A ternary logic photoelectric detector based on pyroelectric photoelectron effect heterojunction and a preparation method and application thereof

Abstract

A ternary logic photoelectric detector based on pyroelectric photoelectron effect heterojunction, a preparation method and application thereof belong to the technical field of optoelectronic devices. The structure of the photoelectric detector comprises a substrate, a heterojunction structure layer, a hole transport layer and an electrode. The heterojunction structure layer is composed of an ETL layer and a material with an asymmetric structure. The thickness of the material with the asymmetric structure is 490-510 nm, and the thickness of the ETL layer is 48-52 nm. The ETL layer is prepared on the FTO by a sol-gel method. The material of the ETL layer is one of -Ga2O3, -Ga2O3 or ZnO. The application realizes ternary logic operation based on double parameters (photocurrent and PPE enhancement factor) by constructing a quasi-two-dimensional perovskite / -Ga2O3 heterojunction and utilizing the interface potential barrier of the two to enhance the pyroelectric photoelectron effect (PPE), and breaks through the density-security trade-off problem of the binary system.

Description

Technical Field

[0001] This invention belongs to the field of optoelectronic device technology, specifically relating to a ternary logic photodetector based on a heterojunction of pyroelectric optoelectronic effect, its fabrication method, and its application. Background Technology

[0002] Traditional binary data transmission faces bottlenecks in terms of speed, capacity, and security. Logic circuits implemented using traditional photodetectors (PDs) often rely on a single parameter (such as current or voltage) output, making it difficult to achieve stable multi-logic states (such as ternary logic), thus limiting their application in encrypted communication and parallel information transmission.

[0003] With the surge in demand for big data transmission, the traditional von Neumann architecture has limitations in information processing efficiency. Ternary logic computation, by introducing a third logic state (0, 1, 2), can significantly improve information density and reduce system complexity. Currently, ternary logic implementations are mostly based on field-effect transistors (such as two-dimensional materials, quantum dots, and nanowire devices), but these are structurally complex and costly. Research on ternary logic based on photodiode-type photodetectors is relatively limited, mainly because they typically only output a single state parameter.

[0004] Existing ternary logic devices mostly rely on circuit-level design or complex material systems (such as inverted bipolar transistors and negative differential resistors), and lack solutions for directly implementing logic operations through optoelectronic devices. For example, the dimensional constraints of two-dimensional materials result in devices with high valley currents, requiring modifications to the device structure, leading to complex design and manufacturing processes, high fabrication difficulty, and low yield (Recent Advances on Multivalued Logic Gates: A Materials Perspective. Adv. Sci. 2021, 2004216); quantum dot-gated transistors require precise control of their size and spatial distribution, resulting in complex manufacturing processes (Recent Advances on Multivalued Logic Gates: A Materials Perspective. Adv. Sci. 2021, 2004216); piezoelectric-based photodiodes (PDs) only respond to mechanical stress, lacking flexibility (Progress and perspectives in 2D piezoelectric materials for piezotronics and piezo-phototronics, Adv. Sci. 2025, 2411422); while traditional perovskite PDs possess excellent photoelectric properties, they lack asymmetric structures, making it difficult to generate PPE (polyelectric properties) or resulting in a weak PPE effect, hindering practical applications (Advances in the application of perovskite). materials, Nano-Micro Lett. 2023, 177; Pyro-phototronic effect: an effective route toward self-powered photodetection, NanoEnergy, 2023, 108172).

[0005] Thermoluminescent photoelectronic effect (PPE) can be achieved using non-centrosymmetric materials (such as ZnO), but these materials suffer from interfacial energy level mismatch and poor compatibility with perovskites, and PPE enhancement is limited (Light-induced pyroelectric effect as an effective approach for ultrafast ultraviolet nanosensing. Nat. Commun. 2015, 8401). Jiang et al. previously regulated the photodetector response of the pyroluminescent photoelectronic effect in Ga2O3 through polar interface engineering (Tunable Pyro-Phototronic Effect by Polar Interface Engineering in Ga2O3. Adv. Funct. Mater. 2025, 2504294), but did not address ternary logic applications. Summary of the Invention

[0006] The problems to be solved by this invention are as follows: a single-parameter output PD cannot distinguish multiple logic states, which makes existing ternary logic devices often rely on complex circuit designs and difficult to integrate; energy level mismatch between traditional PPE materials and perovskite interfaces leads to low efficiency; and there is a lack of logic implementation schemes that can be coordinated and controlled by multiple parameters such as light, electricity and heat.

[0007] This invention constructs quasi-two-dimensional perovskite / -Ga2O3 heterojunction, by utilizing the interface barrier between the two to modulate the enhanced thermoluminescent photoelectron effect (PPE), realized ternary logic operation based on two parameters (photocurrent and PPE enhancement factor), and broke through the density-security trade-off problem of binary system.

[0008] To achieve the above objectives, the technical solution adopted by the present invention is as follows:

[0009] A ternary logic photodetector based on a pyroelectric optoelectronic effect heterojunction is disclosed. The photodetector structure includes a substrate / heterojunction structure layer / hole transport layer / electrode. The heterojunction structure layer is composed of an ETL layer and an asymmetric structure material. The thickness of the asymmetric structure material is 490~510 nm, and the thickness of the ETL layer is 48~52 nm.

[0010] Furthermore, the structure of the photodetector includes an FTO / ETL layer / quasi-two-dimensional perovskite (PVK) / Spiro-OMeTAD (HTL) / Ag (e.g.) Figure 1 (As shown).

[0011] Furthermore, the ETL layer is prepared on FTO using a sol-gel method.

[0012] Furthermore, the material of the ETL layer is -Ga2O3、 - One of Ga2O3 or ZnO.

[0013] Furthermore, the asymmetric material is a quasi-two-dimensional perovskite active layer, employing a Dion-Jacobson type (4-Py)MA2Pb3Br 10 (MA = methylamine), by introducing 4-methylpyridine bromide (4-PyBr2) with an asymmetric charge distribution to induce structural asymmetry, the PPE is enhanced. This invention protects the pyroelectric photoelectronic effect generated by materials with asymmetric structures. This effect allows photodetectors to output not only photocurrent but also the pyroelectric factor (PPE) parameter, thus differing from conventional photodetectors and enabling their use in ternary logic operations. In this invention, it refers to quasi-two-dimensional perovskite (PVK) with an asymmetric structure that produces a pyroelectric effect. Of course, other asymmetric materials can also be used, or a certain structure can be used to create an asymmetric property. The structure in this invention... -Ga2O3 / quasi-two-dimensional perovskite (PVK) further enhances the pyroelectric effect, and other materials can also be used to generate or enhance this effect. Therefore, the innovations of this invention are as follows: (1) Dual-parameter logic definition: combining photocurrent and PPE enhancement factor to achieve ternary state distinction; (2) Heterojunction structure: quasi-two-dimensional perovskite / -Ga2O3 interface design, enhanced PPE through band modulation; (3) Material selection: Dion-Jacobson type quasi-two-dimensional perovskite (4-Py)MA2Pb3Br 10 Its asymmetric structure induces polarization charges.

[0014] A method for fabricating the above-mentioned ternary logic photodetector based on a pyroelectric photoelectronic effect heterojunction, wherein the method comprises:

[0015] Step 1: There are three options:

[0016] Option 1: -Ga₂O₃ ETL Preparation: Dissolve Ga(NO₃)₃·6H₂O and LiOH in anhydrous ethanol to obtain a mixed solution. Stir in a water bath at 78-82℃ for at least 5 min. Add the same mass of Ga(NO₃)₃·6H₂O and LiOH to the mixed solution and stir for at least 5 min to obtain a gel-sol suspension. After standing for at least 1 day, spin-coat 40-60 μL of the supernatant onto an FTO substrate (1×1.5 cm) and anneal at 400-500℃ for 20-30 min to obtain... -Ga2O3 ETL layer;

[0017] Option 2: -Ga₂O₃ ETL Preparation: Dissolve Ga(NO₃)₃·6H₂O and LiOH in anhydrous ethanol to obtain a mixed solution. Stir in a water bath at 78-82℃ for at least 5 min. Add the same mass of Ga(NO₃)₃·6H₂O and LiOH to the mixed solution and stir for at least 5 min to obtain a gel-sol suspension. After standing for at least 1 day, spin-coat 40-60 μL of the supernatant onto an FTO substrate (1×1.5 cm) and anneal at 700-800℃ for 20-30 min to obtain... -Ga2O3 ETL layer;

[0018] Option 3: ZnO ETL preparation: Dissolve Zn(NO3)2·6H2O and LiOH in anhydrous ethanol to obtain a mixed solution. Stir in a water bath at 78~82℃ for at least 5 min. Add the same mass of Zn(NO3)2·6H2O and LiOH to the mixed solution and stir for at least 5 min to obtain a gel-sol suspension. After standing for at least 1 day, take 40~60 μL of the supernatant and spin-coat it onto an FTO substrate (1×1.5 cm). Anneal at 400~700℃ for 30~60 min to obtain a ZnO ETL layer. Adding the raw materials in two stages allows for more precise control of the reaction rate, thereby obtaining smaller, more uniform, and more stable precursor particles, which ultimately affects the gel structure and product performance.

[0019] Step 2: Preparation of Quasi-Two-Dimensional Perovskite Layer

[0020] Dissolve 4-PyABr2, MABr, and PbBr2 in a DMF / DMSO (4:1) mixed solvent to prepare a 0.2–0.4 mol / L solution (using Pb as the solvent). 2+ (Based on molar concentration), after stirring for more than 2 hours until completely dissolved, take 50 μL (1×1.5 cm FTO substrate) and spin-coat it onto the ETL layer at a speed of 4000~5000 rpm for 30~40 seconds. Add 250~300 μL of chlorobenzene solvent dropwise within 9~11 seconds before the end of spin-coating. Anneal at 80~85 ℃ for 8~12 min to form a dense (4-Py)MA2Pb3Br 10 Perovskite polycrystalline thin films; the addition of chlorobenzene will remove some of the good solvents (DMF and DMSO) and promote the crystallization of quasi-two-dimensional perovskite, making the resulting films more dense.

[0021] Step 3: Hole transport layer and electrodes

[0022] 72.3 mg of Spiro-OMeTAD was dissolved in 1 mL of chlorobenzene solvent and stirred at room temperature until completely dissolved. Then, 17.5 μL of lithium bis(trifluoromethane)sulfonamide (Li-TSFI, dissolved in acetonitrile solvent at a concentration of 520 mg / mL) and 28.8 μL of 4-tert-butylpyridine (TBP) were pipetted into the aforementioned solution to obtain a mixed solution mainly composed of Spiro-OMeTAD. Before use, the solution was stirred for 1–2 hours to ensure thorough mixing. This mixed solution (50 μL) was then spin-coated onto a perovskite layer at 4000–4500 rpm for 30–40 seconds, followed by a vacuum of 8 × 10⁻⁶. -4 Ag electrodes are deposited under Pa for 10-15 minutes.

[0023] Furthermore, in Scheme 1 and Scheme 2, the concentration of Ga(NO3)3·6H2O is 0.02~0.04 mol / L and the concentration of LiOH is 0.10~0.2 mol / L during the initial feeding; in Scheme 3, the concentration of Zn(NO3)2·6H2O is 0.02~0.04 mol / L and the concentration of LiOH is 0.10~0.2 mol / L during the initial feeding.

[0024] Further, in step two, the molar ratio of 4-PyABr2, MABr, and PbBr2 is one of 1:2:3, 1:1:2, or 1:3:4. Perovskite dimensional control: It is possible to try preparing (4-Py)MA by changing the molar ratio of 4-PyABr2, MABr, and PbBr2 in step two (1:2:3, 1:1:2, or 1:3:4). n-1 Pb n Br 3n+1 Quasi-two-dimensional perovskites (n=3, n=2 or n=4) with adjusted phase distribution.

[0025] An application of the above-mentioned ternary logic photodetector based on a pyroelectric photoelectroelectronic effect heterojunction, wherein the ternary logic calculation mechanism is as follows: through photocurrent (I photo ) and PPE enhancement factor (E = I pyro+photo / I photo Two-parameter definition of logic state: Logic 0: I photo > -3 μA and E > 2; Logic 1: I photo > -3 μA and E < 2; Logic 2: I photo <-3 μA. Logic protocol extension: The logic threshold can be dynamically adjusted based on input conditions such as modulation optical power and optical input frequency.

[0026] The advantages of this invention over the prior art are as follows:

[0027] (1) Strong process compatibility: prepared by solution method, compatible with flexible electronics technology.

[0028] (2) Self-powered characteristics: The device operates at 0 V bias and has low power consumption;

[0029] (3) Device structure: The structure is simple and does not require input or complex circuits;

[0030] (4) High-throughput transmission: Ternary logic supports multi-channel parallel information transmission, improving data density;

[0031] (5) High security: The two-parameter logic protocol can achieve encrypted communication, which interceptors cannot decrypt;

[0032] Through quasi-two-dimensional perovskite / - Interface engineering of Ga2O3 heterojunction enhances the PPE effect. By using the dual-parameter output of photocurrent and PPE enhancement factor to define ternary logic states, high-throughput, encrypted optical communication and parallel information transmission can be achieved. Attached Figure Description

[0033] Figure 1 This is a schematic diagram of the photodetector of the present invention;

[0034] Figure 2 State diagrams defining logic values ​​for quasi-two-dimensional perovskite PPE devices at different voltages;

[0035] Figure 3 State diagrams defining logic values ​​for quasi-two-dimensional perovskite PPE devices at different wavelengths. Detailed Implementation

[0036] The technical solution of the present invention will be further described below with reference to the accompanying drawings and embodiments, but it is not limited thereto. Any modifications or equivalent substitutions to the technical solution of the present invention that do not depart from the spirit and scope of the technical solution of the present invention should be covered within the protection scope of the present invention.

[0037] The innovations of this invention are as follows: (1) Dual-parameter logic definition: combining photocurrent and PPE enhancement factor to achieve ternary state distinction; (2) Heterojunction structure: quasi-two-dimensional perovskite / -Ga2O3 interface design, enhanced PPE through band modulation; (3) Material selection: Dion-Jacobson type quasi-two-dimensional perovskite (4-Py)MA2Pb3Br 10 Its asymmetric structure induces polarization charges.

[0038] Example 1:

[0039] 1. Weigh 1.275 g of Ga(NO3)3·6H2O and 0.29 g of LiOH, dissolve them in 100 mL of anhydrous ethanol, and stir in an 80°C water bath for 5 minutes. Add equal masses of Ga(NO3)3·6H2O and LiOH to the anhydrous ethanol mixture and continue stirring in an 80°C water bath for 5 minutes to prepare a gel-sol suspension.

[0040] 2. Take an FTO conductive substrate and cut it into 1×1.5 cm pieces. Take 50 μL of the supernatant from the gel-sol suspension that has been left to stand for one day and spin-coat it onto the cleaned FTO substrate at 3000 rpm for 30 seconds. After completing the above steps, anneal the spin-coated FTO at 450℃ for 20 minutes to obtain the desired result. -Ga2O3 ETL layer.

[0041] 3. Dissolve 4-PyABr2 (0.3 mmol), MABr (0.6 mmol), and PbBr2 (0.9 mmol) in a mixed solution of DMF / DMSO (4:1, 3 mL) and stir for 2 hours to obtain a quasi-two-dimensional perovskite precursor solution.

[0042] 4. Spin-coat the quasi-two-dimensional perovskite precursor solution (at a speed of 4000 rpm for 30 seconds) as described in step two. The Ga2O3 ETL layer was deposited on an FTO substrate. 250 μL of chlorobenzene solvent was added dropwise 10 seconds before the end of spin coating. After spin coating, the substrate was annealed at 80°C for 10 minutes. Following these steps, a layer of Ga2O3 ETL layer was successfully fabricated on the FTO substrate. -Ga2O3 ETL layer and quasi-two-dimensional perovskite (4-Py)MA2Pb3Br 10 Perovskite polycrystalline thin film layer.

[0043] 5. Take 72.3 mg of Spiro-OMeTAD and place it in 1 mL of chlorobenzene and stir to obtain a clear solution. Then add 17.5 μL of a solution containing Li-TSFI (130 mg of Li-TSFI dissolved in 250 μL of acetonitrile) and 28.8 μL of TBP to the solution and stir for 1 h to mix the solution thoroughly to obtain a mixed solution of the hole transport layer.

[0044] 6. Spin-coat the mixed solution from step five onto the FTO from step four (spin-coat at 4000 rpm for 30 seconds) to prepare the HTL layer.

[0045] 7. After completing the above six steps, at a vacuum degree of 8×10 -4 An Ag electrode was obtained by vapor deposition at Pa for 12 minutes. -Ga2O3 / quasi-two-dimensional perovskite photodetector.

[0046] 8. Current-time plots of the photodetector at 0 V, 0.3 V, and 0.5 V were obtained under monochromatic light irradiation at 400 nm. Figure 2 (Upper part) As can be seen from the figure, the device has a significant PPE effect, proving that a quasi-two-dimensional photodetector with thermoluminescent photoelectron effect has been successfully fabricated.

[0047] 9. Based on the current-time graph obtained in step 8, and using the formula E = I... pyro+photo / I photo Calculate the enhancement factor without voltage ( Figure 2 (Lower half). When I photo When I > -3 μA and E > 2, it is defined as a logic value of 0; when I photo When I > -3 μA and E < 2, the logic value is defined as 1; when I photo When the current is less than -3 μA, the logic value is defined as 2. At this point, the logic value of the ternary logic is determined, and the device achieves the capability for ternary logic computation.

[0048] Example 2:

[0049] 1. Weigh 1.275 g of Ga(NO3)3·6H2O and 0.29 g of LiOH, dissolve them in 100 mL of anhydrous ethanol, and stir in an 80°C water bath for 5 minutes. Add equal masses of Ga(NO3)3·6H2O and LiOH to the anhydrous ethanol mixture and continue stirring in an 80°C water bath for 5 minutes to prepare a gel-sol suspension.

[0050] 2. Take an FTO conductive substrate and cut it into 1×1.5 cm pieces. Take 50 μL of the supernatant from the gel-sol suspension that has been left to stand for one day and spin-coat it onto the cleaned FTO substrate at 3000 rpm for 30 seconds. After completing the above steps, anneal the spin-coated FTO at 700℃ for 20 minutes to obtain the desired result. -Ga2O3 ETL layer.

[0051] 3. Dissolve 4-PyABr2 (0.3 mmol), MABr (0.6 mmol), and PbBr2 (0.9 mmol) in a mixed solution of DMF / DMSO (4:1, 3 mL) and stir for 2 hours to obtain a quasi-two-dimensional perovskite precursor solution.

[0052] 4. Spin-coat the quasi-two-dimensional perovskite precursor solution (at a speed of 4000 rpm for 30 seconds) as described in step two. The Ga2O3 ETL layer was deposited on an FTO substrate. 250 μL of chlorobenzene solvent was added dropwise 10 seconds before the end of spin coating. After spin coating, the substrate was annealed at 80°C for 10 minutes. Following these steps, a layer of Ga2O3 ETL layer was successfully fabricated on the FTO substrate. -Ga2O3 ETL layer and quasi-two-dimensional perovskite (4-Py)MA2Pb3Br 10 Perovskite polycrystalline thin film layer.

[0053] 5. Take 72.3 mg of Spiro-OMeTAD and place it in 1 mL of chlorobenzene and stir to obtain a clear solution. Then add 17.5 μL of a solution containing Li-TSFI (130 mg of Li-TSFI dissolved in 250 μL of acetonitrile) and 28.8 μL of TBP to the solution and stir for 1 h to mix the solution thoroughly to obtain a mixed solution of the hole transport layer.

[0054] 6. Spin-coat the mixed solution from step five onto the FTO from step four (spin-coat at 4000 rpm for 30 seconds) to prepare the HTL layer.

[0055] 7. After completing the above six steps, at a vacuum degree of 8×10 -4 An Ag electrode was obtained by vapor deposition at Pa for 12 minutes. -Ga2O3 / quasi-two-dimensional perovskite photodetector.

[0056] 8. The testing section is the same as in Example 1.

[0057] Example 3:

[0058] 1. Weigh 1.041 g of Zn(NO3)2·6H2O and 0.29 g of LiOH, dissolve them in 100 mL of anhydrous ethanol, and stir in an 80°C water bath for 5 minutes. Add equal masses of Zn(NO3)3·6H2O and LiOH to the anhydrous ethanol mixture and continue stirring in an 80°C water bath for 5 minutes to prepare a gel-sol suspension.

[0059] 2. Take an FTO conductive substrate and cut it into 1×1.5 cm pieces. Take 50 μL of the supernatant from the gel-sol suspension that has been left to stand for one day and spin-coat it onto the cleaned FTO substrate at 3000 rpm for 30 seconds. After completing the above steps, anneal the spin-coated FTO at 700℃ for 30 minutes to obtain a ZnO ETL layer.

[0060] 3. Dissolve 4-PyABr2 (0.3 mmol), MABr (0.6 mmol), and PbBr2 (0.9 mmol) in a mixed solution of DMF / DMSO (4:1, 3 mL) and stir for 2 hours to obtain a quasi-two-dimensional perovskite precursor solution.

[0061] 4. Spin-coat the quasi-two-dimensional perovskite precursor solution (at 4000 rpm for 30 seconds) onto the FTO substrate with the ZnO ETL layer from step two. Add 250 μL of chlorobenzene solvent 10 seconds before the end of the spin-coating. After spin-coating, anneal at 80°C for 10 minutes. After completing the above steps, a ZnO ETL layer and a quasi-two-dimensional perovskite (4-Py)MA2Pb3Br layer have been successfully formed on the FTO substrate. 10 Perovskite polycrystalline thin film layer.

[0062] 5. Take 72.3 mg of Spiro-OMeTAD and place it in 1 mL of chlorobenzene and stir to obtain a clear solution. Then add 17.5 μL of a solution containing Li-TSFI (130 mg of Li-TSFI dissolved in 250 μL of acetonitrile) and 28.8 μL of TBP to the solution and stir for 1 h to mix the solution thoroughly to obtain a mixed solution of the hole transport layer.

[0063] 6. Spin-coat the mixed solution from step five onto the FTO from step four (spin-coat at 4000 rpm for 30 seconds) to prepare the HTL layer.

[0064] 7. After completing the above six steps, at a vacuum degree of 8×10 -4 Ag electrodes were obtained by vapor deposition at Pa for 12 minutes, resulting in a ZnO / quasi-two-dimensional perovskite photodetector.

[0065] 8. The testing section is the same as in Example 1.

Claims

1. A ternary logic photodetector based on a heterojunction of pyroelectric photoelectronic effect, characterized in that: The structure of the photodetector includes a substrate / heterojunction structure layer / hole transport layer / electrode, wherein the heterojunction structure layer is composed of an ETL layer and asymmetric structure materials.

2. A ternary logic photodetector based on a pyroelectric photoelectroelectronic effect heterojunction according to claim 1, characterized in that: The structure of the photodetector includes an FTO / ETL layer / quasi-two-dimensional perovskite (PVK) / Spiro-OMeTAD (HTL) / Ag.

3. A ternary logic photodetector based on a heterojunction of pyroelectric photoelectronic effect according to claim 2, characterized in that: The ETL layer was prepared on FTO using the sol-gel method.

4. A ternary logic photodetector based on a heterojunction of pyroelectric photoelectronic effect according to any one of claims 1 to 3, characterized in that: The material of the ETL layer is -Ga2O3、 - One of Ga2O3 or ZnO.

5. A ternary logic photodetector based on a heterojunction of pyroelectric photoelectronic effect according to claim 1 or 2, characterized in that: The asymmetric material is a quasi-two-dimensional perovskite active layer, employing a Dion-Jacobson type (4-Py)MA2Pb3Br. 10 (MA = methylamine), by introducing 4-methylpyridine bromide (4-PyBr2) with an asymmetric charge distribution to induce structural asymmetry, PPE is enhanced.

6. A method for fabricating a ternary logic photodetector based on a heterojunction of pyroelectric photoelectroelectronic effect as described in any one of claims 1 to 5, characterized in that: The method is as follows: Step 1: There are three options: Option 1: -Ga₂O₃ ETL Preparation: Dissolve Ga(NO₃)₃·6H₂O and LiOH in anhydrous ethanol to obtain a mixed solution. Stir in a water bath at 78-82℃ for at least 5 min. Add the same mass of Ga(NO₃)₃·6H₂O and LiOH to the mixed solution and stir for at least 5 min to obtain a gel-sol suspension. After standing for at least 1 day, spin-coat 40-60 μL of the supernatant onto an FTO substrate (1×1.5 cm) and anneal at 400-500℃ for 20-30 min to obtain... -Ga2O3 ETL layer; Option 2: -Ga₂O₃ ETL Preparation: Dissolve Ga(NO₃)₃·6H₂O and LiOH in anhydrous ethanol to obtain a mixed solution. Stir in a water bath at 78-82℃ for at least 5 min. Add the same mass of Ga(NO₃)₃·6H₂O and LiOH to the mixed solution and stir for at least 5 min to obtain a gel-sol suspension. After standing for at least 1 day, spin-coat 40-60 μL of the supernatant onto an FTO substrate (1×1.5 cm) and anneal at 700-800℃ for 20-30 min to obtain... -Ga2O3 ETL layer; Option 3: ZnO ETL preparation: Dissolve Zn(NO3)2·6H2O and LiOH in anhydrous ethanol to obtain a mixed solution. Stir in a water bath at 78~82℃ for at least 5 min. Add the same mass of Zn(NO3)2·6H2O and LiOH to the mixed solution and stir for at least 5 min to obtain a gel-sol suspension. After standing for at least 1 day, take 40~60 μL of the supernatant and spin-coat it onto an FTO substrate (1×1.5 cm). Anneal at 400~700℃ for 30~60 min to obtain a ZnO ETL layer. Step 2: Preparation of Quasi-Two-Dimensional Perovskite Layer Dissolve 4-PyABr2, MABr, and PbBr2 in a DMF / DMSO (4:1) mixed solvent to prepare a 0.2–0.4 mol / L solution (using Pb as the solvent). 2+ (Based on molar concentration), after stirring until completely dissolved, take 50 μL (1×1.5 cm FTO substrate) and spin-coat it onto the ETL layer at a speed of 4000~5000 rpm for 30~40 seconds. Add 250~300 μL of chlorobenzene solvent dropwise within 9~11 seconds before the end of spin-coating. Anneal at 80~85 ℃ for 8~12 min to generate MA2Pb3Br. 10 Perovskite polycrystalline thin films; Step 3: Hole transport layer and electrodes 72.3 mg of Spiro-OMeTAD was dissolved in 1 mL of chlorobenzene solvent and stirred at room temperature until completely dissolved. Then, 17.5 μL of lithium bis(trifluoromethane)sulfonamide (Li-TSFI, dissolved in acetonitrile solvent at a concentration of 520 mg / mL) and 28.8 μL of 4-tert-butylpyridine (TBP) were added to the aforementioned solution to obtain a mixed solution mainly composed of Spiro-OMeTAD. Before use, the solution was stirred for 1–2 hours to ensure thorough mixing. This mixed solution (50 μL) was then spin-coated onto a perovskite layer at 4000–4500 rpm for 30–40 seconds, followed by a vacuum of 8 × 10⁻⁶. -4 Ag electrodes are deposited under Pa for 10-15 minutes.

7. The preparation method according to claim 6, characterized in that: In Scheme 1 and Scheme 2, the initial concentration of Ga(NO3)3·6H2O is 0.02~0.04 mol / L and the concentration of LiOH is 0.10~0.2 mol / L; in Scheme 3, the initial concentration of Zn(NO3)2·6H2O is 0.02~0.04 mol / L and the concentration of LiOH is 0.10~0.2 mol / L.

8. The preparation method according to claim 6, characterized in that: In step two, the molar ratio of 4-PyABr2, MABr, and PbBr2 is one of 1:2:3, 1:1:2, or 1:3:

4.

9. An application of the ternary logic photodetector based on a heterojunction of pyroelectric photoelectroelectronic effect as described in any one of claims 1 to 5, characterized in that: The ternary logic calculation mechanism is implemented by: using photocurrent (I0) photo ) and PPE enhancement factor (E = I pyro+photo / I photo Two-parameter definition of logic state: Logic 0: I photo > -3 μA and E > 2; Logic 1: I photo >-3 μA and E < 2; Logic 2: I photo < -3 μA.

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