CN109686844A - A kind of photosensitive sensor based on perovskite self-powered behavior - Google Patents
A kind of photosensitive sensor based on perovskite self-powered behavior Download PDFInfo
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- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
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- H—ELECTRICITY
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- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/10—Deposition of organic active material
- H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
- H10K71/125—Deposition of organic active material using liquid deposition, e.g. spin coating using electrolytic deposition e.g. in-situ electropolymerisation
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Abstract
The present invention relates to a kind of photosensitive sensors based on perovskite self-powered behavior, including successively layered distribution silicon dioxide layer, calcium titanium ore bed and metal electrode layer, silicon dioxide layer, calcium titanium ore bed and metal electrode layer are connected to forming circuit by external wire, silicon dioxide layer is for reducing dark current, ammeter is in series on external wire, when illumination is incident upon calcium titanium ore bed, circuit generates photoelectric current.The present invention is using silica to the barrier effect of carrier, so that being reduced under the conditions of dark-state to dark-state electric current, the excitation of perovskite light, generate carrier, it is compared due to its carrier generated and is substantially increased for dark-state, overcome the barrier effect of silicon dioxide layer, form photogenerated current in the loop, and detected by ammeter, thus judge the calcium titanium ore bed whether by illumination.Furthermore silicon dioxide layer can also provide current ratio bigger under illumination and under dark-state.
Description
[technical field]
The present invention relates to a kind of photosensitive sensors based on perovskite self-powered behavior, belong to sensor field.
[background technique]
In photovoltaic art, perovskite is as a kind of excellent monocrystal thin films material, so that the solar battery of its preparation
Present photoelectric conversion efficiency has been able to reach 23%, therefore perovskite is applied in other field by few people, such as benefit
With characteristics such as the dielectric constant of perovskite, current-voltage lag, used so that other perovskite devices are made.Because it is advanced by leaps and bounds
Photoelectric conversion efficiency and material source extremely abundant, ten big sciences in 2013 are chosen as by " Science " and one of are broken through.Together
When, which also has been used to the application study of optical detector, and this material has higher response from visible light to near-infrared.
Photodetector is a kind of novel Detection Techniques, is widely used in astronomy, environmental monitoring, defense military and leads to
The fields such as letter.Photodetector is mainly used for radionetric survey and detection, industry automatic control, light in visible light or near infrared band
Degree metering etc.；Infrared band be mainly used for missile guidance, infrared thermal imaging, in terms of optical detection used at present
Body product is larger, and operating voltage is high, and equipment is expensive.Inorganic semiconductor such as Si and GaN are most common photodetector (PD), especially
It is for ultraviolet light detection.GaN detector has superior performance under ultraviolet radioactive, but invalid to visible light.In addition, it
It is at high cost, quantum efficiency is low (< 40%, responsiveness < 0.2WA-1).In order to detect very weak light, some traditional PD
(including Si PD) needs low temperature to reduce dark current.Therefore, in order to detect superweak light, it is always necessary to which preamplifier, this can band
Carry out new noise source, and keeps system more expensive.Therefore, there is an urgent need to have wide light detection, high-quantum efficiency and highly sensitive now
The inexpensive PD spent without low-temperature operation.Photoelectron material (such as organic material, the nanometer material of low cost and solution-processible
Material and nanocomposite) its prospect as active layer is shown in large area PDs.However, their detection
The obstruction for further increasing the charge carrier mobility low by its of energy.Therefore which kind of material and technique is selected to prepare high-quality
The photodetector of amount becomes particularly important.Perovskite material is compared to organic material mobility with higher compared to inorganic
Material is had lower cost and can be detected with wide spectrum.Before these all make halide perovskite become one kind with development
The detector new material of scape.
[summary of the invention]
A kind of high sensitivity, structure are provided technical problem to be solved by the present invention lies in overcome the deficiencies in the prior art
Simply, the photosensitive sensor of wide spectrum response, low cost, low-power consumption, preparation easily based on perovskite self-powered behavior.
Above-mentioned technical problem is solved, the present invention adopts the following technical scheme:
A kind of photosensitive sensor based on perovskite self-powered behavior, including successively layered distribution silicon dioxide layer, calcium titanium
Ore bed and metal electrode layer, silicon dioxide layer, calcium titanium ore bed and metal electrode layer are connected to forming circuit by external wire, and two
Silicon oxide layer is in series with ammeter on external wire for reducing dark current, and when illumination is incident upon calcium titanium ore bed, circuit generates photoelectricity
Stream.
The invention has the benefit that using silica to the barrier effect of carrier, so that right under the conditions of dark-state
Dark-state electric current is reduced, and the excitation of perovskite light generates carrier, since the carrier that it is generated is very big compared to for dark-state
Ground increases, and overcomes the barrier effect of silicon dioxide layer, forms photogenerated current in the loop, and detected by ammeter,
Thus judge the calcium titanium ore bed whether by illumination.Furthermore silicon dioxide layer can also provide electric current bigger under illumination and under dark-state
Ratio；2, the wide scope spectrum from deep ultraviolet to near-infrared can be detected；3, responsiveness and detectivity with higher, have simultaneously
There are low dark current density and high external quantum efficiency；4, the panel detector structure is simple, high-efficient, response is fast, the operation is stable, makes
Long with the service life, production cost is low, the advantages that without expensive instrument and equipment.
The present invention does not include electron transfer layer and hole transmission layer.
Metal electrode layer of the present invention is Pt electrode.
Photosensitive sensor of the present invention based on perovskite self-powered behavior further includes aluminium electrode and silicon layer, aluminium electrode,
Silicon layer, silicon dioxide layer, calcium titanium ore bed and metal electrode layer successively layered distribution.
The present invention is in dark-state when calcium titanium ore bed, and dark current is less than 50pA, when illumination to calcium titanium ore bed, ammeter number
Value is 100-10000 times of dark current.
External power supply is in series on external wire of the present invention.
Electrode of metal layer is metal electrode layer.The present invention includes electrode, heavily doped silicon layer, dioxy under successively laminated metal
SiClx layer, calcium titanium ore bed and electrode of metal layer, lower metal electrode are connected to be formed by external wire with electrode of metal layer
Circuit, silicon dioxide layer are in series with ammeter on external wire, when illumination is incident upon calcium titanium ore bed, circuit for reducing dark current
Generate photoelectric current.
The present invention does not include electron transfer layer and hole transmission layer.
Lower metal electrode layer of the present invention is Al electrode, is also possible to Au, Ag, Ni, Ti, Pt, Pd, FTO, ITO electrode
One of or it is a variety of, with a thickness of 50-200nm, growing method is one of magnetron sputtering, vacuum evaporation.Its object is to
Above-mentioned electrode can form suitable conduction band and valence band gradient between heavily doped silicon layer, so that carrier is crossed under illumination condition
Silica reaches heavily doped silicon layer and is then collected by lower metal electrode layer.
Heavily doped silicon layer of the present invention primarily serves the effect of substrate supports, is also possible to other conductive substrates, such as weight
Adulterate GaN, SiC, Ga2O3, the conductive substrates such as ZnO.Above-mentioned material, will not be to illumination condition firstly the need of there is good electric conductivity
Under cross the carrier of silicon dioxide layer and generate excessive hinder.It, also will be to leaking through silicon dioxide layer simultaneously under the conditions of dark-state
Part carrier plays obstruction, to further decrease dark current.Reach to increase with this and compare between illumination electric current and dark-state electric current
The purpose of value.
Silicon dioxide layer of the present invention primarily serves the effect for reducing dark current, material SiO2、Al2O3、HfO2、
Zr2O5Or Y2O3, above-mentioned material have semi-insulating characteristic, the oxidated layer thickness be 30-300nm, growing method be thermal oxide,
One of hot spin coating, atomic layer deposition, Pulsed laser deposition, chemical vapor deposition.Furthermore SiO2、Al2O3、HfO2、Zr2O5、
Y2O3GaN, SiC, Ga can be cooperated2O3, ZnO form suitable energy level, meet the carrier under the conditions of above-mentioned illumination and dark-state and pass
Defeated process.
Calcium titanium ore bed of the present invention is light-sensitive layer, including CH3NH3PbI3、CH3NH3SnI3、CH3NH3PbCl3-xIx、
CsPbI3Deng, for perovskite with a thickness of 300-500nm, growing method is a step solwution method, in two step solwution methods, coevaporation method
It is a kind of.Self poling effect is different under the different types of illumination of perovskite, in order to guarantee to have enough illumination electric currents and dark-state electric current
Ratio.
Electrode of metal layer of the present invention is Pt electrode.
Photosensitive sensor of the present invention based on perovskite self-powered behavior successively includes aluminium electrode, silicon layer, titanium dioxide
Silicon layer, perovskite photosensitive layer and platinum electrode, aluminium electrode, silicon layer, silicon dioxide layer, calcium titanium ore bed and platinum electrode layer successively stratiform
Distribution.
The present invention is in dark-state when calcium titanium ore bed, and dark current is less than 50pA, when illumination to calcium titanium ore bed, ammeter numerical value
It is 100-10000 times of dark current.
There is no external power supply on external wire of the present invention, can work under the conditions of self-powered, it can also be with external electricity
Source works under the conditions of applying bias.
An embodiment provides a kind of preparation sides of photosensitive sensor based on perovskite self-powered behavior
Method, comprising:
(a) conductive substrates are chosen；
(b) in the substrate surface deposited oxide layer；
(c) electrode under substrate back deposit；
(d) in the oxidation layer surface spin coating calcium titanium ore bed；
(e) top electrode is formed in the calcium titanium ore bed surface deposition, to complete the preparation of the photosensitive sensor.
The present invention does not include electron transfer layer and hole transmission layer.
Lower metal electrode layer of the present invention is Al electrode.
Electrode of metal layer of the present invention is Pt electrode.
The other features and advantages of the invention will the detailed exposure in following specific embodiment, attached drawing.
[Detailed description of the invention]
Following further describes the present invention with reference to the drawings:
Fig. 1 is the embodiment of the present invention 1 in 5mW/cm2IV schemes under illumination condition and under the conditions of dark-state；
Fig. 2 is that the IV under different illumination intensity of the embodiment of the present invention 1 schemes；
Fig. 3 is the It curve when applied voltage is 0V of the embodiment of the present invention 1 and 2；
Fig. 4 is It curve under the conditions of different applied voltages of the embodiment of the present invention 1.
[specific embodiment]
The technical solution of the embodiment of the present invention is explained and illustrated below with reference to the attached drawing of the embodiment of the present invention, but under
It states embodiment to be merely a preferred embodiment of the present invention, and not all.Based on the implementation example in the implementation mode, those skilled in the art
Obtained other embodiments without making creative work, belong to protection scope of the present invention.
In the following description, occur term "inner", "outside", "upper", "lower", the indicating positions such as "left", "right" or
Positional relationship description embodiment merely for convenience and simplified description, rather than the device or element of indication or suggestion meaning must
There must be specific orientation, be constructed and operated in a specific orientation, therefore be not considered as limiting the invention.
Embodiment 1:
A kind of photosensitive sensor based on perovskite self-powered behavior is present embodiments provided, preparation process is as follows:
(a1) conductive silicon substrate is chosen；
(a2) conductive silicon substrate is cleaned using RCA standard cleaning technique.
(b) thermal oxidation technology is utilized, in the silica material that the conductive substrates surface heat oxide thickness is 100-500nm
Material.
(c1) magnetron sputtering technique is utilized, in the Al metal that conductive silicon substrate surface growth thickness is 50-200nm；
(c2) under the atmosphere of nitrogen and argon gas, using rapid thermal anneal process the conductive silicon substrate surface with it is described
The contact position metal Al forms Ohmic contact to complete the preparation of the lower electrode.
(d1) spin coating precursor solution: ethanol solution (methylamine mass fraction is 34%) and the 15ml hydrogen of 34ml methylamine is prepared
The aqueous solution (hydroiodic acid mass fraction is 57%) of acid iodide stirs at 0 DEG C, and water then is evaporated off in 60 DEG C of backspins, rotates out
CH3NH3I uses ether cleaning stirring drying.CH3NH3I、PbI2, DMSO, DMF with molar ratio 1:1:4:4 mixing,
(d2) it is spin-coated to silica surface under nitrogen atmosphere using spin-coating method: firstly, precursor solution is heated to
100 DEG C of crystallizations, anneal at 80 DEG C after cooling.Calcium titanium ore bed spin coating is with a thickness of 300-500nm.
(e1) magnetron sputtering technique is utilized, utilizes physical mask version splash-proofing sputtering metal Pt on the calcium titanium ore bed surface；
(e2) under the atmosphere of nitrogen and argon gas, using rapid thermal anneal process in the calcium titanium ore bed and the Pt metal
Ohmic contact is formed at material to complete the preparation of the top electrode.
(f) it is formed into a loop by being connected between platinum electrode and aluminium electrode by external wire, is in series on external wire
External power supply is scanned characterization.
Wherein Pt/CH3NH3PbI3/SiO2/ Si/Al forms MOS structure.Si piece is n-type doping, 500 microns of thickness, SiO2
With a thickness of 300nm.Platinum electrode and aluminium electrode area are 6.4 × 10-3cm2。
Embodiment 2:
The present embodiment the difference from embodiment 1 is that, Pt electrode replaces with Au electrode.
Referring to Fig. 1, in embodiment 1, it is arranged between 0- ± 10V in external scanning voltage, under the conditions of dark-state, dark current
In magnitude 10-12-10-10Between A, and in 5mW/cm2Electric current magnitude is 10 under illumination condition-9-10-7A, scanning voltage be ±
Near 3.8V or so, dark current 10-12A or so, and electric current is 10 under illumination-7A or so, therefore may determine that photoelectric current is remote
Greater than dark current, ratio is up to 10000 or so between photoelectric current and dark current, by illumination effect, therefore curent change is
MOS structure can detect illumination, and ignore the influence of dark current and noise current.It is simultaneously 0V in bias voltage
When, still there is decades of times difference between photoelectric current and dark current, has absolutely proved CH3NH3PbI3The generation of self-powered behavior.
Furthermore it is shown in Fig. 1, under the conditions of dark-state, electric current has a hysteresis, the lag with scanning voltage variation
Scanning voltage range between ± 3.8V, which is greater than the diode structure of electron transfer layer or hole transmission layer, former
Because being under no illumination condition, applied voltage enables to electron transfer layer or hole transmission layer that can uniformly accommodate ion,
And silica can and Pt electrode can greatly under dark-state ion transmission obstruct, under the conditions of dark-state, MOS
The built in field of structure makes carrier be limited in Pt/CH respectively3NH3PbI3The both sides of the edge of structure, and non-uniform Distribution,
So that it is different from diode structure.
Response rate R is the ratio under illumination between current density and intensity of illumination, and specific detectivity D and R is linearly positively correlated.Ginseng
See Fig. 2, in embodiment 1, scanning voltage is still arranged between ± 10V, respectively with 2mW/cm2、4mW/cm2、6mW/cm2、8mW/
cm2、10mW/cm2It carries out, even if in 2mW/cm2In the case of this low intensity light is shone, IV variation still shows approximately linear
Variation tendency, in the case where illustrating that intensity of illumination is constant, R is constant, therefore can be determined that MOS structure can be approximate as a kind of
Photoconductor carry out using.Furthermore it by calculating curve matching, is linearly positively correlated between intensity of illumination and R.Pass through IV song
The slope of line is scaled intensity of illumination, i.e. MOS structure not only has higher sensitivity to illumination, secondly can also to illumination into
Row quantitative measurment.Its reason is to dramatically increase with the promotion of applied voltage, photo-generated carrier, and can cross SiO2Resistance
Gear forms the photoelectric current for being much larger than dark current.When applied voltage is 0V, D=8.8 × 10 of the present embodiment10Jones。
Referring to Fig. 3, embodiment 1 and embodiment 2 are 0V in applied voltage and are in 5mW/cm2It is tested under illumination condition, no
By practical Au or Pt as electrode, circuit is periodically disconnected, electric current generates cyclically-varying at any time, illustrates perovskite
The generation of self-powered behavior, and generated to be lasting, and the response speed of photoelectric current remains relatively stable.In addition, different metal
Manufactured metal electrode layer has a significant effect to photoelectric current numerical value.
When wherein Pt is as metal electrode layer, electric current is 3.25nA under illumination, electric under illumination when Au is as metal electrode layer
Stream is 1.25nA.Ohmic contact is formed between Au and perovskite, and Pt is about the latter 2.5 as illumination electric current under electrode case
Times, illustrating to be formed between Pt and perovskite in embodiment 1 is Fei Xiaojite knot.
Furthermore also in 5mW/cm in embodiment2Respectively in 1V under light intensity, 2V and 5V applied voltage condition carries out MOS in advance
Ionic polarization 30s measures under dark current and illumination electric current without significant difference later, therefore MOS structure also eliminates ionic polarization
A possibility that.
Referring to fig. 4, in embodiment 1, in 5mW/cm2Under illumination condition, periodically switching switch, bias voltage be respectively ±
0.1V, ± 1V, and ± 5V, with the promotion of bias voltage, photoelectric current is gradually increased, and photoelectric current is synchronous with the ratio of dark current
Increase.But when applied voltage is ± 0.1V, the lifting speed of photoelectric current is still very gentle, illustrates in low applied voltage feelings
Carrier is difficult to cross SiO under condition2。
For this purpose, photoelectric current, which reaches, stablizes required time as 25.8ms, and photoelectric current when applied voltage is ± 0.1V
Extinction time only needs 620 μ s.Its reason is to need to complete Light polarizing and two steps of carrier transport under illumination condition.
In embodiment 1, due to conduction band offset (2.07eV) huge between perovskite and silica and valence band offset
(4.55eV), therefore it is generally acknowledged that CH3NH3PbI3/SiO2Interface be difficult to form hetero-junctions.Under the conditions of dark-state, perovskite
Interior uniform ion distribution, therefore the perovskite under dark-state regards intrinsic semiconductor.Corresponding dark-state electric current is noise current.Illumination
Under the conditions of, due to CH3NH3PbI3Self poling effect, negative ions shift to the two sides boundary of calcium titanium ore bed respectively, in calcium titanium
Built in field is formed in ore bed, flows to Pt electrode and Al electrode respectively under built-in electric field action later.Even if without outer power-up
In the case where pressure and electrons transport layer, observable photoinduction self-powered behavior can be also obtained, thus as one kind
Optical sensor uses.
Furthermore it is found through experiments that, CH3NH3SnI3、CH3NH3PbCl3-xIx、CsPbI3Shown when replacement with
CH3NH3PbI3Similar numerical value change trend and numberical range.But using such as CH3NH3BaCl3-xIxIn the case where, dark-state
Electric current is 50pA or so, but when bias is between ± 10V, 2mW/cm2Under light intensity, photoelectric current is only floating in 500pA-2000pA
It is dynamic, in other words there can not be enough ratio between photoelectric current and dark current so that MOS structure is used as optical sensor.
The above description is merely a specific embodiment, but scope of protection of the present invention is not limited thereto, is familiar with
The those skilled in the art should be understood that the present invention includes but is not limited to attached drawing and interior described in specific embodiment above
Hold.Any modification without departing from function and structure principle of the invention is intended to be included in the range of claims.
Claims (6)
1. a kind of photosensitive sensor based on perovskite self-powered behavior, it is characterised in that: including successively layered distribution titanium dioxide
Silicon layer, calcium titanium ore bed and metal electrode layer, silicon dioxide layer, calcium titanium ore bed and metal electrode layer are connected to shape by external wire
At circuit, silicon dioxide layer is in series with ammeter on external wire for reducing dark current, when illumination is incident upon calcium titanium ore bed, returns
Road generates photoelectric current.
2. the photosensitive sensor according to claim 1 based on perovskite self-powered behavior, it is characterised in that: do not include electricity
Sub- transport layer and hole transmission layer.
3. the photosensitive sensor according to claim 2 based on perovskite self-powered behavior, it is characterised in that: the metal
Electrode layer is Pt electrode.
4. the photosensitive sensor according to claim 3 based on perovskite self-powered behavior, it is characterised in that: described to be based on
The photosensitive sensor of perovskite self-powered behavior further includes aluminium electrode and silicon layer, aluminium electrode, silicon layer, silicon dioxide layer, perovskite
Layer and metal electrode layer successively layered distribution.
5. the photosensitive sensor according to claim 4 based on perovskite self-powered behavior, it is characterised in that: work as perovskite
Layer is in dark-state, and dark current is less than 50pA, and when illumination to calcium titanium ore bed, ammeter numerical value is the 100-10000 of dark current
Times.
6. the photosensitive sensor according to claim 5 based on perovskite self-powered behavior, it is characterised in that: described external
External power supply is in series on conducting wire.
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| CN112420929A (en) * | 2020-12-08 | 2021-02-26 | 湖南师范大学 | Perovskite solar cell with cesium-doped tin dioxide thin film as electron transport layer and preparation method thereof |
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| CN112420929A (en) * | 2020-12-08 | 2021-02-26 | 湖南师范大学 | Perovskite solar cell with cesium-doped tin dioxide thin film as electron transport layer and preparation method thereof |
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