CN119153571B - Perovskite-like CsAg-based2I3Pin type ultraviolet photoelectric detector of polycrystalline film and preparation method thereof - Google Patents
Perovskite-like CsAg-based2I3Pin type ultraviolet photoelectric detector of polycrystalline film and preparation method thereof Download PDFInfo
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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Abstract
The invention discloses a pin type ultraviolet photoelectric detector based on perovskite-like CsAg 2I3 polycrystalline films and a preparation method thereof, and belongs to the technical field of novel polycrystalline film material preparation technology and photoelectric detectors. The detector uses CsAg 2I3 polycrystalline film as light absorption layer, and hole transmission layer and electron transmission layer are respectively prepared on two sides of light absorption layer to form pin junction. The invention adopts the lead-free perovskite CsAg 2I3 polycrystalline film as the main light absorbing layer, has intrinsic ultraviolet absorption and good stability, and the hole transmission layer and the electron transmission layer with wide forbidden band are matched with the CsAg 2I3 polycrystalline film energy band to form a pin junction, and the built-in electric field formed by the pin junction can separate photon-generated carriers under the condition of no bias voltage, so that the device can work in a self-driving mode. The invention has promotion effect on the further development of the non-lead perovskite ultraviolet photoelectric detector.
Description
Technical Field
The invention belongs to the technical field of new material preparation and photoelectric detectors, and particularly relates to a pin type ultraviolet photoelectric detector with perovskite CsAg 2I3 -like polycrystalline films as main light absorption layers and a preparation method thereof.
Background
With the continuous progress of science and technology, ultraviolet (UV) is becoming more and more popular in many fields such as integrated circuits, space observation, ultraviolet communication, environmental monitoring, water purification, and biomedical applications. In order to meet the use of ultraviolet rays in various scenes, the rapid development of ultraviolet detection technology is of great importance. Commercial silicon-based photodetectors have evolved rapidly over the past few decades, but because of the relatively narrow band gap width of silicon, silicon-based photodetectors have an optimal response in the visible and near infrared regions of the spectrum, and a lower sensitivity to the response in the ultraviolet band. Therefore, the filter is required to be added to reduce interference of visible light and infrared radiation on ultraviolet detection, so that the overall structure of the detector is complex and the price is high.
Perovskite has excellent photoelectric characteristics and adjustable band gap, so that the perovskite has wide prospects in the fields of Light Emitting Diodes (LEDs), solar cells, detectors and the like. Cesium lead chloride (CsPbCl 3) and methyl amine lead chloride (CH 3NH3PbCl3) have been used for ultraviolet detection, but traditional lead-based perovskite is toxic and potential hazards to the human body and environment do not follow the green and safe development route.
Disclosure of Invention
The invention aims to provide a pin type ultraviolet photoelectric detector based on perovskite-like CsAg 2I3 polycrystalline films and a preparation method thereof. The detector uses lead-free perovskite as a light absorption layer, and simultaneously, a hole transmission layer and an electron transmission layer are respectively prepared on two sides of the light absorption layer to form a pin junction. In order to facilitate the electrical connection with an external circuit, electrodes are also required to be respectively prepared at two sides of the hole transmission layer and the electron transmission layer, so that the complete pin type ultraviolet photoelectric detector is formed. Specifically, the invention is realized by adopting the following technical scheme:
The pin type ultraviolet photoelectric detector based on the perovskite-like CsAg 2I3 polycrystalline film comprises a GaN substrate, a light absorbing layer and a hole transmission layer, wherein the GaN substrate comprises a GaN layer and a sapphire layer (Al 2O3), the GaN layer is used as an electron transmission layer, the sapphire layer is used as a basal layer, the GaN layer and the hole transmission layer are respectively connected with an electrode, the light absorbing layer is a lead-free perovskite-like material, a cesium silver iodine (CsAg 2I3) polycrystalline film is preferably used as the light absorbing layer, the GaN electron transmission layer is an n type semiconductor and is matched with the energy band structure of a light absorbing layer material, the hole transmission layer is cuprous salt and comprises at least one of cuprous iodide (CuI), cuprous bromide (CuBr) and cuprous thiocyanate (CuSCN), and the hole transmission layer is preferably 30-100 nm. The hole transport layer is a p-type semiconductor and is matched with the energy band structure of the light absorption layer material. The GaN substrate of the invention can directly adopt GaN of a commercial GaN substrate, namely a sapphire substrate.
The electrode comprises a first electrode and a second electrode, wherein the first electrode is in contact connection with the hole transmission layer, and the second electrode is in contact connection with the electron transmission layer. The electrode is stable In property and good In conductivity, ohmic contact is required to be formed between the electrode I and the contact material, specifically, a high work function material such as gold (Au), nickel (Ni), carbon (C) and the like is required to be used for contact between the electrode II and the electron transport layer, and a low work function material such as indium (In), gallium (Ga), indium-gallium alloy (InGa) and the like is required to be used for contact between the electrode II and the electron transport layer;
The invention also provides a preparation method of the pin type ultraviolet photoelectric detector based on the perovskite-like CsAg 2I3 polycrystalline film, which comprises the steps of preparing an electron transport layer or a substrate, preparing a light absorption layer, preparing a hole transport layer and preparing an electrode.
Preferably, the preparation of the electron transport layer or the substrate comprises the steps of GaN substrate cleaning, electrode position reservation and hydrophilic treatment.
Preferably, the preparation of the light absorbing layer comprises CsAg 2I3 preparation of a precursor solution, spin coating and step annealing. The concentration of the CsAg 2I3 precursor solution is preferably 0.8 to 2mol/L, particularly preferably 0.8 to 1.2 mol/L.
Preferably, the hole transport layer is prepared by vacuum evaporation deposition of cuprous salt by using thermal evaporation.
Preferably, the preparation of the electrode comprises the steps of depositing an electrode I with the thickness of 60-100 nm on a hole transport layer by using a thermal evaporation mode and preparing an electrode II on a reserved area of the electrode on a GaN substrate by using a thermal evaporation or knife coating mode.
Thirdly, the photoelectric detector can be applied to ultraviolet light detection. I-V characteristics show that the pin type ultraviolet photoelectric detector based on perovskite has obvious rectification characteristics, which indicates the formation of pin junctions, so that the device can work in a self-driving mode. Because the built-in electric field formed by the pin junction reduces electron-hole recombination, the device has dark current as low as 10 -11 A level, is very beneficial to weak light detection, and meanwhile, the detector performs 1500 times of cyclic tests, the dark current is almost unchanged, and the photocurrent only decays by 3%, so that good stability is shown.
Compared with the prior art, the invention has the beneficial effects that:
the CsAg 2I3 polycrystalline film does not contain lead, and belongs to a nontoxic green material;
Csag 2I3 polycrystalline films have a relatively wide direct band gap (E g =3.4 eV) and thus an intrinsic uv response;
the CsAg 2I3 polycrystalline film is used as an all-inorganic material and has good stability;
4. The wide forbidden band hole transport layer and the electron transport layer are matched with CsAg 2I3 polycrystal film energy bands to form a pin junction, so that the device can work without external power supply.
Drawings
Fig. 1 is a device structure diagram of a pin-type ultraviolet photodetector based on perovskite-like.
Fig. 2 is an energy band diagram of a perovskite-like based pin-type ultraviolet photodetector.
FIG. 3 is an electron micrograph of CsAg 2I3 polycrystalline thin films prepared in example 1.
FIG. 4 is an I-V characteristic curve of the pin type ultraviolet photodetector prepared in example 1.
FIG. 5 is an I-T characteristic curve of the pin type ultraviolet photodetector prepared in example 1.
Fig. 6 is a cycle stability test curve of the pin type uv photodetector prepared in example 1.
FIG. 7 is an electron micrograph of the CsAg 2I3 polycrystalline film prepared in example 2.
FIG. 8 is an I-V characteristic curve of the pin type ultraviolet photodetector prepared in example 2.
FIG. 9 is an I-T characteristic curve of the pin type ultraviolet photodetector prepared in example 2.
FIG. 10 is an I-V characteristic curve of the pin type ultraviolet photodetector prepared in example 3.
FIG. 11 is an I-T characteristic curve of the pin type ultraviolet photodetector prepared in example 3.
Detailed Description
The pin type ultraviolet photoelectric detector based on perovskite-like material comprises the following steps:
Preparation of gan substrate:
(1) Cleaning, namely sequentially using deionized water, acetone and absolute ethyl alcohol to ultrasonically clean a substrate, and then using nitrogen to blow-dry;
(2) Reserving an electrode position, namely reserving a position of an electrode II on one side of the GaN substrate;
(3) Hydrophilic treatment, namely placing the substrate into an ultraviolet ozone box for treatment for 10-15 min to make the surface hydrophilic;
Preparation of csag 2I3 polycrystalline thin film:
(1) Preparing a precursor solution, namely dissolving CsI and AgI in DMF according to a molar ratio of 1:2, putting the mixture on a mixing instrument to completely dissolve the mixture, and filtering the mixture by using a needle filter with the diameter of 0.22 mu m before using the mixture to obtain a clarified precursor solution;
(2) Spin coating, namely placing the substrate on a spin coater, and dripping CsAg 2I3 solution with the concentration of 40-60 mu L, wherein the spin coating speed is 2000-2500 rpm, and the duration time is 40-60 s;
(3) Step annealing, namely transferring the substrate to a 50-80 ℃ hot stage for annealing for 30min after spin coating, and then raising the temperature of the hot stage to 80-110 ℃ for annealing for 30 min.
3. Preparation of hole transport layer:
Preparing a hole transport layer by using a thermal evaporation mode, placing the substrate obtained in the last step into a vacuum cavity, placing a medicine (purity is more than 99.999%) on a tungsten boat, starting evaporation after the vacuum degree is superior to 1X 10 -4 Pa, depositing 5nm by using an evaporation speed of 0.1A/s, and then depositing 30-100 nm by using a speed of 0.5-0.8A/s.
4. Preparation of an electrode:
(1) The first electrode is prepared by adopting a thermal evaporation mode, fixing an electrode mask plate on the substrate obtained in the last step, then placing the substrate into a vacuum cavity, placing electrode metal particles (purity is more than 99.99%) on a tungsten boat, starting evaporation after the vacuum degree is superior to 1X 10 -4 Pa, firstly depositing 5nm at an evaporation speed of 0.1A/s, and then depositing 60-100 nm at a speed of 0.5-0.8A/s.
(2) The preparation of the electrode II comprises the steps of preparing In and Ga by using a thermal evaporation mode, wherein the specific steps are the same as those of the electrode I, and the preparation of the electrode I comprises the steps of dipping InGaon a hot plate, uniformly scraping the dipped InGaon the hot plate by using a plastic rod, and coating the dipped InGaon a reserved position on a GaN substrate, wherein the reserved position is not connected with other parts of the device.
5. And testing the performance of the device.
To illustrate the performance of the perovskite detector of the present invention, we have used a photodetector test system to perform electrical performance testing on devices, consisting essentially of the following test items:
(1) I-V characteristic, namely placing a sample on a probe platform, applying scanning voltage to a left electrode and a right electrode, obtaining I-V characteristic under dark state under dark condition, and continuously irradiating the sample by using 365 nm light source to obtain I-V characteristic curve under illumination;
(2) I-T characteristic, namely placing a sample on a probe station, applying no bias voltage, and irradiating the sample with a 365 nm light source at a fixed period to obtain an I-T characteristic curve;
(3) The circuit connection is tested with I-T characteristics, the light source frequency is 1Hz, and the test is continuously carried out for more than 1000 cycles until the waveform is obviously attenuated.
The invention is further described in connection with the following examples and comparative examples, which are intended to be illustrative of the invention rather than limiting. The invention is not limited to the specific examples and embodiments described herein. Further modifications and improvements may readily occur to those skilled in the art without departing from the spirit and scope of the invention.
Example 1
Preparing a GaN substrate, namely processing the GaN substrate by using the process;
Preparation of CsAg 2I3 polycrystalline film 1mol/L CsAg 2I3 precursor solution is prepared by the process to prepare CsAg 2I3 film, 50 mu L CsAg 2I3 solution is dripped during spin coating, 40s is continuously carried out at a speed of 2500 rpm, a step annealing mode is 70 ℃ annealing 30min, and then 100 ℃ annealing 30 min. Characterization of the prepared CsAg 2I3 polycrystalline thin film using electron microscopy, as shown in fig. 3;
3. preparing a hole transport layer, namely preparing a CuI film with the thickness of 100 nm a by using the process;
4. the preparation of the electrode comprises the steps of preparing the electrode I by using Au, preparing the electrode II by using InGa, and preparing the electrode by using the process;
5. device performance test the I-V characteristics, I-T characteristics and cycling stability of the samples were tested using the test methods described above, see FIGS. 4, 5, and 6, respectively.
As shown in fig. 4, the I-V characteristic shows a remarkable rectifying characteristic, indicating the formation of the pin junction. Since the built-in electric field formed by the pin junction reduces electron-hole recombination, the device has dark current as low as 10 -11 A, which is very beneficial to weak light detection. The I-T characteristics shown in fig. 5 demonstrate good device performance in self-driven mode. The detector in fig. 6 performs 1500 cycles of testing, the dark current is almost unchanged, and the photocurrent only decays by 3%, thus showing good stability.
Example 2
Preparation of GaN substrate the same as in example 1;
Preparation of csag 2I3 polycrystalline thin film 0.3 mol/L of CsAg 2I3 precursor solution was prepared for CsAg 2I3 polycrystalline thin film using the above process, and the spin coating was continued at 2000 rpm for 40 s, with the remainder being the same as in example 1. Characterization of the CsAg 2I3 films prepared using electron microscopy was performed as shown in figure 7;
3. preparation of hole transport layer the same as in example 1;
4. the electrode was prepared as in example 1;
5. device performance test the I-V and I-T characteristics of the samples were tested as shown in fig. 8 and 9.
As shown in FIG. 7, the film at 0.3 mol/L was discontinuous and had a large number of voids. This is due to insufficient solute in the solution, rapid solvent evaporation in high speed rotation, large amounts of solute nucleation but insufficient solute to support continued crystal growth, thus forming a discontinuous film. CsAg 2I3 the polycrystalline film acts as an intermediate layer of the pin structure, and the discontinuous film allows the electron transport layer to be in direct contact with the hole transport layer, which results in a large leakage current. As shown in fig. 8, the dark current is only 10 -10 a, which indicates that the continuous and dense CsAg 2I3 polycrystalline film can well reduce the dark current of the device, increase the on-off ratio, and thus improve the dark light detection capability of the device.
Example 3
Preparation of GaN substrate the same as in example 1;
Preparation of CsAg 2I3 polycrystalline film, namely changing the step annealing mode in the embodiment 1 into 50 ℃ annealing 30 min and 80 ℃ annealing 30 min, and the rest is the same as the embodiment 1;
3. preparation of hole transport layer the same as in example 1;
4. the electrode was prepared as in example 1;
5. device performance test the I-V and I-T characteristics of the samples were tested as shown in fig. 10 and 11.
The invention adopts the lead-free perovskite CsAg 2I3 polycrystalline film as the main light absorbing layer, has intrinsic ultraviolet absorption and good stability, and the hole transmission layer and the electron transmission layer with wide forbidden band are matched with the CsAg 2I3 polycrystalline film energy band to form a pin junction, and the built-in electric field formed by the pin junction can separate photon-generated carriers under the condition of no bias voltage, so that the device can work in a self-driving mode. The invention has great promotion effect on the further development of the non-lead perovskite ultraviolet photoelectric detector.
It should be noted that the above-mentioned embodiments of the present invention are merely explained and illustrated to enable those skilled in the art to obtain the technical spirit of the present invention, and the technical content is not to limit the scope of the present invention. The essential scope of the invention is as defined in the appended claims. Those skilled in the art should understand that any modification, equivalent substitution, improvement, etc. made based on the spirit of the present invention should fall within the spirit and scope of the present invention.
Claims (9)
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Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN111834487A (en) * | 2020-07-24 | 2020-10-27 | 西安电子科技大学 | All-inorganic perovskite nanowire self-powered-short-wave photodetector and preparation method |
Non-Patent Citations (1)
| Title |
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| High Detectivity and Stability Self-Powered UV Photodetector Based on the GaN/CsAg2I3 Microbelt Heterojunction;Wang, Xin, et.al;《 IEEE ELECTRON DEVICE LETTERS》;20240809;第45卷(第8期);全文 * |
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