CN109830497A - A kind of list conductance layer ultraviolet photoelectron device - Google Patents
A kind of list conductance layer ultraviolet photoelectron device Download PDFInfo
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- CN109830497A CN109830497A CN201910020024.6A CN201910020024A CN109830497A CN 109830497 A CN109830497 A CN 109830497A CN 201910020024 A CN201910020024 A CN 201910020024A CN 109830497 A CN109830497 A CN 109830497A
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Abstract
The present invention provides a kind of single conductance layer ultraviolet photoelectron devices, comprising: single conductance layer, the potential barrier insulating layer being arranged on single conductance layer, the transparent electrode layer being arranged on potential barrier insulating layer and the metal electrode being electrically connected with single conductance layer of substrate, setting on substrate;There is the window for exposing single conductance layer on the potential barrier insulating layer, the metal electrode is electrically connected by the window with single conductance layer formation, the list conductance layer is the wide bandgap semiconductor layer of N-shaped or p-type doping, and the transparent electrode layer is the conductive, transparent two-dimensional material of nano wire or atom level thickness.Ultraviolet double-side may be implemented in above-mentioned opto-electronic device, and has good optical detection performance, helps to improve luminescent properties and optical detection performance, and the manufacture craft for reducing complexity reduces cost.
Description
Technical field
The present invention relates to a kind of single conductance layer ultraviolet photoelectron devices.
Background technique
Since Thomas Alva Edison et al. has invented osram lamp, the life style of the mankind has occurred earth-shaking
Variation." as the sun rises, resting together with sunset " is no longer a kind of life style.The invention of electroluminescent device is direct
Accelerate the development of technological progress and civilization.After that, scientists are constantly looked for more energy conservations and practical application
New light sources.1961, Robert Biard and Gary Pittman had found the infra-red radiation and second year Nick of GaAs
Holonyak has invented first visible light emitting diode.Recently, Nakamura Sh ū ji et al. has invented brightness blue light
LED simultaneously obtains Nobel Prize in physics.Light emitting diode (LED) is this can be by the development day of device of the light together with being electrically coupled
Beneficial mature, compared with conventional light source, LED has small in size, and luminous efficiency is ideal, and the service life is long, and switch time is fast, conducting voltage phase
To the advantages that lower, mercury environmental pollution is small;LED is applied not only to illuminate, and is also used for the optic communication even fields such as industry and medical treatment.One
As high-brightness LED manufacturing process it is considerably complicated, include more than ten a manufacturing steps, this need a large amount of time and raw material at
This.
Deep ultraviolet LED is still one of the goal in research field that scientist continues research in recent years, because they have extensively
General application value, including biomedicine, environmental protection and public health etc.;But compared to other LED, the system of deep ultraviolet LED
It makes in the presence of more challenges.This be primarily due to the ignorance to the powder injection molding of crystalline substrates and III-V nitride-based semiconductor with
And technical obstacle, these challenges not only increase the difficulty of manufacture, also add cost of manufacture.
Therefore, it is necessary to manufacture a kind of new deep ultraviolet LED structure, to meet various competition features, including the fast of batch production
Fast manufacturing process, it is inexpensive and multi-functional.Firstly, being exactly to find a kind of structure to replace p-n junction, because excessive p, n are adulterated
Process may be along with the destruction of lattice structure;In addition, many semiconductors inherently are difficult to obtain p-type and n-type doping, this
So that p-n junction is manufactured as challenge.
Summary of the invention
The main technical problem to be solved by the present invention is to provide a kind of single conductance layer ultraviolet photoelectron devices, realize device
Ultraviolet double-side, and there is good optical detection performance, help to improve luminescent properties and optical detection performance, and reduce multiple
Miscellaneous manufacture craft reduces cost.
In order to solve the above technical problems, the present invention provides a kind of single conductance layer ultraviolet photoelectron devices, comprising: lining
Bottom, setting single conductance layer on substrate, the potential barrier insulating layer being arranged on single conductance layer, be arranged in it is saturating on potential barrier insulating layer
Prescribed electrode layer and the metal electrode being electrically connected with single conductance layer;
There is the window for exposing single conductance layer, the metal electrode passes through the window and single electricity on the potential barrier insulating layer
Conducting shell forms electrical connection, and the list conductance layer is the wide bandgap semiconductor layer of N-shaped or p-type doping, and the transparent electrode layer is to receive
The conductive, transparent two-dimensional material of rice noodles or atom level thickness.
In a preferred embodiment: the list conductance layer includes but is not limited to n-AlGaN.
In a preferred embodiment: the potential barrier insulating layer includes but is not limited to SiO2, AlN, two dimension h-BN, MoS2、
MoSe2、WS2, silene, one of germanium alkene or black phosphorus or a variety of.
In a preferred embodiment: the transparent electrode layer includes but is not limited to Ag nano wire, Cu nano wire, alloy nano
One of line, graphene are a variety of.
In a preferred embodiment: the metal electrode is Ohmic contact with single conductance layer.
In a preferred embodiment: the opto-electronic device is optical detector.
The technical program compared with the background art, it has the following advantages:
1. the present invention uses a kind of " metal (Metal)-insulator (Insulator)-semiconductor
(Semiconductor) " structure replaces p-n junction, and excessive p, n is avoided to adulterate the destruction of the adjoint lattice structure of process,
And solve the problems, such as that many semiconductors inherently are difficult to obtain p-type and n-type doping;
2. the invention avoids complicated manufacture crafts, and reduce the defect generated in prolonged deposition process, together
When reduce the production cost;
3. the ultraviolet double-side of device may be implemented in the present invention, and luminous efficiency is high, and luminescence band reaches ultraviolet light wave band;
4. the present invention has good optical detection performance, a kind of optical detector can be obtained with this, there is fast photoresponse
Time and high responsiveness.
Detailed description of the invention
Fig. 1 shows the structural schematic diagram of single conductance layer ultraviolet photoelectron device of the embodiment of the present invention;
Fig. 2 shows the manufacturing method flow diagrams of single conductance layer ultraviolet photoelectron device of the embodiment of the present invention;
Fig. 3 shows the structural schematic diagram of single conductance layer of the embodiment of the present invention;
Fig. 4 shows luminescence generated by light (PL) spectrum of the embodiment of the present invention;
Fig. 5 has shown the insulating layer h-BN film SEM characterization and insulating properties test of the embodiment of the present invention;
Fig. 6 shows the SEM characterization and transmissivity test of the transparent electrode layer Cu nano wire of the embodiment of the present invention;
Fig. 7 shows the Ohmic contact test of the metal electrode of the embodiment of the present invention;
Fig. 8 shows the I-V curve of the rectification characteristic of single conductance layer ultraviolet photoelectron device of the embodiment of the present invention;
Fig. 9 shows electroluminescent (EL) spectrum of single conductance layer ultraviolet photoelectron device of the embodiment of the present invention;
Figure 10 shows the optical detection performance of the transient response of single conductance layer ultraviolet photoelectron device of the embodiment of the present invention.
Specific embodiment
Hereafter by the drawings and specific embodiments, the present invention will be further described.
With reference to Fig. 1-2, a kind of manufacturing method of single conductance layer ultraviolet photoelectron device is present embodiments provided, including as follows
Step:
1. the preparation of list conductance layer n-Al GaN, the list conductance layer is the wide bandgap semiconductor layer of N-shaped or p-type doping.
1) it is prepared using Metallo-Organic Chemical Vapor deposition (MOCVD) method: not being mixed including 600nm on a sapphire substrate
Miscellaneous Al0.3Ga0.7N buffer layer and 100nm Al0.4Ga0.6N;
2) Al adulterated using 1.5 μm of molecular beam epitaxial growth of N-shaped Si0.3Ga0.7N thin film, as shown in Figure 3, Figure 4;
3) n-AlGaN active layer is rinsed with ultrasonic impact in ethyl alcohol and DI water, cleans surface completely, finally utilizes
Nitrogen gun removes surface water droplet and dust.
2. the preparation of potential barrier insulating layer h-BN:
1) it is prepared on Cu substrate using low-pressure chemical vapor deposition (LPCVD) method;
2) big quartz ampoule is set as reaction cavity, for providing vacuum environment and whole cavity gaseous environment and occurring to sink
Product reaction;Big quartz pipe end is connected with vacuum pump by flange, including mechanical pump and molecular pump two-stage vacuum device, sealing
Cavity can be evacuated to required vacuum degree after good, it is ensured that reaction is protected from airborne pollution, while by the exhaust gas generated in reaction process and
By-product takes cavity out of.
3) setting tubule constitutes independent ventilation pipeline, is directly connected with independent gas circuit, and length is by BN predecessor warm area, out
Mouth setting and reaction chamber section start.
4) there is mass flow controller to connect gas cylinder inside and outside outside pipeline, gas mass flow can be made using software accurate
Control, and do the mixed gas supply of multiple gases.
5) predecessor of Borazane (ammonia borane) as B, N is chosen, after weighing 0.0120g, is placed in a small-sized quartz
In boat and the center for being located at the first warm area is pushed it in tubule;Cu foil substrate is placed in the center of third warm area.
6) it sets temperature control panel and ventilation and starts to warm up program, when reaction temperature-raising region temperature raising is to 800-1000 DEG C,
Outer tube passes to a certain proportion of hydrogen and argon gas mixed gas (10sccm H2 and 20sccm Ar), makes annealing treatment to substrate
About 20-60 minutes, to remove substrate surface oxide layer and other absorption pollutants, increase the domain of Cu close with big reduction nucleation
Degree, is conducive to the growth of high-quality thin film.
7) after the completion of annealing, reaction chamber temperature is promoted to 1050-1060 DEG C, meanwhile, warm area locating for predecessor is promoted to pre-
If temperature (85-100 DEG C, 700~800 DEG C), starts growth phase at this time: being changed to be passed through 8sccm H from inner tube2And 20sccm
Ar conveys Borazane (gas flow and ratio can need to be scaled according to doping concentration and reaction speed).
8) heating schedule is automatically closed after reaction, and changes and continue to be passed through 5sccm H in outer tube2It is used with 20sccm Ar
Make protective gas, finally after naturally cooling to room temperature, close vacuum pump, opens after cavity restores vacuum degree and take out sample differentiation
Front and back sides are placed in drying box stand-by.
3. potential barrier insulating layer h-BN film is transferred to single conductance layer;1) PMMA (polymethyl methacrylate) conduct is used
The transfer method of medium.
2) boron nitride is protected in hexagonal boron nitride one layer of PMMA laid on, prepares a certain concentration ammonium persulfate ((NH4)2S2O8) solution, growth substrate copper sheet is removed, obtains the hexagonal boron nitride film floating of PMMA covering on etching solution.
3) it is transferred on single conductance layer n-Al GaN after rinsing in deionized water, the hexagonal boron nitride of PMMA covering is thin
There are the windows for placing metal electrode on film, and part list conductance layer n-Al GaN is exposed.Then it is heating and curing, makes
The hexagonal boron nitride film of PMMA covering is sufficiently contacted with single conductance layer n-Al GaN, and sample is placed in acetone soln
Except PMMA.
4) it is finally annealed and further removes remaining PMMA.
4. the preparation of Ohmic electrode Ti/Al/Ti/Au:
1) Cu nano line electrode mask is made with aluminium-foil paper, and be wrapped on h-BN/n-Al GaN, pay attention to making electrode position
It is corresponding with the window.
2) Ti (40nm)/Al (120nm)/Ti (40nm)/Au (80nm) metal electricity is sputtered using magnetron sputtering method respectively
Pole.
3) reach Ohmic contact after short annealing 30s at 950 DEG C.
5. the preparation of transparent electrode Cu nano wire:
1) pre-reaction material of the 0.8mmol Copper dichloride dihydrate (CuCl22H2O) as copper atom is weighed
(Precursor);0.4mmol nickel acetylacetonate-Ni (acac) 2 is used as reducing agent;10ml oleyl amine is measured as reducing agent, dispersion
Agent and structure directing agent (protective agent), three is mixed in three-necked flask.
2) three-necked flask is placed in constant-temperature heating magnetic stirring apparatus and carries out heating reaction, heating dress is adjusted by setting
It sets, the accurate control to reaction temperature and reaction rate may be implemented.To avoid in reaction process Cu nano wire at high temperature
It is oxidized, needs constantly to be passed through 50sccm high pure nitrogen (or argon gas) into container as protection gas.
3) when unit temp is increased to 80 DEG C, heated at constant temperature 20min.
4) by reaction unit continuous heating to 185 DEG C, 4 hours of heated at constant temperature.
5) after reaction, stop heating, after reaction solution is cooled to room temperature, Cu is centrifugated out from reaction product
Nano wire, and be sealed in hexane solution.
6. transparent electrode Cu nano wire is transferred to insulating layer h-BN:
1) Cu nano wire transparent metal electrode is prepared using vacuum filtration stamping technique.
2) Cu nano line electrode mask is made with aluminium-foil paper, and be wrapped on h-BN/n-Al GaN, pay attention to making transparent electrode
Part is located at the position for having h-BN to cover.
3) a certain amount of Cu nano wire-n-hexane ink is taken out, is diluted to a certain proportion of hexane solution certain dense
(thickness that the amount by changing addition n-hexane can regulate and control transparent electrode influences the ginseng such as its transmissivity and square resistance to degree
Number) and ultrasound, oscillation so that it is uniformly dispersed several minutes.
4) the Cu nano wire ink diluted is poured into the container of Suction filtration device, open vacuum mechanical pump take out just oneself
Alkane, being formed on filter membrane has certain thickness equally distributed Cu nano wire film.
5) it takes the filter membrane for being covered with uniform Cu nano wire film off from suction filtration head with tweezers, makes to be covered with Cu nano wire
It is fitted closely together with target substrate on one side.
6) apply certain pressure and uniformly rolling transfer at the filter membrane back side using boat-shaped seal, under the action of compression,
Cu nano wire film comes into full contact with target substrate surface, and enables Cu nano wire so complete that be transferred in target substrate.
7) it is taken out after short annealing 20min at 300-400 DEG C after removing mask, it is organic on nano wire to remove
Object, while copper nano-wire grid electric conductivity and mechanical performance are improved, to obtain the metallic film conductive grid being evenly distributed.
As the simple replacement of the present embodiment, it is readily modified as preparing potential barrier insulation directly on single conductance layer n-Al GaN
Layer;The preparation sequence of otherwise see-through electrode and metal electrode can overturn, i.e., first production transparent electrode prepares metal electrode again.
Single conductance layer ultraviolet photoelectron device has been obtained by the above method, comprising: the single electricity of substrate, setting on substrate
Conducting shell, the potential barrier insulating layer being arranged on single conductance layer, the transparent electrode layer being arranged on potential barrier insulating layer and with the list
The metal electrode of conductance layer electrical connection;
There is the window for exposing single conductance layer, the metal electrode passes through the window and single electricity on the potential barrier insulating layer
Conducting shell forms electrical connection, and the list conductance layer is the wide bandgap semiconductor layer of N-shaped or p-type doping, and the transparent electrode layer is to receive
The conductive, transparent two-dimensional material of rice noodles or atom level thickness.
For the feasibility and beneficial effect for verifying this programme, to single conductance layer ultraviolet photoelectron device of this programme production into
Row test and analysis:
1) the photoelectric properties test of list conductance layer n-Al GaN;
For the quality for studying n-Al GaN, measure room temperature PL spectrum: under 248nm laser excitation, front receives light and exists for discovery
There are glow peaks at 282nm and 325nm, and through preliminary analysis, 324nm, which shines, is not as the impurity energy level of Si, because Si exists
Ionization energy only has 0.2eV in Al GaN, but the transition between the acceptor level from Si impurity energy level to certain defects, be with
The related nearly band-edge emission of defect;And luminous at 282nm then equally will not be from defect luminescence, because defect luminescence must
It is generated in longer position, but it is ensured that photoluminescence wavelength has reached ultraviolet band, if attempting optimization n-Al GaN
Structure or component, then be expected to step into deep ultraviolet band.
2) pattern of potential barrier insulating layer h-BN film and insulating properties test:
From fig. 5, it can be seen that there are some folds (Wrinkles) and the h-BN of single triangle for h-BN film
Domain, fold are due to a complete h-BN film of engagement, its coefficient of expansion and the coefficient of expansion of copper foil are different institutes
It causes, it can be determined that the integrality of h-BN film.
Test for insulating properties, we are illustrated using the measurement of I-V curve: it can be seen that under the voltage of 5V,
The even h-BN film being covered on n-AlGaN shows the characteristic of insulation, equally illustrates that h-BN keeps good in transfer process
Good integrality, while also explanation can use h-BN film as insulating layer, and the generation of leakage current can be prevented with this, can also be
Free carrier is gathered in interface, to improve the luminous efficiency of opto-electronic device.
3) pattern of transparent electrode Cu nano wire and transmissivity test:
From fig. 6, it can be seen that the nano wire of preparation is uniformly dispersed, do not gather into bundles, impurity particle is few, nano wire purity
It is high.In terms of nano wire pattern, diameter thickness is uniform, and diameter is averagely in 30nm hereinafter, have superelevation draw ratio (> 1600), explanation
The Cu nano wire prepared has better quality, compared with the Cu nano wire that other technologies obtain in current report, we
The result is that most thin in the world, draw ratio highest, surface be the most smooth, the highest nano wire of quality.
The photoelectric characteristic of transparent electrode material be measure whether the most important index with practical application value, it is general and
Speech, it is intended that the higher the better for the transmissivity (T, optical properties) of transparent electrode, and the lower sheet resistance (Rs electrical properties) the better.I
Cu nano wire is transferred on the quartz glass of high light transmittance, test its transmissivity using ultraviolet-visible photometer, can be with
Find out that Cu nano wire has very high transmissivity in a very wide wavelength band (ultraviolet-infrared): sheet resistance Rs is 23 Ω/sq
When, transmissivity T is up to 86.6%;And it is worth noting that, we can prepare different thickness by changing the concentration of nano wire
The transparent electrode thin film of degree, Cu nano wire concentration is higher, and film is thicker, and transparent electrode electric conductivity is better, and transmissivity is then lower.
4) the Ohmic contact test of metal electrode:
By measuring the n-Al after having sputtered Ti (40nm)/Al (120nm)/Ti (40nm)/Au (80nm) metal electrode
The I-V curve of GaN device, such as Fig. 7, discovery can achieve good Ohmic contact, and this Ohmic contact will not make in semiconductor
Significant changes occur for the equilibrium carrier concentration in portion, the I-E characteristic of device are nor affected on, hence it is demonstrated that selected metal is electric
It is extremely more appropriate.
5) the I-V measurement of opto-electronic device:
In order to confirm the reason of tunneling mechanism is carrier transport in the device, we measure the I- from -10V to+10V
V curve, such as Fig. 8, finding the device, there are apparent rectification characteristics, and electric current reaches greatly tens mA very much;In addition, binding isotherm
Knowledge can find that direct tunnelling process is the leading mechanism of carrier transport in our devices.
6) electroluminescent (EL) spectral measurement of opto-electronic device:
For the luminous efficiency for measuring the device, the electroluminescent light of our the different tunnelling currents under room temperature forward bias
Spectrum, such as Fig. 9 a, it can be seen from the figure that light emitting near 328nm belongs to nearly band edge hair under medium Injection Current
It penetrates, and with the increase of tunnelling current, luminous intensity also occurs significantly increasing phenomenon.Due to the presence of h-BN insulating layer sum,
It generates electric field and results in the accumulation of electronics;Tunneled holes in n-Al GaN film conductive strips are combined rapidly with electronics,
328nm nearby generates ultraviolet radioactive.The monopolizing characteristic that we realize is double-side, it is from Cu nanometers of high transparency
Line electrode and Sapphire Substrate.EL spectrum in figure to be received from positive and negative.The luminous efficiency measured from the negative is positive
53%.
7) test of the optical detection performance of opto-electronic device:
Structural similarity based on light emitting diode and photodetector, device of the invention can show and be imitated by photovoltaic
The light detection that should be generated.When being excited with 325nm laser (0.75mw/mm2), discovery detector has a transient response, dark current and
Photoelectric current is with good stability and repeated.Compared with other structures such as MSM and p-i-n photodetector, we are measured
The dark current arrived is much smaller;Response time is fast~90ms and responsiveness up to 0.133A/W, such as Figure 10, illustrate device of the invention
Part keeps excellent in responsiveness, therefore has good ultraviolet detection performance.
Skilled person will appreciate that when technical parameter of the invention changes in the following range, it is contemplated that obtain
Same as the previously described embodiments or similar technical effect:
The potential barrier insulating layer is SiO2, AlN and two dimension h-BN, MoS2、MoSe2、WS2, silene, germanium alkene or black phosphorus etc.
One of two-dimensional material is a variety of.
The transparent electrode layer is that the atom levels such as Ag nano wire, Cu nano wire, alloy nano-wire or graphene are thick conductive saturating
One of bright two-dimensional material is a variety of.
The above is only a preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and those skilled in the art can
To readily appreciate that variation disclosed in this invention or technical scope.Alternative solution is intended to cover within the scope of the invention.Cause
This, protection scope of the present invention should be determined by the scope of the claims.
Claims (6)
1. a kind of list conductance layer ultraviolet photoelectron device, characterized by comprising: substrate, setting single conductance layer on substrate,
The potential barrier insulating layer that is arranged on single conductance layer, the transparent electrode layer being arranged on potential barrier insulating layer and with single conductance
The metal electrode of layer electrical connection;
There is the window for exposing single conductance layer, the metal electrode passes through the window and single conductance layer on the potential barrier insulating layer
Electrical connection is formed, the list conductance layer is the wide bandgap semiconductor layer of N-shaped or p-type doping, and the transparent electrode layer is nano wire
Or the conductive, transparent two-dimensional material of atom level thickness.
2. a kind of single conductance layer ultraviolet photoelectron device according to claim 1, it is characterised in that: the list conductance layer packet
It includes but is not limited to n-AlGaN.
3. a kind of single conductance layer ultraviolet photoelectron device according to claim 1, it is characterised in that: the potential barrier insulating layer
Including but not limited to SiO2, AIN, two dimension h-BN, MoS2、MoSe2、WS2, silene, one of germanium alkene or black phosphorus or a variety of.
4. a kind of single conductance layer ultraviolet photoelectron device according to claim 1, it is characterised in that: the transparent electrode layer
Including but not limited to one of Ag nano wire, Cu nano wire, alloy nano-wire, graphene or a variety of.
5. a kind of single conductance layer ultraviolet photoelectron device according to claim 1, it is characterised in that: the metal electrode with
The list conductance layer is Ohmic contact.
6. a kind of single conductance layer ultraviolet photoelectron device according to claim 1, it is characterised in that: the opto-electronic device
For optical detector.
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