that, During the internal filling process, the pretreated single-chiral single-walled carbon nanotube device and the filling material are placed in the same closed processing container and spaced apart along the axial direction of the closed processing container.

5. The method for controlling the internal filling of a single-walled carbon nanotube device according to claim 4, characterized in that, The sealed processing container is a quartz tube; The filling material and the pretreated single-chiral single-walled carbon nanotube device are placed in different regions of the quartz tube, so that they are spatially separated, so that the filling material can migrate and fill to the device side under subsequent heat treatment conditions.

6. The method for controlling the internal filling of a single-walled carbon nanotube device according to claim 4, characterized in that, The sealed container is subjected to heat treatment, which causes the filling material to migrate under heating conditions and enter the internal cavity structure and / or interface region of the single-walled carbon nanotube under the drive of concentration gradient, chemical potential difference and / or interface interaction, thereby forming an internal filling structure.

7. The method for controlling the internal filling of a single-walled carbon nanotube device according to claim 1, characterized in that, The heat treatment is carried out under vacuum, inert atmosphere or protective atmosphere conditions; the heat treatment temperature is 300~700 ℃; the heat treatment time is 30~600 min.

8. The method for controlling the internal filling of a single-walled carbon nanotube device according to claim 1, characterized in that, The amount of the filler material used is 1~50 mg.

9. A single-walled carbon nanotube device, wherein the device is prepared by the internal filling control method for single-walled carbon nanotube devices as described in any one of claims 1 to 8, characterized in that, The filling material exists stably inside or at the inner interface of single-walled carbon nanotubes, forming an internal filling control structure.

10. The application of a single-walled carbon nanotube device as described in claim 9 in photoelectric detection and field-effect transistor devices.

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