CN107093663B - The ultra-thin longitudinal multilayer cascaded structure thermal electric film of editable and thermo-electric device unit - Google Patents
The ultra-thin longitudinal multilayer cascaded structure thermal electric film of editable and thermo-electric device unit Download PDFInfo
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- CN107093663B CN107093663B CN201710232389.6A CN201710232389A CN107093663B CN 107093663 B CN107093663 B CN 107093663B CN 201710232389 A CN201710232389 A CN 201710232389A CN 107093663 B CN107093663 B CN 107093663B
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
- H10N10/10—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects
- H10N10/17—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects characterised by the structure or configuration of the cell or thermocouple forming the device
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
- H10N10/01—Manufacture or treatment
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N19/00—Integrated devices, or assemblies of multiple devices, comprising at least one thermoelectric or thermomagnetic element covered by groups H10N10/00 - H10N15/00
- H10N19/101—Multiple thermocouples connected in a cascade arrangement
Abstract
The present invention relates to a kind of ultra-thin longitudinal multilayer cascaded structure thermal electric films of editable and preparation method and thermo-electric device unit, the film to be formed by multilayer material lontitudinal series.The layers of material for being composed in series film can be used one of following methods or a variety of film be made, including liquid phase method, physical vapor method, electrochemical process etc., such as magnetron sputtering, electron beam evaporation or molecular beam epitaxy deposition film in physical vapor method, it wherein can be used simultaneously above-mentioned one of film preparation mode for every layer, two or more film preparation modes can also be used respectively.Thermo-electric device unit includes the substrate (1) being sequentially overlapped, hearth electrode (2), ultra-thin longitudinal multilayer cascaded structure thermal electric film column (3), top electrode (4).Compared with prior art, the ultra-thin longitudinal multilayer cascaded structure thermal electric film structure of the present invention and performance editable, manufactured thermo-electric device size and self weight are smaller, and relative to the block thermo-electric device of body structure, performance boost space is bigger, and application range is wider.
Description
Technical field
The present invention relates to thermal electric film technical fields, relate in particular to the ultra-thin longitudinal multilayer cascaded structure thermoelectricity of editable
Film and preparation method and thermo-electric device unit containing longitudinal multilayer cascaded structure thermal electric film.
Background technique
Thermoelectric material can utilize solid interior carrier moving, realize that thermal energy and electric energy are directly converted mutually, effectively will
Hot-cast socket is a kind of all solid state energy conversion regime at electric energy, without chemical reaction or fluid media (medium).Thermo-electric device is often by two kinds
Different types of thermoelectric material (such as P-type semiconductor and N-type semiconductor) is made into column structure (P column and N column), and by one end
In conjunction with being placed under the condition of high temperature, the other end is opened a way in low-temperature condition, due to the effect of high temperature, so that the hole of temperature end and electronics
Concentration is different from low-temperature end, forms concentration difference, to realize the migration of carrier, and then potential difference is realized, by face
Multipair P column and N column connect to obtain bigger voltage.Thermo-electric device is a kind of clean energy resource process units, have movement-less part,
Noiseless, small in size, light-weight, conveniently moving, long service life, stablizes output electricity at pollution-free, easily controllable, high reliablity
The series of advantages such as energy.
The main evaluation index for measuring thermo-electric device transfer efficiency is the thermoelectric figure of merit (ZT value) of thermoelectric material, ZT=
S2·σ·κ-1T, wherein S indicates that Seebeck coefficient, σ indicate conductivity, and κ indicates thermal conductivity, and thermal conductivity includes electronics thermal conductivity
Rate κeWith lattice thermal conductivity κl, by Wiedemann-Franz law κe=L σ T shows that electron thermal conductivity and conductance are linearly related,
And for semiconductor, electron thermal conductivity is much smaller than lattice thermal conductivity.ZT value is bigger, and thermoelectricity capability is better.By the expression of ZT
Formula is it is found that the approach for improving the ZT value of thermoelectric material is exactly the Seebeck coefficient for increasing material, the conductivity for improving material, drop
The thermal conductivity of low material.However, these parameters in thermoelectric material intercouple together, it is difficult to it is adjusted in synchronism, so that
Thermoelectric figure of merit and conversion efficiency of thermoelectric are difficult to increase substantially.And lattice thermal conductivity is that only one is not determined by electronic structure
Parameter has relatively independent space, increases phon scattering by introducing the methods of point defect, crystal boundary, to reduce lattice heat
Conductance, while the transmission of electronics is not influenced or enhancing, to achieve the purpose that " electron crystal-phonon glasses " channel, effectively improve
ZT value improves thermoelectricity capability.
Apply the thermo-electric device of comparative maturity that body processing method is mainly used to manufacture at present, thickness reaches several centimeters grades
Not, size and self weight are larger.In order to be further reduced device self weight and promote thermoelectrical efficiency, the in recent years low-dimensional of thermoelectric material
Change is a hot spot trend, and the thin film thermoelectric device thickness being currently in research also reaches hundreds of microns to millimeter rank, is concentrated
Still immature in single thin film, the performance of thermal electric film device is restricted to a certain extent.
Summary of the invention
It is ultra-thin vertical that it is an object of the present invention to overcome the above-mentioned drawbacks of the prior art and provide a kind of editables
To multilayer cascaded structure thermal electric film and preparation method and thermo-electric device unit.
The purpose of the present invention can be achieved through the following technical solutions: a kind of ultra-thin longitudinal multilayer cascaded structure of editable
Thermal electric film, which is characterized in that the film is formed by multilayer material lontitudinal series.
The thickness of every layer material is less than 1000nm in the film.Ultra-thin multilayer lontitudinal series structure thermal electric film total thickness
Degree is less than 10 μm.
The layers of material that the film of lontitudinal series composition uses includes metal, oxide, semiconductor, organic matter or inorganization
Object is closed, when series connection, at least a kind of material containing more than one with thermoelectric property, i.e. thermoelectric material.For to sum up enumerating (including
Material with thermoelectric property), metal such as Au, Ag, Cu, Pt, Pd etc..Organic matter such as conducting polymer etc., semiconductor is such as
Bi2Te3、Sb2Te3, PbTe, Si, Ge, Bi, Te, Sb, Sn, Se, Pb etc..Oxide such as SiO2、ZnO、Al2O3、In2O3、SnO2
Deng.Inorganic compound such as Skutterudite and Clathrate filling compound etc..
Layers of material can be the period or aperiodic in longitudinal multilayer cascaded structure thermal electric film, if periodicity, then period
It is 1~1000.
It is preferred that the film is alternately connected by n kind material, m period is formed, wherein n and m is the integer greater than 1.
Further preferably, the n is 2, m 2, and vertical structure alternant is A1A2A1A2。
It is preferred that the film is composed in series by n kind material aperiodicity, n is the integer greater than 1, meanwhile, in n kind material
Expect in aperiodicity series connection, same material may occur in which repeatedly.If m is 3, vertical structure such as A1A2A3。
In the film multilayer material lontitudinal series mode include one or more thermoelectric materials and metal, oxide,
Semiconductor or inorganic compound series connection, or connected by thermoelectric material with thermoelectric material.
In the multilayer material for forming film, it can lead to and control generation hole using preparation means in uniform material or mix
Enter tiny impurity particle, it is pore layer that there is hole, which to be less than 50nm, and it is doping stratum granulosum that there is particle, which to be less than 50nm,
The remaining uniform material of constituent is conforming layer.Wherein pore layer, stratum granulosum can be described as functional layer again, have excitation carrier
(excitation layer) or the effect for absorbing phonon (absorbed layer).
In view of multilayer cascaded structure layer thermal electric film and interelectrode combination problem, adhesive layer, thickness 3 can be added
~100nm.
The preparation method of the ultra-thin longitudinal multilayer cascaded structure thermal electric film of a kind of editable, which is characterized in that be composed in series
The layers of material of film can be used one of following methods or a variety of film, including liquid phase method, physical vapor method, electrification be made
Method etc., such as magnetron sputtering, electron beam evaporation or molecular beam epitaxy deposition film in physical vapor method, wherein every layer can be same
When using above-mentioned one of film preparation mode, two or more film preparation modes can also be used respectively.
Thermo-electric device unit comprising the ultra-thin longitudinal multilayer cascaded structure thermal electric film of editable, including successively fold
The substrate that adds, hearth electrode, ultra-thin longitudinal multilayer cascaded structure thermal electric film column, top electrode, wherein if binding force between layers
It is weak, adhesive layer can be increased in interlayer.
The substrate requirements meet it is smooth, can bearing structure, insulation, such as silicon wafer, sheet glass, stainless steel plate (if
It is conductive substrates, a layer insulating, such as SiO is deposited between substrate and hearth electrode2, Si3N4, AlN etc., thickness is greater than 50nm), base
Base thickness degree is greater than 50 μm；
The hearth electrode is placed in substrate, top electrode is placed on thermal electric film, thick using material such as Au, Ag, Cu, Pt etc.
Degree is greater than 50nm；
Compared with prior art, the thickness of thermal electric film device is thinned further in the method for the present invention, and self weight is further
Reduce, can apply to the fields such as Aerospace Satellite station, chip cooling power generation, the power generation of automobile exhaust pipe Waste Heat Reuse, while designing logical
Cross the functional layer material cascaded structure, including pore layer, stratum granulosum, conforming layer etc. of suitable longitudinal multilayer, wherein pore layer,
Granulosa has the function of exciting carrier (excitation layer) or absorbs phonon (absorbed layer).Pass through different structure layer series connection shape simultaneously
At boundary layer, enhances phon scattering, do not influence or enhance the transmission of electronics, to form " electron crystal-phonon glasses " channel,
Further increase thermoelectricity capability.
Detailed description of the invention
Fig. 1 is the ultra-thin longitudinal multilayer cascaded structure thin film thermoelectric unit schematic cross-section of editable；
Fig. 2 is the ultra-thin longitudinal multilayer cascaded structure thermal electric film schematic cross-section of editable；A is ultra-thin longitudinal multilayer n kind
M periodic structure thermal electric film schematic diagram of material in series；B is ultra-thin longitudinal multilayer n kind material aperiodicity cascaded structure thermoelectricity
Film schematic diagram；C is ultra-thin longitudinal multilayer cascaded structure thermal electric film schematic diagram；
Fig. 3 is the ultra-thin longitudinal multilayer cascaded structure thermal electric film equivalent circuit diagram of editable；A is ultra-thin longitudinal multilayer n kind
M periodic structure thermal electric film equivalent circuit diagram of material in series；B is ultra-thin longitudinal multilayer n kind material aperiodicity cascaded structure
Thermal electric film equivalent circuit diagram；
Fig. 4 is the ultra-thin longitudinal multilayer cascaded structure thermal electric film section example schematic of editable；A be uniform layer material,
Particle layer material and m periodic structure schematic diagram of pore layer material in series；B is stratum granulosum A1, pore layer A2... uniform thermoelectric layer
An-2, uniform alumina nitride layer An-1, homogenous metal layer AnAperiodicity cascaded structure schematic diagram；
Fig. 5 is ultra-thin longitudinal 1 sectional view of multilayer cascaded structure thin film thermoelectric unit example of editable；A is ultra-thin multilayer string
It is coupled in structure thermoelectric material Si/Ge (section SEM), b is ultra-thin multilayer cascaded structure thermoelectric material Si/Ge schematic diagram；C is ultra-thin more
Layer cascaded structure thermoelectric material Si/Ge equivalent circuit diagram；
Fig. 6 is ultra-thin longitudinal 2 sectional view of multilayer cascaded structure thin film thermoelectric unit example of editable；A is ultra-thin multilayer string
It is coupled structure thermoelectric material Au/Sb2Te3(section SEM), b are ultra-thin multilayer cascaded structure thermoelectric material Au/Sb2Te3Schematic diagram；c
For ultra-thin multilayer cascaded structure thermoelectric material Au/Sb2Te3Equivalent circuit diagram.
Specific embodiment
It is enumerated below by way of attached drawing of the invention, and magnetron sputtering deposition film thermoelectric unit in conjunction with specific embodiments,
The more detailed description present invention.It should be pointed out that the present invention can realize in different forms, and should be according to practical feelings
Condition makes corresponding adjustment.It proposes that these examples are intended to reach sufficient complete disclosure, keeps those skilled in the art complete
Understand the scope of the present invention, should not be construed as being limited by the embodiment of this proposition.It is all such as when selecting the technique of deposition film
Such as liquid phase method, electrochemical process and the electron beam evaporation in physical vapor method or molecular beam epitaxy can deposition film mode
, it is not limited to the magnetron sputtering in example, example does not enumerate herein.
It is illustrated first against the ultra-thin multilayer lontitudinal series structure thermal electric film thermoelectric unit of editable, Fig. 1 is in fact
One of schematic diagram is applied, it is thin that vertical structure is followed successively by the ultra-thin multilayer lontitudinal series structure thermoelectricity of dielectric base 1, hearth electrode 2, editable
Film 3, top electrode 4.It is poor by longitudinal both ends formation temperature, potential difference is generated, the difference of hot and cold side is placed according to upper and lower surface,
The positive and negative difference of the potential difference of generation.
Wherein for ultra-thin 3 structure of multilayer lontitudinal series structure thermal electric film of editable as shown, such as Fig. 2 (a), longitudinal direction can
It alternately connects m period for n kind material, it is 2, m 2 if n that n and m, which are the integer greater than 1, then vertical structure alternating shape
Formula is A1A2A1A2.Such as Fig. 2 (b), or the series connection of n kind material aperiodicity, n are the integer greater than 1, longitudinal if m is 3
Structure such as A1A2A3.Meanwhile in the series connection of n kind material aperiodicity, same material be may occur in which repeatedly.
Fig. 3 is the ultra-thin multilayer lontitudinal series structure thermal electric film equivalent circuit diagram of editable, and Fig. 3 (a) is n kind material in series
M period film equivalent circuit diagram, Fig. 3 (b) are n kind material aperiodicity tandem thin-film equivalent circuit diagram.
Fig. 4 is the ultra-thin longitudinal multilayer cascaded structure thermal electric film example schematic of editable, and Fig. 4 (a) is conforming layer, particle
Layer and m period schematic diagram of pore layer lontitudinal series, Fig. 4 (b) are stratum granulosum A1, pore layer A2... uniform thermoelectric layer An-2, uniformly
Oxide skin(coating) An-1, homogenous metal layer AnLongitudinal aperiodicity series connection schematic diagram.
Secondly it is directed to ultra-thin longitudinal multilayer cascaded structure thermal electric film and can be directly used for the preparation of the thermoelectric unit to generate electricity,
In conjunction with magnetron sputtering deposited thermoelectric Films Example 1 and embodiment 2, it is illustrated.
Embodiment 1
Wherein substrate uses the oxidized silicon chip of 3 cun of single-sided polishings, and Si is doped to P, crystal orientation<100>, resistivity 1-20 Ω
Cm, 400 ± 10 μm of thickness, 500 ± 30nm of oxidated layer thickness.
Substrate steeps 10min using acetone clear liquid, then takes out rapidly, is rinsed with dehydrated alcohol, and deionized water is rinsed, and uses N2
Drying.
It is 10 that substrate, which is placed in background vacuum,-6In the Denton multi-target magnetic control sputtering coating system of Torr, first using height
Pure Ar cleans 1min, then starts to carry out deposition film.
In view of the combination problem in physical vapour deposition (PVD) between layers, adhesive layer is added, adhesive layer uses material such as
Cr, Ni, Ti etc., 5~100nm of thickness.In the present embodiment using 20nm Cr as adhesive layer, wherein in substrate in sequence according to
Secondary deposition 20nm Cr (adhesive layer), 200nm Au (hearth electrode), 20nm Cr (adhesive layer),
Then depositing ultrathin longitudinal direction multilayer cascaded structure thermal electric film in the present embodiment, first deposits 20nm Si, then sinks
Product 20nm Ge, successively 25 periods of alternating deposit, totally 1 μm, Fig. 5 is prepared ultra-thin longitudinal multilayer cascaded structure thermal electric film
The section Si/Ge SEM figure.
Embodiment 2
Substrate and hearth electrode processing are same as Example 1, at the ultra-thin multilayer lontitudinal series structure thermal electric film of editable
It manages as follows: first depositing 20nm Au on hearth electrode, then deposit 20nm Sb2Te3, successively 25 periods of alternating deposit, totally 1 μ
M, Fig. 6 are prepared ultra-thin longitudinal multilayer cascaded structure thermal electric film Au/Sb2Te3Section SEM figure.
20nm Cr (adhesive layer), 200nm Au (top electrode) are deposited on ultra-thin longitudinal multilayer cascaded structure thermal electric film,
Obtain thermo-electric device unit.
Following table is to prepare the ultra-thin longitudinal multilayer cascaded structure thermal electric film of editable obtained in film implementation process
Partial properties are enumerated, and ultralow thermal conductivity (0.30Wm has been obtained-1·K-1) film.Pass through preferred preparation method, material simultaneously
Material, structure, period, the combination of thickness degree are expected to obtain the lower film of thermal conductivity, while obtaining matched suitable plug
Seebeck coefficient and conductivity obtain better conversion efficiency of thermoelectric.
Therefore it is middle using in different method for manufacturing thin film and combination, such as physical vapor method through the invention
Ultra-thin longitudinal multilayer string of magnetron sputtering, electron beam evaporation or molecular beam epitaxy, the different-thickness that can be obtained and different micro-structures
Be coupled structure thermal electric film, and can by this film design at thermoelectric unit device is made, realize the preparation of ultra-thin thermo-electric device with
And the expansion of application range.
The above is only a specific embodiment of the invention citing, it should be pointed out that the present invention is not intended to be limited to herein
Shown in example, but want compound widest range consistent with the principles and novel features disclosed in this article.
Claims (3)
1. a kind of thermo-electric device unit containing the ultra-thin longitudinal multilayer cascaded structure thermal electric film of editable, which is characterized in that packet
Include the substrate (1) being sequentially overlapped, hearth electrode (2), ultra-thin longitudinal multilayer cascaded structure thermal electric film column (3), top electrode (4), institute
The ultra-thin longitudinal multilayer cascaded structure thermal electric film column (3) stated is formed by multilayer material lontitudinal series, multilayer cascaded structure thermoelectricity
Adhesive layer, 3~100nm of thickness are added between film and hearth electrode (2), top electrode (4)；It is more in multilayer cascaded structure thermal electric film
Layer material lontitudinal series mode includes one or more thermoelectric materials and metal, oxide, semiconductor, organic matter or inorganic chemical
Object series connection, or connected by thermoelectric material with thermoelectric material；
The metal includes Au, Ag, Cu, Pt or Pd, and the organic matter includes conducting polymer, and the semiconductor includes
Bi2Te3, PbTe, Si, Ge, Bi, Te, Sb, Sn, Se, the oxide includes ZnO, Al2O3、In2O3Or SnO2, the nothing
Machine compound includes Skutterudite and Clathrate filling compound；
By n kind material, alternately the m period of series connection forms the multilayer cascaded structure thermal electric film, wherein n and m is greater than 2
Integer；
Alternatively, multilayer cascaded structure thermal electric film is composed in series by n kind material aperiodicity, n is the integer greater than 2, meanwhile,
In the series connection of n kind material aperiodicity, same material be may occur in which repeatedly；
It is pore layer that forming in the multilayer material of multilayer cascaded structure thermal electric film, there is hole, which to be less than 50nm, has doping
It is doping stratum granulosum that grain, which is less than 50nm, remaining ingredient is uniformly conforming layer；Wherein pore layer, doping stratum granulosum are known as function
Layer has the function of exciting carrier or absorbs phonon.
2. a kind of thermo-electric device containing the ultra-thin longitudinal multilayer cascaded structure thermal electric film of editable according to claim 1
Unit, which is characterized in that the thickness of every layer material is less than 1000nm in the multilayer cascaded structure thermal electric film.
3. a kind of thermo-electric device containing the ultra-thin longitudinal multilayer cascaded structure thermal electric film of editable according to claim 1
Unit, which is characterized in that the layers of material in multilayer cascaded structure thermal electric film is using one of following methods or a variety of systems
At film, including liquid phase method, physical vapor method or electrochemical process, wherein physical vapor method includes magnetron sputtering, electron beam evaporation
Or molecular beam epitaxy.
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