WO2007076843A1 - Composition composite pour cellule solaire, structure semi-conductrice p-i-n comportant cette composition, cellule solaire et procede de realisation de compositions composites - Google Patents

Composition composite pour cellule solaire, structure semi-conductrice p-i-n comportant cette composition, cellule solaire et procede de realisation de compositions composites Download PDF

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WO2007076843A1
WO2007076843A1 PCT/DE2006/002334 DE2006002334W WO2007076843A1 WO 2007076843 A1 WO2007076843 A1 WO 2007076843A1 DE 2006002334 W DE2006002334 W DE 2006002334W WO 2007076843 A1 WO2007076843 A1 WO 2007076843A1
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matrix
electron
composition according
guest material
donor
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PCT/DE2006/002334
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Thomas Mayer
Wolfram Jaegermann
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Technische Universität Darmstadt
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
    • H01L31/036—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their crystalline structure or particular orientation of the crystalline planes
    • H01L31/0384—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their crystalline structure or particular orientation of the crystalline planes including other non-monocrystalline materials, e.g. semiconductor particles embedded in an insulating material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y10/00—Nanotechnology for information processing, storage or transmission, e.g. quantum computing or single electron logic
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L31/04—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices
    • H01L31/06—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices characterised by potential barriers
    • H01L31/075—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices characterised by potential barriers the potential barriers being only of the PIN type, e.g. amorphous silicon PIN solar cells
    • H01L31/077—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices characterised by potential barriers the potential barriers being only of the PIN type, e.g. amorphous silicon PIN solar cells the devices comprising monocrystalline or polycrystalline materials
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
    • H10K30/40—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising a p-i-n structure, e.g. having a perovskite absorber between p-type and n-type charge transport layers
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
    • H10K30/10—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising heterojunctions between organic semiconductors and inorganic semiconductors
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
    • H10K30/30—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising bulk heterojunctions, e.g. interpenetrating networks of donor and acceptor material domains
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
    • H10K30/50—Photovoltaic [PV] devices
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
    • H10K85/20—Carbon compounds, e.g. carbon nanotubes or fullerenes
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
    • H10K85/30—Coordination compounds
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E10/00—Energy generation through renewable energy sources
    • Y02E10/50—Photovoltaic [PV] energy
    • Y02E10/547—Monocrystalline silicon PV cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E10/00—Energy generation through renewable energy sources
    • Y02E10/50—Photovoltaic [PV] energy
    • Y02E10/549—Organic PV cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a composite composition, comprising at least one semiconductor material as a matrix and at least one embedded therein at least one guest material, which is suitable to absorb radiation of at least one wavelength and generate at least one electron-hole pair under the action of radiation. Furthermore, the invention relates to a p-i-n semiconductor structure containing this composition, a solar cell and a method for producing the composite composition according to the invention.
  • Crystalline silicon layers generally have too low absorption for solar cell applications because silicon is a semiconductor having an indirect bandgap between the valence band and the conduction band. At the same time, however, silicon has a high intrinsic carrier lifetime due to this indirect band gap. Accordingly, mono- and multicrystalline silicon layer materials for solar cells have hitherto always been at least about 300 ⁇ m thick and therefore very complicated and expensive to produce. Amorphous silicon, however, brings with it stability problems.
  • EP 0 525 070 B1 proposes the use of dye-sensitized solar cells.
  • a dye absorber forms a monomolecular layer, and, in order to achieve a sufficiently strong absorption, porous layers of nanocrystalline TiO 2 are used.
  • the surface of this monomolecular layer must be adjacent to an electrolyte into which a hole of an electron-hole pair generated by light absorption in the dye absorber is injected and transported to a back contact.
  • the excited electron of the electron-hole pair is injected into a conduction band of an oxide semiconductor.
  • the electron and the hole of the excited electron-hole pair are accordingly to be injected into two different materials, whereby the absorption is limited to a single interface.
  • a difficulty here is to keep excited charge carriers in the intermediate band for a long enough time to recombine into the valence band in order instead to reach the conduction band by means of excitation by another photon. Radiation-free recombination processes have proven to be particularly disadvantageous which call into question the above concept.
  • US Pat. No. 6,852,920 B2 discloses a solar cell with a nano-architecture in which two or more different materials with different electron affinities regularly alternate. For example, photons are absorbed and converted into pairs of holes and electrons, which are transported away separately by the different electron affinities.
  • the nano-architecture of US Pat. No. 6,852,920 B2 is produced by a mesoporous template.
  • the object of the invention is therefore to develop the generic composition such that it overcomes the disadvantages of the prior art, in particular improves the optical absorption of solar cells. In particular, the efficiency of solar cells should be increased and simpler device structures can be realized. It is a further object of the invention to provide a process for producing suitable solar cell materials.
  • the object of the composite composition is achieved according to the invention in that at least one domain of the stored guest material is dimensioned such that the average lifetime of the electron-hole pair that can be generated in the guest material by the action of radiation is sufficient for a transfer of the electron-hole pair into the matrix material ,
  • a domain is to be understood as meaning a coherent volume in the matrix which is formed or filled in by the guest material. Accordingly, the range of such a domain ranges from only a single absorbing molecule, such as an organic molecule such as polythiophene, through clusters to crystallites or (amorphous) agglomerates. Crystallites and agglomerates usually have an average diameter of up to 500 nm, preferably up to 100 nm.
  • the invention is based on the surprising finding that a composite composition which comprises a matrix material and at least one domain of at least one absorbent guest material, for example an organic dye pigment or an inorganic semiconductor cluster, is suitable for photovoltaic solar cells with a very high degree of efficiency in a structurally simple manner To make available.
  • a composite composition which comprises a matrix material and at least one domain of at least one absorbent guest material, for example an organic dye pigment or an inorganic semiconductor cluster, is suitable for photovoltaic solar cells with a very high degree of efficiency in a structurally simple manner To make available.
  • the separation of charge carriers from the matrix material ie in particular from a homogeneous semiconductor layer, is taken over.
  • the wavelength of the absorbed radiation should be such as to allow an electron-hole pair in the guest material.
  • the guest material essentially serves to absorb radiation under the effect of radiation and as a rule does not participate in the transport of the charges produced.
  • the function of the radiation absorption is separated from that of the charge carrier separation or the charge carrier transport.
  • This also has the advantage that the different materials, ie the guest material on the one hand and the matrix material on the other hand, can be optimized independently of each other.
  • the absorption of radiation of at least one wavelength occurs preferentially in the volume itself due to the domains embedded in the matrix.
  • the guest material is preferably selected so that radiation in the region of the terrestrial solar radiation is sufficient to produce an electron-hole pair.
  • a preferred embodiment of the invention is characterized in that the average diffusion length of the electron-hole pair formed in a domain is larger than the average diameter of the domain.
  • the diffusion length or the lifetime of an electron or a hole in the guest particle or the guest material generally depends on this material and the material quality.
  • a small particle size should be sought for organic pigments or an organic guest material in order to allow an effective charge transfer of the electron or the hole into the matrix.
  • transition domain / matrix is at least partially such that a charge carrier recombination is completely or partially suppressed.
  • the interface between the stored guest material and the host material, in particular silicon, should be prepared as free as possible from recombination states, so that no or almost no effective charge carrier recombination is to be expected at an internal phase boundary, in particular between the guest material and the matrix material.
  • the domain / matrix transition in particular the phase interface, is at least partially H-passivated in order to suppress the charge carrier recombination.
  • the embedded guest material domains have congruently grown into the matrix and / or c) at least one domain at least partially has at least one passivation layer.
  • An H-passivation represents, for example, a saturation of silicon-binding sites on a surface or interface such saturation can be achieved, for example, during a manufacturing process by adding hydrogen as a process gas.
  • the three alternative measures proposed above are intended to eliminate or suppress internal interfaces or problems which arise with internal interfaces between domain and matrix.
  • Interfaces in the matrix for example in a matrix of microcrystalline silicon, are impurities at which undesired recombination of the electron / hole pair formed can take place.
  • lattice-matched guest materials These guest materials preferably have the same lattice constant as the matrix material. This applies, for example, to FeSi 2 (guest material) and microcrystalline silicon (matrix).
  • the semiconductor material of the matrix is an indirect semiconductor.
  • An indirect semiconductor usually has good conduction properties due to its band structure of the conduction band and valence band. The intrinsic carrier lifetime and thus the diffusion length are generally sufficiently high to be considered as matrix material.
  • the indirect semiconductor material of the matrix preferably comprises crystalline, in particular microcrystalline, silicon.
  • the inventive composition according to the first embodiment makes it possible, in particular for thin-film solar cells made of silicon, to have a high level of absorptivity, for example using pigments as the guest material, while retaining the good transport properties of silicon.
  • the first embodiment of the composite composition is preferably resorted to a guest material, from whose valence band or HOMO from a hole of an electron-hole pair in the valence band of the matrix, in particular energetically favored, is transferable, and from its conduction band or LUMO from an electron of the electron-hole pair in the conduction band of the matrix, in particular energetically favored, is transferable.
  • An electron is transported by absorption of a photon from the HOMO or the valence band into the LUMO or the conduction band of the guest material.
  • the valence band or HOMO of the guest material generally has a lower energy level than the valence band of the matrix, so that the hole of a generated electron-hole pair without a Energy barrier can be transferred into the valence band of the matrix.
  • the conduction band or LUMO of the guest material is preferably arranged energetically above the conduction band of the matrix, so that the electron of the electron-hole pair can likewise be transmitted into the conduction band of the matrix without an energetic barrier.
  • the radiation energy absorbed in the guest materials by excitation of an electron-hole pair can be transferred into the matrix via a dipole-dipole interaction or via an exciton transfer.
  • this orbital arrangement that is, the placement of the LUMO or HOMO or guest band conduction band or valence band relative to the conduction band and valence band of the matrix, permits a direct, energetically favored transfer of excitons, i. of excited electrons or holes to get from the guest material into the matrix (Dexter transfer). If the excitation energy is transferred from the guest material into the matrix via a dipole-dipole interaction, this is also referred to as a so-called Förster transfer.
  • the guest material comprises at least one direct semiconductor material.
  • a guest material is preferably used in the first embodiment of the composite composition according to the invention together with an indirect semiconductor as matrix, in particular microcrystalline silicon.
  • a further preferred embodiment may provide that the guest material comprises at least one group II element and group VI element absorbing compound semiconductor and / or at least one Group III element and group V element absorbing compound semiconductor.
  • a guest material is preferably used in the first embodiment of the composite composition according to the invention having a matrix of an indirect semiconductor, in particular microcrystalline silicon.
  • the guest material comprises at least one semiconducting metal silicide compound, in particular FeSi 2 , preferably incorporated as a cluster.
  • a guest material is preferably used in the first embodiment of the composite composition according to the invention together with a matrix of an indirect semiconductor, in particular microcrystalline silicon.
  • the guest material comprises at least one organic pigment, in particular porphyrins and / or phthalocyanines, and / or organic semiconductors, especially polythiophenes.
  • a guest material in the first embodiment of the composite composition according to the invention is used together with a matrix of an indirect semiconductor, in particular microcrystalline silicon.
  • the composite composition according to the invention comprises zinc phthalocyanine (ZnPc) as intercalated guest material and microcrystalline silicon as semiconductor material of the matrix.
  • the guest material comprises an organic nanostructure, in particular in the form of fullerenes or nanotube structures.
  • such a guest material in the first embodiment of the composite composition according to the invention is used together with a matrix of an indirect semiconductor, in particular microcrystalline silicon.
  • the guest material comprises an inorganic nanostructure, in particular in the form of fullerenes or nanotube structures, preferably MoS 2 .
  • an indirect semiconductor in particular microcrystalline silicon.
  • the semiconductor material of the matrix is a direct semiconductor.
  • a direct semiconductor it is possible to further photon transition from the valence band to the conduction band of the matrix provide.
  • the semiconductor material of the matrix preferably comprises inorganic oxidic and / or chalcogenic materials.
  • a guest material which represents a donor / acceptor system capable of multiphoton absorption.
  • donor / acceptor systems incorporated in oxide or chalcogenide halides as matrix material
  • absorption of Radiation multiple photon transitions possible, which can realize very high efficiencies.
  • With a large bandgap donor / acceptor guest material embedded in a matrix material it is possible to use different photons of different energy or wavelength with their chemical potentials for energy conversion from radiation to electrical energy.
  • direct optical transitions in the matrix material can be utilized in the donor / acceptor guest material.
  • a donor / acceptor guest material is preferred in which a hole of an electron-hole pair in the valence band of the matrix, in particular energetically favored transferable from a HOMO of the donor, in which further of a LUMO of the donor from an electron of the electron-hole pair in a first LUMO of the acceptor, in particular energetically favored, is transferable, in which further from a second LUMO of the acceptor from the electron in the conduction band of the matrix, in particular energetically favored transferable ,
  • an electron which is located in the HOMO of a donor, which is arranged below the energy level of the valence band of the matrix is preferably transported into the LUMO of the donor by a first photon.
  • an electron in the LUMO of the donor generally has higher energy than an electron in the first LUMO of the acceptor, so that the electron in the LUMO of the donor can be transferred to the first LUMO of the acceptor.
  • the electron can then be transferred into the second LUMO of the acceptor. Since this generally has a higher energy level than the conduction band of the matrix, then finally a transfer of the electron takes place in its conduction band.
  • a donor / acceptor guest material is preferred in which a HOMO of the donor of a hole of an electron-hole pair in the valence band of the matrix, in particular energetically favored, is transferable from a LUMO of Donors from an electron of the electron-hole pair in a first LUMO of the acceptor, in particular energetically favorable transferable, and from a second energetically higher, unoccupied orbital (SUMO) of the acceptor from the electron into the conduction band of the matrix, in particular energetically favored , is transferable.
  • SUMO unoccupied orbital
  • an electron located in the HOMO of the donor which is located below the energy level of the valence band of the matrix, is transported by a first photon into the LUMO of the donor.
  • an electron in the LUMO of the donor generally has a higher energy than an electron in the LUMO of the acceptor, so that the electron in the LUMO of the donor can be transferred into the LUMO of the acceptor.
  • the electron can be transferred into the SUMO of the acceptor. Since this generally has a higher energy level than the conduction band of the matrix, then a transfer of the electron then takes place in its conduction band.
  • a donor-acceptor guest material in which an electron of an electron-hole pair is transferable from a LUMO of the donor into the conduction band of the matrix, particularly energetically favorably, from a HOMO of the donor from a hole of the electron-hole pair in a first HOMO of the acceptor, in particular energetically favored, is transferable, and transferable from an energetically deeper, occupied orbital (SOMO) of the acceptor from the hole in the valence band of the matrix, in particular energetically favored is.
  • SOMO energetically deeper, occupied orbital
  • an electron located in the donor's HOMO is excited by a photon to thereby first be transported into the LUMO of the donor and subsequently transferred to the valence band of the matrix.
  • the hole in the HOMO of the donor can then be transferred into a HOMO of the acceptor, if the HOMO of the acceptor for a hole is located more energetically favorably than the HOMO of the donor.
  • an electron can be transferred from the acceptor's SOMO to the acceptor's HOMO and, consequently, the hole from the acceptor's HOMO to the acceptor's SOMO.
  • the SOMO of the acceptor is usually arranged lower in energy than the valence band of the matrix. In this way, the hole from the acceptor's SOMO can enter the valence band of the matrix.
  • a donor / acceptor guest material is preferred in which a hole of a first electron-hole pair can be transferred from a HOMO of a donor into the valence band of the matrix, in particular energetically favored a LUMO of the acceptor from an electron of a second electron-hole pair in the conduction band of the matrix, in particular energetically favored, is transferable, and from a LUMO of the donor of an electron of the first electron-hole pair in the HOMO of the acceptor, in particular energetically favored, transferable.
  • an electron located in the acceptor's HOMO and transferred by photon excitation into the acceptor's LUMO can be derived from the acceptor LUMO of the acceptor are transferred into the conduction band of the matrix.
  • a second photon to be absorbed can then be used to transfer an electron from the donor's HOMO to the donor's LUMO so that the hole in the donor's HOMO, which is typically lower in energy than the valence band of the donor, enters the valence band is transferable.
  • the electron of the electron-hole pair produced by the second photon, when the acceptor HOMO is located lower in energy than the donor LUMO, can be transferred to the acceptor's HOMO.
  • suitable donor / acceptor systems have at least one organic color pigment system, in particular a porphyrin / quinone system and / or a thiophene / fullerene system.
  • a donor / acceptor system is preferably used in the second embodiment of the composite composition according to the invention with a direct semiconductor as the matrix.
  • the donor / acceptor system may comprise a combination of at least one first compound semiconductor of a group II element and one element of group VI and at least one second compound semiconductor of a group II element and a group VI element , in particular HgTe / CdTe.
  • a donor / acceptor system is used in the second embodiment of the composite composition according to the invention together with a direct semiconductor as the matrix.
  • the donor / acceptor system may comprise a combination of at least one group III element compound semiconductor and one element of group V and at least one second compound element II group member and one group VI element.
  • a donor / acceptor system in the second embodiment of the composite composition according to the invention is also used together with a direct semiconductor as the matrix.
  • the donor / acceptor system at least one biological absorber system, in particular chlorophyll and / or bacteriochlorophyll having.
  • a donor / acceptor system is used in the second embodiment of the composite composition according to the invention together with a direct semiconductor as a matrix.
  • the composite composition according to the invention comprises as embedded guest material F 16 ZnPc and as direct semiconductor material of the matrix ZnSe.
  • weight ratio of semiconductor material of the matrix / guest material in a range from 2: 1 to 500: 1, in particular from 5: 1 to 100: 1. Most preferred is a weight ratio of about 10: 1.
  • weight ratios are set with a matrix of an indirect semiconductor, in particular microcrystalline silicon.
  • the guest material domains are preferably present in the matrix as embedded clusters.
  • Clusters in the sense of the present invention are understood to mean small homogeneous phase regions of the material with virtually volume properties in a nanoscopic dimension, in particular to the limit of isolated molecular units. Accordingly, clusters in the sense of the present invention are understood as meaning those accumulations of guest material in a matrix which do not comprise a single molecule on the one side and are not present as crystallites on the other side. Guest material present as cluster in the matrix no longer has all the macroscopic properties of this guest material. For example, a guest material present in the form of a cluster may have a different melting point or, in the case of a semiconductor, a different energy gap than the guest material that is not in the form of a cluster.
  • the average diameter of the clusters used according to the invention is below 1 nm, preferably in the range of a few angstroms to a few hundred angstroms, for example 500 angstroms.
  • this information also depends on the nature of the guest material used.
  • the total volume of all the clusters incorporated therein is preferably in the range from 0.2 to 50%, particularly preferably in the range from 0.5 to 20% and in particular in the range from 2 to 10%.
  • the inventively embedded in the matrix domains of at least one guest material for example in the form of molecules or clusters in the composite composition according to the second embodiment as additional absorber (Generation Centers) for radiation.
  • Suitable guest materials generally include organic pigments, dye systems or inorganic semiconductors having a high absorptivity, for example direct semiconductors, with additional optical transitions.
  • the matrix material, also called host material may in particular comprise an elemental semiconductor, such as silicon, or a compound semiconductor, for example ZnSe, whose fundamental absorption can likewise be utilized photovoltaically.
  • the object on which the invention is based is furthermore achieved by a p-i-n semiconductor structure in which the intrinsic semiconductor material represents a composition according to the composite composition according to the invention.
  • the generated electron-hole pairs can thus be effectively separated and transported in the matrix material by electric fields from the manufactured component structure.
  • a photovoltaic solar cell which comprises at least one pin semiconductor structure according to the invention.
  • transparent oxidic layers This may be, for example, indium oxide doped with tin (In 2 O 3 : Sn, also called ITO) or tin oxide doped with antimony, thalium, niobium or tungsten (SnO 2 ISb, Ta Nb, W; ITO is essentially an In 2 O 3 / SnO 2 alloy.
  • this material is applied by sputtering.
  • TCO transparent contactive oxides
  • ZnO Al is also to be counted among these TCOs.
  • the intrinsic region is formed by the composition according to the invention, preferably a matrix of microcrystalline silicon added to domains of semiconducting guest material. By interaction with electromagnetic radiation, a field can be generated via such an intrinsic region.
  • the solar cell according to the invention preferably has an average thickness of less than 300 ⁇ m, particularly preferably less than 150 ⁇ m and in particular less than 30 ⁇ m. Thus, it is technically possible for the first time to offer effective thin-film solar cells.
  • the object relating to the method is achieved by co-depositing the guest material and the matrix material, in particular microcrystalline silicon, simultaneously or in particular sequentially from the gas phase on a substrate.
  • the most favorable deposition conditions are often dependent on the respective material combinations of matrix and guest material.
  • the guest material can be co-deposited simultaneously with the reactive components obtained from the starting material for the matrix, for example silane, from the gas phase.
  • the starting material for the matrix preparation and the guest material for example ZnPc
  • the material for the silicon matrix is continuously vapor deposited and the guest material sequentially, ie, at intervals.
  • the periods for the release intervals of silane or the reactive components obtained therefrom with a heating wire in a time window of, for example, 10 to 60 minutes, preferably 20 to 40 minutes, and the vaporization intervals for the guest material in the range of 1 to 10 minutes, preferably 3 to 7 minutes.
  • time interval windows adapted thereto can be selected.
  • microcrystalline silicon is carried out in the presence of hydrogen.
  • This hydrogen has the function, where appropriate, in addition to microcrystalline silicon also deposited amorphous silicon again to passivate and passivate any impurities.
  • the matrix, in particular microcrystalline silicon, and / or the guest material are co-deposited, in particular on a glass substrate.
  • Be particularly advantageous has proved to be the matrix material in particular microcrystalline silicon, and / or the guest material, such as organic absorbent materials, at temperatures ranging from 230 0 C to 290 ° C, in particular of 25O 0 C to 270 ° C to deposit. At these temperatures it is generally ensured that, on the one hand, the guest material is not destroyed and, on the other hand, that the matrix material grows up in a desired crystal form, for example in the case of silicon in microcrystalline form. Particularly suitable are temperatures in the range of about 260 ° C. This is particularly preferred for the production of microcrystalline silicon as a matrix material, in particular next to a temperature in the range of about 26O 0 C, with relatively low silane concentrations especially high pressures worked.
  • the concentration of silane in the preparation of the silicon matrix is in the range of 0.5 to 10%, preferably in the range of 1 to 5%, and more preferably in the range of 1.5 to 3%, for example 2%.
  • the pressure in the production of microcrystalline silicon in evaporator deposition is preferably in the range of 2 to 10 Pa, more preferably in the range of 4 to 8 Pa and most preferably in the range of 5 to 7 Pa, for example at 6 Pa.
  • a preferred embodiment is characterized by the use of a, in particular thermally shielded, hot-wire CVD or a Knudsen cell.
  • the use of a thermally at least partially shielded heating wire is to be understood, so that formed on this heating wire in the presence of silane reactive gaseous species can escape substantially only in the direction of the substrate support for the purpose of deposition and the co-vaporized guest material is no longer exposed to the direct thermal load of the heating wire, but can reach the substrate carrier non-destructive.
  • the use of a shutter e.g. with a narrow exit slit or hole, thus preferably not required.
  • An alternative embodiment of the method according to the invention provides layer sequences, in particular multilayer systems, containing at least one layer of a semiconductor material of the matrix, in particular of microcrystalline silicon, and at least one layer of at least one guest material, in particular FeSi 2 or Fe, an annealing and / or a Undergo laser annealing step.
  • a further alternative embodiment of the method according to the invention provides chemically deposited guest materials, in particular pigment clusters, dissolved in the liquid phase or in electrolytes on a layer of a semiconductor material of the matrix, in particular by sol-gel method or solvothermal method as well as hydrothermal synthesis.
  • a further alternative embodiment of the method according to the invention provides for mechanically mixing the semiconductor material of the matrix and the guest material, in particular by means of a ball mill, and then sintering.
  • a further alternative embodiment of the method according to the invention provides infiltrating porous semiconductor material of the matrix with liquefied or dissolved guest material, in particular pigments, and subjecting the infiltrated semiconductor material to an annealing step.
  • hydrogen it is possible for hydrogen to be used as the process gas in the process according to the invention. This serves, in particular, to saturate bonding sites on a surface or interface in the case of a silicon matrix, in order to achieve H passivation.
  • the proportion of hydrogen in a microcrystalline silicon matrix can be varied by the process control.
  • hydrogen in the production of microcrystalline silicon generally also serves to reverse the undesirable formation of amorphous silicon.
  • inorganic clusters of highly absorbent semiconductor materials as a guest material the absorption by excitation of an electron via an energy gap between valence band and conduction band of the guest material and the transfer of the excited electrons or holes from the conduction band of the semiconductor cluster of the guest material in the conduction band of the matrix material, in particular a silicon host material, and the hole from the valence band of the guest material into the valence band of the matrix material or of the host material.
  • both components of the excited electron-hole pair are transferred to the same matrix material, particularly microcrystalline silicon.
  • the absorption and transfer process is not limited only to an interface, but can take place in the volume. Therefore, solid solar cells according to the invention are also possible using the established semiconductor material silicon without the use of electrolyte contacts, so that in particular the resulting stability problems can be avoided.
  • a strongly directly absorbing constituent is preferably incorporated as guest material in microcrystalline silicon as matrix material.
  • thin-film solar cells made of silicon become accessible with high absorptivity.
  • the use of bulk silicon composites as a matrix material containing embedded domains of a guest material thus provides the opportunity to couple the benefits of silicon as an electronically highly manageable matrix material with high light absorption of the guest material.
  • Silicon-based solar cells can be produced inexpensively and energetically advantageously, for example as thin-film semiconductor material, and thus help to establish photovoltaics as an economically competitive source of primary energy.
  • the established silicon deposition methods can be used further. These methods are generally only to be modified with regard to the code positions of the guest materials.
  • FIG. 1 shows a schematic representation of a p + -i-n + component of a solar cell with a composition according to the invention in the first embodiment
  • Figure 2 the electronic band structure of a solar cell with an inventive
  • FIG. 4 shows the optical absorption of pure ZnPc films in ⁇ - and ⁇ -modification and of compositions according to FIG. 3;
  • FIG. 5 shows a schematic representation of a p-i-n component of a solar cell with a composition according to the invention according to the second embodiment
  • FIG. 6 shows a donor-acceptor system of the second embodiment of the inventive composition
  • FIG. 7 a shows a first schematic electronic band structure and optical transitions of the composition according to the invention according to the second embodiment
  • Figure 7b the first schematic electronic band structure and optical transitions in the composition according to the invention according to the second embodiment in a simplified scheme
  • FIG. 7c shows a second schematic electronic band structure and optical transitions of the inventive composition according to the second embodiment
  • FIG. 7d shows a third schematic electronic band structure and optical transitions of the composition according to the invention according to the second embodiment
  • FIG. 8 Raman spectra of ZnSe / F 16 ZnPc composites with different ZnPc
  • FIG. 9 the optical absorption of pure F 16 ZnPc and of ZnSe / F 16 ZnPc
  • Figure 10 photographs of ZnSe, F 16 ZnPc and ZnSe / F 16 ZnPc compositions with increasing concentration
  • FIG. 11 shows a reactor for producing a composition according to the invention
  • FIG. 12 shows an alternative embodiment according to the invention of the reactor according to FIG. 11.
  • FIG. 13 a schematic representation of a section of the reactor according to FIG. 12.
  • the p + -i-n + device 1 of the solar cell further has, opposite and adjacent to the top and bottom of the intrinsic semiconductor layer comprising the composition 2, an n + region 7 (heavily n-doped region) and a p + region 9 (heavily p-doped region).
  • FIG. 2 shows a schematic electronic band structure of the p + -i-n + component 1 of the solar cell according to FIG.
  • the inventive composition according to the first embodiment functions as intrinsic semiconductor i between the p + -doped region 9 and the n + -doped region 7.
  • the Fermi level is denoted by Ep, the valence band by EV B, and the conduction band by EL.
  • Crystalline silicon has good electrical transport properties due to its characteristic indirect band gap, but also a low absorptivity of radiation.
  • the electron from the guest occupied LUMO 13 is transferred to the conduction band E L of the matrix material and the hole from the HOMO 11 of the guest material is transferred to the valence band E VB of the matrix material (injection). Subsequently, electron and hole are transported separately in the quasi-homogeneous semiconductor matrix material, ie in the indirect semiconductor silicon, by electric fields of the pin device structure, which is represented in FIG. 2 by a hole movement direction 17 and electron movement direction 19.
  • FIG. 3 shows Raman spectra of pure microcrystalline silicon, pure ZnPc and composite compositions of these materials which were deposited as the substrate temperature increased.
  • Raman spectra reflect molecular vibrations and are therefore a sensitive criterion for the survival of molecular bonds.
  • a substrate temperature of 260 ° C all the excitations characteristic of ZnPc and microcrystalline silicon are found, with the excitations of microcrystalline silicon indicated by an arrow.
  • the intensity ratios of ZnPc vibrations are partially varied due to different environments in the composite.
  • the spectrum at 26O 0 C shows that organic pigments and microcrystalline silicon can be codepositioned in a sequential process. From 300 0 C substrate temperature are traces only of ZnPc.
  • FIG. 4 shows the optical absorption of pure ZnPc in ⁇ - and ⁇ -modification and of composite compositions according to FIG. 2.
  • the optical absorption also indicates the integrity of the molecules used.
  • the basic function of the Sorption of photons of a radiation checked.
  • the structures in the range of 550 nm to 850 nm show that the Q-band absorption of ZnPc in the composite is retained.
  • FIG. 5 shows a pin component 100 of a solar cell according to the second embodiment of the composition 102 according to the invention.
  • the composition 102 comprises a matrix material 105 having a large energy gap of an oxide semiconductor or a chalcogenide semiconductor in which domains 103 of a guest material containing a donor / acceptor system are intercalated.
  • the pin component 100 of the solar cell comprises an opposing n + region 107 and a p + region 109. Like the solar cell 1 from FIG. 1, the solar cell also has a pin component structure.
  • the charge carrier separation does not take place on a single hetero-interface, as in the case of the solar cell with an absorber / electrolyte boundary layer discussed above in the prior art, but within the matrix material 105
  • Figures 6 and 7a illustrate the function of the donor / acceptor system.
  • the matrix material 105 in the second embodiment of the composition 102 has a valence band EV B and a conduction band EL.
  • a direct transition 110 of an electron from the valence band EV B into the conduction band E L of the matrix material 105 can take place by a first absorption of a first photon 111.
  • a second electron can pass from the HOMO 1 to the LUMO 1 of the donor 114. Subsequently, the second electron is transferred to the energetically favorable LUMO 2 of the acceptor 116. By absorption of a third photon 118, the second electron is transferred from LUMO 2 to (LUMO + 1) 2 of the acceptor. Finally, from the (LUMO + 1) 2, the second electron passes into the conduction band E L. Thus, the LUMO 2 state of the acceptor is filled by transfer of the excited second electron from LUMO 1 of the donor.
  • This charge transfer suppresses a back reaction from the LUMO 1 of the donor to the HOMO 1 .
  • the hole in the HOMO 1 state of the donor is injected into the valence band EVB of the matrix material 105 and the absorption process can start anew. In this way, multiple photons with their respective chemical potentials are used for the energy conversion of radiation, allowing theoretical efficiencies of up to 42%.
  • the electron-hole pairs injected into the matrix material 105 are separated by electric fields transmitted through the pinhole.
  • Component structure 100 of the solar cell can be produced with the inventive composition 102 as an intrinsic absorber.
  • FIG. 7b shows the first electronic band structure of FIG. 7a of a donor / acceptor system in a simplified scheme.
  • the HOMO 1 of the donor 211 is located lower in energy than the valence band EVB of the matrix.
  • the donor 214 provides a first optical junction 212 from the donor 214 HOMO 1 211 to the donor 214 LUMO 1 213 so that upon absorption of a photon, an electron is transferred from the HOMOj 211 to the LUMO 1 213, thereby forming an electron hole pair is produced.
  • the electron is transferred from LUMO 1 213 of donor 214 to LUMO 2 215 of acceptor 216 because LUMO 2 215 of acceptor 216 has a lower energy level than LUMO 1 213 of donor 214.
  • a second optical junction 218 can transmit the electron from the LUMO 2 215 to the SUMO 219 of the acceptor 216.
  • the electron of the electron-hole pair transitions into the conduction band Ei of the matrix.
  • the LUMO 2 215 of the acceptor 216 is filled above the LUMO 1 213 state of the donor 214.
  • FIG. 7c shows a second electronic band structure of a donor / acceptor system according to the second embodiment.
  • the electron is first transferred into the LUMO 1 313 of the donor 314 by means of a first optical junction 312, that is, an excitation by absorption of a first photon, so that an electron hole Pair is generated.
  • the electron can then pass into it due to the lower energy position of the conduction band E L of the matrix material.
  • the hole of this first electron-hole pair located in the HOMOi 311 of the donor is then transferred to the HOMO 2 315 of the acceptor 316, since the HOMO 2 315 of the acceptor 316 for the hole is located more energetically than the HOMOi 311 of the donor 314.
  • a second optical junction 318 may transmit an electron from the SOMO 2 located lower than the valence band EVB of the matrix material into the HOMO 2 315 of the acceptor 316.
  • the hole of the electron-hole pair is now in the SOMO 2 317 of the acceptor 316 and can finally be inserted into the valence energy that is more favorable for the hole. band EVB of the matrix material are transferred. Now also the absorption process can start anew.
  • FIG. 7d shows a third schematic electronic band structure of the composition according to the invention in the second embodiment.
  • a donor 414 has a HOMO 2 411 and a LUMO 2 413
  • an acceptor 416 has a HOMO 1 415 and a LUMO 417.
  • the HOMO 1 of the acceptor 416 is located lower in energy than the LUMO 2 413 of the donor 414.
  • both the HOMO 1 415 of the acceptor 416 and the HOMO 2 411 of the donor are filled with at least one electron.
  • first optical transition 418 produced by absorption of a first photon, that is to say an excitation of a first electron
  • the first electron is first transferred from the HOMO 1 415 to the LUMO 1 417, so that a first electron-hole pair is formed.
  • a second photon By absorption of a second photon, a second electron is transferred via the second optical junction 412 from the donor's HOMO 2 411 to the donor's LUMO 2 413 to form a second electron-hole pair.
  • the electron of the second electron-hole pair then passes from the donor's LUMO 2 413 to the more energetically favorable HOMO 1 415 of the acceptor, or the hole of the first electron-hole pair passes from the HOMO 1 415 into the energy that is more favorable for the hole LUMO 2 413 of the donor over.
  • the electron from the first electron-hole pair is transferred from the LUMO 1 417 of the acceptor into the more energy-efficient conduction band EL of the matrix material, as well as the hole of the second electron-hole pair transferred into the valence band E VB which is more energy-efficient for the hole becomes.
  • the intercalated domains 103 of the donor / acceptor guest material are spatially in the form of the appropriate passivation of the matrix material of the invention Matrix material 105 separated, whereby also an electronic separation between the guest material and the matrix material is made possible.
  • the advantage is that the desired electron and hole transfer enters the bands of the matrix material (downhill charge injection).
  • Figure 8 shows the Raman spectra of ZnSe / Fi ö ZnPc composite compositions with increasing ZnPc concentration.
  • ZnPc shows in the composites all the typical excitations of the pure material.
  • FIG. 9 shows the optical absorption of pure F 16 ZnPc and of ZnSe / F 16 ZnPc composite compositions. Due to different environments, the width of the Q band is lower for the dye molecules in the composite.
  • Figure 10 shows photographs of ZnSe, F 16 ZnPC and ZnSe / F 16 ZnPc compositions with increasing concentration.
  • FIG. 11 shows a reactor 1000 in which a microcrystalline silicon sample 1004 which has already been deposited is arranged in a reactor vessel 1001 under a sample heater 1002.
  • the reactor 1000 further includes a source 1006 for the vaporization of one, especially organic, guest material, e.g. ZnPc on.
  • the reactor 1000 includes a pump system 1008 fluidly connected to the reactor vessel 1001 via a throttle valve 1010 upstream of the pump system. On the other side, ie downstream of the pump system 1008, an exhaust pipe 1012 is provided.
  • the reactor 1000 has a cooling water inlet 1014, a pyrometer 1016 and an electrical feedthrough 1018.
  • thermally shielded "hot wire” (HW) source for the deposition of SiH 4.
  • the thermal shielding of the heating wire succeeds, for example, by attaching a lateral jacket 1020 of the heating wire 1022, as shown in Figures 11 and 12.
  • the thermal shield 1020 may surround the heating wire 1022 laterally full extent, for example by using a cylindrical shield, or this heating wire only partially regionally. cover, so that still always sufficient thermal shielding succeeds. In this way, the gaseous guest material fed via the source 1006 can be applied to the sample without damage.
  • the thermal sheath 1020 may partially cover the side facing the carrier or silicon sample and, as shown, leave only one exit gap or hole open, as in the case of a diaphragm.
  • the opening diameter of the silane source should not be too small.
  • an opening having a diameter of 20 mm is used at a helix length of the HW source of 12 mm.
  • the thermal shield 1020 may be limited only to the side regions of the heating wire, so that it is not necessary to shield the heating wire in the direction of the substrate carrier or the silicon sample.
  • the silicon deposition for the matrix material is usually carried out in the flow.
  • the flows of silane and H 2 are controlled by two mass flow controllers to a constant value. With the ratio of the flow rates of silane and H 2 , the desired concentration is set.
  • the pressure in the reactor vessel 1001 by a regulation between the mass flow controllers and the throttle valve 1010 should, which is advantageously present in a butterfly valve of a suction pipe is to be kept constant at about 10 '2 bar. This applies in particular when using a 2% silane concentration in the process gas.
  • For sequential deposition see also FIG.
  • the gas supply of a silicon source is alternately interrupted via a first cutter 1024 and opened via a second shutter 1026 of a guest material source 1006 and vice versa, as shown schematically in FIG. 13, process gas supplied while the second shutter 1026 of the guest material source 1006 is closed.
  • Hot Wire Chemical Vapor Deposition a reaction product of a process gas separates out as a solid layer on a substrate surface.
  • the activation energy required for this purpose is supplied by the hot substrate.
  • Hot wire CVD activates the deposition process by reacting the process gas in the gas phase on a hot wire.
  • the hot wire acts in two ways, it provides the activation energy for the desired reactions and acts as a catalyst for this reaction. Actions. In this way, the deposition process can be carried out at lower substrate temperature.
  • the composite composition according to the invention by means of a Physical Vapor Deposition (PVD).
  • PVD Physical Vapor Deposition
  • a guest material is converted by heating in the gas phase, whereupon it deposits on a substrate.
  • This deposition process is particularly advantageous for organic absorber pigments as a guest material.
  • the control of the flow is via the source temperature.

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Abstract

L'invention concerne une composition composite comprenant au moins un matériau semi-conducteur en tant que matrice, dans laquelle est inséré au moins un domaine d'au moins un matériau hôte apte à absorber le rayonnement d'au moins une longueur d'onde et à générer au moins une paire d'électron-trou sous l'effet du rayonnement. Au moins un domaine du matériau hôte inséré est dimensionné de manière à ce que la durée de vie moyenne de la paire d'électron-trou générée sous l'effet du rayonnement dans le matériau hôte suffise pour un transfert de la paire d'électron-trou dans le matériau de la matrice. La présente invention porte également sur une structure semi-conductrice p-i-n dont le matériau semi-conducteur intrinsèque a une composition correspondant à une des revendications préalables. L'invention concerne aussi une cellule solaire photovoltaïque comportant au moins une structure semi-conductrice p-i-n selon l'invention. Enfin, l'invention porte sur un procédé de réalisation des compositions composites susmentionnées.
PCT/DE2006/002334 2005-12-23 2006-12-22 Composition composite pour cellule solaire, structure semi-conductrice p-i-n comportant cette composition, cellule solaire et procede de realisation de compositions composites WO2007076843A1 (fr)

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WO2014001817A1 (fr) * 2012-06-29 2014-01-03 Cambridge Enterprise Limited Dispositif photovoltaïque et son procédé de fabrication
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