CN108598266B - Perovskite photoelectric device based on tunneling effect and preparation method thereof - Google Patents
Perovskite photoelectric device based on tunneling effect and preparation method thereof Download PDFInfo
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- H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
- H10K85/50—Organic perovskites; Hybrid organic-inorganic perovskites [HOIP], e.g. CH3NH3PbI3
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Abstract
The present invention relates to a kind of perovskite photoelectric device and preparation method thereof based on tunneling effect, the preparation method include: to choose Si substrate；Lower electrode is formed in a side surface deposited metal material of the Si substrate；HfO is deposited in another side surface of the Si substrate2Form tunnel layer；CH is deposited on the tunnel layer3NH3PbI3Form light absorbing layer；Deposited metal material forms top electrode on the light absorbing layer, forms the perovskite photoelectric device based on tunneling effect.The perovskite photoelectric device successively includes top electrode, CH3NH3PbI3Light absorbing layer, HfO2Tunnel layer, Si substrate and lower electrode.Perovskite photoelectric device of the invention is in Si substrate and CH3NH3PbI3Between include HfO2Tunnel layer, structure and preparation process are simple, reduce the compound of light induced electron and photohole, increase photoelectric current, improve the sensitivity and efficiency of photoelectric device.
Description
Technical field
The invention belongs to microelectronics technologies, and in particular to a kind of perovskite photoelectric device based on tunneling effect and its
Preparation method.
Background technique
In recent years, sensitive for photoelectric device in terms of life, military affairs and scientific research along with the rapid development of electronic technology
Degree demand is higher and higher, wherein the research of structure, technique and material etc. is that photoelectricity is made to mention device performance and sensitivity
High Main way.
Perovskite (CH3NH3PbI3) a kind of hybrid inorganic-organic materials are used as, it is a kind of novel optoelectronic materials, has
The crystal structure of long-range order takes into account organic and inorganic advantage.In terms of inorganic component, perovskite have strong covalent bond with
Ionic bond makes it have very high mobility and thermal stability and good electrology characteristic.Have benefited from organic component formation
Self assembly and film forming characteristics allow spin-coating method to prepare perovskite and complete under conditions of low temperature and low cost.Perovskite tool
The high absorption coefficient of light and long charge carriers carrier diffusion length having, make it show up prominently in field of photoelectric devices.
Traditional perovskite optoelectronic device structure is Si and CH3NH3PbI3It directly contacts, contact surface conduction band is bent so that light
Raw electronics is by CH3NH3PbI3Flow to Si, but valence-band level stops photohole from Si to CH3NH3PbI3Effective transfer, therefore
A large amount of holes in contact area, so as to cause a large amount of compound of light induced electron and photohole, light induced electron and photohole
Separation is reduced, and causes photoelectric current weaker, therefore, the sensitivity of manufactured photoelectric device and efficiency are relatively low.
Summary of the invention
In order to solve the above-mentioned problems in the prior art, the present invention provides a kind of perovskites based on tunneling effect
Photoelectric device and preparation method thereof.The technical problem to be solved in the present invention is achieved through the following technical solutions:
One aspect of the present invention provides a kind of preparation method of perovskite photoelectric device based on tunneling effect, packet
It includes:
Choose Si substrate；
Lower electrode is formed in a side surface deposited metal material of the Si substrate；
HfO is deposited in another side surface of the Si substrate2Form tunnel layer；
CH is deposited on the tunnel layer3NH3PbI3Form light absorbing layer；
Deposited metal material forms top electrode on the light absorbing layer, forms the perovskite phototube based on tunneling effect
Part.
In one embodiment of the invention, Si substrate is chosen, comprising:
The intrinsic Si with a thickness of 200-600 μm is chosen as Si substrate.
In one embodiment of the invention, the metal material is Al, Ti, Ni, Au, Pt or Cu.
In one embodiment of the invention, lower electrode is formed in a side surface deposited metal material of the Si substrate,
Include:
Magnetron sputtering apparatus cavity is cleaned and is vacuumized with the argon gas that mass percent purity is 99.999%,
In, scavenging period 5min；
Sputtering chamber is passed through as sputter gas using the argon gas that mass percent purity is 99.999%；
It is 6 × 10 in vacuum degree-4-1×10-3Pa, argon flow 20-30cm3/ s, target cardinal distance are 10cm and magnetic control
Under conditions of the operating power of sputtering equipment is 20W-80W, using mask plate, using magnetically controlled sputter method in the Si substrate one
Side surface depositing Al material forms lower electrode, mass percent purity > 99.99% of the Al material.
In one embodiment of the invention, HfO is deposited in another side surface of the Si substrate2Form tunnel layer, packet
It includes:
Magnetron sputtering apparatus cavity is cleaned and is vacuumized with the argon gas that mass percent purity is 99.999%,
In, scavenging period 5min；
Sputtering chamber is passed through as sputter gas using the argon gas that mass percent purity is 99.999%；
It is 6 × 10 in vacuum degree-4-1.1×10-3Pa, argon flow 20-30cm3/ s, target cardinal distance are 10cm and magnetic
Under conditions of the operating power for controlling sputtering equipment is 20W-80W, using mask plate, using magnetically controlled sputter method in the Si substrate
One side surface deposits HfO2Material forms tunnel layer.
In one embodiment of the invention, CH is deposited on the tunnel layer3NH3PbI3Form light absorbing layer, comprising:
The light absorbing layer is deposited on the tunnel layer using single spin-coating method, solvent evaporated method or gel method.
In one embodiment of the invention, CH is deposited on the tunnel layer3NH3PbI3Form light absorbing layer, comprising:
By the PbI of 650-655mg2With the CH of 215-220mg3NH3I is successively added in DMSO:GBL, obtains PbI2With
CH3NH3The mixed solution of I；
By PbI2And CH3NH3The mixed solution of I stirs 2h at 80 DEG C, by the solution after stirring in 80 DEG C of standing 1h, obtains
To CH3NH3PbI3Solution；
By CH3NH3PbI3Solution is added drop-wise to HfO2It is uniform using single spin-coating method spin coating on sol evenning machine on tunnel layer；
By CH3NH3PbI3The uniform HfO of solution spin coating2Tunnel layer is annealed 20min at 100 DEG C, forms CH3NH3PbI3Light
Absorbed layer.
In one embodiment of the invention, deposited metal material forms top electrode on the light absorbing layer, forms base
In the perovskite photoelectric device of tunneling effect, comprising:
Magnetron sputtering apparatus cavity is cleaned and is vacuumized with the argon gas that mass percent purity is 99.999%,
In, scavenging period 5min；
Sputtering chamber is passed through as sputter gas using the argon gas that mass percent purity is 99.999%；
It is 6 × 10 in vacuum degree-4-1×10-3Pa, argon flow 20cm3/ s, target cardinal distance are that 10cm and magnetic control splash
Under conditions of the operating current of jet device is 1A, using mask plate, splashed using magnetically controlled sputter method in light absorbing layer surface magnetic control
It penetrates Au material and forms top electrode, mass percent purity > 99.99% of the Au material.
Another aspect provides a kind of perovskite photoelectric device based on tunneling effect, including by above-mentioned implementation
Example any one of described in preparation method be prepared top electrode, CH3NH3PbI3Light absorbing layer, HfO2Tunnel layer, Si substrate
With lower electrode.
In one embodiment of the invention, the top electrode with a thickness of 100nm-300nm；The CH3NH3PbI3Light
Absorbed layer with a thickness of 200nm-300nm；The HfO2Tunnel layer with a thickness of 2nm-10nm；The Si substrate with a thickness of
200μm-600μm；The lower electrode with a thickness of 100nm-300nm.
Compared with prior art, the beneficial effects of the present invention are:
1, the perovskite photoelectric device of the invention based on tunneling effect is in Si substrate and CH3NH3PbI3Between light absorbing layer
Including one layer of very thin HfO2Tunnel layer, at conduction band, the light induced electron that perovskite generates can not be directly migrated to by perovskite
HfO2, but it is transferred to Si by tunneling effect, then received by metal electrode；Photohole is then directly received by metal electrode,
Reduce the compound of light induced electron and photohole in this way, photoelectric current is increased, so as to improve the sensitivity of photoelectric device
And efficiency.
2, the present invention is based on the perovskite optoelectronic device structure and preparation process of tunneling effect are simple, fast response time, effect
Rate is high, low in cost, is easy to scale of mass production.
Detailed description of the invention
Fig. 1 is the preparation method flow chart of the perovskite photoelectric device provided in an embodiment of the present invention based on tunneling effect；
Fig. 2 is the structural schematic diagram of the perovskite photoelectric device provided in an embodiment of the present invention based on tunneling effect；
Fig. 3 is HfO in the perovskite photoelectric device provided in an embodiment of the present invention based on tunneling effect2Tunnel layer,
CH3NH3PbI3The double heterojunction energy band schematic diagram that light absorbing layer and Si substrate are formed.
Specific embodiment
The content of present invention is further described combined with specific embodiments below, but embodiments of the present invention are not limited to
This.
Embodiment one
Referring to Figure 1, Fig. 1 is the preparation side of the perovskite photoelectric device provided in an embodiment of the present invention based on tunneling effect
Method flow chart.The preparation method of perovskite photoelectric device of the present embodiment based on tunneling effect the following steps are included:
S1: Si substrate is chosen；
Specifically, the intrinsic Si with a thickness of 400 μm is chosen as Si substrate.The Si substrate plays the entire photoelectricity of support and visits
Survey the effect of device structure.
S2: lower electrode is formed in a side surface deposited metal material of the Si substrate；
Specifically, the S2 includes:
S21: the argon gas for being 99.999% with mass percent purity carries out 5min to magnetron sputtering apparatus cavity and cleans, and
It is evacuated to 6 × 10-4-1×10-3Pa；
S22: sputtering chamber is passed through as sputter gas using the argon gas that mass percent purity is 99.999%；
S23: being 6 × 10 in vacuum degree-4-1×10-3Pa, argon flow 20-30cm3/ s, target cardinal distance be 10cm and
Under conditions of the operating power of magnetron sputtering apparatus is 20W-80W, using mask plate, served as a contrast using magnetically controlled sputter method in the Si
One side surface depositing Al material of bottom forms lower electrode, mass percent purity > 99.99% of the Al material.
In the present embodiment, under the Al material of generation electrode with a thickness of 100nm-300nm.
Further, in other embodiments, the lower electrode can be by material any in Al, Ti, Ni, Au, Pt or Cu
Material deposits, and the material has low cost, is easy to the features such as depositing.
In addition, in other embodiments, the lower electrode can also use chemical vapor deposition, molecular beam epitaxy and original
The other technologies method such as sublayer deposition technique is deposited.
S3: HfO is deposited in another side surface of the Si substrate2Form tunnel layer；
Specifically, the S3 includes:
S31: the argon gas for being 99.999% with mass percent purity carries out 5min to magnetron sputtering apparatus cavity and cleans, and
It is evacuated to 6 × 10-4-1×10-3Pa；
S32: sputtering chamber is passed through as sputter gas using the argon gas that mass percent purity is 99.999%；
S33: being 6 × 10 in vacuum degree-4-1×10-3Pa, argon flow 20-30cm3/ s, target cardinal distance be 10cm and
Under conditions of the operating power of magnetron sputtering apparatus is 20W-100W, using mask plate, using magnetically controlled sputter method in the Si
One side of substrate surface deposits HfO2Material forms tunnel layer.
In the present embodiment, the thickness of the tunnel layer of generation can be 2nm-10nm.HfO2Thick layer cannot be too high, because
If too high for the distance that the light induced electron that perovskite generates passes through, may cause in HfO2It is mutually multiple to occur a large amount of body in layer
It closes.
In other embodiments, the tunnel layer can also be formed using chemical vapor deposition or molecular beam epitaxy.To divide
For beamlet epitaxy, it is placed in high vacuum cavity in the Si substrate, by HfO2Material is placed in jeting furnace, is heated to
HfO when certain temperature2Material generates molecular beam by high temperature evaporation, glow discharge etc., and incoming molecular beam is exchanged with Si substrate
After energy, form a film through adsorption, migration, nucleation, growth.
S4: CH is deposited on the tunnel layer3NH3PbI3Form light absorbing layer；
Usually the light absorption can be deposited on the tunnel layer using single spin-coating method, solution cooling method or gel method
Layer deposits CH using single spin-coating method in the present embodiment3NH3PbI3Form light absorbing layer.
Specifically, the S4 includes:
S41: by the PbI of 654mg2With the CH of 217mg3NH3I is successively added in DMSO:GBL, obtains PbI2And CH3NH3I's
Mixed solution；
S42: by PbI2And CH3NH3The mixed solution of I stirs 2h at 80 DEG C, and the solution after stirring is stood at 80 DEG C
1h obtains CH3NH3PbI3Solution；
S43: by CH3NH3PbI3Solution is added drop-wise to HfO2It is equal using single spin-coating method spin coating on sol evenning machine on tunnel layer
It is even；
S44: by CH3NH3PbI3The uniform HfO of solution spin coating2Tunnel layer is annealed 20min at 100 DEG C, is formed
CH3NH3PbI3Light absorbing layer.In the present embodiment, the light absorbing layer of generation with a thickness of 200n-300nm.
Further, in other embodiments, the light absorbing layer can using solution cooling method or gel method etc. other
Method is made.By taking solution cooling method as an example, specific preparation flow is at relatively high temperatures, will to have calculated stoicheiometry
PbI2And CH3NH3I dissolves respectively in same solvent, then dissolved two kinds of solution is mixed again, by temperature
It is slowly reduced under room temperature, the monocrystalline of high quality will be crystallized out at this time.
S5: deposited metal material forms top electrode on the light absorbing layer, and ultimately generates the calcium based on tunneling effect
Titanium ore photoelectric device.
Specifically, the S5 includes:
S51: the argon gas for being 99.999% with mass percent purity carries out 5min to magnetron sputtering apparatus cavity and cleans, and
It is evacuated to 6 × 10-4-1×10-3Pa；
S52: sputtering chamber is passed through as sputter gas using the argon gas that mass percent purity is 99.999%；
S53: being 6 × 10 in vacuum degree-4-1×10-3Pa, argon flow 20cm3/ s, target cardinal distance are 10cm and magnetic
Under conditions of the operating current for controlling sputtering equipment is 1A, using mask plate, using magnetically controlled sputter method in light absorbing layer surface magnetic
Control sputtering Au material forms top electrode, mass percent purity > 99.99% of the Au material.
In the present embodiment, the top electrode of generation with a thickness of 100nm-300nm.
Further, in other embodiments, the top electrode can also use chemical vapor deposition, molecular beam epitaxy
It is deposited with other technologies methods such as technique for atomic layer deposition.
Fig. 3 is referred to, Fig. 3 is HfO in the perovskite photoelectric device provided in an embodiment of the present invention based on tunneling effect2Tunnel
Wear layer, CH3NH3PbI3The double heterojunction energy band schematic diagram that light absorbing layer and Si substrate are formed.Traditional perovskite photoelectric device knot
Structure is Si substrate and CH3NH3PbI3Light absorbing layer directly contacts, and contact surface conduction band is bent so that light induced electron is by CH3NH3PbI3Light
Absorbed layer flows to Si substrate, but valence-band level stops photohole from Si substrate to CH3NH3PbI3Effective transfer of light absorbing layer,
Therefore a large amount of holes in contact area, cause light induced electron largely compound with photohole, light induced electron is separated with photohole
It reduces, so that photoelectric current weakens.
As shown in figure 3, in the perovskite photoelectric device made of the present embodiment preparation method, Si substrate with
CH3NH3PbI3One layer of very thin HfO is added between light absorbing layer2Metal oxide forms HfO2Tunnel layer.HfO2Tunnel layer,
CH3NH3PbI3Heterostructure band is formed between light absorbing layer and Si substrate, in conduction band, light induced electron can not be by CH3NH3PbI3Light
Absorbed layer directly migrates to tunnel layer, but light induced electron is by CH3NH3PbI3Light absorbing layer passes through after generating by tunneling mechanism
HfO2Tunnel layer directly reaches Si substrate, after received by electrode under Al；And photohole is then by CH3NH3PbI3Light absorbing layer generates
It is directly received afterwards by Au top electrode.In this way compared with Si substrate and CH3NH3PbI3Light absorbing layer directly contacts, and reduces light induced electron
It is compound with photohole, so that photoelectric current is increased, so as to improve the sensitivity and efficiency of photoelectric device.
Embodiment two
Fig. 2 is referred to, Fig. 2 is a kind of knot of the perovskite photoelectric device based on tunneling effect provided in an embodiment of the present invention
Structure schematic diagram.The perovskite photoelectric device based on tunneling effect of the present embodiment is multilayered structure, in order successively includes powering on
Pole 1, light absorbing layer 2, tunnel layer 3, substrate 4 and lower electrode 5.In the present embodiment, top electrode 1 uses Au material；Light absorbing layer 2
Using CH3NH3PbI3Material；Tunnel layer 3 uses HfO2Material；Substrate 4 uses intrinsic Si；Lower electrode 5 uses Al material.This reality
The perovskite photoelectric device based on tunneling effect for applying example can be prepared using preparation method described in embodiment one.
Specifically, the preparation method of perovskite photoelectric device of the present embodiment based on tunneling effect includes:
Step a: intrinsic Si substrate is chosen；
Step b: lower electrode is formed in a side surface of Si substrate deposition Au material using magnetically controlled sputter method；
Step c: HfO is deposited in another side surface of the Si substrate using magnetically controlled sputter method2Form tunnel layer；
Step d: CH is deposited on the tunnel layer using single spin-coating method3NH3PbI3Form light absorbing layer；
Step e: using magnetically controlled sputter method, depositing Al material forms top electrode on the light absorbing layer, generates and is based on tunnel
Wear the perovskite photoelectric device of effect.
Specific preparation process refers to embodiment one, and which is not described herein again.
In the present embodiment, the thickness of top electrode 1 can be 100nm-300nm；CH3NH3PbI3The thickness of light absorbing layer 2
It can be 200nm-300nm；HfO2The thickness of tunnel layer 3 can be 2nm-10nm；The thickness of Si substrate 4 can for 200 μm-
600μm；The thickness of lower electrode 5 can be 100nm-300nm.
In the perovskite photoelectric device of the present embodiment, in Si substrate and CH3NH3PbI3One layer is added between light absorbing layer
Very thin HfO2Metal oxide forms HfO2Tunnel layer.HfO2Tunnel layer, CH3NH3PbI3Shape between light absorbing layer and Si substrate
At heterostructure band, reduce the compound of light induced electron and photohole, so that photoelectric current is increased, so as to improve photoelectricity
The sensitivity and efficiency of device.In addition, the perovskite optoelectronic device structure and preparation process are simple, fast response time is high-efficient,
It is low in cost, it is easy to scale of mass production.
The above content is a further detailed description of the present invention in conjunction with specific preferred embodiments, and it cannot be said that
Specific implementation of the invention is only limited to these instructions.For those of ordinary skill in the art to which the present invention belongs, In
Under the premise of not departing from present inventive concept, a number of simple deductions or replacements can also be made, all shall be regarded as belonging to of the invention
Protection scope.
Claims (7)
1. a kind of preparation method of the perovskite photoelectric device based on tunneling effect, which is characterized in that the preparation method includes:
The intrinsic Si with a thickness of 200-600 μm is chosen as Si substrate；
Lower electrode is formed in a side surface deposited metal material of the Si substrate；
The HfO for being 2nm-10nm in another side surface deposition thickness of the Si substrate2Form tunnel layer；
CH is deposited on the tunnel layer3NH3PbI3Form light absorbing layer；
Deposited metal material forms top electrode on the light absorbing layer, forms the perovskite photoelectric device based on tunneling effect.
2. preparation method according to claim 1, which is characterized in that the metal material be Al, Ti, Ni, Au, Pt or
Cu。
3. preparation method according to claim 1, which is characterized in that in a side surface deposited metal material of the Si substrate
Material forms lower electrode, comprising:
Magnetron sputtering apparatus cavity is cleaned and is vacuumized with the argon gas that mass percent purity is 99.999%, wherein
Scavenging period is 5min；
Sputtering chamber is passed through as sputter gas using the argon gas that mass percent purity is 99.999%；
It is 6 × 10 in vacuum degree-4-1×10-3Pa, argon flow 20-30cm3/ s, target cardinal distance are 10cm and magnetron sputtering
Under conditions of the operating power of equipment is 20W-80W, using mask plate, using magnetically controlled sputter method in the one side of substrate Si table
Face depositing Al material forms lower electrode, mass percent purity > 99.99% of the Al material.
4. preparation method according to claim 3, which is characterized in that deposit HfO in another side surface of the Si substrate2
Form tunnel layer, comprising:
Magnetron sputtering apparatus cavity is cleaned and is vacuumized with the argon gas that mass percent purity is 99.999%, wherein
Scavenging period is 5min；
Sputtering chamber is passed through as sputter gas using the argon gas that mass percent purity is 99.999%；
It is 6 × 10 in vacuum degree-4-1.1×10-3Pa, argon flow 20-30cm3/ s, target cardinal distance are that 10cm and magnetic control splash
Under conditions of the operating power of jet device is 20W-80W, using mask plate, using magnetically controlled sputter method in the one side of substrate Si
Surface deposits HfO2Material forms tunnel layer.
5. preparation method according to claim 1, which is characterized in that deposit CH on the tunnel layer3NH3PbI3It is formed
Light absorbing layer, comprising:
The light absorbing layer is deposited on the tunnel layer using single spin-coating method, solvent evaporated method or gel method.
6. preparation method according to claim 1, which is characterized in that deposit CH on the tunnel layer3NH3PbI3It is formed
Light absorbing layer, comprising:
By the PbI of 650-655mg2With the CH of 215-220mg3NH3I is successively added in DMSO:GBL, obtains PbI2And CH3NH3I's
Mixed solution；
By PbI2And CH3NH3The mixed solution of I stirs 2h at 80 DEG C, by the solution after stirring in 80 DEG C of standing 1h, obtains
CH3NH3PbI3Solution；
By CH3NH3PbI3Solution is added drop-wise to HfO2It is uniform using single spin-coating method spin coating on sol evenning machine on tunnel layer；
By CH3NH3PbI3The uniform HfO of solution spin coating2Tunnel layer is annealed 20min at 100 DEG C, forms CH3NH3PbI3Light absorption
Layer.
7. preparation method according to claim 1, which is characterized in that deposited metal material is formed on the light absorbing layer
Top electrode forms the perovskite photoelectric device based on tunneling effect, comprising:
Magnetron sputtering apparatus cavity is cleaned and is vacuumized with the argon gas that mass percent purity is 99.999%, wherein
Scavenging period is 5min；
Sputtering chamber is passed through as sputter gas using the argon gas that mass percent purity is 99.999%；
It is 6 × 10 in vacuum degree-4-1×10-3Pa, argon flow 20cm3/ s, target cardinal distance are that 10cm and magnetron sputtering are set
Under conditions of standby operating current is 1A, using mask plate, using magnetically controlled sputter method in light absorbing layer surface magnetic control sputtering Au
Material forms top electrode, mass percent purity > 99.99% of the Au material.
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