Plasma as afterglow excitation source

Abstract

The invention discloses a plasma as an afterglow excitation source. Specifically, the plasma is used as the afterglow excitation source for exciting a material to generate afterglow. The plasma serves as a novel afterglow excitation source, the afterglow excitation mode is expanded, and the plasma can flexibly adapt to different scene requirements. By regulating and controlling plasma generation parameters, accurate excitation control and uniform energy transfer can be realized, and the surface quenching risk is reduced; plasma can excite part of materials which cannot be excited by a traditional excitation source to generate afterglow, and the range of the materials capable of expressing afterglow characteristics is expanded. In addition, the technology has good biocompatibility and equipment integration flexibility, and safety, reliability and flexibility can be improved.

Description

Technical Field

[0001] This invention relates to the field of luminescent materials technology, and in particular to plasma as an afterglow excitation source, and further to the application of plasma as an afterglow excitation source in the generation of afterglow in excitation materials. Background Technology

[0002] Afterglow materials are a class of functional materials that continue to emit light after external excitation ceases. Their luminescence mechanism primarily relies on the slow release of excited-state electrons through defect energy levels or energy storage states. These materials exhibit characteristics such as long-lived luminescence (from milliseconds to hours), absence of background autofluorescence interference, high signal-to-noise ratio, and low signal-to-background ratio, showing broad application prospects in biomedical imaging (e.g., tumor diagnosis and in vivo tracking), information encryption, anti-counterfeiting labels, and photocatalysis. However, currently, the main excitation methods for afterglow materials are limited to three categories: photoexcitation, ultrasonic excitation, and ion radiation excitation. This limited range of excitation methods and the scarcity of afterglow luminescence excitation sources restricts the application and development of afterglow luminescence technology. Summary of the Invention

[0003] This invention aims to at least solve one of the technical problems existing in the prior art. To this end, one object of this invention is to provide the application of plasma as an afterglow excitation source in the generation of afterglow in excitation materials.

[0004] A second objective of this invention is to provide a method for afterglow excitation.

[0005] A third objective of this invention is to provide a method for afterglow imaging.

[0006] The fourth objective of this invention is to provide an afterglow imaging system.

[0007] In a first aspect, the present invention proposes the application of plasma as an afterglow excitation source in the generation of afterglow in excitation materials.

[0008] According to embodiments of the present invention, the application of plasma as an afterglow excitation source in the generation of afterglow from materials has at least the following beneficial effects: The present invention proposes a novel afterglow excitation source, specifically using plasma as an afterglow excitation source to excite materials to generate afterglow. This expands the excitation methods of afterglow and facilitates the application expansion of afterglow luminescence technology. Due to the atoms, electrons, free radicals, and other particles generated by plasma, as well as various active components such as electromagnetic fields and photons, plasma, as a novel afterglow excitation source, can flexibly adapt to different scenario requirements. Precise and uniform energy transfer can be achieved by controlling the plasma generation parameters, realizing uniform and controllable energy deposition on the excited material, thereby effectively optimizing surface interactions and reducing the risk of quenching. Furthermore, the application range of plasma can be extended to the excitation of some inert materials that cannot be excited by traditional excitation sources, thus expanding the range of materials that can exhibit afterglow characteristics. In addition, the efficient energy transfer mechanism of plasma can improve the brightness and duration of afterglow, reducing dependence on high-power light sources and photobleaching. Moreover, this technology combines good biocompatibility (avoiding radiation and light damage) and equipment integration flexibility, improving safety, reliability, and flexibility.

[0009] According to some embodiments of the present invention, the material may include, but is not limited to, at least one of the following: clinical medical materials that can be excited by plasma to produce afterglow, fluorescent probe materials that can be excited by plasma to produce afterglow, and optoelectronic materials that can be excited by plasma to produce afterglow.

[0010] According to some embodiments of the present invention, the clinical pharmaceutical material that can be excited by plasma to produce afterglow may include, but is not limited to, at least one of 1-(4-amino-2-(ethoxymethyl)-1H-imidazo[4,5-c]quinolin-1-yl)-2-methylprop-2-ol (CAS No.: 144875-48-9) and 9-methyl-3-((2-methyl-1H-imidazo-1-yl)methyl)-2,3-dihydro-1H-carbazole-4-(9H)-one (CAS No.: 99614-02-5).

[0011] According to some embodiments of the present invention, the fluorescent probe material that can be excited by plasma to produce afterglow may include, but is not limited to, at least one of 9-(2-(ethoxycarbonyl)phenyl)-3,6-di(ethylamino)-2,7-dimethylchlorooxanethene (CAS No.: 989-38-8) and 7-diethylamino-4-methylcoumarin (CAS No.: 91-44-1).

[0012] According to some embodiments of the present invention, the photoelectric material that can be excited by plasma to produce afterglow may include, but is not limited to, at least one of the following: non-fullerene acceptor ITIC (CAS No.: 1664293-06-4) and 4'-(4-carboxyphenyl)-2,2'-6'-2'-terpyridine (CAS No.: 158014-74-5).

[0013] According to some embodiments of the present invention, the plasma includes at least one of non-thermal plasma and thermal plasma.

[0014] According to some embodiments of the present invention, the non-thermal plasma may include, but is not limited to, at least one of radio frequency glow discharge plasma, DC glow discharge plasma, microwave glow discharge plasma, capacitive coupling plasma, low-pressure glow discharge plasma, atmospheric pressure glow discharge plasma, corona discharge plasma, and dielectric barrier discharge plasma.

[0015] According to some embodiments of the present invention, the thermal plasma may include, but is not limited to, at least one of arc discharge plasma and inductively coupled plasma.

[0016] According to some embodiments of the present invention, the application includes: controlling plasma to contact the material, wherein the plasma excites the material to produce afterglow.

[0017] According to some embodiments of the present invention, the excitation material generating afterglow may include, but is not limited to, exciting the material to generate afterglow in afterglow imaging. That is, in some embodiments, plasma may be used as an afterglow excitation source to excite the material to generate afterglow in afterglow imaging.

[0018] A second aspect of the present invention provides a method for afterglow excitation, comprising the following steps: providing plasma, controlling the plasma to contact a target excitation material, and the plasma exciting the target excitation material to generate afterglow.

[0019] The technical solution of the afterglow excitation method of the present invention has at least the following beneficial effects: In the afterglow excitation method of this invention, plasma is used as the afterglow excitation source. The plasma is controlled to contact the target excitation material, and the plasma excites the target excitation material to generate afterglow. That is, the afterglow excitation method involves the application of plasma as the afterglow excitation source in the generation of afterglow by the excitation material. Therefore, the afterglow excitation method has at least all the excellent effects of the aforementioned application of plasma as the afterglow excitation source in the generation of afterglow by the excitation material, which will not be elaborated further.

[0020] According to some embodiments of the present invention, the target excitation material includes at least one of the following: clinical and pharmaceutical materials that can be excited by plasma to produce afterglow, fluorescent probe materials that can be excited by plasma to produce afterglow, and optoelectronic materials that can be excited by plasma to produce afterglow.

[0021] Clinical and pharmaceutical materials capable of generating afterglow upon plasma excitation may include, but are not limited to, at least one of 1-(4-amino-2-(ethoxymethyl)-1H-imidazo[4,5-c]quinoline-1-yl)-2-methylprop-2-ol and 9-methyl-3-((2-methyl-1H-imidazo-1-yl)methyl)-2,3-dihydro-1H-carbazole-4-(9H)-one. Fluorescent probe materials capable of generating afterglow upon plasma excitation may include, but are not limited to, at least one of 9-(2-(ethoxycarbonyl)phenyl)-3,6-di(ethylamino)-2,7-dimethylchlorooxanthracene and 7-diethylamino-4-methylcoumarin. Photoelectric materials capable of generating afterglow upon plasma excitation may include, but are not limited to, at least one of the non-fullerene acceptor ITIC and 4'-(4-carboxyphenyl)-2,2'-6'-2'-terpyridine.

[0022] According to some embodiments of the present invention, the plasma may be provided by at least one of gas discharge (including but not limited to corona discharge, glow discharge, arc discharge, dielectric barrier discharge, radio frequency discharge, microwave discharge) and thermal ionization (such as an arc plasma torch).

[0023] A third aspect of the present invention provides a afterglow imaging method, including any of the afterglow excitation methods described above.

[0024] The technical solution of the afterglow imaging method of the present invention has at least the following beneficial effects: The afterglow imaging method of this invention uses plasma as the afterglow excitation source and controls the plasma to contact the target excitation material, thereby exciting it to generate afterglow for imaging. Plasma, as a novel afterglow excitation source, expands the excitation methods for afterglow by exciting materials, and can flexibly adapt to different scenario requirements. Furthermore, precise and uniform energy transfer can be achieved by controlling plasma generation parameters, enabling uniform and controllable energy deposition on the target excitation material, thereby effectively optimizing surface interactions and reducing quenching risk. The application scope of plasma can be extended to the excitation of some inert materials that cannot be excited by traditional excitation sources, thus expanding the range of materials that can exhibit afterglow characteristics. In addition, the efficient energy transfer mechanism of plasma can improve afterglow brightness and duration, reducing dependence on high-power light sources and photobleaching. Using plasma as an afterglow excitation source for afterglow imaging, leveraging the spatiotemporal decoupling characteristics of afterglow imaging, can avoid interference from real-time light sources, significantly improving the signal-to-noise ratio, and is suitable for high-contrast imaging of deep tissues. Moreover, the afterglow excitation methods in the above afterglow imaging methods combine good biocompatibility (avoiding radiation and light damage) and equipment integration flexibility, enabling high-quality afterglow imaging and application expansion of deep tissues while ensuring safety.

[0025] According to some embodiments of the present invention, the method further includes: acquiring the afterglow signal generated by the target excitation material and constructing an image.

[0026] A fourth aspect of the present invention provides an afterglow imaging system, comprising: An afterglow generation device includes an excitation source module, wherein the excitation source module includes a plasma generator, and the plasma generator is used to generate plasma to excite a target excitation material to generate afterglow. The afterglow imaging device includes a signal acquisition module and an imaging module; the signal acquisition module is used to acquire the afterglow signal generated by the target excitation material; the imaging module is communicatively connected to the signal acquisition module and is used to receive the afterglow signal acquired by the signal acquisition module and construct an image.

[0027] The technical solution of the afterglow imaging system of the present invention has at least the following beneficial effects: The excitation source module of the afterglow generation device in the afterglow imaging system of this invention includes a plasma generator. The plasma generator is used to generate plasma to excite the target excitation material to generate afterglow. That is, the afterglow imaging system involves the application of plasma as an afterglow excitation source in the generation of afterglow by the excitation material. Therefore, the afterglow imaging system also has at least all the excellent effects of the aforementioned application of plasma as an excitation source in the generation of afterglow by the excitation material, which will not be elaborated further.

[0028] According to some embodiments of the present invention, the afterglow generation device further includes a sample carrying module, which is used to carry an imaging sample containing the target excitation material.

[0029] According to some embodiments of the present invention, a central control module is further included, which is communicatively connected to the excitation source module and is used at least to control the excitation time of the excitation source module.

[0030] According to some embodiments of the present invention, the excitation source module further includes a gas supply device connected to the plasma generator for supplying the plasma generator with the gas required to generate plasma.

[0031] According to some embodiments of the present invention, the central control module is also communicatively connected to the gas supply device, and is at least used to regulate the gas supply from the gas supply device to the plasma generator. Attached Figure Description

[0032] The present invention will be further described below with reference to the accompanying drawings and embodiments, wherein: Figure 1 This is a schematic diagram of the structure of an embodiment of the afterglow imaging system of the present invention; Figure 2 This is a bright-field diagram of the sample solution in the experimental examples of this invention; Figure 3 This is a sample material diagram of the third group of sample solutions in the experimental examples of this invention after plasma excitation; Figure 4 This is a post-luminescence image of the sample solution in the experimental example of this invention after being stimulated by different excitation methods. Detailed Implementation

[0033] The following will describe the concept and technical effects of the present invention clearly and completely with reference to embodiments, so as to fully understand the purpose, features and effects of the present invention. Obviously, the described embodiments are only some embodiments of the present invention, not all embodiments. Other embodiments obtained by those skilled in the art based on the embodiments of the present invention without creative effort are all within the scope of protection of the present invention.

[0034] Afterglow materials can continue to emit light after excitation stops. By eliminating autofluorescence interference from biological tissues, they exhibit high signal-to-background ratio, high sensitivity, and potential for deep tissue detection in fields such as biomedical imaging (e.g., tumor diagnosis), security and anti-counterfeiting, optoelectronic devices, and information displays. Existing excitation methods for afterglow materials are limited. Traditional excitation methods mainly fall into three categories: photoexcitation (e.g., ultraviolet / visible / near-infrared), ultrasonic excitation, and ion radiation excitation (e.g., X-rays). The limited variety of afterglow luminescence excitation sources restricts the application and development of afterglow luminescence technology. Furthermore, these traditional excitation methods typically have the following limitations: photoexcitation suffers from insufficient tissue penetration depth, and high-energy light sources can easily cause photodamage and photobleaching; while ultrasonic excitation offers deep penetration and high safety, it produces low afterglow intensity, has a short wavelength, and limited penetration ability; and while ion radiation excitation has extremely strong penetration, it presents radiation risks, complex material design, and potential biosafety issues. In addition, existing excitation strategies lack versatility, making it difficult to flexibly adapt to different application scenarios and to balance efficient excitation, deep penetration, and biosafety, thus limiting their widespread application in in vivo imaging and portable devices.

[0035] In view of the above, the present invention provides a novel afterglow excitation strategy to expand the excitation methods of afterglow. It can even overcome the limitations of traditional excitation sources in terms of penetration, safety, excitation efficiency and system integration, thereby promoting the development of afterglow technology towards a safer, more efficient, flexible, portable and widely applicable direction.

[0036] In one aspect, the present invention proposes the application of plasma as an afterglow excitation source in the generation of afterglow in excitation materials.

[0037] As an emerging tool, plasma technology has demonstrated broad application potential in multiple fields, including skin inflammation relief, gene expression regulation, and material surface modification. Its mechanism of action mainly stems from the various active components generated by plasma, such as atoms, electrons, free radicals including reactive oxygen species and nitrogen (RONS), as well as electromagnetic fields and photons. Plasma (such as non-equilibrium plasma) can simultaneously integrate photon energy, kinetic effects, and chemical stimulation to form a unique source with multidimensional energy distribution. It can serve as a novel afterglow excitation source. The synergistic combination of its energy forms can interact with the target excitation material through the unconventional pathway of the combined action of multiple active components (possibly including particle collision energy transfer, field-induced excitation, etc.), thereby stimulating the target excitation material to produce afterglow characteristics. Furthermore, it can flexibly adapt to different scenario requirements.

[0038] Plasma, as a novel afterglow excitation source, not only expands the excitation methods of afterglow but also demonstrates significant advantages in terms of control precision, application flexibility, and biosafety. On the one hand, using plasma as an afterglow excitation source allows for precise excitation control and uniform energy transfer. Specifically, by adjusting plasma generation parameters (such as gas type, processing time, power, and other discharge parameters), the surface charge and electric field intensity of the plasma afterglow region can be finely controlled. For example, ferroelectric discharge can be used to enhance the electric field in the afterglow region, achieving more uniform and controllable energy transfer and deposition onto the target excitation material. This effectively optimizes surface interactions (such as catalytic reactions or biological interface coupling) and reduces the risk of surface quenching, overcoming the problem of unstable energy transfer in traditional excitation methods. On the other hand, plasma can excite some inert materials that cannot be excited by traditional photoexcitation or ultrasonic excitation, including some clinical drug materials, fluorescent probe materials, and optoelectronic materials, expanding the range of materials that can exhibit afterglow characteristics. Furthermore, the efficient energy transfer mechanism of plasma (such as storing energy through induced defect states) helps to improve the brightness and duration of the afterglow while reducing dependence on high-power light sources and related photobleaching phenomena. Furthermore, plasma excitation offers high safety and biocompatibility, avoiding the radiation risks of traditional ion radiation excitation and the potential photodamage caused by high-energy light sources such as ultraviolet light. It exhibits significant safety advantages in in vivo tissue and cell imaging, making it suitable for non-invasive or minimally invasive biomedical applications. Its non-invasive and low-damage characteristics provide a reliable tool for developing next-generation biocompatible probes and safety tags. Moreover, plasma devices are easily miniaturized and lightweight, allowing for integration with handheld, wearable, or endoscopic optical imaging devices, greatly expanding the application scenarios of afterglow luminescence technology in bedside diagnosis, intraoperative navigation, and home health monitoring.

[0039] This invention uses plasma as an afterglow excitation source to excite materials to generate afterglow. The form of plasma used to excite the material to generate afterglow is not limited; for example, it can be generated through various forms such as gas discharge (including but not limited to corona discharge, glow discharge, arc discharge, dielectric barrier discharge, radio frequency discharge, and microwave discharge) and thermal ionization (such as an arc plasma torch). Correspondingly, this invention is not limited to the type of plasma used to excite the material to generate afterglow, and can include at least one of non-thermal plasma and thermal plasma. Non-thermal plasma can include, but is not limited to, at least one of radio frequency glow discharge plasma, DC glow discharge plasma, microwave glow discharge plasma, capacitively coupled plasma, low-voltage glow discharge plasma (i.e., non-equilibrium plasma generated by gas ionization under pressures of 0.1~10 Torr), atmospheric pressure glow discharge plasma, corona discharge plasma, and dielectric barrier discharge plasma; thermal plasma can include, but is not limited to, at least one of arc discharge plasma and inductively coupled plasma. Any device capable of generating plasma, the form of plasma that can be generated, or the type of plasma is applicable to this invention.

[0040] Plasma is rich in a variety of active ions, which can efficiently excite target materials and can also excite some materials that cannot be excited by traditional excitation sources (such as ultraviolet light and ultrasound), including but not limited to clinical and medical materials that can be excited by plasma to produce afterglow, fluorescent probe materials that can be excited by plasma to produce afterglow, and optoelectronic materials that can be excited by plasma to produce afterglow.

[0041] Some non-limiting examples of clinical and pharmaceutical materials capable of producing afterglow upon plasma excitation include 1-(4-amino-2-(ethoxymethyl)-1H-imidazo[4,5-c]quinolin-1-yl)-2-methylprop-2-ol and 9-methyl-3-((2-methyl-1H-imidazo-1-yl)methyl)-2,3-dihydro-1H-carbazole-4-(9H)-one. Some non-limiting examples of fluorescent probe materials capable of producing afterglow upon plasma excitation include 9-(2-(ethoxycarbonyl)phenyl)-3,6-di(ethylamino)-2,7-dimethyloxyxanthracene chloride and 7-diethylamino-4-methylcoumarin. Some non-limiting examples of optoelectronic materials capable of producing afterglow upon plasma excitation include the non-fullerene acceptor ITIC and 4'-(4-carboxyphenyl)-2,2'-6'-2'-terpyridine.

[0042] The above materials remain completely inert under prolonged light exposure (such as ultraviolet light) or ultrasonic stimulation, but can be rapidly ignited and produce a lasting afterglow upon brief exposure to plasma. Plasma, as a universal and unique non-invasive stimulation source, has a broad excitation spectrum and is applicable to a wide variety of materials. It can effectively activate inert materials that cannot be excited by traditional excitation sources (such as ultraviolet light and ultrasound), producing a strong and lasting afterglow. Therefore, the application of plasma as an afterglow excitation source proposed in this invention not only provides an innovative tool for the regulation of luminescence dynamics but also expands the range of materials capable of exhibiting afterglow characteristics. It opens new avenues for the development of novel biocompatible afterglow probes, secure anti-counterfeiting labels, drug tracing, and imaging technologies, significantly expanding the research frontier of afterglow materials and demonstrating strong competitiveness and broad application prospects in the field of biomedical optical imaging.

[0043] This invention relates to the application of plasma as an afterglow excitation source in the generation of afterglow in excitation materials. Specifically, it includes: controlling plasma contact with a material (or a target excitation material), thereby exciting the material to generate afterglow. After the material is excited by plasma, the excitation operation can be terminated, and the excited material can still generate continuous afterglow. Furthermore, plasmas excited from different gas sources can be used as different excitation sources, and the processing time of plasma contact with the target excitation material can be controlled to excite afterglow of different intensities. This allows for "on-demand" excitation of the afterglow signal, achieving precise excitation control and improving the flexibility of afterglow material excitation and application.

[0044] In some embodiments of the present invention, plasma is used as an afterglow excitation source to excite materials to generate afterglow in afterglow imaging. That is, plasma can be used as an afterglow excitation source for afterglow imaging. The afterglow imaging process typically has a "spatiotemporal decoupling" characteristic, where the excitation process and signal acquisition are separated in time. Signal acquisition is performed after excitation, which can effectively avoid the use of real-time light sources, eliminate interference from scattering and autofluorescence of biological tissues, significantly reduce background noise, and improve the signal-to-noise ratio (SBR), making it particularly suitable for high-contrast imaging of deep tissues.

[0045] Of course, in other embodiments, plasma can also be used as an afterglow excitation source to excite materials in other fields to generate afterglow. That is, plasma can be used as an afterglow excitation source in any field that involves and can achieve afterglow excitation.

[0046] In another aspect, the present invention proposes an afterglow excitation method, which includes the following steps: providing plasma, controlling the plasma to contact a target excitation material, and the plasma exciting the target excitation material to generate afterglow.

[0047] In some embodiments, plasma supply is stopped after the target excitation material is excited by plasma. The excited target excitation material continues to produce a persistent afterglow after the excitation operation ends.

[0048] Similar to the above application of plasma as an afterglow excitation source in the generation of afterglow in excitation materials, the present invention is not limited to the form of providing or generating plasma. For example, plasma can be provided through gas discharge (including but not limited to corona discharge, glow discharge, arc discharge, dielectric barrier discharge, radio frequency discharge, microwave discharge), thermal ionization (such as an arc plasma torch), etc.

[0049] The target excitation materials that can be excited by plasma to produce afterglow in the above afterglow excitation methods include some afterglow materials that can be excited by traditional excitation sources (light, ultrasound, ionizing radiation), such as 2,8-diethyl-5,5-difluoro-1,3,7,9-tetramethyl-10-phenyl-5H-4l4,5l4-dipyrrolo[1,2-c:2',1'-f][1,3,2]diazacyclohexaborane (CAS No.: 189264-25-3). It also includes some materials that cannot be excited by traditional excitation sources, including but not limited to some clinical and medical materials, fluorescent probe materials, and optoelectronic materials. Among them, some non-limiting examples of clinical pharmaceutical materials include 1-(4-amino-2-(ethoxymethyl)-1H-imidazo[4,5-c]quinolin-1-yl)-2-methylprop-2-ol and 9-methyl-3-((2-methyl-1H-imidazo-1-yl)methyl)-2,3-dihydro-1H-carbazole-4-(9H)-one; some non-limiting examples of fluorescent probe materials include 9-(2-(ethoxycarbonyl)phenyl)-3,6-di(ethylamino)-2,7-dimethylchlorooxanthracene and 7-diethylamino-4-methylcoumarin; and some non-limiting examples of optoelectronic materials include the non-fullerene acceptor ITIC and 4'-(4-carboxyphenyl)-2,2'-6'-2'-terpyridine. In addition, target excitation materials that can be excited by plasma to produce afterglow include, but are not limited to, (Z)-3-(((4-(N-methyl-2-(4-methylpiperazin-1-yl)acetamido)phenyl)amino)(phenyl)methylene)-2-oxoindoline-6-carboxylic acid methyl ester (i.e., nintedanib, CAS No.: 656247-17-5), 2,8-diethyl-5,5-difluoro-1,3,7,9-tetramethyl-10-phenyl-5H-4l4,5l4-dipyrrolo[1,2-c:2',1'-f][1,3,2]diazacyclohexaneborane (CAS No.: 189264-25-3), and indole (CAS No.: 120-72-9).

[0050] In another aspect, the present invention also proposes a afterglow imaging method, which includes any of the afterglow excitation methods described above. Specifically, the afterglow can be generated by exciting a target excitation material using the above afterglow excitation methods for imaging.

[0051] Furthermore, afterglow imaging methods typically include: acquiring the afterglow signal generated by the target excitation material and constructing an image. Specifically, this afterglow imaging method may include the following steps: providing plasma, controlling the plasma to contact the target excitation material, and the plasma exciting the target excitation material to generate afterglow; acquiring the afterglow signal generated by the target excitation material (i.e., the afterglow signal generated when the target excitation material is excited), and constructing an image.

[0052] In another aspect, the present invention proposes a persistence imaging system, see [link to relevant documentation]. Figure 1 In some embodiments, the afterglow imaging system includes an afterglow generating device 10 and an afterglow imaging device 20. The afterglow generating device 10 includes a sample carrying module 11 and an excitation source module 12; the sample carrying module 11 carries an imaging sample containing a target excitation material; the excitation source module 12 includes a plasma generator, which generates plasma to excite the target excitation material to produce afterglow. The afterglow imaging device 20 includes a signal acquisition module 21 and an imaging module 22; the signal acquisition module 21 acquires the afterglow signal generated by the target excitation material; the imaging module 22 is communicatively connected to the signal acquisition module 21 and receives the afterglow signal acquired by the signal acquisition module 21 to construct an image.

[0053] In some embodiments, the sample carrying module 11 in the afterglow generation device includes a sample holding unit, which may include, but is not limited to, sample containers of various sizes such as multi-well plates, culture dishes, glass slides, or live animal trays. In some embodiments, the sample carrying module 11 includes a support carrying unit configured to fix and position the imaging sample, which may include, but is not limited to, general-purpose or special-purpose clamps, supports, or platforms suitable for sample containers of various sizes such as multi-well plates, culture dishes, glass slides, or live animal trays. Of course, in some embodiments, the sample carrying module 11 may include both the sample holding unit and the support carrying unit.

[0054] In some embodiments, the sample carrying module 11 may integrate a temperature control unit (such as a cooling element) and / or a gas environment control unit (such as a gas mixing interface). The inclusion of the temperature control unit and the gas environment control unit helps maintain sample activity, effectively extends the observable time window, and avoids attenuation or anomalies in the afterglow signal due to sample inactivation, thereby ensuring the authenticity and reliability of the imaging data. Furthermore, in some embodiments, the sample carrying module 11 may also integrate a displacement mechanism (such as an XYZ three-dimensional translation stage) to sequentially move different samples or different regions of the same sample to the imaging field of view, thereby facilitating high-throughput and precise observation. Integrating multiple functions into one system enhances the system's integration and applicability, avoids the cumbersome and unstable nature of external equipment, and enables the system to flexibly handle afterglow imaging experiments of different scales and requirements, from in vitro cells to live animals, thus expanding its application range.

[0055] In some embodiments, the afterglow imaging system may also omit the sample carrying module 11.

[0056] In the afterglow generator, the excitation source module 12 includes a plasma generator for generating plasma. The specific implementation of the plasma generator may include, but is not limited to, a dielectric barrier discharge device, an atmospheric pressure plasma jet device, a capacitively coupled plasma device, and an inductively coupled plasma device.

[0057] In this embodiment, the excitation source module 12 is a plasma generator, which includes a power supply 121, an electrode structure (not shown in the figure), and a plasma excitation unit 122. The output terminal of the power supply 121 is electrically connected to the electrode structure to provide electrical energy to the electrode structure. The electrode structure is configured to form an ionization electric field therebetween after the power supply 121 powers it. The plasma excitation unit 122 penetrates the ionization region of the electrode structure to guide the working gas through the ionization electric field and generate plasma. Further, the electrode structure is configured to generate a uniformly distributed ionization electric field after being powered on. The electrode structure may include, but is not limited to, needle-needle electrodes, needle-ring electrodes, ring-ring electrodes, needle-plate electrodes, etc.

[0058] The above-mentioned plasma generating device can ionize the working gas to generate plasma rich in high-energy electrons, active particles and other active components. The working gas may include, but is not limited to, helium, argon, air and their mixtures.

[0059] In some embodiments, the excitation source module 12 further includes a gas supply device connected to the plasma generator for supplying the plasma generator with the gas (i.e., working gas) required to generate plasma. Specifically, the outlet of the gas supply device is connected to the plasma excitation unit 122 of the plasma generator for supplying working gas to the plasma excitation unit 122 of the plasma generator.

[0060] In some embodiments, the gas supply device includes only one gas path connected to the plasma generator, specifically the plasma excitation unit 122 in the plasma generator.

[0061] In some embodiments, the gas supply device may be a multi-channel gas supply device, comprising at least two independent gas paths, each directly or indirectly connected to the plasma generator, and each gas path is equipped with a flow control unit. Specifically, in some embodiments, each gas path in the multi-channel gas supply device may be directly connected to the plasma generator; while in other embodiments, each gas path in the multi-channel gas supply device is connected to the plasma generator through a gas collecting component, and during use, the gas entering each path is collected by the gas collecting component before being delivered to the plasma generator.

[0062] The above-mentioned multi-channel gas supply device is used to deliver and precisely mix different types or proportions of working gases to the plasma generator, achieving adjustable gas supply. Specifically, by switching or mixing gases from different channels, the chemically active components and optical properties of the generated plasma can be dynamically controlled. These plasmas from different gas sources can constitute a series of selectable and tunable afterglow excitation sources, making the excitation source diverse. Users can select the appropriate gas excitation source according to the optimal response band of the target sample to optimize the excitation efficiency.

[0063] In the afterglow imaging device 20, the signal acquisition module 21 is used to acquire the afterglow (or afterglow signal) generated by the target excitation material. The signal acquisition module 21 may include an optical collection component 211, such as a charge-coupled device (CCD) camera, which can collect the afterglow. In some embodiments, the signal acquisition module 21 can be designed to be time-linked with the excitation source module 12 to acquire the afterglow signal without background interference after the excitation source module 12 has completed the excitation operation. After acquiring the afterglow signal of the target excitation material, the signal acquisition module 21 transmits the acquired afterglow signal to the imaging module 22 for image construction. The image construction process of the imaging module 22 generally includes data processing and image generation.

[0064] For the convenience of system control, in some embodiments, the afterglow imaging system further includes a central control module, which is communicatively connected to the excitation source module 12 and is at least used to regulate the excitation time of the excitation source module 12; for example, the central control module can be used to control the switch and operation duration of the plasma generating device. In this way, programmable excitation of the afterglow intensity can be achieved. Specifically, by controlling the processing time of the plasma on the target excitation material, different doses of excitation energy can be accurately "injected", so as to effectively regulate the afterglow luminescence intensity in the target excitation material. For example, the central control module can be used to control the excitation source module to process the target excitation material for a short time to generate a weak afterglow, which is suitable for high-sensitivity detection; while controlling the excitation source module to process the target excitation material for a long time to generate a strong afterglow through the central control module is suitable for imaging of signals with weak intensity or deep tissues.

[0065] In some embodiments, the central control module can also be communicatively connected to the gas supply device and is at least used to regulate the gas supply of the gas supply device to the plasma generating device. For example, in some embodiments, the central control module can be communicatively connected to the flow control units on each gas path of the gas supply device to control the gas flow of each gas path.

[0066] In some embodiments, the central control module can also be communicatively connected to the sample carrier module 11, specifically communicatively connected to the temperature control unit, gas environment control unit and displacement mechanism integrated on the sample carrier module 11. In addition, the central control module can also be communicatively connected to the signal acquisition module 21 to control the parameter settings of the signal acquisition module to control signal acquisition.

[0067] In some embodiments, the central control module and the imaging module 22 can also be integrated into the central host. Among them, the central control module can be configured as the command center of the system to achieve high-precision timing coordination of the excitation, acquisition and processing imaging processes. Specifically, the central control module is communicatively connected to other modules for the linkage control of each module to coordinate the orderly operation of each module. In the specific working process, the central control module can first send an excitation instruction to the excitation source module 12, and the plasma generating device in the excitation source module 12 generates plasma to excite the target excitation material. After the preset excitation period ends, the central control module sends a collection trigger signal to the signal acquisition module 21 to ensure that a pure afterglow signal rather than an excitation source interference signal is collected. The afterglow signal collected by the signal acquisition module 21 is transmitted to the imaging module 22, and the imaging module 22 receives the signal data transmitted by the signal acquisition module 21 and constructs an image.

[0068] The inventors conducted a large number of experiments during the research process and verified that the plasma can be used as an afterglow excitation source to excite materials to generate afterglow. For a clear description of the present invention, some experiments and effects are listed as follows: The inventors selected two representative materials from each of the three major categories of materials: fluorescent probes, optoelectronic materials, and small chemical molecules for clinical medicine. After exciting each material, they studied its luminescence properties.

[0069] Specifically, in the clinical medicine materials category, two materials were selected: 1-(4-amino-2-(ethoxymethyl)-1H-imidazo[4,5-c]quinoline-1-yl)-2-methylprop-2-ol (denoted as A1) and 9-methyl-3-((2-methyl-1H-imidazo-1-yl)methyl)-2,3-dihydro-1H-carbazole-4-(9H)-one (denoted as A2); in the fluorescent probe materials category, two materials were selected: 9-(2-(ethoxycarbonyl)phenyl)-3,6-di(ethylamino)-2,7-dimethylchlorooxanthracene (denoted as B1) and 7-diethylamino-4-methylcoumarin (denoted as B2); and in the optoelectronic materials category, two materials were selected: the non-fullerene acceptor ITIC (denoted as C1) and 4'-(4-carboxyphenyl)-2,2'-6'-2'-terpyridine (denoted as C2).

[0070] The above materials were dissolved in dimethyl sulfoxide (DMSO) to increase their solubility, and then diluted with ultrapure water at a mass ratio of 1:9 to prepare 1% sample solutions for subsequent experiments. Three sample solutions were prepared for each material using the same method, and then all sample solutions were divided into three groups, each containing six different sample solutions.

[0071] The prepared sample solutions were observed under a bright-field imaging system, and the resulting bright-field images are shown below. Figure 2 As shown. Tests have shown that the sample solutions prepared from the selected materials cover systems ranging from transparent to various colors.

[0072] Three groups of sample solutions were subjected to excitation treatment using different excitation methods: Group 1: Each sample solution was stimulated with white light generated by a white LED for 10 minutes. Group 2: Using 1W / cm 3 Each sample solution was stimulated with ultrasound for 10 minutes. The third group: each sample solution was excited by an argon plasma jet. The working parameters were set as follows: voltage 8.5V, current 0.7A, gas flow rate 2.5 L / min, and excitation time 3min. During the processing, the state of the material samples was recorded in real time via video. Testing revealed that the first and second groups of sample solutions showed no change under white light and ultrasonic stimulation, respectively; however, some sample solutions in the third group were excited and emitted light under plasma stimulation, exhibiting different colors, specifically as follows... Figure 3 As shown.

[0073] After undergoing the above excitation treatment, the sample solutions from each group were subjected to afterglow imaging using an imaging system comprising a signal acquisition module and an imaging module. The signal acquisition module includes an imaging cassette and an optical collection component. The imaging cassette is from an IVIS Lumina XR imaging system, and the optical collection component is a cooled charge-coupled device (CCD) from an IVIS Lumina XR imaging system (Caliper, USA). The optical collection component is housed within the imaging cassette and is used to collect the afterglow signal of the sample. The imaging module is communicatively connected to the optical collection component in the signal acquisition module to receive the afterglow signal collected by the optical collection component and construct an image. The afterglow imaging of the sample solutions from each group using this imaging system yielded the following results: Figure 4 As shown, Figure 4 (a) is the image of the first group of sample solutions after being stimulated by white light; (b) is the image of the second group of sample solutions after being stimulated by ultrasound; (c) is the afterglow emission image of the third group of sample solutions after being excited by plasma.

[0074] according to Figure 4 Tests showed that neither white light stimulation nor ultrasound stimulation could excite the above-mentioned fluorescent probes, optoelectronic materials, and small chemical molecule clinical pharmaceutical materials. However, plasma could excite the sample solutions to produce significant afterglow. This indicates that plasma can excite some materials that remain completely inert under light or ultrasound to produce strong afterglow. Thus, plasma provides a new platform for activating and studying persistent luminescent materials, thereby greatly expanding the range of materials that can exhibit afterglow characteristics, and opening up new avenues for the development of anti-counterfeiting, bioimaging, and intelligent sensing.

[0075] The above-described embodiments are merely illustrative of several implementations of the present invention, and while the descriptions are relatively specific and detailed, they should not be construed as limiting the scope of the present invention. It should be noted that those skilled in the art can make various modifications and improvements without departing from the concept of the present invention, and these modifications and improvements all fall within the scope of protection of the present invention.

Claims

1. Application of plasma as an afterglow excitation source in the generation of afterglow in excitation materials.

2. The application according to claim 1, characterized in that, The material includes at least one of the following: clinical medical materials that can be excited by plasma to produce afterglow; fluorescent probe materials that can be excited by plasma to produce afterglow; and optoelectronic materials that can be excited by plasma to produce afterglow.

3. The application according to claim 2, characterized in that, The clinical and pharmaceutical materials that can be excited by plasma to produce afterglow include at least one of 1-(4-amino-2-(ethoxymethyl)-1H-imidazo[4,5-c]quinolin-1-yl)-2-methylprop-2-ol and 9-methyl-3-((2-methyl-1H-imidazo-1-yl)methyl)-2,3-dihydro-1H-carbazole-4-(9H)-one; the fluorescent probe materials that can be excited by plasma to produce afterglow include at least one of 9-(2-(ethoxycarbonyl)phenyl)-3,6-di(ethylamino)-2,7-dimethylchlorooxanthracene and 7-diethylamino-4-methylcoumarin; the optoelectronic materials that can be excited by plasma to produce afterglow include at least one of the non-fullerene acceptor ITIC and 4'-(4-carboxyphenyl)-2,2'-6'-2'-terpyridine.

4. The application according to claim 1, characterized in that, The plasma includes at least one of non-thermal plasma and thermal plasma.

5. The application according to claim 4, characterized in that, The non-thermal plasma includes at least one of radio frequency glow discharge plasma, DC glow discharge plasma, microwave glow discharge plasma, capacitive coupling plasma, low-pressure glow discharge plasma, atmospheric pressure glow discharge plasma, corona discharge plasma, and dielectric barrier discharge plasma; the thermal plasma includes at least one of arc discharge plasma and inductively coupled plasma.

6. The application according to any one of claims 1 to 5, characterized in that, The application includes: controlling plasma to contact the material, wherein the plasma excites the material to produce afterglow.

7. The application according to claim 6, characterized in that, The excitation material generating afterglow includes exciting the material to generate afterglow in afterglow imaging.

8. A method for afterglow excitation, characterized in that, Includes the following steps: Plasma is provided, and the plasma is controlled to contact a target excitation material, thereby exciting the target excitation material to produce afterglow.

9. A method for afterglow imaging, characterized in that it includes the afterglow excitation method as described in claim 8.

10. The afterglow imaging method according to claim 9, characterized in that, Also includes: The afterglow signal generated by the target excitation material is collected to construct an image.

11. A persistence imaging system, characterized in that, include: An afterglow generation device includes an excitation source module, wherein the excitation source module includes a plasma generator, and the plasma generator is used to generate plasma to excite a target excitation material to generate afterglow. Afterglow imaging device, including signal acquisition module and imaging module; The signal acquisition module is used to acquire the afterglow signal generated by the target excitation material; the imaging module is communicatively connected to the signal acquisition module and is used to receive the afterglow signal acquired by the signal acquisition module and construct an image.

12. The afterglow imaging system according to claim 11, characterized in that, The afterglow generation device also includes a sample carrying module, which is used to carry an imaging sample containing the target excitation material.

13. The afterglow imaging system according to claim 11 or 12, characterized in that, It also includes a central control module, which is communicatively connected to the excitation source module and is used to control the excitation time of the excitation source module.

14. The afterglow imaging system according to claim 13, characterized in that, The excitation source module also includes a gas supply device, which is connected to the plasma generator and is used to supply the plasma generator with the gas required to generate plasma.

15. The afterglow imaging system according to claim 14, characterized in that, The central control module is also communicatively connected to the gas supply device, and is used at least to regulate the gas supply from the gas supply device to the plasma generator.

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