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Sample records for layered perovskite structure

  1. Electronic structure of the superconducting layered perovskite niobate

    NASA Astrophysics Data System (ADS)

    Hase, Izumi; Nishihara, Yoshikazu

    1998-07-01

    The electronic energy-band structure for RbLaNb2O7, which is closely related to the layered perovskite niobate superconducting KCa2Nb3O10 and metallic KLaNb2O7 with Li intercalation, has been calculated by using the scalar-relativistic full-potential linearized augmented-plane-wave method within the local-density approximation. The result of the calculation shows that this compound is a band insulator with a small gap, and its conduction band is a typical two-dimensional one and the valence band is rather three dimensional. We can conclude that the layered perovskite niobate KCa2Nb3O10 is a band insulator that can be superconducting with electron doping, and have the highly two-dimensional electronic structure.

  2. Crystal Structure of a Layered Perovskite Niobate KCa 2Nb 3O 10

    NASA Astrophysics Data System (ADS)

    Fukuoka, Hiroshi; Isami, Toshiyuki; Yamanaka, Shoji

    2000-04-01

    The crystal structure of a layered perovskite niobate KCa2Nb3O10 was investigated through single-crystal X-ray analysis. The niobate crystallized in the orthorhombic system Cmcm with lattice constants of a=3.8802(9) Å, b=29.508(6) Å, c=7.714(1) Å, V=883.2(2) Å3. The final refinement using the 908 independent reflections converged into R=4.1%, and Rw=4.7%. The structure of KCa2Nb3O10 was composed of triple-layered perovskite slabs, potassium ions being situated between the slabs. The adjacent perovskite slabs, stacking along the c axis, were mutually displaced with a displacement vector of a→/2. The potassium ions were coordinated by six oxygen atoms to form two short and four long bonds. Apparent disordering was observed in the equatorial oxygen sites of the central niobium atoms in the triple perovskite slabs.

  3. Research Update: The electronic structure of hybrid perovskite layers and their energetic alignment in devices

    NASA Astrophysics Data System (ADS)

    Olthof, Selina

    2016-09-01

    In recent years, the interest in hybrid organic-inorganic perovskites has increased at a rapid pace due to their tremendous success in the field of thin film solar cells. This area closely ties together fundamental solid state research and device application, as it is necessary to understand the basic material properties to optimize the performances and open up new areas of application. In this regard, the energy levels and their respective alignment with adjacent charge transport layers play a crucial role. Currently, we are lacking a detailed understanding about the electronic structure and are struggling to understand what influences the alignment, how it varies, or how it can be intentionally modified. This research update aims at giving an overview over recent results regarding measurements of the electronic structure of hybrid perovskites using photoelectron spectroscopy to summarize the present status.

  4. New hybrid lead iodides: From one-dimensional chain to two-dimensional layered perovskite structure

    SciTech Connect

    Xiong, Kecai; Liu, Wei; Teat, Simon J.; An, Litao; Wang, Hao; Emge, Thomas J.; Li, Jing

    2015-10-15

    Two new hybrid lead halides (H{sub 2}BDA)[PbI{sub 4}] (1) (H{sub 2}BDA=1,4-butanediammonium dication) and (HNPEIM)[PbI{sub 3}] (2) (HNPEIM=N-​phenyl-ethanimidamidine cation) have been synthesized and structurally characterized. X-ray diffraction analyses reveal that compound 1 features a two-dimensional corner-sharing perovskite layer whereas compound 2 contains one-dimensional edge-sharing double chains. The N-​phenyl-ethanimidamidine cation within compound 2 was generated in-situ under solvothermal conditions. The optical absorption spectra collected at room temperature suggest that both compounds are semiconductors having direct band gaps, with estimated values of 2.64 and 2.73 eV for 1 and 2, respectively. Results from the density functional theory (DFT) calculations are consistent with the experimental data. Density of states (DOS) analysis reveals that in both compounds 1 and 2, the energy states in the valence band maximum region are iodine 5p atomic orbitals with a small contribution from lead 6s, while in the region of conduction band minimum, the major contributions are from the inorganic (Pb 6p atomic orbitals) and organic components (C and N 2p atomic orbitals) in compound 1 and 2, respectively. - Graphical abstract: Two new hybrid lead halides built on one-dimensional edge-sharing double chains and two-dimensional corner-sharing perovskite layers are synthesized and their structural and electronic properties are analyzed. - Highlights: • Two new hybrid lead iodides are designed, synthesized, and characterized. • They are closely related to, but different from, perovskite structures. • The electronic properties of both compounds are analyzed by DFT calculations.

  5. A two-layer structured PbI2 thin film for efficient planar perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Ying, Chao; Shi, Chengwu; Wu, Ni; Zhang, Jincheng; Wang, Mao

    2015-07-01

    In this paper, a two-layer structured PbI2 thin film was constructed by the spin-coating procedure using a 0.80 M PbI2 solution in DMF and subsequent close-spaced vacuum thermal evaporation using PbI2 powder as a source. The bottom PbI2 thin film was compact with a sheet-like appearance, parallel to the FTO substrate, and can be easily converted to a compact perovskite thin film to suppress the charge recombination of the electrons of the TiO2 conduction band and the holes of the spiro-OMeTAD valence band. The top PbI2 thin film was porous with nano-sheet arrays, perpendicular to the FTO substrate, and can be easily converted to a porous perovskite thin film to improve the hole migration from the perovskite to spiro-OMeTAD and the charge separation at the perovskite/spiro-OMeTAD interface. The planar perovskite solar cells based on the two-layer structured PbI2 thin film exhibited a photoelectric conversion efficiency of 11.64%, along with an open-circuit voltage of 0.90 V, a short-circuit photocurrent density of 19.29 mA cm-2 and a fill factor of 0.67.

  6. A two-layer structured PbI2 thin film for efficient planar perovskite solar cells.

    PubMed

    Ying, Chao; Shi, Chengwu; Wu, Ni; Zhang, Jincheng; Wang, Mao

    2015-07-28

    In this paper, a two-layer structured PbI2 thin film was constructed by the spin-coating procedure using a 0.80 M PbI2 solution in DMF and subsequent close-spaced vacuum thermal evaporation using PbI2 powder as a source. The bottom PbI2 thin film was compact with a sheet-like appearance, parallel to the FTO substrate, and can be easily converted to a compact perovskite thin film to suppress the charge recombination of the electrons of the TiO2 conduction band and the holes of the spiro-OMeTAD valence band. The top PbI2 thin film was porous with nano-sheet arrays, perpendicular to the FTO substrate, and can be easily converted to a porous perovskite thin film to improve the hole migration from the perovskite to spiro-OMeTAD and the charge separation at the perovskite/spiro-OMeTAD interface. The planar perovskite solar cells based on the two-layer structured PbI2 thin film exhibited a photoelectric conversion efficiency of 11.64%, along with an open-circuit voltage of 0.90 V, a short-circuit photocurrent density of 19.29 mA cm(-2) and a fill factor of 0.67. PMID:26118756

  7. Hierarchically Structured Hole Transport Layers of Spiro-OMeTAD and Multiwalled Carbon Nanotubes for Perovskite Solar Cells.

    PubMed

    Lee, Jiyong; Menamparambath, Mini Mol; Hwang, Jae-Yeol; Baik, Seunghyun

    2015-07-20

    The low electrical conductivity of spiro-OMeTAD hole transport layers impedes further enhancements of the power conversion efficiency (PCE) of perovskite solar cells. We embedded multiwalled carbon nanotubes (MWNTs) in spiro-OMeTAD (spiro-OMeTAD/MWNTs) to increase carrier mobility and conductivity. However, direct electrical contact between CH3 NH3 PbI3 and the MWNTs created pathways for undesirable back-electron transfer, owing to the large work function of MWNTs, limiting enhancements of the PCE. A hierarchical structure of pure spiro-OMeTAD and spiro-OMeTAD/MWNTs was designed to block back-electron transfer and fully exploit the enhanced charge transport of spiro-OMeTAD/MWNTs. The enhanced fill factor, short-circuit current density, open-circuit voltage, and PCE (15.1 %) were achieved by using this hierarchical hole transport layer structure (MWNT concentration=2 wt %). The perovskite solar cells were fabricated by a low-temperature solution process, further decreasing their per-Watt cost.

  8. Structure and dehydration of layered perovskite niobate with bilayer hydrates prepared by exfoliation/self-assembly process

    SciTech Connect

    Chen Yufeng; Zhao Xinhua; Ma Hui; Ma Shulan; Huang Gailing; Makita, Yoji; Bai Xuedong; Yang Xiaojing

    2008-07-15

    The crystals of an H-form niobate of HCa{sub 2}Nb{sub 3}O{sub 10}.xH{sub 2}O (x=0.5) being tetragonal symmetry (space group P4/mbm) with unit cell parameters a=5.4521(6) and c=14.414(2) A were exfoliated into nanosheets with the triple-layered perovskite structure. The colloid suspension of the nanosheets was put into dialysis membrane tubing and allowed self-assembly in a dilute KCl solution. By this method, a novel layered K-form niobate KCa{sub 2}Nb{sub 3}O{sub 10}.xH{sub 2}O (x=1.3, typically) with bilayer hydrates in the interlayer was produced. The Rieveld refinement and transmission electron microscope (TEM)/selected-area electron diffraction (SAED) observation indicated that the orientations of the a-/b-axis of each nanosheet as well as the c-axis are uniform, and the self-assembled compound had the same symmetry, tetragonal (P4/mbm) with a=5.453(2) and c=16.876(5) A, as the H-form precursor; the exfoliation/self-assembly process does not markedly affect the two-dimensional lattice of the layer. The large basal spacing resulted from the interlayer K{sup +} ions solvated by two layers of water molecules. The interlayer bilayers-water was gradually changed to monolayer when the temperatures higher than 100 deg. C, and all the water molecules lost when over 600 deg. C. Accompanying the dehydration, the crystal structure transformed from tetragonal to orthorhombic symmetry. Water molecules may take an important role for the layer layered compound to adjust the unit cell to tetragonal symmetry. - Graphical abstract: The structure of layered perovskite niobate KCa{sub 2}Nb{sub 3}O{sub 10}.xH{sub 2}O (x=1.3) having a bilayers-hydrates interlayer, obtained via the exfoliation of an H-form precursor and the self-assembly of Ca{sub 2}Nb{sub 3}O{sub 10}{sup -} nanosheets, was first discussed in detail and determined to be tetragonal symmetry (P4/mbm). The dehydration resulted in the structural transformation to orthorhombic structure.

  9. Perovskite thin films via atomic layer deposition.

    PubMed

    Sutherland, Brandon R; Hoogland, Sjoerd; Adachi, Michael M; Kanjanaboos, Pongsakorn; Wong, Chris T O; McDowell, Jeffrey J; Xu, Jixian; Voznyy, Oleksandr; Ning, Zhijun; Houtepen, Arjan J; Sargent, Edward H

    2015-01-01

    A new method to deposit perovskite thin films that benefit from the thickness control and conformality of atomic layer deposition (ALD) is detailed. A seed layer of ALD PbS is place-exchanged with PbI2 and subsequently CH3 NH3 PbI3 perovskite. These films show promising optical properties, with gain coefficients of 3200 ± 830 cm(-1) .

  10. Layered hybrid perovskites with micropores created by alkylammonium functional silsesquioxane interlayers.

    PubMed

    Kataoka, Sho; Banerjee, Subhabrata; Kawai, Akiko; Kamimura, Yoshihiro; Choi, Jun-Chul; Kodaira, Tetsuya; Sato, Kazuhiko; Endo, Akira

    2015-04-01

    Layered organic-inorganic hybrid perovskites that consist of metal halides and organic interlayers are a class of low-dimensional materials. Here, we report the fabrication of layered hybrid perovskites using metal halides and silsesquioxane with a cage-like structure. We used a silsesquioxane as an interlayer to produce a rigid structure and improve the functionality of perovskite layers. Propylammonium-functionalized silsesquioxane and metal halide salts (CuCl2, PdCl2, PbCl2, and MnCl2) were self-assembled to form rigid layered perovskite structures with high crystallinity. The rigid silsesquioxane structure produces micropores between the perovskite layers that can potentially be filled with different molecules to tune the dielectric constants of the interlayers. The obtained silsesquioxane-metal halide hybrid perovskites exhibit some characteristic properties of layered perovskites including magnetic ordering (CuCl4(2-) and MnCl4(2-)) and excitonic absorption/emission (PbCl4(2-)). Our results indicate that inserting silsesquioxane interlayers into hybrid perovskites retains and enhances the low-dimensional properties of the materials.

  11. p-i-n/n-i-p type planar hybrid structure of highly efficient perovskite solar cells towards improved air stability: synthetic strategies and the role of p-type hole transport layer (HTL) and n-type electron transport layer (ETL) metal oxides.

    PubMed

    Mali, Sawanta S; Hong, Chang Kook

    2016-05-19

    There has been fast recent progress in perovskite solar cells (PSCs) towards low cost photovoltaic technology. Organometal mixed halide (MAPbX or FAPbX) perovskites are the most promising light absorbing material sandwiched between the electron transport layer (ETL) and hole transport layer (HTL). These two layers play a critical role in boosting the power conversion efficiency (PCE) and maintaining air stability. However, the device stability is a serious issue in regular as well as p-i-n inverted type perovskite solar cells. This mini-review briefly outlines the state-of-art of p-i-n/n-i-p type planar hybrid perovskite solar cells using MAPbX/FAPbX perovskite absorbing layers. Later, we will focus on recent trends, progress and further opportunities in exploring the air stable hybrid planar structure PSCs.

  12. p-i-n/n-i-p type planar hybrid structure of highly efficient perovskite solar cells towards improved air stability: synthetic strategies and the role of p-type hole transport layer (HTL) and n-type electron transport layer (ETL) metal oxides

    NASA Astrophysics Data System (ADS)

    Mali, Sawanta S.; Hong, Chang Kook

    2016-05-01

    There has been fast recent progress in perovskite solar cells (PSCs) towards low cost photovoltaic technology. Organometal mixed halide (MAPbX or FAPbX) perovskites are the most promising light absorbing material sandwiched between the electron transport layer (ETL) and hole transport layer (HTL). These two layers play a critical role in boosting the power conversion efficiency (PCE) and maintaining air stability. However, the device stability is a serious issue in regular as well as p-i-n inverted type perovskite solar cells. This mini-review briefly outlines the state-of-art of p-i-n/n-i-p type planar hybrid perovskite solar cells using MAPbX/FAPbX perovskite absorbing layers. Later, we will focus on recent trends, progress and further opportunities in exploring the air stable hybrid planar structure PSCs.

  13. Synthesis and structure of Ba{sub 6}Co{sub 6}ClO{sub 16}, a new cobalt oxychloride with a layered perovskite-related structure

    SciTech Connect

    Tancret, Nathalie; Roussel, Pascal; Abraham, Francis . E-mail: francis.abraham@ensc-lille.fr

    2005-10-15

    Well-developed single crystals of the title compound were prepared using a BaCl{sub 2} flux and investigated by X-ray diffraction methods using Mo(K{alpha}) radiation and a Charge Coupled Device (CCD) detector. The crystal structure was solved and refined in the hexagonal symmetry with P6-bar m2 space group, a=5.6698(2)A and c=14.4654(5)A to a final R{sub 1}=0.022 for 44 parameters with 1418 individual reflections. The structure of Ba{sub 6}Co{sub 6}ClO{sub 16}, which is related to the 6H-perovkite-type structure of BaMnO{sub 2.88}, is formed by the periodic stacking along [001] of five [BaO{sub 3}] layers separated by a [BaOCl] with a (hhhchc) stacking sequence. The [BaO{sub 3}] stacking creates tetranuclear face sharing octahedra units Co{sub 4}O{sub 15} containing Co(III) connected by dimers of corner-sharing CoO{sub 4} tetrahedra. This new oxychloride belongs to the family of compounds formulated as [BaOCl]M'{sub 2}[Ba{sub n+1}M{sub n}O{sub 3n+3}] where n represents the thickness of the octahedral string in hexagonal perovskite slabs.

  14. Aluminum-Doped Zinc Oxide as Highly Stable Electron Collection Layer for Perovskite Solar Cells.

    PubMed

    Zhao, Xingyue; Shen, Heping; Zhang, Ye; Li, Xin; Zhao, Xiaochong; Tai, Meiqian; Li, Jingfeng; Li, Jianbao; Li, Xin; Lin, Hong

    2016-03-01

    Although low-temperature, solution-processed zinc oxide (ZnO) has been widely adopted as the electron collection layer (ECL) in perovskite solar cells (PSCs) because of its simple synthesis and excellent electrical properties such as high charge mobility, the thermal stability of the perovskite films deposited atop ZnO layer remains as a major issue. Herein, we addressed this problem by employing aluminum-doped zinc oxide (AZO) as the ECL and obtained extraordinarily thermally stable perovskite layers. The improvement of the thermal stability was ascribed to diminish of the Lewis acid-base chemical reaction between perovskite and ECL. Notably, the outstanding transmittance and conductivity also render AZO layer as an ideal candidate for transparent conductive electrodes, which enables a simplified cell structure featuring glass/AZO/perovskite/Spiro-OMeTAD/Au. Optimization of the perovskite layer leads to an excellent and repeatable photovoltaic performance, with the champion cell exhibiting an open-circuit voltage (Voc) of 0.94 V, a short-circuit current (Jsc) of 20.2 mA cm(-2), a fill factor (FF) of 0.67, and an overall power conversion efficiency (PCE) of 12.6% under standard 1 sun illumination. It was also revealed by steady-state and time-resolved photoluminescence that the AZO/perovskite interface resulted in less quenching than that between perovskite and hole transport material. PMID:26960451

  15. Aluminum-Doped Zinc Oxide as Highly Stable Electron Collection Layer for Perovskite Solar Cells.

    PubMed

    Zhao, Xingyue; Shen, Heping; Zhang, Ye; Li, Xin; Zhao, Xiaochong; Tai, Meiqian; Li, Jingfeng; Li, Jianbao; Li, Xin; Lin, Hong

    2016-03-01

    Although low-temperature, solution-processed zinc oxide (ZnO) has been widely adopted as the electron collection layer (ECL) in perovskite solar cells (PSCs) because of its simple synthesis and excellent electrical properties such as high charge mobility, the thermal stability of the perovskite films deposited atop ZnO layer remains as a major issue. Herein, we addressed this problem by employing aluminum-doped zinc oxide (AZO) as the ECL and obtained extraordinarily thermally stable perovskite layers. The improvement of the thermal stability was ascribed to diminish of the Lewis acid-base chemical reaction between perovskite and ECL. Notably, the outstanding transmittance and conductivity also render AZO layer as an ideal candidate for transparent conductive electrodes, which enables a simplified cell structure featuring glass/AZO/perovskite/Spiro-OMeTAD/Au. Optimization of the perovskite layer leads to an excellent and repeatable photovoltaic performance, with the champion cell exhibiting an open-circuit voltage (Voc) of 0.94 V, a short-circuit current (Jsc) of 20.2 mA cm(-2), a fill factor (FF) of 0.67, and an overall power conversion efficiency (PCE) of 12.6% under standard 1 sun illumination. It was also revealed by steady-state and time-resolved photoluminescence that the AZO/perovskite interface resulted in less quenching than that between perovskite and hole transport material.

  16. New Physical Deposition Approach for Low Cost Inorganic Hole Transport Layer in Normal Architecture of Durable Perovskite Solar Cells.

    PubMed

    Nejand, Bahram Abdollahi; Ahmadi, Vahid; Shahverdi, Hamid Reza

    2015-10-01

    In this work we reported sputter deposited NiOx/Ni double layer as an HTM/contact couple in normal architecture of perovskite solar cell. A perovskite solar cell that is durable for more than 60 days was achieved, with increasing efficiency from 1.3% to 7.28% within 6 days. Moreover, low temperature direct deposition of NiOx layer on perovskite layer was introduced as a potential hole transport material for an efficient cost-effective solar cell applicable for various morphologies of perovskite layers, even for perovskite layers containing pinholes, which is a notable challenge in perovskite solar cells. The angular deposition of NiOx layers by dc reactive magnetron sputtering showed uniform and crack-free coverage of the perovskite layer with no negative impact on perovskite structure that is suitable for nickel back contact layer, surface shielding against moisture, and mechanical damages. Replacing the expensive complex materials in previous perovskite solar cells with low cost available materials introduces cost-effective scalable perovskite solar cells.

  17. Reduced thermal conductivity by nanoscale intergrowths in perovskite like layered structure La{sub 2}Ti{sub 2}O{sub 7}

    SciTech Connect

    Khaliq, Jibran; Chen, Kan; Li, Chunchun; Shi, Baogui; Ye, Haitao; Grande, Antonio M.; Yan, Haixue; Reece, Michael J.

    2015-02-21

    The effect of substitution and oxidation-reduction on the thermal conductivity of perovskite-like layered structure (PLS) ceramics was investigated in relation to mass contrast and non-stoichiometry. Sr (acceptor) was substituted on the A site, while Ta (donor) was substituted on the B site of La{sub 2}Ti{sub 2}O{sub 7}. Substitution in PLS materials creates atomic scale disorders to accommodate the non-stoichiometry. High resolution transmission electron microscopy and X ray diffraction revealed that acceptor substitution in La{sub 2}Ti{sub 2}O{sub 7} produced nanoscale intergrowths of n = 5 layered phase, while donor substitution produced nanoscale intergrowths of n = 3 layered phase. As a result of these nanoscale intergrowths, the thermal conductivity value reduced by as much as ∼20%. Pure La{sub 2}Ti{sub 2}O{sub 7} has a thermal conductivity value of ∼1.3 W/m K which dropped to a value of ∼1.12 W/m K for Sr doped La{sub 2}Ti{sub 2}O{sub 7} and ∼0.93 W/m K for Ta doped La{sub 2}Ti{sub 2}O{sub 7} at 573 K.

  18. Development of new layered selenide oxides with perovskite-type oxide layers

    NASA Astrophysics Data System (ADS)

    Ushiyama, Koichi; Ogino, Hiraku; Kishio, Kohji; Shimoyama, Jun-Ichi

    2010-03-01

    Several Fe-based superconductors with perovskite-type oxide layers, such as Sr2ScFePO3 (Tc ˜ 17 K)^[1], were discovered in our previous study. These compounds are composed of alternate stacking of superconducting layers with antifluorite structure and perovskite-type blocking layers. Since both layers are flexible in terms of chemical composition, development of various new functional materials can be expected from this family. In the present study, we have attempted to synthesize new layered selenide oxides with CuSe layers and discovered more than ten compounds, such as Sr2MCu2Se2O2 (M = Mn, Co, Ni, Cu, Zn) and Sr2MCuSeO3 (M = Sc, Cr, Mn, Fe, Ga, In), thus far. These indicated that the CuSe layer can accommodate various types of blocking layers, which may lead various functions. Among them, Sr2Cu3Se2O2 has a potential as for the mother compound of superconductor, if appropriate concentration of carrier is introduced to the CuO2 layer. Crystal structure and physical properties of these newly found compounds will be reported. [1] H. Ogino et al., Supercond. Sci. Technol. 22 (2009) 075008

  19. Ferroelastic switching in a layered-perovskite thin film

    PubMed Central

    Wang, Chuanshou; Ke, Xiaoxing; Wang, Jianjun; Liang, Renrong; Luo, Zhenlin; Tian, Yu; Yi, Di; Zhang, Qintong; Wang, Jing; Han, Xiu-Feng; Van Tendeloo, Gustaaf; Chen, Long-Qing; Nan, Ce-Wen; Ramesh, Ramamoorthy; Zhang, Jinxing

    2016-01-01

    A controllable ferroelastic switching in ferroelectric/multiferroic oxides is highly desirable due to the non-volatile strain and possible coupling between lattice and other order parameter in heterostructures. However, a substrate clamping usually inhibits their elastic deformation in thin films without micro/nano-patterned structure so that the integration of the non-volatile strain with thin film devices is challenging. Here, we report that reversible in-plane elastic switching with a non-volatile strain of approximately 0.4% can be achieved in layered-perovskite Bi2WO6 thin films, where the ferroelectric polarization rotates by 90° within four in-plane preferred orientations. Phase-field simulation indicates that the energy barrier of ferroelastic switching in orthorhombic Bi2WO6 film is ten times lower than the one in PbTiO3 films, revealing the origin of the switching with negligible substrate constraint. The reversible control of the in-plane strain in this layered-perovskite thin film demonstrates a new pathway to integrate mechanical deformation with nanoscale electronic and/or magnetoelectronic applications. PMID:26838483

  20. Ferroelastic switching in a layered-perovskite thin film

    NASA Astrophysics Data System (ADS)

    Wang, Chuanshou; Ke, Xiaoxing; Wang, Jianjun; Liang, Renrong; Luo, Zhenlin; Tian, Yu; Yi, Di; Zhang, Qintong; Wang, Jing; Han, Xiu-Feng; van Tendeloo, Gustaaf; Chen, Long-Qing; Nan, Ce-Wen; Ramesh, Ramamoorthy; Zhang, Jinxing

    2016-02-01

    A controllable ferroelastic switching in ferroelectric/multiferroic oxides is highly desirable due to the non-volatile strain and possible coupling between lattice and other order parameter in heterostructures. However, a substrate clamping usually inhibits their elastic deformation in thin films without micro/nano-patterned structure so that the integration of the non-volatile strain with thin film devices is challenging. Here, we report that reversible in-plane elastic switching with a non-volatile strain of approximately 0.4% can be achieved in layered-perovskite Bi2WO6 thin films, where the ferroelectric polarization rotates by 90° within four in-plane preferred orientations. Phase-field simulation indicates that the energy barrier of ferroelastic switching in orthorhombic Bi2WO6 film is ten times lower than the one in PbTiO3 films, revealing the origin of the switching with negligible substrate constraint. The reversible control of the in-plane strain in this layered-perovskite thin film demonstrates a new pathway to integrate mechanical deformation with nanoscale electronic and/or magnetoelectronic applications.

  1. Toward Revealing the Critical Role of Perovskite Coverage in Highly Efficient Electron-Transport Layer-Free Perovskite Solar Cells: An Energy Band and Equivalent Circuit Model Perspective.

    PubMed

    Huang, Like; Xu, Jie; Sun, Xiaoxiang; Du, Yangyang; Cai, Hongkun; Ni, Jian; Li, Juan; Hu, Ziyang; Zhang, Jianjun

    2016-04-20

    Currently, most efficient perovskite solar cells (PVKSCs) with a p-i-n structure require simultaneously electron transport layers (ETLs) and hole transport layers (HTLs) to help collecting photogenerated electrons and holes for obtaining high performance. ETL free planar PVKSC is a relatively new and simple structured solar cell that gets rid of the complex and high temperature required ETL (such as compact and mesoporous TiO2). Here, we demonstrate the critical role of high coverage of perovskite in efficient ETL free PVKSCs from an energy band and equivalent circuit model perspective. From an electrical point of view, we confirmed that the low coverage of perovskite does cause localized short circuit of the device. With coverage optimization, a planar p-i-n(++) device with a power conversion efficiency of over 11% was achieved, implying that the ETL layer may not be necessary for an efficient device as long as the perovskite coverage is approaching 100%. PMID:27020395

  2. Toward Revealing the Critical Role of Perovskite Coverage in Highly Efficient Electron-Transport Layer-Free Perovskite Solar Cells: An Energy Band and Equivalent Circuit Model Perspective.

    PubMed

    Huang, Like; Xu, Jie; Sun, Xiaoxiang; Du, Yangyang; Cai, Hongkun; Ni, Jian; Li, Juan; Hu, Ziyang; Zhang, Jianjun

    2016-04-20

    Currently, most efficient perovskite solar cells (PVKSCs) with a p-i-n structure require simultaneously electron transport layers (ETLs) and hole transport layers (HTLs) to help collecting photogenerated electrons and holes for obtaining high performance. ETL free planar PVKSC is a relatively new and simple structured solar cell that gets rid of the complex and high temperature required ETL (such as compact and mesoporous TiO2). Here, we demonstrate the critical role of high coverage of perovskite in efficient ETL free PVKSCs from an energy band and equivalent circuit model perspective. From an electrical point of view, we confirmed that the low coverage of perovskite does cause localized short circuit of the device. With coverage optimization, a planar p-i-n(++) device with a power conversion efficiency of over 11% was achieved, implying that the ETL layer may not be necessary for an efficient device as long as the perovskite coverage is approaching 100%.

  3. Improved air stability of perovskite solar cells via solution-processed metal oxide transport layers.

    PubMed

    You, Jingbi; Meng, Lei; Song, Tze-Bin; Guo, Tzung-Fang; Yang, Yang Michael; Chang, Wei-Hsuan; Hong, Ziruo; Chen, Huajun; Zhou, Huanping; Chen, Qi; Liu, Yongsheng; De Marco, Nicholas; Yang, Yang

    2016-01-01

    Lead halide perovskite solar cells have recently attracted tremendous attention because of their excellent photovoltaic efficiencies. However, the poor stability of both the perovskite material and the charge transport layers has so far prevented the fabrication of devices that can withstand sustained operation under normal conditions. Here, we report a solution-processed lead halide perovskite solar cell that has p-type NiO(x) and n-type ZnO nanoparticles as hole and electron transport layers, respectively, and shows improved stability against water and oxygen degradation when compared with devices with organic charge transport layers. Our cells have a p-i-n structure (glass/indium tin oxide/NiO(x)/perovskite/ZnO/Al), in which the ZnO layer isolates the perovskite and Al layers, thus preventing degradation. After 60 days storage in air at room temperature, our all-metal-oxide devices retain about 90% of their original efficiency, unlike control devices made with organic transport layers, which undergo a complete degradation after just 5 days. The initial power conversion efficiency of our devices is 14.6 ± 1.5%, with an uncertified maximum value of 16.1%.

  4. Improved air stability of perovskite solar cells via solution-processed metal oxide transport layers

    NASA Astrophysics Data System (ADS)

    You, Jingbi; Meng, Lei; Song, Tze-Bin; Guo, Tzung-Fang; Yang, Yang (Michael); Chang, Wei-Hsuan; Hong, Ziruo; Chen, Huajun; Zhou, Huanping; Chen, Qi; Liu, Yongsheng; De Marco, Nicholas; Yang, Yang

    2016-01-01

    Lead halide perovskite solar cells have recently attracted tremendous attention because of their excellent photovoltaic efficiencies. However, the poor stability of both the perovskite material and the charge transport layers has so far prevented the fabrication of devices that can withstand sustained operation under normal conditions. Here, we report a solution-processed lead halide perovskite solar cell that has p-type NiOx and n-type ZnO nanoparticles as hole and electron transport layers, respectively, and shows improved stability against water and oxygen degradation when compared with devices with organic charge transport layers. Our cells have a p-i-n structure (glass/indium tin oxide/NiOx/perovskite/ZnO/Al), in which the ZnO layer isolates the perovskite and Al layers, thus preventing degradation. After 60 days storage in air at room temperature, our all-metal-oxide devices retain about 90% of their original efficiency, unlike control devices made with organic transport layers, which undergo a complete degradation after just 5 days. The initial power conversion efficiency of our devices is 14.6 ± 1.5%, with an uncertified maximum value of 16.1%.

  5. Effects of hole-transporting layers of perovskite-based solar cells

    NASA Astrophysics Data System (ADS)

    Suzuki, Atsushi; Kida, Tomoyasu; Takagi, Tatsuru; Oku, Takeo

    2016-02-01

    Fabrication and characterization of the photovoltaic and optical properties, and microstructure of perovskite-based solar cells with lead phthalocyanine (PbPc), zinc phthalocyanine, poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine], and copper(I) thiocyanate as hole-transporting layers were investigated. X-ray diffraction analysis and energy-dispersive X-ray spectroscopy were used to identify surface morphologies of the crystal structure and the elemental composition. Introducing PbPc into perovskite solar cells extended the retaining period of photovoltaic activity and performance. The effects of the hole-transporting layer on incident photon-to-current efficiency were investigated. The energy diagram and photovoltaic mechanism of the perovskite solar cells with the hole-transporting layer are discussed.

  6. Effect of Mesostructured Layer upon Crystalline Properties and Device Performance on Perovskite Solar Cells.

    PubMed

    Listorti, Andrea; Juarez-Perez, Emilio J; Frontera, Carlos; Roiati, Vittoria; Garcia-Andrade, Laura; Colella, Silvia; Rizzo, Aurora; Ortiz, Pablo; Mora-Sero, Ivan

    2015-05-01

    One of the most fascinating characteristics of perovskite solar cells (PSCs) is the retrieved obtainment of outstanding photovoltaic (PV) performances withstanding important device configuration variations. Here we have analyzed CH3NH3PbI3-xClx in planar or in mesostructured (MS) configurations, employing both titania and alumina scaffolds, fully infiltrated with perovskite material or presenting an overstanding layer. The use of the MS scaffold induces to the perovskite different structural properties, in terms of grain size, preferential orientation, and unit cell volume, in comparison to the ones of the material grown with no constraints, as we have found out by X-ray diffraction analyses. We have studied the effect of the PSC configuration on photoinduced absorption and time-resolved photoluminescence, complementary techniques that allow studying charge photogeneration and recombination. We have estimated electron diffusion length in the considered configurations observing a decrease when the material is confined in the MS scaffold with respect to a planar architecture. However, the presence of perovskite overlayer allows an overall recovering of long diffusion lengths explaining the record PV performances obtained with a device configuration bearing both the mesostructure and a perovskite overlayer. Our results suggest that performance in devices with perovskite overlayer is mainly ruled by the overlayer, whereas the mesoporous layer influences the contact properties. PMID:26263326

  7. Anisotropy of Earth's D'' layer and stacking faults in the MgSiO3 post-perovskite phase.

    PubMed

    Oganov, Artem R; Martonák, Roman; Laio, Alessandro; Raiteri, Paolo; Parrinello, Michele

    2005-12-22

    The post-perovskite phase of (Mg,Fe)SiO3 is believed to be the main mineral phase of the Earth's lowermost mantle (the D'' layer). Its properties explain numerous geophysical observations associated with this layer-for example, the D'' discontinuity, its topography and seismic anisotropy within the layer. Here we use a novel simulation technique, first-principles metadynamics, to identify a family of low-energy polytypic stacking-fault structures intermediate between the perovskite and post-perovskite phases. Metadynamics trajectories identify plane sliding involving the formation of stacking faults as the most favourable pathway for the phase transition, and as a likely mechanism for plastic deformation of perovskite and post-perovskite. In particular, the predicted slip planes are {010} for perovskite (consistent with experiment) and {110} for post-perovskite (in contrast to the previously expected {010} slip planes). Dominant slip planes define the lattice preferred orientation and elastic anisotropy of the texture. The {110} slip planes in post-perovskite require a much smaller degree of lattice preferred orientation to explain geophysical observations of shear-wave anisotropy in the D'' layer.

  8. Magnetic coupling at perovskite and rock-salt structured interfaces

    SciTech Connect

    Matvejeff, M.; Ahvenniemi, E.; Takahashi, R.; Lippmaa, M.

    2015-10-05

    We study magnetic coupling between hole-doped manganite layers separated by either a perovskite or a rock-salt barrier of variable thickness. Both the type and the quality of the interface have a strong impact on the minimum critical barrier thickness where the manganite layers become magnetically decoupled. A rock-salt barrier layer only 1 unit cell (0.5 nm) thick remains insulating and is able to magnetically de-couple the electrode layers. The technique can therefore be used for developing high-performance planar oxide electronic devices such as magnetic tunnel junctions and quantum well structures that depend on magnetically and electronically sharp heterointerfaces.

  9. Autothermal reforming catalyst having perovskite structure

    DOEpatents

    Krumpel, Michael; Liu, Di-Jia

    2009-03-24

    The invention addressed two critical issues in fuel processing for fuel cell application, i.e. catalyst cost and operating stability. The existing state-of-the-art fuel reforming catalyst uses Rh and platinum supported over refractory oxide which add significant cost to the fuel cell system. Supported metals agglomerate under elevated temperature during reforming and decrease the catalyst activity. The catalyst is a perovskite oxide or a Ruddlesden-Popper type oxide containing rare-earth elements, catalytically active firs row transition metal elements, and stabilizing elements, such that the catalyst is a single phase in high temperature oxidizing conditions and maintains a primarily perovskite or Ruddlesden-Popper structure under high temperature reducing conditions. The catalyst can also contain alkaline earth dopants, which enhance the catalytic activity of the catalyst, but do not compromise the stability of the perovskite structure.

  10. A new layered nano hybrid perovskite film with enhanced resistance to moisture-induced degradation

    NASA Astrophysics Data System (ADS)

    Jiang, Wenlong; Ying, Jifei; Zhou, Wei; Shen, Kongchao; Liu, Xing; Gao, Xingyu; Guo, Fuqiang; Gao, Yanmin; Yang, Tieying

    2016-08-01

    In this paper, a new layered hybrid perovskite film ((EDA)(MA)2[Pb3I10]) was synthesized through one-step method. Ethylenediamine (EDA) cation was introduced into the perovskite lattice to synthesize a layered structure with improved resistance to degradation by humidity. The effects of humidity and time on crystal structure, composition, morphology and absorption spectra of (EDA)(MA)2[Pb3I10] were analyzed by in situ grazing incidence X-ray diffraction (GIXRD), scanning electron microscope (SEM), and UV-Vis spectroscope. The results reveal that a (EDA)(MA)2[Pb3I10] film is more moisture resistant than a CH3NH3PbI3 film which is widely used in the perovskite solar cell now. UV-Vis spectroscopy result also shows that the layered structure film is a suitable solar absorber with a bandgap (1.67 eV), which is close to the optimum value for solar photoelectric conversion. Compared to CH3NH3PbI3, the low-cost perovskite structure offers greater tunability on a molecular level for further material optimization and possibility for widely used in the future.

  11. Multifunctional MgO Layer in Perovskite Solar Cells.

    PubMed

    Guo, Xudong; Dong, Haopeng; Li, Wenzhe; Li, Nan; Wang, Liduo

    2015-06-01

    A multifunctional magnesium oxide (MgO) layer was successfully introduced into perovskite solar cells (PSCs) to enhance their performance. MgO was coated onto the surface of mesoporous TiO(2) by the decomposition of magnesium acetate and, therefore, could block contact between the perovskite and TiO(2). X-ray photoelectron spectroscopy and infrared spectroscopy showed that the amount of H(2)O/hydroxyl absorbed on the TiO(2) decreased after MgO modification. The UV/Vis absorption spectra of the perovskite with MgO modification revealed an enhanced photoelectric performance compared with that of unmodified perovskite after UV illumination. In addition to the photocurrent, the photovoltage and fill factor also showed an enhancement after modification, which resulted in an increase in the overall efficiency of the cell from 9.6 to 13.9 %. Electrochemical impedance spectroscopy (EIS) confirmed that MgO acts as an insulating layer to reduce charge recombination. PMID:25851999

  12. Multifunctional MgO Layer in Perovskite Solar Cells.

    PubMed

    Guo, Xudong; Dong, Haopeng; Li, Wenzhe; Li, Nan; Wang, Liduo

    2015-06-01

    A multifunctional magnesium oxide (MgO) layer was successfully introduced into perovskite solar cells (PSCs) to enhance their performance. MgO was coated onto the surface of mesoporous TiO(2) by the decomposition of magnesium acetate and, therefore, could block contact between the perovskite and TiO(2). X-ray photoelectron spectroscopy and infrared spectroscopy showed that the amount of H(2)O/hydroxyl absorbed on the TiO(2) decreased after MgO modification. The UV/Vis absorption spectra of the perovskite with MgO modification revealed an enhanced photoelectric performance compared with that of unmodified perovskite after UV illumination. In addition to the photocurrent, the photovoltage and fill factor also showed an enhancement after modification, which resulted in an increase in the overall efficiency of the cell from 9.6 to 13.9 %. Electrochemical impedance spectroscopy (EIS) confirmed that MgO acts as an insulating layer to reduce charge recombination.

  13. Ab initio modeling of 2D layered organohalide lead perovskites.

    PubMed

    Fraccarollo, Alberto; Cantatore, Valentina; Boschetto, Gabriele; Marchese, Leonardo; Cossi, Maurizio

    2016-04-28

    A number of 2D layered perovskites A2PbI4 and BPbI4, with A and B mono- and divalent ammonium and imidazolium cations, have been modeled with different theoretical methods. The periodic structures have been optimized (both in monoclinic and in triclinic systems, corresponding to eclipsed and staggered arrangements of the inorganic layers) at the DFT level, with hybrid functionals, Gaussian-type orbitals and dispersion energy corrections. With the same methods, the various contributions to the solid stabilization energy have been discussed, separating electrostatic and dispersion energies, organic-organic intralayer interactions and H-bonding effects, when applicable. Then the electronic band gaps have been computed with plane waves, at the DFT level with scalar and full relativistic potentials, and including the correlation energy through the GW approximation. Spin orbit coupling and GW effects have been combined in an additive scheme, validated by comparing the computed gap with well known experimental and theoretical results for a model system. Finally, various contributions to the computed band gaps have been discussed on some of the studied systems, by varying some geometrical parameters and by substituting one cation in another's place. PMID:27131557

  14. Rapid Topochemical Modification of Layered Perovskites via Microwave Reactions.

    PubMed

    Akbarian-Tefaghi, Sara; Teixeira Veiga, Elaine; Amand, Guillaume; Wiley, John B

    2016-02-15

    An effective microwave approach to the topochemical modification of different layered oxide perovskite hosts is presented where cation exchange, grafting, and intercalation reactions with acid, n-alkyl alcohols, and n-alkylamines, respectively, are successfully carried out. Microwave-assisted proton exchange reactions involving double- and triple-layered Dion-Jacobson and Ruddlesden-Popper perovskite family members, RbLnNb2O7 (Ln = La, Pr), KCa2Nb3O10, Li2CaTa2O7, and Na2La2Ti3O10, were found to be quite efficient, decreasing reaction times from several days to ≤3 h. Grafting and intercalation reactions involving double-layered perovskites were also quite rapid with full conversions occurring in as fast as an hour. Interestingly, triple-layered hosts were found to show different behavior; when complete intercalations were possible, grafting reactions were limited at best. Utilization of this rapid synthetic approach could help facilitate the fabrication of new organic-inorganic hybrids. PMID:26835716

  15. Efficient methylammonium lead iodide perovskite solar cells with active layers from 300 to 900 nm

    SciTech Connect

    Momblona, C.; Malinkiewicz, O.; Soriano, A.; Gil-Escrig, L.; Bandiello, E.; Scheepers, M.; Bolink, H. J.; Edri, E.

    2014-08-01

    Efficient methylammonium lead iodide perovskite-based solar cells have been prepared in which the perovskite layer is sandwiched in between two organic charge transporting layers that block holes and electrons, respectively. This configuration leads to stable and reproducible devices that do not suffer from strong hysteresis effects and when optimized lead to efficiencies close to 15%. The perovskite layer is formed by using a dual-source thermal evaporation method, whereas the organic layers are processed from solution. The dual-source thermal evaporation method leads to smooth films and allows for high precision thickness variations. Devices were prepared with perovskite layer thicknesses ranging from 160 to 900 nm. The short-circuit current observed for these devices increased with increasing perovskite layer thickness. The main parameter that decreases with increasing perovskite layer thickness is the fill factor and as a result optimum device performance is obtained for perovskite layer thickness around 300 nm. However, here we demonstrate that with a slightly oxidized electron blocking layer the fill factor for the solar cells with a perovskite layer thickness of 900 nm increases to the same values as for the devices with thin perovskite layers. As a result the power conversion efficiencies for the cells with 300 and 900 nm are very similar, 12.7% and 12%, respectively.

  16. Layering fabrication, structure, and electromagnetic properties of perovskite phases by hybrid process: self-propagated high-temperature synthesis and selective laser sintering

    NASA Astrophysics Data System (ADS)

    Shishkovsky, I.; Morozov, Yu.; Kuznetsov, M.

    2013-11-01

    The paper discusses the fundamentals and the requirements for layer-by-layer manufacturing of three-dimensional porous parts from complex metal oxide systems (piezoceramics PbTi1-xZrxO3; hexaferrites - BaFe12-xCrxO19 and SrFe12O19; spinels - Li0.5Fe2.5-xCrxO4 and high-temperature superconducting ceramics (HTSC) - YBa2Cu3O7-y) and examines the main aspects of the overlapped processes associated with the self-propagated high-temperature synthesis (SHS) and selective laser sintering (SLS). These two techniques presently offered are joined as the original solutions in this external magnetic field. The perovskite phase compositions, morphology, and element distribution of the fabricated samples were analyzed by the X-ray diffraction (XRD), scanning electron microscopy (SEM) equipped the EDX analysis. Optimal regimes for the three-dimensional (3D) parts laser synthesis and some of their electro physical properties were estimated for conducting the concurrent SHS-SLS reactions, both for the case with the applied dc magnetic field and without it.

  17. Ferroelastic switching in a layered-perovskite thin film

    DOE PAGES

    Wang, Chuanshou; Ke, Xiaoxing; Wang, Jianjun; Liang, Renrong; Luo, Zhenlin; Tian, Yu; Yi, Di; Zhang, Qintong; Wang, Jing; Han, Xiu -Feng; et al

    2016-02-03

    Here, a controllable ferroelastic switching in ferroelectric/multiferroic oxides is highly desirable due to the non-volatile strain and possible coupling between lattice and other order parameter in heterostructures. However, a substrate clamping usually inhibits their elastic deformation in thin films without micro/nano-patterned structure so that the integration of the non-volatile strain with thin film devices is challenging. Here, we report that reversible in-plane elastic switching with a non-volatile strain of approximately 0.4% can be achieved in layeredperovskite Bi2WO6 thin films, where the ferroelectric polarization rotates by 90 within four in-plane preferred orientations. Phase-field simulation indicates that the energy barrier of ferroelasticmore » switching in orthorhombic Bi2WO6 film is ten times lower than the one in PbTiO3 films, revealing the origin of the switching with negligible substrate constraint. The reversible control of the in-plane strain in this layered-perovskite thin film demonstrates a new pathway to integrate mechanical deformation with nanoscale electronic and/or magnetoelectronic applications.« less

  18. Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films.

    PubMed

    Chong, Wee Kiang; Thirumal, Krishnamoorthy; Giovanni, David; Goh, Teck Wee; Liu, Xinfeng; Mathews, Nripan; Mhaisalkar, Subodh; Sum, Tze Chien

    2016-05-25

    Semiconductors are ubiquitous gain media for coherent light sources. Solution-processed three-dimensional (3D) halide perovskites (e.g., CH3NH3PbI3) with their outstanding room temperature optical gain properties are the latest members of this family. Their two-dimensional (2D) layered perovskite counterparts with natural multiple quantum well structures exhibit strong light-matter interactions and intense excitonic luminescence. However, despite such promising traits, there have been no reports on room temperature optical gain in 2D layered perovskites. Herein, we reveal the challenges towards achieving amplified spontaneous emission (ASE) in the archetypal (C6H5C2H4NH3)2PbI4 (or PEPI) system. Temperature-dependent transient spectroscopy uncovers the dominant free exciton trapping and bound biexciton formation pathways that compete effectively with biexcitonic gain. Phenomenological rate equation modeling predicts a large biexciton ASE threshold of ∼1.4 mJ cm(-2), which is beyond the damage threshold of these materials. Importantly, these findings would rationalize the difficulties in achieving optical gain in 2D perovskites and provide new insights and suggestions for overcoming these challenges. PMID:27184073

  19. Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films.

    PubMed

    Chong, Wee Kiang; Thirumal, Krishnamoorthy; Giovanni, David; Goh, Teck Wee; Liu, Xinfeng; Mathews, Nripan; Mhaisalkar, Subodh; Sum, Tze Chien

    2016-05-25

    Semiconductors are ubiquitous gain media for coherent light sources. Solution-processed three-dimensional (3D) halide perovskites (e.g., CH3NH3PbI3) with their outstanding room temperature optical gain properties are the latest members of this family. Their two-dimensional (2D) layered perovskite counterparts with natural multiple quantum well structures exhibit strong light-matter interactions and intense excitonic luminescence. However, despite such promising traits, there have been no reports on room temperature optical gain in 2D layered perovskites. Herein, we reveal the challenges towards achieving amplified spontaneous emission (ASE) in the archetypal (C6H5C2H4NH3)2PbI4 (or PEPI) system. Temperature-dependent transient spectroscopy uncovers the dominant free exciton trapping and bound biexciton formation pathways that compete effectively with biexcitonic gain. Phenomenological rate equation modeling predicts a large biexciton ASE threshold of ∼1.4 mJ cm(-2), which is beyond the damage threshold of these materials. Importantly, these findings would rationalize the difficulties in achieving optical gain in 2D perovskites and provide new insights and suggestions for overcoming these challenges.

  20. Fine control of perovskite-layered morphology and composition via sequential deposition crystallization process towards improved perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Luo, Yi; Meng, Fanli; Zhao, Erfei; Zheng, Yan-Zhen; Zhou, Yali; Tao, Xia

    2016-04-01

    The ability to prepare high coverage and compact perovskite films via solution-based crystallization manipulation processes still represents a vital issue towards improving the ultimate photoelectric conversion efficiency of devices. In this work, we prepare the active perovskite layer by means of sequential deposition crystallization process i.e. dipping PbI2-infiltrated TiO2 film within CH3NH3I solution from 20s to 60s. The morphology and thickness of the as-prepared perovskite layer, and its overall performance superiority are investigated. X-ray diffraction (XRD) reveals that a maximum conversion of PbI2 to perovskite is completed upon applying a sequential deposition crystallization process of 40s. Field emission scanning electron microscope (FESEM) demonstrates that the coverage of the perovskite capping layer exhibits a trend from rise to decline in the whole dipping time from 20s to 60s. By fine control of the dipping time, a 620 nm-thickness compact perovskite active layer is obtained at the optimized dipping time of 40s and is verified to possess strong light absorption and high electron extraction efficiency, leading to a higher photocurrent. By further optimizing the mesoporous TiO2 film thickness, a high photocurrent of 23.98 mA cm-2 and an efficiency of 13.47% are achieved.

  1. Atomically thin two-dimensional materials as hole extraction layers in organolead halide perovskite photovoltaic cells

    NASA Astrophysics Data System (ADS)

    Kim, Yu Geun; Kwon, Ki Chang; Le, Quyet Van; Hong, Kootak; Jang, Ho Won; Kim, Soo Young

    2016-07-01

    Atomically thin two-dimensional materials such as MoS2, WS2, and graphene oxide (GO) are used as hole extraction layers (HEL) in organolead halide perovskites solar cells (PSCs) instead of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) HEL. MoS2 and WS2 layers with a polycrystalline structure were synthesized by a chemical deposition method using a uniformly spin-coated (NH4)MoS4 and (NH4)WS4 precursor solution. GO was synthesized by the oxidation of natural graphite powder using Hummers' method. The work functions of MoS2, WS2, and GO are measured to be 5.0, 4.95, and 5.1 eV, respectively. The X-ray diffraction spectrum indicated that the synthesized perovskite material is CH3NH3PbI3-xClx. The PSCs with the p-n junction structure were fabricated based on the CH3NH3PbI3-xClx perovskite layer. The power conversion efficiencies of the MoS2, WS2, and GO-based PSCs were 9.53%, 8.02%, and 9.62%, respectively, which are comparable to those obtained from PEDOT:PSS-based devices (9.93%). These results suggest that two-dimensional materials such as MoS2, WS2, and GO can be promising candidates for the formation of HELs in the PSCs.

  2. Structural, electrochemical and magnetic characterization of the layered-type PrBa{sub 0.5}Sr{sub 0.5}Co{sub 2}O{sub 5+δ} perovskite

    SciTech Connect

    Azad, Abul K.; Kim, Jung H.; Irvine, John T.S.

    2014-05-01

    Structural, electrical and magnetic properties of the layered cobaltite PrBa{sub 0.5}Sr{sub 0.5}Co{sub 2}O{sub 5+δ} have been investigated by means of neutron diffraction, electron diffraction, thermogravimetric analysis and SQUID magnetometry. Rietveld analysis of neutron diffraction data shows the ordered distribution of oxygen vacancies in [PrO{sub δ}] planes which doubles the lattice parameters from the simple perovskite cell parameter as a≈2a{sub p} and c≈2a{sub p} (a{sub p} is the cell parameter of the simple Perovskite) yielding tetragonal symmetry in the P4/mmm space group. On heating, above 573 K in air, structural rearrangement takes place and the structure can be defined as a≈a{sub p} and c≈2a{sub p} in the same space group. Oxygen occupancies have been determined as a function of temperature from neutron diffraction results. Initially (≥373 K), oxygen occupancy was increased and then decreased with increasing temperature. It was found that at 973 K the total oxygen loss is calculated about 0.265 oxygen/formula unit. Oxygen vacancy ordering was observed below 573 K, and the oxygen occupancy decreases as cell volume increases with increasing temperature. Area specific resistance (ASR) measurements show a resistance of 0.153 Ωcm{sup 2} and 0.286 Ωcm{sup 2} at 973 K and 923 K, respectively. On cooling, paramagnetic to ferromagnetic and an incomplete ferromagnetic to antiferromagnetic transition takes place. Different behaviours in field cooled and zero-field-cooled measurements leads to a coexistence of ferromagnetic and antiferromagnetic order. - Graphical abstract: Structural phase changes in PrBa{sub 0.5}Sr{sub 0.5}Co{sub 2}O{sub 5+δ} at elevated temperatures determined by neutron powder diffraction. Depending on oxygen occupancy it form different phases at different temperatures. This pictures show the schematic 3D diagram of PrBa{sub 0.5}Sr{sub 0.5}Co{sub 2}O{sub 5+δ} at 295 K (a), 373 K (b) and 573 K (c). Co atoms are inside the

  3. Recent Advances in the Inverted Planar Structure of Perovskite Solar Cells.

    PubMed

    Meng, Lei; You, Jingbi; Guo, Tzung-Fang; Yang, Yang

    2016-01-19

    Inorganic-organic hybrid perovskite solar cells research could be traced back to 2009, and initially showed 3.8% efficiency. After 6 years of efforts, the efficiency has been pushed to 20.1%. The pace of development was much faster than that of any type of solar cell technology. In addition to high efficiency, the device fabrication is a low-cost solution process. Due to these advantages, a large number of scientists have been immersed into this promising area. In the past 6 years, much of the research on perovskite solar cells has been focused on planar and mesoporous device structures employing an n-type TiO2 layer as the bottom electron transport layer. These architectures have achieved champion device efficiencies. However, they still possess unwanted features. Mesoporous structures require a high temperature (>450 °C) sintering process for the TiO2 scaffold, which will increase the cost and also not be compatible with flexible substrates. While the planar structures based on TiO2 (regular structure) usually suffer from a large degree of J-V hysteresis. Recently, another emerging structure, referred to as an "inverted" planar device structure (i.e., p-i-n), uses p-type and n-type materials as bottom and top charge transport layers, respectively. This structure derived from organic solar cells, and the charge transport layers used in organic photovoltaics were successfully transferred into perovskite solar cells. The p-i-n structure of perovskite solar cells has shown efficiencies as high as 18%, lower temperature processing, flexibility, and, furthermore, negligible J-V hysteresis effects. In this Account, we will provide a comprehensive comparison of the mesoporous and planar structures, and also the regular and inverted of planar structures. Later, we will focus the discussion on the development of the inverted planar structure of perovskite solar cells, including film growth, band alignment, stability, and hysteresis. In the film growth part, several

  4. Block Copolymer-Tuned Fullerene Electron Transport Layer Enhances the Efficiency of Perovskite Photovoltaics.

    PubMed

    Lin, Hsi-Kuei; Su, Yu-Wei; Chen, Hsiu-Cheng; Huang, Yi-Jiun; Wei, Kung-Hwa

    2016-09-21

    In this study, we enhanced the power conversion efficiency (PCE) of perovskite solar cells by employing an electron transfer layer (ETL) comprising [6,6]phenyl-C61-butyric acid methyl ester (PC61BM) and, to optimize its morphology, a small amount of the block copolymer polystyrene-b-poly(ethylene oxide) (PS-b-PEO), positioned on the perovskite active layer. When incorporating 0.375 wt % PS-b-PEO into PC61BM, the PCE of the perovskite photovoltaic device increased from 9.4% to 13.4%, a relative increase of 43%, because of a large enhancement in the fill factor of the device. To decipher the intricate morphology of the ETL, we used synchrotron grazing-incidence small-angle X-ray scattering for determining the PC61BM cluster size, atomic force microscopy and scanning electron microscopy for probing the surface, and transmission electron microscopy for observing the aggregation of PC61BM in the ETL. We found that the interaction between PS-b-PEO and PC61BM resulted in smaller PC61BM clusters that further aggregated into dendritic structures in some domains, a result of the similar polarities of the PS block and PC61BM; this behavior could be used to tune the morphology of the ETL. The optimal PS-b-PEO-mediated PC61BM cluster size in the ETL was 17 nm, a large reduction from 59 nm for the pristine PC61BM layer. This approach of incorporating a small amount of nanostructured block copolymer into a fullerene allowed us to effectively tune the morphology of the ETL on the perovskite active layer and resulted in enhanced fill factors of the devices and thus their device efficiency.

  5. Block Copolymer-Tuned Fullerene Electron Transport Layer Enhances the Efficiency of Perovskite Photovoltaics.

    PubMed

    Lin, Hsi-Kuei; Su, Yu-Wei; Chen, Hsiu-Cheng; Huang, Yi-Jiun; Wei, Kung-Hwa

    2016-09-21

    In this study, we enhanced the power conversion efficiency (PCE) of perovskite solar cells by employing an electron transfer layer (ETL) comprising [6,6]phenyl-C61-butyric acid methyl ester (PC61BM) and, to optimize its morphology, a small amount of the block copolymer polystyrene-b-poly(ethylene oxide) (PS-b-PEO), positioned on the perovskite active layer. When incorporating 0.375 wt % PS-b-PEO into PC61BM, the PCE of the perovskite photovoltaic device increased from 9.4% to 13.4%, a relative increase of 43%, because of a large enhancement in the fill factor of the device. To decipher the intricate morphology of the ETL, we used synchrotron grazing-incidence small-angle X-ray scattering for determining the PC61BM cluster size, atomic force microscopy and scanning electron microscopy for probing the surface, and transmission electron microscopy for observing the aggregation of PC61BM in the ETL. We found that the interaction between PS-b-PEO and PC61BM resulted in smaller PC61BM clusters that further aggregated into dendritic structures in some domains, a result of the similar polarities of the PS block and PC61BM; this behavior could be used to tune the morphology of the ETL. The optimal PS-b-PEO-mediated PC61BM cluster size in the ETL was 17 nm, a large reduction from 59 nm for the pristine PC61BM layer. This approach of incorporating a small amount of nanostructured block copolymer into a fullerene allowed us to effectively tune the morphology of the ETL on the perovskite active layer and resulted in enhanced fill factors of the devices and thus their device efficiency. PMID:27574718

  6. PbBr-Based Layered Perovskite Organic-Inorganic Superlattice Having Carbazole Chromophore; Hole-Mobility and Quantum Mechanical Calculation.

    PubMed

    Era, Masanao; Yasuda, Takeshi; Mori, Kento; Tomotsu, Norio; Kawano, Naoki; Koshimizu, Masanori; Asai, Keisuke

    2016-04-01

    We have successfully evaluated hole mobility in a spin-coated film of a lead-bromide based layered perovskite having carbazole chromophore-linked ammonium molecules as organic layer by using FET measurement. The values of hole mobility, threshold voltage and on/off ratio at room temperature were evaluated.to.be 1.7 x 10(-6) cm2 V-1 s-1, 27 V and 28 V, respectively. However, the spin-coated films on Si substrates were not so uniform compared with those on fused quartz substrates. To improve the film uniformity, we examined the relationship between substrate temperature during spin-coating and film morphology in the layered perovskite spin-coated films. The mean roughness of the spin-coated films on Si substrates was dependent on the substrate temperature. At 353 K, the mean roughness was minimized and the carrier mobility was enhanced by one order of magnitude; the values of hole mobility and threshold voltage were .estimated to be 3.4 x 10(-5) cm2 V-1 s-1, and 22 V at room temperature in a preliminary FET evaluation, respectively. In addition, we determined a crystal structure of the layered perovskite by X-ray diffraction analysis. To gain a better understanding of the observed hole transports, we conducted quantum mechanical calculations using the obtained crystal structure information. The calculated band structure of the layered organic perovskite showed that the valence band is composed of the organic carbazole layer, which confirms that.the measured hole mobility is mainly derived from the organic part of the layered perovskite. Band and hopping transport mechanisms were discussed by calculating the effective masses and transfer integrals for the 2D periodic system of the organic layer in isolation. PMID:27451598

  7. Efficient Planar Perovskite Solar Cells with Reduced Hysteresis and Enhanced Open Circuit Voltage by Using PW12-TiO2 as Electron Transport Layer.

    PubMed

    Huang, Chun; Liu, Canjun; Di, Yunxiang; Li, Wenzhang; Liu, Fangyang; Jiang, Liangxing; Li, Jie; Hao, Xiaojing; Huang, Haitao

    2016-04-01

    An electron transport layer is essential for effective operation of planar perovskite solar cells. In this Article, PW12-TiO2 composite was used as the electron transport layer for the planar perovskite solar cell in the device structure of fluorine-doped tin oxide (FTO)-glass/PW12-TiO2/perovskite/spiro-OMeTAD/Au. A proper downward shift of the conduction band minimum (CBM) enhanced electron extraction from the perovskite layer to the PW12-TiO2 composite layer. Consequently, the common hysteresis effect in TiO2-based planar perovskite solar cells was significantly reduced and the open circuit voltage was greatly increased to about 1.1 V. Perovskite solar cells using the PW12-TiO2 compact layer showed an efficiency of 15.45%. This work can contribute to the studies on the electron transport layer and interface engineering for the further development of perovskite solar cells.

  8. Influence of void-free perovskite capping layer on the charge recombination process in high performance CH3NH3PbI3 perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Fu, Kunwu; Nelson, Christopher T.; Scott, Mary Cooper; Minor, Andrew; Mathews, Nripan; Wong, Lydia Helena

    2016-02-01

    The stunning rise of methylammonium lead iodide perovskite material as a light harvesting material in recent years has drawn much attention in the photovoltaic community. Here, we investigated in detail the uniform and void-free perovskite capping layer in the mesoscopic perovskite devices and found it to play a critical role in determining device performance and charge recombination process. Compared to the rough surface with voids of the perovskite layer, surface of the perovskite capping layer obtained from sequential deposition process is much more uniform with less void formation and distribution within the TiO2 mesoscopic scaffold is more homogeneous, leading to much improved photovoltaic parameters of the devices. The impact of void free perovskite capping layer surface on the charge recombination processes within the mesoscopic perovskite solar cells is further scrutinized via charge extraction measurement. Modulation of precursor solution concentrations in order to further improve the perovskite layer surface morphology leads to higher efficiency and lower charge recombination rates. Inhibited charge recombination in these solar cells also matches with the higher charge density and slower photovoltage decay profiles measured.The stunning rise of methylammonium lead iodide perovskite material as a light harvesting material in recent years has drawn much attention in the photovoltaic community. Here, we investigated in detail the uniform and void-free perovskite capping layer in the mesoscopic perovskite devices and found it to play a critical role in determining device performance and charge recombination process. Compared to the rough surface with voids of the perovskite layer, surface of the perovskite capping layer obtained from sequential deposition process is much more uniform with less void formation and distribution within the TiO2 mesoscopic scaffold is more homogeneous, leading to much improved photovoltaic parameters of the devices. The impact of

  9. Perovskite oxides: Oxygen electrocatalysis and bulk structure

    NASA Technical Reports Server (NTRS)

    Carbonio, R. E.; Fierro, C.; Tryk, D.; Scherson, D.; Yeager, Ernest

    1987-01-01

    Perovskite type oxides were considered for use as oxygen reduction and generation electrocatalysts in alkaline electrolytes. Perovskite stability and electrocatalytic activity are studied along with possible relationships of the latter with the bulk solid state properties. A series of compounds of the type LaFe(x)Ni1(-x)O3 was used as a model system to gain information on the possible relationships between surface catalytic activity and bulk structure. Hydrogen peroxide decomposition rate constants were measured for these compounds. Ex situ Mossbauer effect spectroscopy (MES), and magnetic susceptibility measurements were used to study the solid state properties. X ray photoelectron spectroscopy (XPS) was used to examine the surface. MES has indicated the presence of a paramagnetic to magnetically ordered phase transition for values of x between 0.4 and 0.5. A correlation was found between the values of the MES isomer shift and the catalytic activity for peroxide decomposition. Thus, the catalytic activity can be correlated to the d-electron density for the transition metal cations.

  10. Magnetic and electrical properties of quadruple perovskites with 12 layer structures Ba{sub 4}LnM{sub 3}O{sub 12} (Ln=rare earths; M=Ru, Ir): The role of metal-metal bonding in perovskite-related oxides

    SciTech Connect

    Shimoda, Yuki; Doi, Yoshihiro; Wakeshima, Makoto; Hinatsu, Yukio

    2010-09-15

    Structures and magnetic and electrical properties of quadruple perovskites containing rare earths Ba{sub 4}LnM{sub 3}O{sub 12} (Ln=rare earths; M=Ru, Ir) were investigated. They crystallize in the 12L-perovskite-type structure. Three MO{sub 6} octahedra are connected to each other by face-sharing and form a M{sub 3}O{sub 12} trimer. The M{sub 3}O{sub 12} trimers and LnO{sub 6} octahedra are alternately linked by corner-sharing, forming the perovskite-type structure with 12 layers. For Ln=Ce, Pr, and Tb, both the Ln and M ions are in the tetravalent state (Ba{sub 4}Ln{sup 4+}M{sup 4+}{sub 3}O{sub 12}), and for other Ln ions, Ln ions are in the trivalent state and the mean oxidation state of M ions is +4.33 (Ba{sub 4}Ln{sup 3+}M{sup 4.33+}{sub 3}O{sub 12}). All the Ba{sub 4}Ln{sup 3+}Ru{sup 4.33+}{sub 3}O{sub 12} compounds show magnetic ordering at low temperatures, while any of the corresponding iridium-containing compounds Ba{sub 4}Ln{sup 3+}Ir{sup 4.33+}{sub 3}O{sub 12} is paramagnetic down to 1.8 K. Ba{sub 4}Ce{sup 4+}Ir{sup 4+}{sub 3}O{sub 12} orders antiferromagnetically at 10.5 K, while the corresponding ruthenium-containing compound Ba{sub 4}Ce{sup 4+}Ru{sup 4+}{sub 3}O{sub 12} is paramagnetic. These magnetic results were well understood by the magnetic behavior of M{sub 3}O{sub 12}. The effective magnetic moments and the entropy change for the magnetic ordering show that the trimers Ru{sup 4.33+}{sub 3}O{sub 12} and Ir{sup 4+}{sub 3}O{sub 12} have the S=1/2 ground state, and in other cases there is no magnetic contribution from the trimers Ru{sup 4+}{sub 3}O{sub 12} or Ir{sup 4.33+}{sub 3}O{sub 12}. Measurements of the electrical resistivity of Ba{sub 4}LnM{sub 3}O{sub 12} and its analysis show that these compounds demonstrate two-dimensional Mott-variable range hopping behavior. - Graphical abstract: Structures and magnetic and electrical properties of quadruple perovskites containing rare earths Ba{sub 4}LnM{sub 3}O{sub 12} (Ln=rare earths; M = Ru, Ir

  11. Substantial improvement of perovskite solar cells stability by pinhole-free hole transport layer with doping engineering

    PubMed Central

    Jung, Min-Cherl; Raga, Sonia R.; Ono, Luis K.; Qi, Yabing

    2015-01-01

    We fabricated perovskite solar cells using a triple-layer of n-type doped, intrinsic, and p-type doped 2,2′,7,7′-tetrakis(N,N′-di-p-methoxyphenylamine)-9,9′-spirobifluorene (spiro-OMeTAD) (n-i-p) as hole transport layer (HTL) by vacuum evaporation. The doping concentration for n-type doped spiro-OMeTAD was optimized to adjust the highest occupied molecular orbital of spiro-OMeTAD to match the valence band maximum of perovskite for efficient hole extraction while maintaining a high open circuit voltage. Time-dependent solar cell performance measurements revealed significantly improved air stability for perovskite solar cells with the n-i-p structured spiro-OMeTAD HTL showing sustained efficiencies even after 840 h of air exposure. PMID:25985417

  12. Cooperative tin oxide fullerene electron selective layers for high-performance planar perovskite solar cells

    SciTech Connect

    Ke, Weijun; Zhao, Dewei; Xiao, Chuanxiao; Wang, Changlei; Cimaroli, Alexander J.; Grice, Corey R.; Yang, Mengjin; Li, Zhen; Jiang, Chun-Sheng; Al-Jassim, Mowafak; Zhu, Kai; Kanatzidis, Mercouri G.; Fang, Guojia; Yan, Yanfa

    2016-01-01

    Both tin oxide (SnO2) and fullerenes have been reported as electron selective layers (ESLs) for producing efficient lead halide perovskite solar cells. Here, we report that SnO2 and fullerenes can work cooperatively to further boost the performance of perovskite solar cells. We find that fullerenes can be redissolved during perovskite deposition, allowing ultra-thin fullerenes to be retained at the interface and some dissolved fullerenes infiltrate into perovskite grain boundaries. The SnO2 layer blocks holes effectively; whereas, the fullerenes promote electron transfer and passivate both the SnO2/perovskite interface and perovskite grain boundaries. With careful device optimization, the best-performing planar perovskite solar cell using a fullerene passivated SnO2 ESL has achieved a steady-state efficiency of 17.75% and a power conversion efficiency of 19.12% with an open circuit voltage of 1.12 V, a short-circuit current density of 22.61 mA cm-2, and a fill factor of 75.8% when measured under reverse voltage scanning. We find that the partial dissolving of fullerenes during perovskite deposition is the key for fabricating high-performance perovskite solar cells based on metal oxide/fullerene ESLs.

  13. Toward tailorable surfaces: a combined theoretical and experimental study of lanthanum niobate layered perovskites.

    PubMed

    Di Tommaso, Stefania; Giannici, Francesco; Mossuto Marculescu, Adriana; Martorana, Antonino; Adamo, Carlo; Labat, Frédèric

    2014-07-14

    A comprehensive theoretical investigation of the MLaNb2O7 (M = H, Li, Na, K, Rb, and Cs) series of ion-exchangeable layered perovskite is presented. These perovskites are in particular interesting in view of their potential applications as inorganic supports for the design of new hybrid inorganic-organic proton conductors. In particular, their structural and electronic properties have been investigated by periodic calculations in the framework of Density Functional Theory, using different exchange-correlation functionals. A general very good agreement with the available experimental (XRD, NPD, and EXAFS) data has been found. The structure of the protonated HLaNb2O7 form has also been further clarified and a new tetragonal space group is proposed for this compound, better reproducing the experimental cell parameters and yielding to a more realistic picture of the system. The electronic investigation highlighted that all the compounds considered are very similar to each other and that the interaction between interlayer cations and perovskite slabs is purely ionic, except for the proton that is, instead, covalently bound.

  14. Laser-induced microstructuring of two-dimensional layered inorganic-organic perovskites.

    PubMed

    Kanaujia, Pawan K; Vijaya Prakash, G

    2016-04-14

    Non-contact bi-directional micropatterning of two-dimensional (2D) layered inorganic-organic (IO) perovskite [(R-NH3)2PbI4, R = organic moiety] thin films by direct laser writing (DLW) has been reported. These 2D materials are in the form of natural multiple quantum well (MQW) structures and show excitonic luminescence at room temperature because of quantum and dielectric confinement effects. Systematic optical and structural analyses of these laser processed hybrid systems provide an insight into laser-matter interaction and a pathway to develop technology to define complex 2D material based devices with new functionalities. These laser-matter interaction studies reveal several concurrent processes: single photon absorption, material ablation, melting and agglomeration of nanostructures and chemical/physical modifications. This study also provides an insight into chemical and optical changes in laser processed 2D perovskites which subsequently can be recovered by chemical processing. Apart from controllable feature sizes, the prolonged laser exposure results in material agglomeration in the form of nano-pillars at the laser track boundaries. Low-cost micro/nano-scaffolding of IO perovskites may have several important advantages in scalable optoelectronic devices, the realisation of luminescent photonic architectures (photonic crystals and waveguides), and light harvesting elements for IO LEDs and solar cells.

  15. Toward tailorable surfaces: A combined theoretical and experimental study of lanthanum niobate layered perovskites

    SciTech Connect

    Di Tommaso, Stefania E-mail: frederic.labat@chimie-paristech.fr; Giannici, Francesco; Mossuto Marculescu, Adriana; Martorana, Antonino; Adamo, Carlo; Labat, Frédèric E-mail: frederic.labat@chimie-paristech.fr

    2014-07-14

    A comprehensive theoretical investigation of the MLaNb{sub 2}O{sub 7} (M = H, Li, Na, K, Rb, and Cs) series of ion-exchangeable layered perovskite is presented. These perovskites are in particular interesting in view of their potential applications as inorganic supports for the design of new hybrid inorganic-organic proton conductors. In particular, their structural and electronic properties have been investigated by periodic calculations in the framework of Density Functional Theory, using different exchange-correlation functionals. A general very good agreement with the available experimental (XRD, NPD, and EXAFS) data has been found. The structure of the protonated HLaNb{sub 2}O{sub 7} form has also been further clarified and a new tetragonal space group is proposed for this compound, better reproducing the experimental cell parameters and yielding to a more realistic picture of the system. The electronic investigation highlighted that all the compounds considered are very similar to each other and that the interaction between interlayer cations and perovskite slabs is purely ionic, except for the proton that is, instead, covalently bound.

  16. Laser-induced microstructuring of two-dimensional layered inorganic-organic perovskites.

    PubMed

    Kanaujia, Pawan K; Vijaya Prakash, G

    2016-04-14

    Non-contact bi-directional micropatterning of two-dimensional (2D) layered inorganic-organic (IO) perovskite [(R-NH3)2PbI4, R = organic moiety] thin films by direct laser writing (DLW) has been reported. These 2D materials are in the form of natural multiple quantum well (MQW) structures and show excitonic luminescence at room temperature because of quantum and dielectric confinement effects. Systematic optical and structural analyses of these laser processed hybrid systems provide an insight into laser-matter interaction and a pathway to develop technology to define complex 2D material based devices with new functionalities. These laser-matter interaction studies reveal several concurrent processes: single photon absorption, material ablation, melting and agglomeration of nanostructures and chemical/physical modifications. This study also provides an insight into chemical and optical changes in laser processed 2D perovskites which subsequently can be recovered by chemical processing. Apart from controllable feature sizes, the prolonged laser exposure results in material agglomeration in the form of nano-pillars at the laser track boundaries. Low-cost micro/nano-scaffolding of IO perovskites may have several important advantages in scalable optoelectronic devices, the realisation of luminescent photonic architectures (photonic crystals and waveguides), and light harvesting elements for IO LEDs and solar cells. PMID:26996747

  17. Kinetics of Ion Transport in Perovskite Active Layers and Its Implications for Active Layer Stability.

    PubMed

    Bag, Monojit; Renna, Lawrence A; Adhikari, Ramesh Y; Karak, Supravat; Liu, Feng; Lahti, Paul M; Russell, Thomas P; Tuominen, Mark T; Venkataraman, D

    2015-10-14

    Solar cells fabricated using alkyl ammonium metal halides as light absorbers have the right combination of high power conversion efficiency and ease of fabrication to realize inexpensive but efficient thin film solar cells. However, they degrade under prolonged exposure to sunlight. Herein, we show that this degradation is quasi-reversible, and that it can be greatly lessened by simple modifications of the solar cell operating conditions. We studied perovskite devices using electrochemical impedance spectroscopy (EIS) with methylammonium (MA)-, formamidinium (FA)-, and MA(x)FA(1-x) lead triiodide as active layers. From variable temperature EIS studies, we found that the diffusion coefficient using MA ions was greater than when using FA ions. Structural studies using powder X-ray diffraction (PXRD) show that for MAPbI3 a structural change and lattice expansion occurs at device operating temperatures. On the basis of EIS and PXRD studies, we postulate that in MAPbI3 the predominant mechanism of accelerated device degradation under sunlight involves thermally activated fast ion transport coupled with a lattice-expanding phase transition, both of which are facilitated by absorption of the infrared component of the solar spectrum. Using these findings, we show that the devices show greatly improved operation lifetimes and stability under white-light emitting diodes, or under a solar simulator with an infrared cutoff filter or with cooling. PMID:26414066

  18. Tunable Negative Thermal Expansion in Layered Perovskites from Quasi-Two-Dimensional Vibrations

    NASA Astrophysics Data System (ADS)

    Huang, Liang-Feng; Lu, Xue-Zeng; Rondinelli, James M.

    2016-09-01

    We identify a quasi-two-dimensional (quasi-2D) phonon mode in the layered-perovskite Ca3Ti2O7, which exhibits an acoustic branch with quadratic dispersion. Using first-principles methods, we show this mode exhibits atomic displacements perpendicular to the layered [CaTiO3]2 blocks comprising the structure and a negative Grüneisen parameter. Owing to these quasi-2D structural and dynamical features, we find that the mode can be utilized to realize unusual membrane effects, including a tunable negative thermal expansion (NTE) and a rare pressure-independent thermal softening of the bulk modulus. Detailed microscopic analysis shows that the NTE relies on strong intralayer Ti—O covalent bonding and weaker interlayer interactions, which is in contrast to conventional NTE mechanisms for perovskites, such as rigid-unit modes, structural transitions, and electronic or magnetic ordering. The general application of the quasi-2D lattice dynamics opens exciting avenues for the control of lattice dynamical and thermodynamic responses of other complex layered compounds through rational chemical substitution, as we show in A3Zr2O7 (A =Ca , Sr), and by heterostructuring.

  19. Tunable Negative Thermal Expansion in Layered Perovskites from Quasi-Two-Dimensional Vibrations.

    PubMed

    Huang, Liang-Feng; Lu, Xue-Zeng; Rondinelli, James M

    2016-09-01

    We identify a quasi-two-dimensional (quasi-2D) phonon mode in the layered-perovskite Ca_{3}Ti_{2}O_{7}, which exhibits an acoustic branch with quadratic dispersion. Using first-principles methods, we show this mode exhibits atomic displacements perpendicular to the layered [CaTiO_{3}]_{2} blocks comprising the structure and a negative Grüneisen parameter. Owing to these quasi-2D structural and dynamical features, we find that the mode can be utilized to realize unusual membrane effects, including a tunable negative thermal expansion (NTE) and a rare pressure-independent thermal softening of the bulk modulus. Detailed microscopic analysis shows that the NTE relies on strong intralayer Ti-O covalent bonding and weaker interlayer interactions, which is in contrast to conventional NTE mechanisms for perovskites, such as rigid-unit modes, structural transitions, and electronic or magnetic ordering. The general application of the quasi-2D lattice dynamics opens exciting avenues for the control of lattice dynamical and thermodynamic responses of other complex layered compounds through rational chemical substitution, as we show in A_{3}Zr_{2}O_{7} (A=Ca, Sr), and by heterostructuring. PMID:27661701

  20. Special quasirandom structures for perovskite solid solutions.

    PubMed

    Jiang, Zhijun; Nahas, Yousra; Xu, Bin; Prosandeev, Sergey; Wang, Dawei; Bellaiche, Laurent

    2016-11-30

    Special quasirandom structures (SQS) are presently generated for disordered (A'1-x [Formula: see text] x )BX3 and A(B'1-x [Formula: see text] x )X3 perovskite solid solutions, with x  =  1/2 as well as 1/3 and 2/3. These SQS configurations are obtained by imposing that the so-called Cowley parameters are as close to zero as possible for the three nearest neighboring shells. Moreover, these SQS configurations are slightly larger in size than those available in the literature for x  =  1/2, mostly because of the current capabilities of atomistic techniques. They are used here within effective Hamiltonian schemes to predict various properties, which are then compared to those associated with large random supercells, in a variety of compounds, namely (Ba1-x Sr x )TiO3, Pb(Zr1-x Ti x )O3, Pb(Sc0.5Nb0.5)O3, Ba(Zr1-x Ti x )O3, Pb(Mg1/3Nb2/3)O3 and (Bi1-x Nd x )FeO3. It is found that these SQS configurations can reproduce many properties of large random supercells of most of these disordered perovskite alloys, below some finite material-dependent temperature. Examples of these properties are electrical polarization, anti-phase and in-phase octahedral tiltings, antipolar motions, antiferromagnetism, strain, piezoelectric coefficients, dielectric response, specific heat and even the formation of polar nanoregions (PNRs) in some relaxors. Some limitations of these SQS configurations are also pointed out and explained. PMID:27661191

  1. Special quasirandom structures for perovskite solid solutions

    NASA Astrophysics Data System (ADS)

    Jiang, Zhijun; Nahas, Yousra; Xu, Bin; Prosandeev, Sergey; Wang, Dawei; Bellaiche, Laurent

    2016-11-01

    Special quasirandom structures (SQS) are presently generated for disordered (A‧1-x {{\\text{A}}\\prime \\prime} x )BX3 and A(B‧1-x {{\\text{B}}\\prime \\prime} x )X3 perovskite solid solutions, with x  =  1/2 as well as 1/3 and 2/3. These SQS configurations are obtained by imposing that the so-called Cowley parameters are as close to zero as possible for the three nearest neighboring shells. Moreover, these SQS configurations are slightly larger in size than those available in the literature for x  =  1/2, mostly because of the current capabilities of atomistic techniques. They are used here within effective Hamiltonian schemes to predict various properties, which are then compared to those associated with large random supercells, in a variety of compounds, namely (Ba1-x Sr x )TiO3, Pb(Zr1-x Ti x )O3, Pb(Sc0.5Nb0.5)O3, Ba(Zr1-x Ti x )O3, Pb(Mg1/3Nb2/3)O3 and (Bi1-x Nd x )FeO3. It is found that these SQS configurations can reproduce many properties of large random supercells of most of these disordered perovskite alloys, below some finite material-dependent temperature. Examples of these properties are electrical polarization, anti-phase and in-phase octahedral tiltings, antipolar motions, antiferromagnetism, strain, piezoelectric coefficients, dielectric response, specific heat and even the formation of polar nanoregions (PNRs) in some relaxors. Some limitations of these SQS configurations are also pointed out and explained.

  2. New solid acids in the triple-layer Dion-Jacobson layered perovskite family

    SciTech Connect

    Geselbracht, Margret J.; White, Helen K.; Blaine, Jeanette M.; Diaz, Miranda J.; Hubbs, Jennifer L.; Adelstein, Nicole; Kurzman, Joshua A.

    2011-03-15

    Research highlights: {yields} New triple-layer Dion-Jacobson layered perovskite solid solutions synthesized. {yields} New series of Ta-doped layered perovskite solid acids, HCa{sub 2}Nb{sub 3-x}Ta{sub x}O{sub 10}. {yields} New series of Sr-doped layered perovskite solid acids, HCa{sub 2-x}Sr{sub x}Nb{sub 3}O{sub 10}. {yields} Layered perovskites with highest Ta content are weaker solid acids than HCa{sub 2}Nb{sub 3}O{sub 10}. -- Abstract: Dion-Jacobson type layered perovskites such as A'Ca{sub 2}Nb{sub 3}O{sub 10} (A' = K, Rb, H) have continued to be of great interest due to their compositional variability, rich interlayer chemistry, and wide range of physical properties. In this study, we investigated the range and effects of substitutional doping of Ta{sup 5+} for Nb{sup 5+} and of Sr{sup 2+} for Ca{sup 2+} in A'Ca{sub 2}Nb{sub 3}O{sub 10}. We have prepared and characterized three new solid solutions: KCa{sub 2}Nb{sub 3-x}Ta{sub x}O{sub 10}, RbCa{sub 2}Nb{sub 3-x}Ta{sub x}O{sub 10}, and RbCa{sub 2-x}Sr{sub x}Nb{sub 3}O{sub 10}. These materials all readily undergo proton exchange to form two new series of hydrated solid acid phases, which in most cases can be dehydrated to form stable HCa{sub 2}Nb{sub 3-x}Ta{sub x}O{sub 10} and HCa{sub 2-x}Sr{sub x}Nb{sub 3}O{sub 10} compounds. Intercalation studies with n-hexylamine and pyridine were carried out to gauge the relative Bronsted acidities across the HCa{sub 2}Nb{sub 3-x}Ta{sub x}O{sub 10} series, and we determined that materials with the highest tantalum contents are weaker acids than the parent compound HCa{sub 2}Nb{sub 3}O{sub 10}. Preliminary intercalation studies with pyridine for the HCa{sub 2-x}Sr{sub x}Nb{sub 3}O{sub 10}.yH{sub 2}O solid acids, however, showed no significant difference in acidity with varying strontium content.

  3. Highly Efficient Perovskite Solar Cells with Tunable Structural Color

    PubMed Central

    2015-01-01

    The performance of perovskite solar cells has been progressing over the past few years and efficiency is likely to continue to increase. However, a negative aspect for the integration of perovskite solar cells in the built environment is that the color gamut available in these materials is very limited and does not cover the green-to-blue region of the visible spectrum, which has been a big selling point for organic photovoltaics. Here, we integrate a porous photonic crystal (PC) scaffold within the photoactive layer of an opaque perovskite solar cell following a bottom-up approach employing inexpensive and scalable liquid processing techniques. The photovoltaic devices presented herein show high efficiency with tunable color across the visible spectrum. This now imbues the perovskite solar cells with highly desirable properties for cladding in the built environment and encourages design of sustainable colorful buildings and iridescent electric vehicles as future power generation sources. PMID:25650872

  4. Highly efficient perovskite solar cells with tunable structural color.

    PubMed

    Zhang, Wei; Anaya, Miguel; Lozano, Gabriel; Calvo, Mauricio E; Johnston, Michael B; Míguez, Hernán; Snaith, Henry J

    2015-03-11

    The performance of perovskite solar cells has been progressing over the past few years and efficiency is likely to continue to increase. However, a negative aspect for the integration of perovskite solar cells in the built environment is that the color gamut available in these materials is very limited and does not cover the green-to-blue region of the visible spectrum, which has been a big selling point for organic photovoltaics. Here, we integrate a porous photonic crystal (PC) scaffold within the photoactive layer of an opaque perovskite solar cell following a bottom-up approach employing inexpensive and scalable liquid processing techniques. The photovoltaic devices presented herein show high efficiency with tunable color across the visible spectrum. This now imbues the perovskite solar cells with highly desirable properties for cladding in the built environment and encourages design of sustainable colorful buildings and iridescent electric vehicles as future power generation sources.

  5. In Situ Intercalation Dynamics in Inorganic–Organic Layered Perovskite Thin Films

    PubMed Central

    2014-01-01

    The properties of layered inorganic semiconductors can be manipulated by the insertion of foreign molecular species via a process known as intercalation. In the present study, we investigate the phenomenon of organic moiety (R-NH3I) intercalation in layered metal-halide (PbI2)-based inorganic semiconductors, leading to the formation of inorganic–organic (IO) perovskites [(R-NH3)2PbI4]. During this intercalation strong resonant exciton optical transitions are created, enabling study of the dynamics of this process. Simultaneous in situ photoluminescence (PL) and transmission measurements are used to track the structural and exciton evolution. On the basis of the experimental observations, a model is proposed which explains the process of IO perovskite formation during intercalation of the organic moiety through the inorganic semiconductor layers. The interplay between precursor film thickness and organic solution concentration/solvent highlights the role of van der Waals interactions between the layers, as well as the need for maintaining stoichiometry during intercalation. Nucleation and growth occurring during intercalation matches a Johnson–Mehl–Avrami–Kolmogorov model, with results fitting both ideal and nonideal cases. PMID:24905435

  6. Efficient Light Harvester Layer Prepared by Solid/Mist Interface Reaction for Perovskite Solar Cells.

    PubMed

    Xia, Xiang; Li, Hongcui; Wu, Wenyi; Li, Yanhua; Fei, Dehou; Gao, Chunxiao; Liu, Xizhe

    2015-08-12

    A solid/mist reaction method is developed to produce well-crystallized light harvester layers without pinhole defects for perovskite solar cells. The reaction based on mist precursor can be facilely operated with low process temperature. And it can effectively control the volume of CH3NH3I solution and the reaction temperature, which affect the quality of perovskite harvester layers and the performance of perovskite solar cells remarkably. Under optimized condition, the efficiencies of devices reach 16.2% with the average efficiency of 14.9%. The solid/mist reaction is also used to fabricate planar junction solar cells and a PCE of 14.9% is obtained.

  7. Ab initio study of metastable layered perovskites R2Ti2O7 (R = Sm and Gd)

    NASA Astrophysics Data System (ADS)

    Sayede, Adlane; Bruyer, Emilie; Springborg, Michael

    2012-09-01

    The structural, electronic, and ferroelectric properties of metastable R2Ti2O7(R= Sm and Gd) layered perovskites materials are investigated by first-principles density functional theory calculations. The computed structural parameters are found to be in good agreement with experimental findings. The calculated spontaneous polarizations of the studied titanates are found to be larger than the spontaneous polarization of the usual R2Ti2O7 layered perovskites materials. GGA+U electronic structures predict a good photocatalytic activity for the studied compounds, in particular for Gd2Ti2O7, which lacks electron-carriers trapping in the conduction band. From the results of the total energy and the polarization as functions of structure we estimate the responses of the materials to external electrostatic fields.

  8. Layered-structural monoclinic–orthorhombic perovskite La{sub 2}Ti{sub 2}O{sub 7} to orthorhombic LaTiO{sub 3} phase transition and their microstructure characterization

    SciTech Connect

    Herrera, G.; Jiménez-Mier, J.; Chavira, E.

    2014-03-01

    The layered-structural ceramics, such as lanthanum titanate (La{sub 2}Ti{sub 2}O{sub 7}), have been known for their good temperature and low dielectric loss at microwave frequencies that make them good candidate materials for high frequency applications. However, few studies have been conducted on the synthesis optimization by sol gel reaction, in particular by acrylamide polymerization route. The interest in La{sub 2}Ti{sub 2}O{sub 7} ceramic has been greatly increased recently due to the effect of oriented grains. This anisotropy of the microstructure leads to anisotropy in dielectric, electrical and mechanical properties. In this study, grain oriented lanthanum titanate was produced by the sol–gel acrylamide polymerization route. The characterizations of the samples were achieved by thermal analysis, X-ray diffraction (XRD), scanning electron microscopy (SEM), atomic force microscopy (AFM), and transmission electron microscopy (TEM). X-ray diffraction indicates that the formation of monoclinic perovskite La{sub 2}Ti{sub 2}O{sub 7} nanocrystals is a necessary first step to obtain orthorhombic LaTiO{sub 3} nanocomposites (with space group Pbnm). In this work we identified that the monoclinic perovskite La{sub 2}Ti{sub 2}O{sub 7} with space group P2{sub 1} transforms its structure into one with the orthorhombic space group Cmc2{sub 1} at approximately 1073 K. The microstructure associated consisted of flaky monoclinic La{sub 2}Ti{sub 2}O{sub 7} nanocomposites in comparison with round-shaped LaTiO{sub 3} nanocomposites. - Highlights: • The flaky-like La{sub 2}Ti{sub 2}O{sub 7} compound was synthesized by sol–gel acrylamide route. • Simultaneous monitoring of the DTA and XRD with temperature was performed. • Phase transformation characterization of La{sub 2}Ti{sub 2}O{sub 7} has been carried out. • The variation of the La{sub 2}Ti{sub 2}O{sub 7} and LaTiO{sub 3} grain morphology has been compared.

  9. High Efficiency Tandem Thin-Perovskite/Polymer Solar Cells with a Graded Recombination Layer.

    PubMed

    Liu, Yao; Renna, Lawrence A; Bag, Monojit; Page, Zachariah A; Kim, Paul; Choi, Jaewon; Emrick, Todd; Venkataraman, D; Russell, Thomas P

    2016-03-23

    Perovskite-containing tandem solar cells are attracting attention for their potential to achieve high efficiencies. We demonstrate a series connection of a ∼ 90 nm thick perovskite front subcell and a ∼ 100 nm thick polymer:fullerene blend back subcell that benefits from an efficient graded recombination layer containing a zwitterionic fullerene, silver (Ag), and molybdenum trioxide (MoO3). This methodology eliminates the adverse effects of thermal annealing or chemical treatment that occurs during perovskite fabrication on polymer-based front subcells. The record tandem perovskite/polymer solar cell efficiency of 16.0%, with low hysteresis, is 75% greater than that of the corresponding ∼ 90 nm thick perovskite single-junction device and 65% greater than that of the polymer single-junction device. The high efficiency of this hybrid tandem device, achieved using only a ∼ 90 nm thick perovskite layer, provides an opportunity to substantially reduce the lead content in the device, while maintaining the high performance derived from perovskites. PMID:26918708

  10. High Efficiency Tandem Thin-Perovskite/Polymer Solar Cells with a Graded Recombination Layer.

    PubMed

    Liu, Yao; Renna, Lawrence A; Bag, Monojit; Page, Zachariah A; Kim, Paul; Choi, Jaewon; Emrick, Todd; Venkataraman, D; Russell, Thomas P

    2016-03-23

    Perovskite-containing tandem solar cells are attracting attention for their potential to achieve high efficiencies. We demonstrate a series connection of a ∼ 90 nm thick perovskite front subcell and a ∼ 100 nm thick polymer:fullerene blend back subcell that benefits from an efficient graded recombination layer containing a zwitterionic fullerene, silver (Ag), and molybdenum trioxide (MoO3). This methodology eliminates the adverse effects of thermal annealing or chemical treatment that occurs during perovskite fabrication on polymer-based front subcells. The record tandem perovskite/polymer solar cell efficiency of 16.0%, with low hysteresis, is 75% greater than that of the corresponding ∼ 90 nm thick perovskite single-junction device and 65% greater than that of the polymer single-junction device. The high efficiency of this hybrid tandem device, achieved using only a ∼ 90 nm thick perovskite layer, provides an opportunity to substantially reduce the lead content in the device, while maintaining the high performance derived from perovskites.

  11. Evidence for reduced charge recombination in carbon nanotube/perovskite-based active layers

    NASA Astrophysics Data System (ADS)

    Bag, Monojit; Renna, Lawrence A.; Jeong, Seung Pyo; Han, Xu; Cutting, Christie L.; Maroudas, Dimitrios; Venkataraman, D.

    2016-10-01

    Using impedance spectroscopy and computation, we show that incorporation of multi-walled carbon nanotubes (MWCNTs) in the bulk of the active layer of perovskite-based solar cells reduces charge recombination and increases the open circuit voltage. An ∼87% reduction in recombination was achieved when MWCNTs were introduced in the planar-heterostructure perovskite solar cell containing mixed counterions. The open circuit voltage (Voc) of perovskite/MWCNTs devices was increased by 70 mV, while the short circuit current density (Jsc) and fill factor (FF) remained unchanged.

  12. Epitaxial Growth of Perovskite Strontium Titanate on Germanium via Atomic Layer Deposition.

    PubMed

    Lin, Edward L; Edmondson, Bryce I; Hu, Shen; Ekerdt, John G

    2016-01-01

    Atomic layer deposition (ALD) is a commercially utilized deposition method for electronic materials. ALD growth of thin films offers thickness control and conformality by taking advantage of self-limiting reactions between vapor-phase precursors and the growing film. Perovskite oxides present potential for next-generation electronic materials, but to-date have mostly been deposited by physical methods. This work outlines a method for depositing SrTiO3 (STO) on germanium using ALD. Germanium has higher carrier mobilities than silicon and therefore offers an alternative semiconductor material with faster device operation. This method takes advantage of the instability of germanium's native oxide by using thermal deoxidation to clean and reconstruct the Ge (001) surface to the 2×1 structure. 2-nm thick, amorphous STO is then deposited by ALD. The STO film is annealed under ultra-high vacuum and crystallizes on the reconstructed Ge surface. Reflection high-energy electron diffraction (RHEED) is used during this annealing step to monitor the STO crystallization. The thin, crystalline layer of STO acts as a template for subsequent growth of STO that is crystalline as-grown, as confirmed by RHEED. In situ X-ray photoelectron spectroscopy is used to verify film stoichiometry before and after the annealing step, as well as after subsequent STO growth. This procedure provides framework for additional perovskite oxides to be deposited on semiconductors via chemical methods in addition to the integration of more sophisticated heterostructures already achievable by physical methods. PMID:27501462

  13. A new layered perovskite, KSrNb2O6F, by powder neutron diffraction.

    PubMed

    Yoo, Chung Yul; Hong, Kun Pyo; Kim, Seung Joo

    2007-08-01

    The structure of a new layered oxyfluoride, viz. potassium strontium diniobium hexaoxide fluoride, KSrNb(2)O(6)F, was refined from powder neutron diffraction data in the orthorhombic space group Immm. The oxyfluoride compound is an n = 2 member of the Dion-Jacobson-type family of general formula A[A'(n-1)B(n)X(3n+1)], which consists of double layered perovskite slabs, [SrNb(2)O(6)F](-), between which K(+) ions are located. Within the perovskite slabs, the NbO(5)F octahedra are significantly distorted and tilted about the a axis. A bond-valence-sum calculation gives evidence for O/F ordering in KSrNb(2)O(6)F, with the F(-) ions located in the central sites of the corner-sharing NbO(5)F octahedra along the b axis. All atoms lie on special positions, namely Nb on m, Sr on mmm, K on m2m, F on mm2, and O on sites of symmetry m and m2m.

  14. Flexible perovskite solar cells based on the metal-insulator-semiconductor structure.

    PubMed

    Wei, Jing; Li, Heng; Zhao, Yicheng; Zhou, Wenke; Fu, Rui; Pan, Huiyue; Zhao, Qing

    2016-09-14

    The metal-insulator-semiconductor (MIS) structure is applied to perovskite solar cells, in which the traditional compact layer TiO2 is replaced by Al2O3 as the hole blocking material to realize an all-low-temperature process. Flexible devices based on this structure are also realized with excellent flexibility, which hold 85% of their initial efficiency after bending 100 times. PMID:27524362

  15. Highly stable perovskite solar cells with an all-carbon hole transport layer.

    PubMed

    Wang, Feijiu; Endo, Masaru; Mouri, Shinichiro; Miyauchi, Yuhei; Ohno, Yutaka; Wakamiya, Atsushi; Murata, Yasujiro; Matsuda, Kazunari

    2016-06-01

    Nano-carbon materials (carbon nanotubes, graphene, and graphene oxide) have potential application for photovoltaics because of their excellent optical and electronic properties. Here, we demonstrate that a single-walled carbon nanotubes/graphene oxide buffer layer greatly improves the photovoltaic performance of organo-lead iodide perovskite solar cells. The carbon nanotubes/graphene oxide buffer layer works as an efficient hole transport/electron blocking layer. The photovoltaic conversion efficiency of 13.3% was achieved in the organo-lead iodide perovskite solar cell due to the complementary properties of carbon nanotubes and graphene oxide. Furthermore, the great improvement of photovoltaic performance stability in the perovskite solar cells using carbon nanotubes/graphene oxide/polymethyl methacrylate was demonstrated in comparison with that using a typical organic hole transport layer of 2,2',7,7'-tetrakis-(N,N-di-4-methoxyphenylamino)-9,9'-spirobifluorene.

  16. Highly stable perovskite solar cells with an all-carbon hole transport layer.

    PubMed

    Wang, Feijiu; Endo, Masaru; Mouri, Shinichiro; Miyauchi, Yuhei; Ohno, Yutaka; Wakamiya, Atsushi; Murata, Yasujiro; Matsuda, Kazunari

    2016-06-01

    Nano-carbon materials (carbon nanotubes, graphene, and graphene oxide) have potential application for photovoltaics because of their excellent optical and electronic properties. Here, we demonstrate that a single-walled carbon nanotubes/graphene oxide buffer layer greatly improves the photovoltaic performance of organo-lead iodide perovskite solar cells. The carbon nanotubes/graphene oxide buffer layer works as an efficient hole transport/electron blocking layer. The photovoltaic conversion efficiency of 13.3% was achieved in the organo-lead iodide perovskite solar cell due to the complementary properties of carbon nanotubes and graphene oxide. Furthermore, the great improvement of photovoltaic performance stability in the perovskite solar cells using carbon nanotubes/graphene oxide/polymethyl methacrylate was demonstrated in comparison with that using a typical organic hole transport layer of 2,2',7,7'-tetrakis-(N,N-di-4-methoxyphenylamino)-9,9'-spirobifluorene. PMID:27232674

  17. Highly stable perovskite solar cells with an all-carbon hole transport layer

    NASA Astrophysics Data System (ADS)

    Wang, Feijiu; Endo, Masaru; Mouri, Shinichiro; Miyauchi, Yuhei; Ohno, Yutaka; Wakamiya, Atsushi; Murata, Yasujiro; Matsuda, Kazunari

    2016-06-01

    Nano-carbon materials (carbon nanotubes, graphene, and graphene oxide) have potential application for photovoltaics because of their excellent optical and electronic properties. Here, we demonstrate that a single-walled carbon nanotubes/graphene oxide buffer layer greatly improves the photovoltaic performance of organo-lead iodide perovskite solar cells. The carbon nanotubes/graphene oxide buffer layer works as an efficient hole transport/electron blocking layer. The photovoltaic conversion efficiency of 13.3% was achieved in the organo-lead iodide perovskite solar cell due to the complementary properties of carbon nanotubes and graphene oxide. Furthermore, the great improvement of photovoltaic performance stability in the perovskite solar cells using carbon nanotubes/graphene oxide/polymethyl methacrylate was demonstrated in comparison with that using a typical organic hole transport layer of 2,2',7,7'-tetrakis-(N,N-di-4-methoxyphenylamino)-9,9'-spirobifluorene.Nano-carbon materials (carbon nanotubes, graphene, and graphene oxide) have potential application for photovoltaics because of their excellent optical and electronic properties. Here, we demonstrate that a single-walled carbon nanotubes/graphene oxide buffer layer greatly improves the photovoltaic performance of organo-lead iodide perovskite solar cells. The carbon nanotubes/graphene oxide buffer layer works as an efficient hole transport/electron blocking layer. The photovoltaic conversion efficiency of 13.3% was achieved in the organo-lead iodide perovskite solar cell due to the complementary properties of carbon nanotubes and graphene oxide. Furthermore, the great improvement of photovoltaic performance stability in the perovskite solar cells using carbon nanotubes/graphene oxide/polymethyl methacrylate was demonstrated in comparison with that using a typical organic hole transport layer of 2,2',7,7'-tetrakis-(N,N-di-4-methoxyphenylamino)-9,9'-spirobifluorene. Electronic supplementary information (ESI

  18. Color-Pure Violet-Light-Emitting Diodes Based on Layered Lead Halide Perovskite Nanoplates.

    PubMed

    Liang, Dong; Peng, Yuelin; Fu, Yongping; Shearer, Melinda J; Zhang, Jingjing; Zhai, Jianyuan; Zhang, Yi; Hamers, Robert J; Andrew, Trisha L; Jin, Song

    2016-07-26

    Violet electroluminescence is rare in both inorganic and organic light-emitting diodes (LEDs). Low-cost and room-temperature solution-processed lead halide perovskites with high-efficiency and color-tunable photoluminescence are promising for LEDs. Here, we report room-temperature color-pure violet LEDs based on a two-dimensional lead halide perovskite material, namely, 2-phenylethylammonium (C6H5CH2CH2NH3(+), PEA) lead bromide [(PEA)2PbBr4]. The natural quantum confinement of two-dimensional layered perovskite (PEA)2PbBr4 allows for photoluminescence of shorter wavelength (410 nm) than its three-dimensional counterpart. By converting as-deposited polycrystalline thin films to micrometer-sized (PEA)2PbBr4 nanoplates using solvent vapor annealing, we successfully integrated this layered perovskite material into LEDs and achieved efficient room-temperature violet electroluminescence at 410 nm with a narrow bandwidth. This conversion to nanoplates significantly enhanced the crystallinity and photophysical properties of the (PEA)2PbBr4 samples and the external quantum efficiency of the violet LED. The solvent vapor annealing method reported herein can be generally applied to other perovskite materials to increase their grain size and, ultimately, improve the performance of optoelectronic devices based on perovskite materials. PMID:27336850

  19. Self limiting atomic layer deposition of Al2O3 on perovskite surfaces: a reality?

    NASA Astrophysics Data System (ADS)

    Choudhury, Devika; Rajaraman, Gopalan; Sarkar, Shaibal K.

    2016-03-01

    The feasibility of self-saturated atomic layer deposition of Al2O3 on an organolead halide perovskite (MAPbI3-xClx) surface through a well known trimethylaluminium (TMA)-water (H2O) chemistry is studied. Though the sequential dosages of reactants form films on the perovskite surfaces, a self saturated growth is never observed. Self-saturation leads to the degradation of the material. Both experimental and density functional theory calculations are carried out for complete understanding of the growth mechanism of self-limiting Al2O3 on the perovskite surface.The feasibility of self-saturated atomic layer deposition of Al2O3 on an organolead halide perovskite (MAPbI3-xClx) surface through a well known trimethylaluminium (TMA)-water (H2O) chemistry is studied. Though the sequential dosages of reactants form films on the perovskite surfaces, a self saturated growth is never observed. Self-saturation leads to the degradation of the material. Both experimental and density functional theory calculations are carried out for complete understanding of the growth mechanism of self-limiting Al2O3 on the perovskite surface. Electronic supplementary information (ESI) available: Additional QCM results, FTIR spectra and DFT results. See DOI: 10.1039/c5nr06974b

  20. Photocatalytic activity of layered perovskite-like oxides in practically valuable chemical reactions

    NASA Astrophysics Data System (ADS)

    Rodionov, I. A.; Zvereva, I. A.

    2016-03-01

    The photocatalytic properties of layered perovskite-like oxides corresponding to the Ruddlesen–Popper, Dion–Jacobson and Aurivillius phases are considered. Of the photocatalytic reactions, the focus is on the reactions of water splitting, hydrogen evolution from aqueous solutions of organic substances and degradation of model organic pollutants. Possibilities to conduct these reactions under UV and visible light in the presence of layered perovskite-like oxides and composite photocatalysts based on them are shown. The specific surface area, band gap energy, particle morphology, cation and anion doping and surface modification are considered as factors that affect the photocatalytic activity. Special attention is paid to the possibilities to enhance the photocatalytic activity by intercalation, ion exchange and exfoliation, which are inherent in this class of compounds. Conclusions are made about the prospects for the use of layered perovskite-like oxides in photocatalysis. The bibliography includes 253 references.

  1. Photocatalytic activity of layered perovskite-like oxides in practically valuable chemical reactions

    NASA Astrophysics Data System (ADS)

    Rodionov, I. A.; Zvereva, I. A.

    2016-03-01

    The photocatalytic properties of layered perovskite-like oxides corresponding to the Ruddlesen-Popper, Dion-Jacobson and Aurivillius phases are considered. Of the photocatalytic reactions, the focus is on the reactions of water splitting, hydrogen evolution from aqueous solutions of organic substances and degradation of model organic pollutants. Possibilities to conduct these reactions under UV and visible light in the presence of layered perovskite-like oxides and composite photocatalysts based on them are shown. The specific surface area, band gap energy, particle morphology, cation and anion doping and surface modification are considered as factors that affect the photocatalytic activity. Special attention is paid to the possibilities to enhance the photocatalytic activity by intercalation, ion exchange and exfoliation, which are inherent in this class of compounds. Conclusions are made about the prospects for the use of layered perovskite-like oxides in photocatalysis. The bibliography includes 253 references.

  2. Thermal stability of Dion-Jacobson mixed-metal-niobate double-layered perovskites

    SciTech Connect

    Hermann, Andrew T.; Wiley, John B.

    2009-05-06

    The thermal stability and decomposition pathways of six Dion-Jacobson-related double-layered perovskites, ALaNb{sub 2}O{sub 7} (A = H, Li, Na, Ag) and (ACl)LaNb{sub 2}O{sub 7} (A = Fe, Cu), are investigated. These compounds are made by low temperature (<400 deg. C) ion exchange reactions from RbLaNb{sub 2}O{sub 7}. All the compounds are low temperature phases with some of them exhibiting decomposition exotherms consistent with metastability. Decomposition temperatures and reactions pathways vary with the identity of A with most decompositions resulting in the formation of a niobate (containing A) and LaNbO{sub 4}. Results from differential scanning calorimetry and high temperature X-ray powder diffraction studies are presented and structural parameters pertinent to compound stability discussed.

  3. Ferromagnetic and Photocatalytic Properties of Layered Perovskite LaBaCo₂O₆ Nanostructures.

    PubMed

    Hu, Yongming; Lei, Jinmei; He, Jing; Li, Yuebin; Wang, Zhao; Wang, Yu; Gu, Haoshuang

    2016-01-01

    Cationic ordered layered tetragonal perovskite phase LaBaCo₂O₆ (LBCO) nanomaterials with irregular shape, and an average diameter of about 100 nm were successfully prepared. A precursor material was annealed in an argon atmosphere at 1100 °C for 48 hours, and then heat treated in an oxygen atmosphere pressure at 800 °C for 12 hours. The resulting LBCO nanomaterials show ferromagnetic transition at about 175 K without any structural changes. They show metallic behavior at below 140 K, and adopt the behavior of soft ferromagnetic materials at 80 K. Cationic ordered LBCO nanomaterials display photocatalytic activities, as they successfully degrade MB solutions under both UV irradiation and visible light. The B-site cations act as the active center, and are located in the centre of BO₆ octahedron units. The various valence states of Co ions in LBCO could contribute to the enhancement of photocatalytic activies. PMID:27398548

  4. Structural, magnetic and magnetocaloric properties of layered perovskite La1.1Bi0.3Sr1.6Mn2O7

    NASA Astrophysics Data System (ADS)

    Oubla, M.; Lamire, M.; Boutahar, A.; Lassri, H.; Manoun, B.; Hlil, E. K.

    2016-04-01

    The La1.1Bi0.3Sr1.6Mn2O7 sample was synthesized by coprecipitation method. Its structure has been characterized by X-ray powder diffraction. The diffraction patterns are consistent with the I4/mmm symmetry, with tetragonal lattice parameters a=3.8750±0.0001 Å and c=20.0456±0.0002 Å. Magnetic measurements have shown a ferromagnetic like ordering with second order magnetic phase transition to paramagnetic states. The magnetic entropy change caused by a magnetic field, (-∆Smax), was estimated on the basis of the Maxwell relation. The maximum magnetic entropy change (-∆Smax) and the relative cooling power (RCP) are, 1.65 J kg-1K-1 and 134.4 J kg-1 respectively, for a 5 T magnetic field change at 340 K.

  5. Exclusion of metal oxide by an RF sputtered Ti layer in flexible perovskite solar cells: energetic interface between a Ti layer and an organic charge transporting layer.

    PubMed

    Ameen, Sadia; Akhtar, M Shaheer; Seo, Hyung-Kee; Nazeeruddin, Mohammad Khaja; Shin, Hyung-Shik

    2015-04-14

    In this work, the effects of a titanium (Ti) layer on the charge transport and recombination rates of flexible perovskite solar cells were studied. Ti as an efficient barrier layer was deposited directly on PET-ITO flexible substrates through RF magnetic sputtering using a Ti-source and a pressure of ∼5 mTorr. A Ti coated PET-ITO was used for the fabrication of a flexible perovskite solar cell without using any metal oxide layer. The fabricated flexible perovskite solar cell was composed of a PET-ITO/Ti/perovskite (CH3NH3PbI3)/organic hole transport layer of 2,2',7,7'-tetrakis [N,N'-di-p-methoxyphenylamine]-9,9'-spirobifluorene (spiro-OMeTAD)-Li-TFSI/Ag. A high conversion efficiency of ∼8.39% along with a high short circuit current (JSC) of ∼15.24 mA cm(-2), an open circuit voltage (VOC) of ∼0.830 V and a high fill factor (FF) of ∼0.66 was accomplished by the fabricated flexible perovskite solar cell under a light illumination of ∼100 mW cm(-2) (1.5 AM). Intensity-modulated photocurrent (IMPS)/photovoltage spectroscopy (IMVS) studies demonstrated that the fabricated flexible perovskite solar cell considerably reduced the recombination rate.

  6. Method for fabricating high aspect ratio structures in perovskite material

    DOEpatents

    Karapetrov, Goran T.; Kwok, Wai-Kwong; Crabtree, George W.; Iavarone, Maria

    2003-10-28

    A method of fabricating high aspect ratio ceramic structures in which a selected portion of perovskite or perovskite-like crystalline material is exposed to a high energy ion beam for a time sufficient to cause the crystalline material contacted by the ion beam to have substantially parallel columnar defects. Then selected portions of the material having substantially parallel columnar defects are etched leaving material with and without substantially parallel columnar defects in a predetermined shape having high aspect ratios of not less than 2 to 1. Etching is accomplished by optical or PMMA lithography. There is also disclosed a structure of a ceramic which is superconducting at a temperature in the range of from about 10.degree. K. to about 90.degree. K. with substantially parallel columnar defects in which the smallest lateral dimension of the structure is less than about 5 microns, and the thickness of the structure is greater than 2 times the smallest lateral dimension of the structure.

  7. Efficient hole-blocking layer-free planar halide perovskite thin-film solar cells.

    PubMed

    Ke, Weijun; Fang, Guojia; Wan, Jiawei; Tao, Hong; Liu, Qin; Xiong, Liangbin; Qin, Pingli; Wang, Jing; Lei, Hongwei; Yang, Guang; Qin, Minchao; Zhao, Xingzhong; Yan, Yanfa

    2015-01-01

    Efficient lead halide perovskite solar cells use hole-blocking layers to help collection of photogenerated electrons and to achieve high open-circuit voltages. Here, we report the realization of efficient perovskite solar cells grown directly on fluorine-doped tin oxide-coated substrates without using any hole-blocking layers. With ultraviolet-ozone treatment of the substrates, a planar Au/hole-transporting material/CH₃NH₃PbI₃-xClx/substrate cell processed by a solution method has achieved a power conversion efficiency of over 14% and an open-circuit voltage of 1.06 V measured under reverse voltage scan. The open-circuit voltage is as high as that of our best reference cell with a TiO₂ hole-blocking layer. Besides ultraviolet-ozone treatment, we find that involving Cl in the synthesis is another key for realizing high open-circuit voltage perovskite solar cells without hole-blocking layers. Our results suggest that TiO₂ may not be the ultimate interfacial material for achieving high-performance perovskite solar cells. PMID:25798925

  8. Efficient hole-blocking layer-free planar halide perovskite thin-film solar cells

    NASA Astrophysics Data System (ADS)

    Ke, Weijun; Fang, Guojia; Wan, Jiawei; Tao, Hong; Liu, Qin; Xiong, Liangbin; Qin, Pingli; Wang, Jing; Lei, Hongwei; Yang, Guang; Qin, Minchao; Zhao, Xingzhong; Yan, Yanfa

    2015-03-01

    Efficient lead halide perovskite solar cells use hole-blocking layers to help collection of photogenerated electrons and to achieve high open-circuit voltages. Here, we report the realization of efficient perovskite solar cells grown directly on fluorine-doped tin oxide-coated substrates without using any hole-blocking layers. With ultraviolet-ozone treatment of the substrates, a planar Au/hole-transporting material/CH3NH3PbI3-xClx/substrate cell processed by a solution method has achieved a power conversion efficiency of over 14% and an open-circuit voltage of 1.06 V measured under reverse voltage scan. The open-circuit voltage is as high as that of our best reference cell with a TiO2 hole-blocking layer. Besides ultraviolet-ozone treatment, we find that involving Cl in the synthesis is another key for realizing high open-circuit voltage perovskite solar cells without hole-blocking layers. Our results suggest that TiO2 may not be the ultimate interfacial material for achieving high-performance perovskite solar cells.

  9. Efficient hole-blocking layer-free planar halide perovskite thin-film solar cells.

    PubMed

    Ke, Weijun; Fang, Guojia; Wan, Jiawei; Tao, Hong; Liu, Qin; Xiong, Liangbin; Qin, Pingli; Wang, Jing; Lei, Hongwei; Yang, Guang; Qin, Minchao; Zhao, Xingzhong; Yan, Yanfa

    2015-01-01

    Efficient lead halide perovskite solar cells use hole-blocking layers to help collection of photogenerated electrons and to achieve high open-circuit voltages. Here, we report the realization of efficient perovskite solar cells grown directly on fluorine-doped tin oxide-coated substrates without using any hole-blocking layers. With ultraviolet-ozone treatment of the substrates, a planar Au/hole-transporting material/CH₃NH₃PbI₃-xClx/substrate cell processed by a solution method has achieved a power conversion efficiency of over 14% and an open-circuit voltage of 1.06 V measured under reverse voltage scan. The open-circuit voltage is as high as that of our best reference cell with a TiO₂ hole-blocking layer. Besides ultraviolet-ozone treatment, we find that involving Cl in the synthesis is another key for realizing high open-circuit voltage perovskite solar cells without hole-blocking layers. Our results suggest that TiO₂ may not be the ultimate interfacial material for achieving high-performance perovskite solar cells.

  10. Photocatalytic Hydrogen Production over Chromium Doped Layered Perovskite Sr2TiO4.

    PubMed

    Sun, Xiaoqin; Xie, Yinghao; Wu, Fangfang; Chen, Hongmei; Lv, Meilin; Ni, Shuang; Liu, Gang; Xu, Xiaoxiang

    2015-08-01

    Layered semiconductor photocatalysts have been found to exhibit promising performance levels, probably linked to their interlayer framework that facilitates separation of charge carriers and the reduction/oxidation reactions. Layered titanates, however, generally demonstrate activities under UV irradiation, and therein lies the strong desire to extend their activity into the visible light region. Here, we investigated a series of layered perovskite by doping Sr2TiO4 with Cr and/or La in the hope to improve their visible light responses. Their crystal structures and other physicochemical properties were systematically explored. Our results show that La and Cr can be successfully accommodated in the layered structure and Cr is an efficient dopant for the extension of visible light absorbance. Much enhanced photocatalytic hydrogen evolution was observed after doping and was found to be composition-dependent. The highest hydrogen production rate approaches 97.7 μmol/h for Sr2Ti0.95Cr0.05O4-δ under full range irradiation (λ ≥ 250 nm) and 17 μmol/h for Sr2Ti0.9Cr0.1O4-δ under visible light irradiation (λ ≥ 400 nm), corresponding to an apparent quantum efficiency of 0.16% and 0.05%, respectively. Theoretical calculation reveals that the improved optical and photocatalytic properties are owing to a newly formed spin-polarized valence band from Cr 3d orbitals. The decreased unit cell parameters, reduced band gaps as well as anisotropic properties of layered architectures are likely the reasons for a better activity. Nevertheless, instability of these compounds in the presence of moisture and CO2 was also noticed, suggesting that protective atmospheres are needed for the storage of these photocatalysts.

  11. Towards printed perovskite solar cells with cuprous oxide hole transporting layers: a theoretical design

    NASA Astrophysics Data System (ADS)

    Wang, Yan; Xia, Zhonggao; Liang, Jun; Wang, Xinwei; Liu, Yiming; Liu, Chuan; Zhang, Shengdong; Zhou, Hang

    2015-05-01

    Solution-processed p-type metal oxide materials have shown great promise in improving the stability of perovskite-based solar cells and offering the feasibility for a low cost printing fabrication process. Herein, we performed a device modeling study on planar perovskite solar cells with cuprous oxide (Cu2O) hole transporting layers (HTLs) by using a solar cell simulation program, wxAMPS. The performance of a Cu2O/perovskite solar cell was correlated to the material properties of the Cu2O HTL, such as thickness, carrier mobility, mid-gap defect, and doping concentrations. The effect of interfacial defect densities on the solar cell performance was also investigated. Our simulation indicates that, with an optimized Cu2O HTL, high performance perovskite solar cells with efficiencies above 13% could be achieved, which shows the potential of using Cu2O as an alternative HTL over other inorganic materials, such as NiOx and MoOx. This study provides theoretical guidance for developing perovskite solar cells with inorganic hole transporting materials via a printing process.

  12. Improve efficiency of perovskite solar cells by using Magnesium doped ZnO and TiO2 compact layers

    NASA Astrophysics Data System (ADS)

    Baktash, Ardeshir; Amiri, Omid; Sasani, Alireza

    2016-05-01

    Here the effect of Magnesium doped TiO2 and ZnO as hole blocking layers (HBLs) are investigated by using solar cell capacitance simulator (SCAPS). The Impact of Magnesium concentration into the TiO2 and ZnO and effect of operating temperature on the performance of the perovskite solar cell are investigated. Best cell performance for both TiO2 and ZnO HBLs (with cell efficiencies of 19.86% and 19.57% respectively) are concluded for the doping level of 10% of Mg into the structure of HBLs. Increase in operating temperature from 300 K to 400 K are decreased the performance of the perovskite solar cell with both pure and Mg-doped HBLs. However, the cells with pure ZnO layer and with Zn0.9 Mg0.1O layer show the highest (with a decline of 8.88% in efficiency) and the lowest stability (with a decline of 50.49% in efficiency) at higher temperatures respectively. Moreover, the cell with Ti0.9 Mg0.1O2 layer shows better stability (with 21.85% reduction in efficiency) than the cell with pure TiO2 compact layer (with 23.28% reduction in efficiency) at higher operating temperatures.

  13. Designing rules and probabilistic weighting for fast materials discovery in the Perovskite structure

    NASA Astrophysics Data System (ADS)

    Castelli, I. E.; Jacobsen, K. W.

    2014-07-01

    High-throughput electronic-structure calculations are becoming increasingly popular in materials science and in the design of new compounds. Electronic-structure theory, for example, in the form of density-functional theory, can be used to calculate stabilities and electronic properties as bandgaps of new compounds. However, in practice, the methods are often limited to rather small atomic-scale systems or periodic crystals with only a limited number of atoms in the unit cell. It is therefore of interest to be able to derive generally useful information from simple systems to be applied in other, more complex, crystals. Here, we consider a large database of calculated stabilities and bandgaps of oxides and oxynitrides in the perovskite structure. We use the database as a testing ground for existing ideas about the behavior of these types of compounds and we derive some new simple chemical-based rules which combine structural information, like the ionic radii of the chemical elements, with electronic data, like the number of electrons and the valences of the pure elements. The rules extracted from the ABO3 cubic perovskite are then tested using the ABO2N and A2BO4 stoichiometry in the cubic and layered perovskite structure, respectively. These rules allow a saving in computer time of around 80%.

  14. Cation Ordering within the Perovskite Block of a Six-layer Ruddlesden-Popper Oxide from Layer-by-layer Growth

    NASA Astrophysics Data System (ADS)

    Yan, Lei; Niu, H. J.; Rosseinsky, M. J.

    2011-03-01

    The (AO)(A BO3)n Ruddlesden-Popper structure is an archetypal complex oxide consisting of two distinct structural units, an (AO) rock salt layer separating an n-octahedra thick perovskite block. Conventional high-temperature oxide synthesis methods cannot access members with n > 3 , butlowtemperaturelayer - by - layerthinfilmmethodsallowthepreparationofmaterialswiththickerperovskiteblocks , exploitinghighsurfacemobilityandlatticematchingwiththesubstrate . Thispresentationdescribesthegrowthofann = 6 memberCaO / (ABO 3)n (ABO 3 : CaMnO 3 , La 0.67 Ca 0.33 MnO 3 orCa 0.85 Sm 0.15 MnO 3) epitaxialsinglecrystalfilmsonthe (001) SrTiO 3 substrates by pulsed laser deposition with the assistance of a reflection high energy electron diffraction (RHEED).

  15. Nanometer-Scale Epitaxial Strain Release in Perovskite Heterostructures Using 'SrAlOx' Sliding Buffer Layers

    SciTech Connect

    Bell, Christopher

    2011-08-11

    We demonstrate the strain release of LaAlO{sub 3} epitaxial film on SrTiO{sub 3} (001) by inserting ultra-thin 'SrAlO{sub x}' buffer layers. Although SrAlO{sub x} is not a perovskite, nor stable as a single phase in bulk, epitaxy stabilizes the perovskite structure up to a thickness of 2 unit cells (uc). At a critical thickness of 3 uc of SrAlO{sub x}, the interlayer acts as a sliding buffer layer, and abruptly relieves the lattice mismatch between the LaAlO{sub 3} filmand the SrTiO{sub 3} substrate, while maintaining crystallinity. This technique may provide a general approach for strain relaxation of perovskite film far below the thermodynamic critical thickness. A central issue in heteroepitaxial filmgrowth is the inevitable difference in lattice constants between the filmand substrate. Due to this lattice mismatch, thin film are subjected to microstructural strain, which can have a significan effect on the filmproperties. This challenge is especially prominent in the rapidly developing fiel of oxide electronics, where much interest is focused on incorporating the emergent physical properties of oxides in devices. Although strain can be used to great effect to engineer unusual ground states, it is often deleterious for bulk first-orde phase transitions, which are suppressed by the strain and symmetry constraints of the substrate. While there are some reports discussing the control of the lattice mismatch in oxides using thick buffer layers, the materials choice, lattice-tunable range, and control of misfit dislocations are still limited. In this Letter, we report the fabrication of strain-relaxed LaAlO{sub 3} (LAO) thin film on SrTiO{sub 3} (STO) (001) using very thin 'SrAlO{sub x}' (SAO) buffer layers. Whereas for 1 or 2 pseudo-perovskite unit cells (uc) of SAO, the subsequent LAO filmis strained to the substrate, at a critical thickness of 3 uc the SAO interlayer abruptly relieves the lattice mismatch between the LAO and the STO, although maintaining the

  16. Photovoltaic switching mechanism in lateral structure hybrid perovskite solar cells

    DOE PAGES

    Yuan, Yongbo; Chae, Jungseok; Shao, Yuchuan; Wang, Qi; Xiao, Zhengguo; Centrone, Andrea; Huang, Jinsong

    2015-06-05

    In this study, long range electromigration of methylammonium ions (MA+) in methyl ammonium lead tri-iodide (MAPbI3) film is observed directly using the photo­thermal induced resonance technique. The electromigration of MA+ leads to the formation of a lateral p-i-n structure, which is the origin of the switchable photovoltaic effect in MAPbI3 perovskite devices.

  17. Photovoltaic switching mechanism in lateral structure hybrid perovskite solar cells

    SciTech Connect

    Yuan, Yongbo; Chae, Jungseok; Shao, Yuchuan; Wang, Qi; Xiao, Zhengguo; Centrone, Andrea; Huang, Jinsong

    2015-06-05

    In this study, long range electromigration of methylammonium ions (MA+) in methyl ammonium lead tri-iodide (MAPbI3) film is observed directly using the photo­thermal induced resonance technique. The electromigration of MA+ leads to the formation of a lateral p-i-n structure, which is the origin of the switchable photovoltaic effect in MAPbI3 perovskite devices.

  18. Transition Metal-Oxide Free Perovskite Solar Cells Enabled by a New Organic Charge Transport Layer.

    PubMed

    Chang, Sehoon; Han, Ggoch Ddeul; Weis, Jonathan G; Park, Hyoungwon; Hentz, Olivia; Zhao, Zhibo; Swager, Timothy M; Gradečak, Silvija

    2016-04-01

    Various electron and hole transport layers have been used to develop high-efficiency perovskite solar cells. To achieve low-temperature solution processing of perovskite solar cells, organic n-type materials are employed to replace the metal oxide electron transport layer (ETL). Although PCBM (phenyl-C61-butyric acid methyl ester) has been widely used for this application, its morphological instability in films (i.e., aggregation) is detrimental. Herein, we demonstrate the synthesis of a new fullerene derivative (isobenzofulvene-C60-epoxide, IBF-Ep) that serves as an electron transporting material for methylammonium mixed lead halide-based perovskite (CH3NH3PbI(3-x)Cl(x)) solar cells, both in the normal and inverted device configurations. We demonstrate that IBF-Ep has superior morphological stability compared to the conventional acceptor, PCBM. IBF-Ep provides higher photovoltaic device performance as compared to PCBM (6.9% vs 2.5% in the normal and 9.0% vs 5.3% in the inverted device configuration). Moreover, IBF-Ep devices show superior tolerance to high humidity (90%) in air. By reaching power conversion efficiencies up to 9.0% for the inverted devices with IBF-Ep as the ETL, we demonstrate the potential of this new material as an alternative to metal oxides for perovskite solar cells processed in air.

  19. Effect of Morphology Control of Light Absorbing Layer on CH3NH3PbI3 Perovskite Solar Cells.

    PubMed

    Lei, Binglong; Eze, Vincent Obiozo; Mori, Tatsuo

    2016-04-01

    As one of the most significant components of perovskite solar cells, the perovskite light absorbing layer demands high quality to guarantee extraordinary power conversion efficiency (PCE). We have fabricated series of CH3NH3PbI3 perovskite solar cells by virtue of gas-flowing assisting (GFA), spin coating twice for the Pbl2 layer and dipping the semi-samples in a thermal CH3NH3I solution, by which some undesirable perovskite morphologies can be effectively avoided. The modified conductions have also dramatically improved the perovskite layer and elevated the coverage ratio from 53.6% to 79.5%. All the fabrication processes, except the steps for deposition of the hole transport material (HTM) and back gold electrode, have been conducted in air and an average PCE of 6.6% has been achieved by initiatively applying N,N'-bis(1-naphtyl)-N,N'-diphenyl-1,1'-biphenyl-4,4'-diamine (α-NPD) doped by MoO3 as HTM. The CH3NH3PbI3 perovskite's morphology and its coverage ratio to the underneath TiO2 mesoporic layer are evaluated to account for the cells' performance. It has demonstrated that higher homogeneity and coverage ratio of the CH3NH3PbI3 layer have most significantly contributed to the solar cells' light conversion efficiency. Keywords: Perovskite, Solar Cell, Morphology, Coverage Ratio, Hole Transport Material. PMID:27451600

  20. The effect of skin-depth interfacial defect layer in perovskite solar cell

    NASA Astrophysics Data System (ADS)

    Gebremichael, Bizuneh; Mola, Genene Tessema

    2016-08-01

    The hole transport buffer layer (HTL) known as PEDOT:PSS is found to be sensitive to polar solvents often used in the preparation of solution-processed perovskite-based solar cell. We employed {CH}3 {NH}3 {PbI}3 perovskite absorber sandwiched between two charge transport layers to analyze the effect of precursor solvent. By introducing skin-depth interfacial defect layer (IDL) on PEDOT:PSS film we studied the overall performance of the devices using one-dimensional device simulator. Both enhanced conductivity and variations in valence band offset (VBO) of IDL were considered to analyze device performance. A power conversion efficiency (PCE) of the devices was found to grow by 35 % due to increased conductivity of IDL by a factor of 1000. Furthermore, we noted a drastic reduction in PCE of the device by reducing the work function of IDL by more than 0.3eV . The thickness of interfacial defect layer was also analyzed and found to decrease the PCE of the devices by 18 % for fourfold increase in IDL thickness. The analysis was remarkably reproduced the experimentally generated device parameters and will help to understand the underlying physical process in perovskite-based solar cell.

  1. Process for forming epitaxial perovskite thin film layers using halide precursors

    DOEpatents

    Clem, Paul G.; Rodriguez, Mark A.; Voigt, James A.; Ashley, Carol S.

    2001-01-01

    A process for forming an epitaxial perovskite-phase thin film on a substrate. This thin film can act as a buffer layer between a Ni substrate and a YBa.sub.2 Cu.sub.3 O.sub.7-x superconductor layer. The process utilizes alkali or alkaline metal acetates dissolved in halogenated organic acid along with titanium isopropoxide to dip or spin-coat the substrate which is then heated to about 700.degree. C. in an inert gas atmosphere to form the epitaxial film on the substrate. The YBCO superconductor can then be deposited on the layer formed by this invention.

  2. Atomic layer deposition of perovskite oxides and their epitaxial integration with Si, Ge, and other semiconductors

    SciTech Connect

    McDaniel, Martin D.; Ngo, Thong Q.; Hu, Shen; Ekerdt, John G.; Posadas, Agham; Demkov, Alexander A.

    2015-12-15

    Atomic layer deposition (ALD) is a proven technique for the conformal deposition of oxide thin films with nanoscale thickness control. Most successful industrial applications have been with binary oxides, such as Al{sub 2}O{sub 3} and HfO{sub 2}. However, there has been much effort to deposit ternary oxides, such as perovskites (ABO{sub 3}), with desirable properties for advanced thin film applications. Distinct challenges are presented by the deposition of multi-component oxides using ALD. This review is intended to highlight the research of the many groups that have deposited perovskite oxides by ALD methods. Several commonalities between the studies are discussed. Special emphasis is put on precursor selection, deposition temperatures, and specific property performance (high-k, ferroelectric, ferromagnetic, etc.). Finally, the monolithic integration of perovskite oxides with semiconductors by ALD is reviewed. High-quality epitaxial growth of oxide thin films has traditionally been limited to physical vapor deposition techniques (e.g., molecular beam epitaxy). However, recent studies have demonstrated that epitaxial oxide thin films may be deposited on semiconductor substrates using ALD. This presents an exciting opportunity to integrate functional perovskite oxides for advanced semiconductor applications in a process that is economical and scalable.

  3. TiO2 Sub-microsphere Film as Scaffold Layer for Efficient Perovskite Solar Cells.

    PubMed

    Huang, Yang; Zhu, Jun; Ding, Yong; Chen, Shuanghong; Zhang, Changneng; Dai, Songyuan

    2016-03-01

    TiO2 sub-microspheres composed of anatase granular-like nanocrystallines with an average diameter ∼250 nm are synthesized using sol-gel method and employed as the scaffold layer for efficient mesocopic perovskite solar cells. Compared with mesoporous TiO2 films composed of ∼18 nm nanoparticles, the sub-microsphere films show superior light-trapping characteristics and significantly improve the light-harvesting capability of the solar cells. In addition, the charge-transport performance is also dramatically improved according to the transient photocurrent decay despite there being no significant difference in the perovskite layer surface morphology. As a result, an average power conversion efficiency of 15% with a highly uniform distribution is achieved for the solar cells with TiO2 sub-microsphere films, 12% higher than those with TiO2 nanoparticle films. The combination of light-harvesting capability and fast charge transfer make the TiO2 sub-microsphere film a good candidate as the scaffold layer for efficient perovskite solar cells. PMID:26953635

  4. TiO2 Sub-microsphere Film as Scaffold Layer for Efficient Perovskite Solar Cells.

    PubMed

    Huang, Yang; Zhu, Jun; Ding, Yong; Chen, Shuanghong; Zhang, Changneng; Dai, Songyuan

    2016-03-01

    TiO2 sub-microspheres composed of anatase granular-like nanocrystallines with an average diameter ∼250 nm are synthesized using sol-gel method and employed as the scaffold layer for efficient mesocopic perovskite solar cells. Compared with mesoporous TiO2 films composed of ∼18 nm nanoparticles, the sub-microsphere films show superior light-trapping characteristics and significantly improve the light-harvesting capability of the solar cells. In addition, the charge-transport performance is also dramatically improved according to the transient photocurrent decay despite there being no significant difference in the perovskite layer surface morphology. As a result, an average power conversion efficiency of 15% with a highly uniform distribution is achieved for the solar cells with TiO2 sub-microsphere films, 12% higher than those with TiO2 nanoparticle films. The combination of light-harvesting capability and fast charge transfer make the TiO2 sub-microsphere film a good candidate as the scaffold layer for efficient perovskite solar cells.

  5. New hexagonal perovskite with Mn4+ and Mn5+ at distinct structural positions

    NASA Astrophysics Data System (ADS)

    Tarakina, N. V.; Tyutyunnik, A. P.; Bazuev, G. V.; Vasiliev, A. D.; Berger, I. F.; Gould, C.; Nikolaenko, I. V.

    2015-10-01

    A new hexagonal perovskite, Ba7Li1.75Mn3.5O15.75, has been synthesised using microwave-assisted solid-state synthesis. Its crystal structure has elements typical for the layered hexagonal perovskites and quasi-one-dimensional oxides, hence representing a new polytype. Structural solution based on simultaneous refinement of X-ray and neutron diffraction data shows that Ba7Li1.75Mn3.5O15.75 crystallizes in a hexagonal unit cell with parameters a = 5.66274(2) Å and c = 16.7467(1) Å (V = 465.063(4) Å3). Columns of face- shared octahedra occupied by Mn4+, Li+ cations and vacancies along the c axis are separated in the ab plane by barium atoms, so that every sixth layer, the coordination of Mn5+ and Li+ changes to tetrahedral. Separation of Mn4+ and Mn5+ cations in two distinct structural positions makes the structure unique. A scanning transmission electron microscopy study revealed the formation of a rhombohedrally centered supercell, which might be attributed to the ordering of manganese and lithium atoms among cationic sites.

  6. Novel Solvent-free Perovskite Deposition in Fabrication of Normal and Inverted Architectures of Perovskite Solar Cells.

    PubMed

    Nejand, Bahram Abdollahi; Gharibzadeh, Saba; Ahmadi, Vahid; Shahverdi, H Reza

    2016-01-01

    We introduced a new approach to deposit perovskite layer with no need for dissolving perovskite precursors. Deposition of Solution-free perovskite (SFP) layer is a key method for deposition of perovskite layer on the hole or electron transport layers that are strongly sensitive to perovskite precursors. Using deposition of SFP layer in the perovskite solar cells would extend possibility of using many electron and hole transport materials in both normal and invert architectures of perovskite solar cells. In the present work, we synthesized crystalline perovskite powder followed by successful deposition on TiO2 and cuprous iodide as the non-sensitve and sensitive charge transport layers to PbI2 and CH3NH3I solution in DMF. The post compressing step enhanced the efficiency of the devices by increasing the interface area between perovskite and charge transport layers. The 9.07% and 7.71% cell efficiencies of the device prepared by SFP layer was achieved in respective normal (using TiO2 as a deposition substrate) and inverted structure (using CuI as deposition substrate) of perovskite solar cell. This method can be efficient in large-scale and low cost fabrication of new generation perovskite solar cells.

  7. Novel Solvent-free Perovskite Deposition in Fabrication of Normal and Inverted Architectures of Perovskite Solar Cells

    PubMed Central

    Nejand, Bahram Abdollahi; Gharibzadeh, Saba; Ahmadi, Vahid; Shahverdi, H. Reza

    2016-01-01

    We introduced a new approach to deposit perovskite layer with no need for dissolving perovskite precursors. Deposition of Solution-free perovskite (SFP) layer is a key method for deposition of perovskite layer on the hole or electron transport layers that are strongly sensitive to perovskite precursors. Using deposition of SFP layer in the perovskite solar cells would extend possibility of using many electron and hole transport materials in both normal and invert architectures of perovskite solar cells. In the present work, we synthesized crystalline perovskite powder followed by successful deposition on TiO2 and cuprous iodide as the non-sensitve and sensitive charge transport layers to PbI2 and CH3NH3I solution in DMF. The post compressing step enhanced the efficiency of the devices by increasing the interface area between perovskite and charge transport layers. The 9.07% and 7.71% cell efficiencies of the device prepared by SFP layer was achieved in respective normal (using TiO2 as a deposition substrate) and inverted structure (using CuI as deposition substrate) of perovskite solar cell. This method can be efficient in large-scale and low cost fabrication of new generation perovskite solar cells. PMID:27640991

  8. Novel Solvent-free Perovskite Deposition in Fabrication of Normal and Inverted Architectures of Perovskite Solar Cells

    NASA Astrophysics Data System (ADS)

    Nejand, Bahram Abdollahi; Gharibzadeh, Saba; Ahmadi, Vahid; Shahverdi, H. Reza

    2016-09-01

    We introduced a new approach to deposit perovskite layer with no need for dissolving perovskite precursors. Deposition of Solution-free perovskite (SFP) layer is a key method for deposition of perovskite layer on the hole or electron transport layers that are strongly sensitive to perovskite precursors. Using deposition of SFP layer in the perovskite solar cells would extend possibility of using many electron and hole transport materials in both normal and invert architectures of perovskite solar cells. In the present work, we synthesized crystalline perovskite powder followed by successful deposition on TiO2 and cuprous iodide as the non-sensitve and sensitive charge transport layers to PbI2 and CH3NH3I solution in DMF. The post compressing step enhanced the efficiency of the devices by increasing the interface area between perovskite and charge transport layers. The 9.07% and 7.71% cell efficiencies of the device prepared by SFP layer was achieved in respective normal (using TiO2 as a deposition substrate) and inverted structure (using CuI as deposition substrate) of perovskite solar cell. This method can be efficient in large-scale and low cost fabrication of new generation perovskite solar cells.

  9. Novel Solvent-free Perovskite Deposition in Fabrication of Normal and Inverted Architectures of Perovskite Solar Cells.

    PubMed

    Nejand, Bahram Abdollahi; Gharibzadeh, Saba; Ahmadi, Vahid; Shahverdi, H Reza

    2016-01-01

    We introduced a new approach to deposit perovskite layer with no need for dissolving perovskite precursors. Deposition of Solution-free perovskite (SFP) layer is a key method for deposition of perovskite layer on the hole or electron transport layers that are strongly sensitive to perovskite precursors. Using deposition of SFP layer in the perovskite solar cells would extend possibility of using many electron and hole transport materials in both normal and invert architectures of perovskite solar cells. In the present work, we synthesized crystalline perovskite powder followed by successful deposition on TiO2 and cuprous iodide as the non-sensitve and sensitive charge transport layers to PbI2 and CH3NH3I solution in DMF. The post compressing step enhanced the efficiency of the devices by increasing the interface area between perovskite and charge transport layers. The 9.07% and 7.71% cell efficiencies of the device prepared by SFP layer was achieved in respective normal (using TiO2 as a deposition substrate) and inverted structure (using CuI as deposition substrate) of perovskite solar cell. This method can be efficient in large-scale and low cost fabrication of new generation perovskite solar cells. PMID:27640991

  10. Lateral-Structure Single-Crystal Hybrid Perovskite Solar Cells via Piezoelectric Poling.

    PubMed

    Dong, Qingfeng; Song, Jingfeng; Fang, Yanjun; Shao, Yuchuan; Ducharme, Stephen; Huang, Jinsong

    2016-04-13

    Single-crystal perovskite solar cells with a lateral structure yield an efficiency enhancement 44-fold that of polycrystalline thin films, due to the much longer carrier diffusion length. A piezoelectric effect observed in perovskite single-crystal and the strain-generated grain-boundaries enable ion migration to form a p-i-n structure. PMID:26836224

  11. Lateral-Structure Single-Crystal Hybrid Perovskite Solar Cells via Piezoelectric Poling.

    PubMed

    Dong, Qingfeng; Song, Jingfeng; Fang, Yanjun; Shao, Yuchuan; Ducharme, Stephen; Huang, Jinsong

    2016-04-13

    Single-crystal perovskite solar cells with a lateral structure yield an efficiency enhancement 44-fold that of polycrystalline thin films, due to the much longer carrier diffusion length. A piezoelectric effect observed in perovskite single-crystal and the strain-generated grain-boundaries enable ion migration to form a p-i-n structure.

  12. Calcium manganate: A promising candidate as buffer layer for hybrid halide perovskite photovoltaic-thermoelectric systems

    SciTech Connect

    Zhao, Pengjun; Wang, Hongguang; Kong, Wenwen; Xu, Jinbao Wang, Lei; Ren, Wei; Bian, Liang; Chang, Aimin

    2014-11-21

    We have systematically studied the feasibility of CaMnO{sub 3} thin film, an n-type perovskite, to be utilized as the buffer layer for hybrid halide perovskite photovoltaic-thermoelectric device. Locations of the conduction band and the valence band, spontaneous polarization performance, and optical properties were investigated. Results indicate the energy band of CaMnO{sub 3} can match up well with that of CH{sub 3}NH{sub 3}PbI{sub 3} on separating electron-hole pairs. In addition, the consistent polarization angle helps enlarge the open circuit voltage of the composite system. Besides, CaMnO{sub 3} film shows large absorption coefficient and low extinction coefficient under visible irradiation, demonstrating high carrier concentration, which is beneficial to the current density. More importantly, benign thermoelectric properties enable CaMnO{sub 3} film to assimilate phonon vibration from CH{sub 3}NH3PbI{sub 3}. All the above features lead to a bright future of CaMnO{sub 3} film, which can be a promising candidate as a buffer layer for hybrid halide perovskite photovoltaic-thermoelectric systems.

  13. Reversible Structural Swell-Shrink and Recoverable Optical Properties in Hybrid Inorganic-Organic Perovskite.

    PubMed

    Zhang, Yupeng; Wang, Yusheng; Xu, Zai-Quan; Liu, Jingying; Song, Jingchao; Xue, Yunzhou; Wang, Ziyu; Zheng, Jialu; Jiang, Liangcong; Zheng, Changxi; Huang, Fuzhi; Sun, Baoquan; Cheng, Yi-Bing; Bao, Qiaoliang

    2016-07-26

    Ion migration in hybrid organic-inorganic perovskites has been suggested to be an important factor for many unusual behaviors in perovskite-based optoelectronics, such as current-voltage hysteresis, low-frequency giant dielectric response, and the switchable photovoltaic effect. However, the role played by ion migration in the photoelectric conversion process of perovskites is still unclear. In this work, we provide microscale insights into the influence of ion migration on the microstructure, stability, and light-matter interaction in perovskite micro/nanowires by using spatially resolved optical characterization techniques. We observed that ion migration, especially the migration of MA(+) ions, will induce a reversible structural swell-shrink in perovskites and recoverably affect the reflective index, quantum efficiency, light-harvesting, and photoelectric properties. The maximum ion migration quantity in perovskites was as high as approximately 30%, resulting in lattice swell or shrink of approximately 4.4%. Meanwhile, the evidence shows that ion migration in perovskites could gradually accelerate the aging of perovskites because of lattice distortion in the reversible structural swell-shrink process. Knowledge regarding reversible structural swell-shrink and recoverable optical properties may shed light on the development of optoelectronic and converse piezoelectric devices based on perovskites.

  14. Reversible Structural Swell-Shrink and Recoverable Optical Properties in Hybrid Inorganic-Organic Perovskite.

    PubMed

    Zhang, Yupeng; Wang, Yusheng; Xu, Zai-Quan; Liu, Jingying; Song, Jingchao; Xue, Yunzhou; Wang, Ziyu; Zheng, Jialu; Jiang, Liangcong; Zheng, Changxi; Huang, Fuzhi; Sun, Baoquan; Cheng, Yi-Bing; Bao, Qiaoliang

    2016-07-26

    Ion migration in hybrid organic-inorganic perovskites has been suggested to be an important factor for many unusual behaviors in perovskite-based optoelectronics, such as current-voltage hysteresis, low-frequency giant dielectric response, and the switchable photovoltaic effect. However, the role played by ion migration in the photoelectric conversion process of perovskites is still unclear. In this work, we provide microscale insights into the influence of ion migration on the microstructure, stability, and light-matter interaction in perovskite micro/nanowires by using spatially resolved optical characterization techniques. We observed that ion migration, especially the migration of MA(+) ions, will induce a reversible structural swell-shrink in perovskites and recoverably affect the reflective index, quantum efficiency, light-harvesting, and photoelectric properties. The maximum ion migration quantity in perovskites was as high as approximately 30%, resulting in lattice swell or shrink of approximately 4.4%. Meanwhile, the evidence shows that ion migration in perovskites could gradually accelerate the aging of perovskites because of lattice distortion in the reversible structural swell-shrink process. Knowledge regarding reversible structural swell-shrink and recoverable optical properties may shed light on the development of optoelectronic and converse piezoelectric devices based on perovskites. PMID:27386731

  15. Structured luminescence conversion layer

    DOEpatents

    Berben, Dirk; Antoniadis, Homer; Jermann, Frank; Krummacher, Benjamin Claus; Von Malm, Norwin; Zachau, Martin

    2012-12-11

    An apparatus device such as a light source is disclosed which has an OLED device and a structured luminescence conversion layer deposited on the substrate or transparent electrode of said OLED device and on the exterior of said OLED device. The structured luminescence conversion layer contains regions such as color-changing and non-color-changing regions with particular shapes arranged in a particular pattern.

  16. Epitaxial 1D electron transport layers for high-performance perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Han, Gill Sang; Chung, Hyun Suk; Kim, Dong Hoe; Kim, Byeong Jo; Lee, Jin-Wook; Park, Nam-Gyu; Cho, In Sun; Lee, Jung-Kun; Lee, Sangwook; Jung, Hyun Suk

    2015-09-01

    We demonstrate high-performance perovskite solar cells with excellent electron transport properties using a one-dimensional (1D) electron transport layer (ETL). The 1D array-based ETL is comprised of 1D SnO2 nanowires (NWs) array grown on a F:SnO2 transparent conducting oxide substrate and rutile TiO2 nanoshells epitaxially grown on the surface of the 1D SnO2 NWs. The optimized devices show more than 95% internal quantum yield at 750 nm, and a power conversion efficiency (PCE) of 14.2%. The high quantum yield is attributed to dramatically enhanced electron transport in the epitaxial TiO2 layer, compared to that in conventional nanoparticle-based mesoporous TiO2 (mp-TiO2) layers. In addition, the open space in the 1D array-based ETL increases the prevalence of uniform TiO2/perovskite junctions, leading to reproducible device performance with a high fill factor. This work offers a method to achieve reproducible, high-efficiency perovskite solar cells with high-speed electron transport.We demonstrate high-performance perovskite solar cells with excellent electron transport properties using a one-dimensional (1D) electron transport layer (ETL). The 1D array-based ETL is comprised of 1D SnO2 nanowires (NWs) array grown on a F:SnO2 transparent conducting oxide substrate and rutile TiO2 nanoshells epitaxially grown on the surface of the 1D SnO2 NWs. The optimized devices show more than 95% internal quantum yield at 750 nm, and a power conversion efficiency (PCE) of 14.2%. The high quantum yield is attributed to dramatically enhanced electron transport in the epitaxial TiO2 layer, compared to that in conventional nanoparticle-based mesoporous TiO2 (mp-TiO2) layers. In addition, the open space in the 1D array-based ETL increases the prevalence of uniform TiO2/perovskite junctions, leading to reproducible device performance with a high fill factor. This work offers a method to achieve reproducible, high-efficiency perovskite solar cells with high-speed electron transport

  17. Electro- and photoluminescence imaging as fast screening technique of the layer uniformity and device degradation in planar perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Soufiani, Arman Mahboubi; Tayebjee, Murad J. Y.; Meyer, Steffen; Ho-Baillie, Anita; Sung Yun, Jae; MacQueen, Rowan W.; Spiccia, Leone; Green, Martin A.; Hameiri, Ziv

    2016-07-01

    In this study, we provide insights into planar structure methylammonium lead triiodide (MAPbI3) perovskite solar cells (PSCs) using electroluminescence and photoluminescence imaging techniques. We demonstrate the strength of these techniques in screening relatively large area PSCs, correlating the solar cell electrical parameters to the images and visualizing the features which contribute to the variation of the parameters extracted from current density-voltage characterizations. It is further used to investigate one of the major concerns about perovskite solar cells, their long term stability and aging. Upon storage under dark in dry glovebox condition for more than two months, the major parameter found to have deteriorated in electrical performance measurements was the fill factor; this was elucidated via electroluminescence image comparisons which revealed that the contacts' quality degrades. Interestingly, by deploying electroluminescence imaging, the significance of having a pin-hole free active layer is demonstrated. Pin-holes can grow over time and can cause degradation of the active layer surrounding them.

  18. Metal halide perovskite light emitters

    PubMed Central

    Kim, Young-Hoon; Cho, Himchan; Lee, Tae-Woo

    2016-01-01

    Twenty years after layer-type metal halide perovskites were successfully developed, 3D metal halide perovskites (shortly, perovskites) were recently rediscovered and are attracting multidisciplinary interest from physicists, chemists, and material engineers. Perovskites have a crystal structure composed of five atoms per unit cell (ABX3) with cation A positioned at a corner, metal cation B at the center, and halide anion X at the center of six planes and unique optoelectronic properties determined by the crystal structure. Because of very narrow spectra (full width at half-maximum ≤20 nm), which are insensitive to the crystallite/grain/particle dimension and wide wavelength range (400 nm ≤ λ ≤ 780 nm), perovskites are expected to be promising high-color purity light emitters that overcome inherent problems of conventional organic and inorganic quantum dot emitters. Within the last 2 y, perovskites have already demonstrated their great potential in light-emitting diodes by showing high electroluminescence efficiency comparable to those of organic and quantum dot light-emitting diodes. This article reviews the progress of perovskite emitters in two directions of bulk perovskite polycrystalline films and perovskite nanoparticles, describes current challenges, and suggests future research directions for researchers to encourage them to collaborate and to make a synergetic effect in this rapidly emerging multidisciplinary field. PMID:27679844

  19. Perovskite solar cell using a two-dimensional titania nanosheet thin film as the compact layer.

    PubMed

    Li, Can; Li, Yahui; Xing, Yujin; Zhang, Zelin; Zhang, Xianfeng; Li, Zhen; Shi, Yantao; Ma, Tingli; Ma, Renzhi; Wang, Kunlin; Wei, Jinquan

    2015-07-22

    The compact layer plays an important role in conducting electrons and blocking holes in perovskite solar cells (PSCs). Here, we use a two-dimensional titania nanosheet (TNS) thin film as the compact layer in CH3NH3PbI3 PSCs. TNS thin films with thicknesses ranging from 8 to 75 nm were prepared by an electrophoretic deposition method from a dilute TNS/tetrabutylammonium hydroxide solution. The TNS thin films contact the fluorine-doped tin oxide grains perfectly. Our results show that a 8-nm-thick TNS film is sufficient for acting as the compact layer. Currently, the PSC with a TNS compact layer has a high efficiency of 10.7% and relatively low hysteresis behavior. PMID:26158908

  20. Synthesis, crystal structure, and properties of a perovskite-related bismuth phase, (NH4)3Bi2I9

    NASA Astrophysics Data System (ADS)

    Sun, Shijing; Tominaka, Satoshi; Lee, Jung-Hoon; Xie, Fei; Bristowe, Paul D.; Cheetham, Anthony K.

    2016-03-01

    Organic-inorganic halide perovskites, especially methylammonium lead halide, have recently led to remarkable advances in photovoltaic devices. However, due to environmental and stability concerns around the use of lead, research into lead-free perovskite structures has been attracting increasing attention. In this study, a layered perovskite-like architecture, (NH4)3Bi2I9, is prepared from solution and the structure solved by single crystal X-ray diffraction. The band gap, which is estimated to be 2.04 eV using UV-visible spectroscopy, is lower than that of CH3NH3PbBr3. The energy-minimized structure obtained from first principles calculations is in excellent agreement with the X-ray results and establishes the locations of the hydrogen atoms. The calculations also point to a significant lone pair effect on the bismuth ion. Single crystal and powder conductivity measurements are performed to examine the potential application of (NH4)3Bi2I9 as an alternative to the lead containing perovskites.

  1. A composite light-harvesting layer from photoactive polymer and halide perovskite for planar heterojunction solar cells.

    PubMed

    Wang, Heming; Rahaq, Yaqub; Kumar, Vikas

    2016-01-01

    A new route for fabrication of photoactive materials in organic-inorganic hybrid solar cells is presented in this report. Photoactive materials by blending a semiconductive conjugated polymer with an organolead halide perovskite were fabricated for the first time. The composite active layer was then used to make planar heterojunction solar cells with the PCBM film as the electron-acceptor. Photovoltaic performance of solar cells was investigated by J-V curves and external quantum efficiency spectra. We demonstrated that the incorporation of the conjugated photoactive polymer into organolead halide perovskites did not only contribute to the generation of charges, but also enhance stability of solar cells by providing a barrier protection to halide perovskites. It is expected that versatile of conjugated semi-conductive polymers and halide perovskites in photoactive properties enables to create various combinations, forming composites with advantages offered by both types of photoactive materials. PMID:27411487

  2. A composite light-harvesting layer from photoactive polymer and halide perovskite for planar heterojunction solar cells

    NASA Astrophysics Data System (ADS)

    Wang, Heming; Rahaq, Yaqub; Kumar, Vikas

    2016-07-01

    A new route for fabrication of photoactive materials in organic-inorganic hybrid solar cells is presented in this report. Photoactive materials by blending a semiconductive conjugated polymer with an organolead halide perovskite were fabricated for the first time. The composite active layer was then used to make planar heterojunction solar cells with the PCBM film as the electron-acceptor. Photovoltaic performance of solar cells was investigated by J-V curves and external quantum efficiency spectra. We demonstrated that the incorporation of the conjugated photoactive polymer into organolead halide perovskites did not only contribute to the generation of charges, but also enhance stability of solar cells by providing a barrier protection to halide perovskites. It is expected that versatile of conjugated semi-conductive polymers and halide perovskites in photoactive properties enables to create various combinations, forming composites with advantages offered by both types of photoactive materials.

  3. A composite light-harvesting layer from photoactive polymer and halide perovskite for planar heterojunction solar cells

    PubMed Central

    Wang, Heming; Rahaq, Yaqub; Kumar, Vikas

    2016-01-01

    A new route for fabrication of photoactive materials in organic-inorganic hybrid solar cells is presented in this report. Photoactive materials by blending a semiconductive conjugated polymer with an organolead halide perovskite were fabricated for the first time. The composite active layer was then used to make planar heterojunction solar cells with the PCBM film as the electron-acceptor. Photovoltaic performance of solar cells was investigated by J-V curves and external quantum efficiency spectra. We demonstrated that the incorporation of the conjugated photoactive polymer into organolead halide perovskites did not only contribute to the generation of charges, but also enhance stability of solar cells by providing a barrier protection to halide perovskites. It is expected that versatile of conjugated semi-conductive polymers and halide perovskites in photoactive properties enables to create various combinations, forming composites with advantages offered by both types of photoactive materials. PMID:27411487

  4. A composite light-harvesting layer from photoactive polymer and halide perovskite for planar heterojunction solar cells.

    PubMed

    Wang, Heming; Rahaq, Yaqub; Kumar, Vikas

    2016-01-01

    A new route for fabrication of photoactive materials in organic-inorganic hybrid solar cells is presented in this report. Photoactive materials by blending a semiconductive conjugated polymer with an organolead halide perovskite were fabricated for the first time. The composite active layer was then used to make planar heterojunction solar cells with the PCBM film as the electron-acceptor. Photovoltaic performance of solar cells was investigated by J-V curves and external quantum efficiency spectra. We demonstrated that the incorporation of the conjugated photoactive polymer into organolead halide perovskites did not only contribute to the generation of charges, but also enhance stability of solar cells by providing a barrier protection to halide perovskites. It is expected that versatile of conjugated semi-conductive polymers and halide perovskites in photoactive properties enables to create various combinations, forming composites with advantages offered by both types of photoactive materials.

  5. Amorphous TiO2 Compact Layers via ALD for Planar Halide Perovskite Photovoltaics.

    PubMed

    Kim, In Soo; Haasch, Richard T; Cao, Duyen H; Farha, Omar K; Hupp, Joseph T; Kanatzidis, Mercouri G; Martinson, Alex B F

    2016-09-21

    A low-temperature (<120 °C) route to pinhole-free amorphous TiO2 compact layers may pave the way to more efficient, flexible, and stable inverted perovskite halide device designs. Toward this end, we utilize low-temperature thermal atomic layer deposition (ALD) to synthesize ultrathin (12 nm) compact TiO2 underlayers for planar halide perovskite PV. Although device performance with as-deposited TiO2 films is poor, we identify room-temperature UV-O3 treatment as a route to device efficiency comparable to crystalline TiO2 thin films synthesized by higher temperature methods. We further explore the chemical, physical, and interfacial properties that might explain the improved performance through X-ray diffraction, spectroscopic ellipsometry, Raman spectroscopy, and X-ray photoelectron spectroscopy. These findings challenge our intuition about effective electron selective layers as well as point the way to a greater selection of flexible substrates and more stable inverted device designs. PMID:27598453

  6. Amorphous TiO2 Compact Layers via ALD for Planar Halide Perovskite Photovoltaics.

    PubMed

    Kim, In Soo; Haasch, Richard T; Cao, Duyen H; Farha, Omar K; Hupp, Joseph T; Kanatzidis, Mercouri G; Martinson, Alex B F

    2016-09-21

    A low-temperature (<120 °C) route to pinhole-free amorphous TiO2 compact layers may pave the way to more efficient, flexible, and stable inverted perovskite halide device designs. Toward this end, we utilize low-temperature thermal atomic layer deposition (ALD) to synthesize ultrathin (12 nm) compact TiO2 underlayers for planar halide perovskite PV. Although device performance with as-deposited TiO2 films is poor, we identify room-temperature UV-O3 treatment as a route to device efficiency comparable to crystalline TiO2 thin films synthesized by higher temperature methods. We further explore the chemical, physical, and interfacial properties that might explain the improved performance through X-ray diffraction, spectroscopic ellipsometry, Raman spectroscopy, and X-ray photoelectron spectroscopy. These findings challenge our intuition about effective electron selective layers as well as point the way to a greater selection of flexible substrates and more stable inverted device designs.

  7. Perovskite Solar Cells: Moth-Eye TiO2 Layer for Improving Light Harvesting Efficiency in Perovskite Solar Cells (Small 18/2016).

    PubMed

    Kang, Seong Min; Jang, Segeun; Lee, Jong-Kwon; Yoon, Jungjin; Yoo, Dong-Eun; Lee, Jin-Wook; Choi, Mansoo; Park, Nam-Gyu

    2016-05-01

    A moth-eye patterned mesoporous (mp) TiO2 layer is fabricated in the form of submicron scale by using lithography, nano-imprinting and polydimethyl siloxane (PDMS) stamping methods. On page 2443, M. Choi, N.-G. Park, and co-workers demonstrate an excellent light harvesting property of perovskite solar cell by employing the moth-eye nanostructured mp-TiO2 film. These novel fabrication methods are expected to be optically beneficial to opto-electronic devices.

  8. Improving the performance of perovskite solar cells with glycerol-doped PEDOT:PSS buffer layer

    NASA Astrophysics Data System (ADS)

    Jian-Feng, Li; Chuang, Zhao; Heng, Zhang; Jun-Feng, Tong; Peng, Zhang; Chun-Yan, Yang; Yang-Jun, Xia; Duo-Wang, Fan

    2016-02-01

    In this paper, we investigate the effects of glycerol doping on transmittance, conductivity and surface morphology of poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate)) (PEDOT:PSS) and its influence on the performance of perovskite solar cells. . The conductivity of PEDOT:PSS is improved obviously by doping glycerol. The maximum of the conductivity is 0.89 S/cm when the doping concentration reaches 6 wt%, which increases about 127 times compared with undoped. The perovskite solar cells are fabricated with a configuration of indium tin oxide (ITO)/PEDOT:PSS/CH3NH3PbI3/PC61BM/Al, where PEDOT:PSS and PC61BM are used as hole and electron transport layers, respectively. The results show an improvement of hole charge transport as well as an increase of short-circuit current density and a reduction of series resistance, owing to the higher conductivity of the doped PEDOT:PSS. Consequently, it improves the whole performance of perovskite solar cell. The power conversion efficiency (PCE) of the device is improved from 8.57% to 11.03% under AM 1.5 G (100 mW/cm2 illumination) after the buffer layer has been modified. Project supported by the National Natural Science Foundation of China (Grant Nos. 61264002, 61166002, 91333206, and 51463011), the Natural Science Foundation of Gansu Province, China (Grant No. 1308RJZA159), the New Century Excellent Talents in University of Ministry of Education of China (Grant No. NCET-13-0840), the Research Project of Graduate Teacher of Gansu Province, China (Grant No. 2014A-0042), and the Postdoctoral Science Foundation from Lanzhou Jiaotong University, China.

  9. Properties of Ferroelectric Perovskite Structures under Non-equilibrium Conditions

    NASA Astrophysics Data System (ADS)

    Zhang, Qingteng

    Ferroelectric materials have received lots of attention thanks to their intriguing properties such as the piezoelectric and pyroelectric effects, as well as the large dielectric constants and the spontaneous polarization which can potentially be used for information storage. In particular, perovskite crystal has a very simple unit cell structure yet a very rich phase transition diagram, which makes it one of the most intensively studied ferroelectric materials. In this dissertation, we use effective Hamiltonian, a first-principles-based computational technique to study the finite-temperature properties of ferroelectric perovskites. We studied temperature-graded (BaxSr 1-x)TiO3 (BST) bulk alloys as well as the dynamics of nanodomain walls (nanowalls) in Pb(Zr xTi1-x)O 3 (PZT) ultra-thin films under the driving force of an AC field. Our computations suggest that, for the temperature-graded BST, the polarization responds to the temperature gradient (TG), with the "up" and "down" offset observed in polarization components along the direction of TG, in agreement with the findings from experiments. For the nanowalls in PZT, the dynamics can be described by the damped-harmonic-oscillator model, and we observed a size-driven transition from resonance to relaxational dynamics at a critical thickness of 7.2 nm. The transition originates from the change in the effective mass of a nanowall as a film thickness increases. Some of the findings may find potential applications in various devices, such as thermal sensors, energy converters, or novel memory units.

  10. Fabrication of (110)-one-axis-oriented perovskite-type oxide thin films and their application to buffer layer

    NASA Astrophysics Data System (ADS)

    Sato, Tomoya; Ichinose, Daichi; Kimura, Junichi; Inoue, Takaaki; Mimura, Takanori; Funakubo, Hiroshi; Uchiyama, Kiyoshi

    2016-10-01

    BaCe0.9Y0.1O3-δ (BCYO) and SrZr0.8Y0.2O3-δ (SZYO) thin films of perovskite-type oxides were deposited on (111)Pt/TiO x /SiO2/(100)Si substrates. X-ray diffraction patterns showed that the (110)-oriented BCYO and SZYO thin films were grown on (111)Pt/Si substrates directly without using any buffer layers. Thin films of SrRuO3 (SRO), a conductive perovskite-type oxide, were also deposited on those films and highly (110)-oriented SRO thin films were obtained. We believe that this (110)-oriented SRO works as a buffer layer to deposit (110)-oriented perovskite-type ferroelectric oxide thin films as well as a bottom electrode and can modify the ferroelectric properties of the oxide thin films by controlling their crystallographic orientations.

  11. Doped hole transport layer for efficiency enhancement in planar heterojunction organolead trihalide perovskite solar cells

    SciTech Connect

    Wang, Qi; Bi, Cheng; Huang, Jinsong

    2015-05-06

    We demonstrated the efficiency of a solution-processed planar heterojunction organometallic trihalide perovskite solar cell can be increased to 17.5% through doping the hole transporting layer for reducing the resistivity. Doped Poly(triaryl amine) (PTAA) by 2,3,5,6-Tetrafluoro-7,7,8,8-Tetracyanoquinodimethane (F4-TCNQ) reduced device series resistance by three-folds, increasing the device fill factor to 74%, open circuit voltage to 1.09 V without sacrificing the short circuit current. As a result, this study reveals that the high resistivity of currently broadly applied polymer hole transport layer limits the device efficiency, and points a new direction to improve the device efficiency.

  12. Structure and Growth Control of Organic–Inorganic Halide Perovskites for Optoelectronics: From Polycrystalline Films to Single Crystals

    PubMed Central

    Chen, Yani; He, Minhong; Peng, Jiajun; Sun, Yong

    2016-01-01

    Recently, organic–inorganic halide perovskites have sparked tremendous research interest because of their ground‐breaking photovoltaic performance. The crystallization process and crystal shape of perovskites have striking impacts on their optoelectronic properties. Polycrystalline films and single crystals are two main forms of perovskites. Currently, perovskite thin films have been under intensive investigation while studies of perovskite single crystals are just in their infancy. This review article is concentrated upon the control of perovskite structures and growth, which are intimately correlated for improvements of not only solar cells but also light‐emitting diodes, lasers, and photodetectors. We begin with the survey of the film formation process of perovskites including deposition methods and morphological optimization avenues. Strategies such as the use of additives, thermal annealing, solvent annealing, atmospheric control, and solvent engineering have been successfully employed to yield high‐quality perovskite films. Next, we turn to summarize the shape evolution of perovskites single crystals from three‐dimensional large sized single crystals, two‐dimensional nanoplates, one‐dimensional nanowires, to zero‐dimensional quantum dots. Siginificant functions of perovskites single crystals are highlighted, which benefit fundamental studies of intrinsic photophysics. Then, the growth mechanisms of the previously mentioned perovskite crystals are unveiled. Lastly, perspectives for structure and growth control of perovskites are outlined towards high‐performance (opto)electronic devices. PMID:27812463

  13. Structure of 18R shifted hexagonal perovskite La{sub 6}MgTi{sub 4}O{sub 18} revisited by neutron diffraction

    SciTech Connect

    Lu, Fengqi; Kuang, Xiaojun

    2015-01-15

    The structure of 18-layer shifted B-site deficient hexagonal perovskite La{sub 6}MgTi{sub 4}O{sub 18} compound has been re-examined by neutron powder diffraction. Structural analysis reveals that La{sub 6}MgTi{sub 4}O{sub 18} compound adopts a 18R octahedral-tilted structure with LaO{sub 3} layer stacking sequence of (hhcccc){sub 3} in space group R{sup {sup -}}3, in contrast with the previously proposed R3m. La{sub 6}MgTi{sub 4}O{sub 18} demonstrates partially ordered Mg cation distribution with a preference on the central octahedral sites over the outer octahedral sites in the cubic perovskite blocks isolated by the single vacant octahedral layers between the two consecutive hexagonal layers. The instability of the La{sub 6}MgTi{sub 4}O{sub 18} on alumina ceramic substrate at high temperature and its dependencies of cell parameters and permittivity were characterized as well. - Graphical abstract: 18-layer shifted hexagonal perovskite La{sub 6}MgTi{sub 4}O{sub 18} adopts octahedral-tilted structure in R{sup {sup -}}3 and demonstrates partially ordered Mg distribution in the cubic perovskite blocks isolated by the vacant octahedral layers. - Highlights: • Neutron diffraction reveals an octahedra-tilted structure in R{sup {sup -}}3 for La{sub 6}MgTi{sub 4}O{sub 18}. • Mg/Ti distribution in La{sub 6}MgTi{sub 4}O{sub 18} is partially ordered in the perovskite blocks. • Instability of La{sub 6}MgTi{sub 4}O{sub 18} on alumina ceramic at high temperature is demonstrated.

  14. Well-Defined Nanostructured, Single-Crystalline TiO2 Electron Transport Layer for Efficient Planar Perovskite Solar Cells.

    PubMed

    Choi, Jongmin; Song, Seulki; Hörantner, Maximilian T; Snaith, Henry J; Park, Taiho

    2016-06-28

    An electron transporting layer (ETL) plays an important role in extracting electrons from a perovskite layer and blocking recombination between electrons in the fluorine-doped tin oxide (FTO) and holes in the perovskite layers, especially in planar perovskite solar cells. Dense TiO2 ETLs prepared by a solution-processed spin-coating method (S-TiO2) are mainly used in devices due to their ease of fabrication. Herein, we found that fatal morphological defects at the S-TiO2 interface due to a rough FTO surface, including an irregular film thickness, discontinuous areas, and poor physical contact between the S-TiO2 and the FTO layers, were inevitable and lowered the charge transport properties through the planar perovskite solar cells. The effects of the morphological defects were mitigated in this work using a TiO2 ETL produced from sputtering and anodization. This method produced a well-defined nanostructured TiO2 ETL with an excellent transmittance, single-crystalline properties, a uniform film thickness, a large effective area, and defect-free physical contact with a rough substrate that provided outstanding electron extraction and hole blocking in a planar perovskite solar cell. In planar perovskite devices, anodized TiO2 ETL (A-TiO2) increased the power conversion efficiency by 22% (from 12.5 to 15.2%), and the stabilized maximum power output efficiency increased by 44% (from 8.9 to 12.8%) compared with S-TiO2. This work highlights the importance of the ETL geometry for maximizing device performance and provides insights into achieving ideal ETL morphologies that remedy the drawbacks observed in conventional spin-coated ETLs.

  15. Highly stable, luminescent core-shell type methylammonium-octylammonium lead bromide layered perovskite nanoparticles.

    PubMed

    Bhaumik, Saikat; Veldhuis, Sjoerd A; Ng, Yan Fong; Li, Mingjie; Muduli, Subas Kumar; Sum, Tze Chien; Damodaran, Bahulayan; Mhaisalkar, Subodh; Mathews, Nripan

    2016-06-01

    A new protocol for the synthesis of a highly stable (over 2 months under ambient conditions) solution-processed core-shell type structure of mixed methylammonium-octylammonium lead bromide perovskite nanoparticles (5-12 nm), having spherical shape, color tunability in the blue to green spectral region (438-521 nm) and a high photoluminescence quantum yield (PLQY) of up to 92% is described. The color tunability, high PLQY and stability are due to the quantum confinement imparted by the crystal engineering associated with core-shell nanoparticle formation during growth. PMID:27165565

  16. Significant enhancement of photovoltage in artificially designed perovskite oxide structures

    NASA Astrophysics Data System (ADS)

    Zhou, Wen-jia; Jin, Kui-juan; Guo, Hai-zhong; He, Xu; He, Meng; Xu, Xiu-lai; Lu, Hui-bin; Yang, Guo-zhen

    2015-03-01

    La0.9Sr0.1MnO3/insulator/SrNb0.007Ti0.993O3 multilayer and La0.9Sr0.1MnO3/SrNb0.007Ti0.993O3/In2O3:SnO2(ITO)/La0.9Sr0.1MnO3/SrNb0.007Ti0.993O3 multilayer structures were designed to enhance the photovoltage. The photovoltages of these two structures under an illumination of 308 nm laser are 410 and 600 mV, respectively. The latter is 20 times larger than that (30 mV) observed in La0.9Sr0.1MnO3/SrNb0.007Ti0.993O3 single junction. The origin of such significant enhancement of photovoltage is discussed in this letter. These results suggest that the photoelectric property of perovskite oxides could be much improved by artificial structure designing. The enhanced photovoltaic effects have potential applications in the ultraviolet photodetection and solar cells.

  17. Atomic force microscopy surface analysis of layered perovskite La2Ti2O7 particles grown by molten flux method

    NASA Astrophysics Data System (ADS)

    Orum, Aslihan; Takatori, Kazumasa; Hori, Shigeo; Ikeda, Tomiko; Yoshimura, Masamichi; Tani, Toshihiko

    2016-08-01

    Rectangular platelike particles of La2Ti2O7, a layered perovskite, were synthesized in KCl, NaCl, and LiCl by the molten flux method. The formation mechanism of the equilibrium shape in these alkali chloride fluxes was discussed in terms of the surface and interfacial energies of crystallographic planes. The atomic force microscopy (AFM) observations revealed that the developed plane of the platelike particles is along the interlayers in the {110}-type layered crystal structure, and is considered to represent the lowest surface energy plane in which strong, periodic Ti–O bond chains terminate. Herein, for the first time, a growth mechanism for La2Ti2O7 particles is proposed and discussed. Triangular prism structures along the c-axis were observed on the developed planes of KCl-grown particles whereas no such structures were found on those of LiCl-grown ones. AFM measurements suggest that the prism facets are {210}-La2Ti2O7, which results in lower interfacial energy within KCl.

  18. Atomic force microscopy surface analysis of layered perovskite La2Ti2O7 particles grown by molten flux method

    NASA Astrophysics Data System (ADS)

    Orum, Aslihan; Takatori, Kazumasa; Hori, Shigeo; Ikeda, Tomiko; Yoshimura, Masamichi; Tani, Toshihiko

    2016-08-01

    Rectangular platelike particles of La2Ti2O7, a layered perovskite, were synthesized in KCl, NaCl, and LiCl by the molten flux method. The formation mechanism of the equilibrium shape in these alkali chloride fluxes was discussed in terms of the surface and interfacial energies of crystallographic planes. The atomic force microscopy (AFM) observations revealed that the developed plane of the platelike particles is along the interlayers in the {110}-type layered crystal structure, and is considered to represent the lowest surface energy plane in which strong, periodic Ti-O bond chains terminate. Herein, for the first time, a growth mechanism for La2Ti2O7 particles is proposed and discussed. Triangular prism structures along the c-axis were observed on the developed planes of KCl-grown particles whereas no such structures were found on those of LiCl-grown ones. AFM measurements suggest that the prism facets are {210}-La2Ti2O7, which results in lower interfacial energy within KCl.

  19. A High-Performing Sulfur-Tolerant and Redox-Stable Layered Perovskite Anode for Direct Hydrocarbon Solid Oxide Fuel Cells.

    PubMed

    Ding, Hanping; Tao, Zetian; Liu, Shun; Zhang, Jiujun

    2015-12-09

    Development of alternative ceramic oxide anode materials is a key step for direct hydrocarbon solid oxide fuel cells (SOFCs). Several lanthanide based layered perovskite-structured oxides demonstrate outstanding oxygen diffusion rate, favorable electronic conductivity, and good oxygen surface exchange kinetics, owing to A-site ordered structure in which lanthanide and alkali-earth ions occupy alternate (001) layers and oxygen vacancies are mainly located in [LnOx] planes. Here we report a nickel-free cation deficient layered perovskite, (PrBa)0.95(Fe0.9Mo0.1)2O5 + δ (PBFM), for SOFC anode, and this anode shows an outstanding performance with high resistance against both carbon build-up and sulfur poisoning in hydrocarbon fuels. At 800 °C, the layered PBFM showed high electrical conductivity of 59.2 S cm(-1) in 5% H2 and peak power densities of 1.72 and 0.54 W cm(-2) using H2 and CH4 as fuel, respectively. The cell exhibits a very stable performance under a constant current load of 1.0 A cm(-2). To our best knowledge, this is the highest performance of ceramic anodes operated in methane. In addition, the anode is structurally stable at various fuel and temperature conditions, suggesting that it is a feasible material candidate for high-performing SOFC anode.

  20. A High-Performing Sulfur-Tolerant and Redox-Stable Layered Perovskite Anode for Direct Hydrocarbon Solid Oxide Fuel Cells

    PubMed Central

    Ding, Hanping; Tao, Zetian; Liu, Shun; Zhang, Jiujun

    2015-01-01

    Development of alternative ceramic oxide anode materials is a key step for direct hydrocarbon solid oxide fuel cells (SOFCs). Several lanthanide based layered perovskite-structured oxides demonstrate outstanding oxygen diffusion rate, favorable electronic conductivity, and good oxygen surface exchange kinetics, owing to A-site ordered structure in which lanthanide and alkali-earth ions occupy alternate (001) layers and oxygen vacancies are mainly located in [LnOx] planes. Here we report a nickel-free cation deficient layered perovskite, (PrBa)0.95(Fe0.9Mo0.1)2O5 + δ (PBFM), for SOFC anode, and this anode shows an outstanding performance with high resistance against both carbon build-up and sulfur poisoning in hydrocarbon fuels. At 800 °C, the layered PBFM showed high electrical conductivity of 59.2 S cm−1 in 5% H2 and peak power densities of 1.72 and 0.54 W cm−2 using H2 and CH4 as fuel, respectively. The cell exhibits a very stable performance under a constant current load of 1.0 A cm−2. To our best knowledge, this is the highest performance of ceramic anodes operated in methane. In addition, the anode is structurally stable at various fuel and temperature conditions, suggesting that it is a feasible material candidate for high-performing SOFC anode. PMID:26648509

  1. A High-Performing Sulfur-Tolerant and Redox-Stable Layered Perovskite Anode for Direct Hydrocarbon Solid Oxide Fuel Cells.

    PubMed

    Ding, Hanping; Tao, Zetian; Liu, Shun; Zhang, Jiujun

    2015-01-01

    Development of alternative ceramic oxide anode materials is a key step for direct hydrocarbon solid oxide fuel cells (SOFCs). Several lanthanide based layered perovskite-structured oxides demonstrate outstanding oxygen diffusion rate, favorable electronic conductivity, and good oxygen surface exchange kinetics, owing to A-site ordered structure in which lanthanide and alkali-earth ions occupy alternate (001) layers and oxygen vacancies are mainly located in [LnOx] planes. Here we report a nickel-free cation deficient layered perovskite, (PrBa)0.95(Fe0.9Mo0.1)2O5 + δ (PBFM), for SOFC anode, and this anode shows an outstanding performance with high resistance against both carbon build-up and sulfur poisoning in hydrocarbon fuels. At 800 °C, the layered PBFM showed high electrical conductivity of 59.2 S cm(-1) in 5% H2 and peak power densities of 1.72 and 0.54 W cm(-2) using H2 and CH4 as fuel, respectively. The cell exhibits a very stable performance under a constant current load of 1.0 A cm(-2). To our best knowledge, this is the highest performance of ceramic anodes operated in methane. In addition, the anode is structurally stable at various fuel and temperature conditions, suggesting that it is a feasible material candidate for high-performing SOFC anode. PMID:26648509

  2. A High-Performing Sulfur-Tolerant and Redox-Stable Layered Perovskite Anode for Direct Hydrocarbon Solid Oxide Fuel Cells

    NASA Astrophysics Data System (ADS)

    Ding, Hanping; Tao, Zetian; Liu, Shun; Zhang, Jiujun

    2015-12-01

    Development of alternative ceramic oxide anode materials is a key step for direct hydrocarbon solid oxide fuel cells (SOFCs). Several lanthanide based layered perovskite-structured oxides demonstrate outstanding oxygen diffusion rate, favorable electronic conductivity, and good oxygen surface exchange kinetics, owing to A-site ordered structure in which lanthanide and alkali-earth ions occupy alternate (001) layers and oxygen vacancies are mainly located in [LnOx] planes. Here we report a nickel-free cation deficient layered perovskite, (PrBa)0.95(Fe0.9Mo0.1)2O5 + δ (PBFM), for SOFC anode, and this anode shows an outstanding performance with high resistance against both carbon build-up and sulfur poisoning in hydrocarbon fuels. At 800 °C, the layered PBFM showed high electrical conductivity of 59.2 S cm-1 in 5% H2 and peak power densities of 1.72 and 0.54 W cm-2 using H2 and CH4 as fuel, respectively. The cell exhibits a very stable performance under a constant current load of 1.0 A cm-2. To our best knowledge, this is the highest performance of ceramic anodes operated in methane. In addition, the anode is structurally stable at various fuel and temperature conditions, suggesting that it is a feasible material candidate for high-performing SOFC anode.

  3. K 1- xLa xCa 2- xNb 3O 10, a Layered Perovskite Series with Variable Interlayer Cation Density, and LaCaNb 3O 10, a Novel Layered Perovskite Oxide with No Interlayer Cations

    NASA Astrophysics Data System (ADS)

    Uma, S.; Gopalakrishnan, J.

    1993-02-01

    A series of layered perovskite oxides of the formula K1-xLaxCa2-xNb3O10 for 0 < x ≤ 1.0 have been prepared. All the members are isostructural, possessing the structure of KCa2Nb3O10. The interlayer potassium ions in the new series can be ion-exchanged with protons to give H1-xLaxCa2-xNb3O10. The latter readily forms intercalation compounds of the formula (CnH2n+1NH3)1-x LaxCa2-xNb3O10, just as the parent solid acid HCa2Nb3O10. The end member LaCaNb3O10 containing no interlayer cations is a novel layered perovskite oxide, being a n = 3 member of the series An-1BnX3n+1.

  4. Coordination Chemistry Dictates the Structural Defects in Lead Halide Perovskites.

    PubMed

    Rahimnejad, Sara; Kovalenko, Alexander; Forés, Sergio Martí; Aranda, Clara; Guerrero, Antonio

    2016-09-19

    We show the influence of species present in precursor solution during formation of lead halide perovskite materials on the structural defects of the films. The coordination of lead by competing solvent molecules and iodide ions dictate the type of complexes present in the films. Depending on the processing conditions all PbIS5 (+) , PbI2 S4, PbI3 S3 (-) , PbI4 S2 (2-) , PbI5 S2 (3-) , PbI6 (4-) and 1D (Pb2 I4 )n chains are observed by absorption measurements. Different parameters are studied such as polarity of the solvent, concentration of iodide ions, concentration of solvent molecules and temperature. It is concluded that strongly coordinating solvents will preferentially form species with a low number of iodide ions and less coordinative solvents generate high concentration of PbI6 (-) . We furthermore propose that all these plumbate ions may act as structural defects determining electronic properties of the photovoltaic films.

  5. High-performance and environmentally stable planar heterojunction perovskite solar cells based on a solution-processed copper-doped nickel oxide hole-transporting layer.

    PubMed

    Kim, Jong H; Liang, Po-Wei; Williams, Spencer T; Cho, Namchul; Chueh, Chu-Chen; Glaz, Micah S; Ginger, David S; Jen, Alex K-Y

    2015-01-27

    An effective approach to significantly increase the electrical conductivity of a NiOx hole-transporting layer (HTL) to achieve high-efficiency planar heterojunction perovskite solar cells is demonstrated. Perovskite solar cells based on using Cu-doped NiOx HTL show a remarkably improved power conversion efficiency up to 15.40% due to the improved electrical conductivity and enhanced perovskite film quality. General applicability of Cu-doped NiOx to larger bandgap perovskites is also demonstrated in this study. PMID:25449020

  6. Stable and null current hysteresis perovskite solar cells based nitrogen doped graphene oxide nanoribbons hole transport layer

    PubMed Central

    Kim, Jeongmo; Mat Teridi, Mohd Asri; Mohd Yusoff, Abd. Rashid bin; Jang, Jin

    2016-01-01

    Perovskite solar cells are becoming one of the leading technologies to reduce our dependency on traditional power sources. However, the frequently used component poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) has several shortcomings, such as an easily corroded indium-tin-oxide (ITO) interface at elevated temperatures and induced electrical inhomogeneity. Herein, we propose solution-processed nitrogen-doped graphene oxide nanoribbons (NGONRs) as a hole transport layer (HTL) in perovskite solar cells, replacing the conducting polymer PEDOT:PSS. The conversion efficiency of NGONR-based perovskite solar cells has outperformed a control device constructed using PEDOT:PSS. Moreover, our proposed NGONR-based devices also demonstrate a negligible current hysteresis along with improved stability. This work provides an effective route for substituting PEDOT:PSS as the effective HTL. PMID:27277388

  7. Stable and null current hysteresis perovskite solar cells based nitrogen doped graphene oxide nanoribbons hole transport layer

    NASA Astrophysics Data System (ADS)

    Kim, Jeongmo; Mat Teridi, Mohd Asri; Mohd Yusoff, Abd. Rashid Bin; Jang, Jin

    2016-06-01

    Perovskite solar cells are becoming one of the leading technologies to reduce our dependency on traditional power sources. However, the frequently used component poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) has several shortcomings, such as an easily corroded indium-tin-oxide (ITO) interface at elevated temperatures and induced electrical inhomogeneity. Herein, we propose solution-processed nitrogen-doped graphene oxide nanoribbons (NGONRs) as a hole transport layer (HTL) in perovskite solar cells, replacing the conducting polymer PEDOT:PSS. The conversion efficiency of NGONR-based perovskite solar cells has outperformed a control device constructed using PEDOT:PSS. Moreover, our proposed NGONR-based devices also demonstrate a negligible current hysteresis along with improved stability. This work provides an effective route for substituting PEDOT:PSS as the effective HTL.

  8. Electrodeposited Ultrathin TiO2 Blocking Layers for Efficient Perovskite Solar Cells

    PubMed Central

    Su, Tzu-Sen; Hsieh, Tsung-Yu; Hong, Cheng-You; Wei, Tzu-Chien

    2015-01-01

    In this study, the electrodeposition (ED) of ultrathin, compact TiO2 blocking layers (BLs) on fluorine-doped tin oxide (FTO) glass for perovskite solar cells (PSCs) is evaluated. This bottom-up method allows for controlling the morphology and thickness of TiO2 films by simply manipulating deposition conditions. Compared with BLs produced using the spin-coating (SC) method, BLs produced using ED exhibit satisfactory surface coverage, even with a film thickness of 29 nm. Evidence from cyclic voltammetry shows that an ED BL suppresses interfacial recombination more profoundly than an SC BL does, consequently improving the photovoltaic properties of the PSC significantly. A PSC equipped with an ED TiO2 BL having a 13.6% power conversion efficiency is demonstrated. PMID:26526771

  9. Electrodeposited Ultrathin TiO2 Blocking Layers for Efficient Perovskite Solar Cells

    NASA Astrophysics Data System (ADS)

    Su, Tzu-Sen; Hsieh, Tsung-Yu; Hong, Cheng-You; Wei, Tzu-Chien

    2015-11-01

    In this study, the electrodeposition (ED) of ultrathin, compact TiO2 blocking layers (BLs) on fluorine-doped tin oxide (FTO) glass for perovskite solar cells (PSCs) is evaluated. This bottom-up method allows for controlling the morphology and thickness of TiO2 films by simply manipulating deposition conditions. Compared with BLs produced using the spin-coating (SC) method, BLs produced using ED exhibit satisfactory surface coverage, even with a film thickness of 29 nm. Evidence from cyclic voltammetry shows that an ED BL suppresses interfacial recombination more profoundly than an SC BL does, consequently improving the photovoltaic properties of the PSC significantly. A PSC equipped with an ED TiO2 BL having a 13.6% power conversion efficiency is demonstrated.

  10. Perovskite Solar Cells: Moth-Eye TiO2 Layer for Improving Light Harvesting Efficiency in Perovskite Solar Cells (Small 18/2016).

    PubMed

    Kang, Seong Min; Jang, Segeun; Lee, Jong-Kwon; Yoon, Jungjin; Yoo, Dong-Eun; Lee, Jin-Wook; Choi, Mansoo; Park, Nam-Gyu

    2016-05-01

    A moth-eye patterned mesoporous (mp) TiO2 layer is fabricated in the form of submicron scale by using lithography, nano-imprinting and polydimethyl siloxane (PDMS) stamping methods. On page 2443, M. Choi, N.-G. Park, and co-workers demonstrate an excellent light harvesting property of perovskite solar cell by employing the moth-eye nanostructured mp-TiO2 film. These novel fabrication methods are expected to be optically beneficial to opto-electronic devices. PMID:27151831

  11. Role of 4-tert-Butylpyridine as a Hole Transport Layer Morphological Controller in Perovskite Solar Cells.

    PubMed

    Wang, Shen; Sina, Mahsa; Parikh, Pritesh; Uekert, Taylor; Shahbazian, Brian; Devaraj, Arun; Meng, Ying Shirley

    2016-09-14

    Hybrid organic-inorganic materials for high-efficiency, low-cost photovoltaic devices have seen rapid progress since the introduction of lead based perovskites and solid-state hole transport layers. Although majority of the materials used for perovskite solar cells (PSC) are introduced from dye-sensitized solar cells (DSSCs), the presence of a perovskite capping layer as opposed to a single dye molecule (in DSSCs) changes the interactions between the various layers in perovskite solar cells. 4-tert-Butylpyridine (tBP), commonly used in PSCs, is assumed to function as a charge recombination inhibitor, similar to DSSCs. However, the presence of a perovskite capping layer calls for a re-evaluation of its function in PSCs. Using TEM (transmission electron microscopy), we first confirm the role of tBP as a HTL morphology controller in PSCs. Our observations suggest that tBP significantly improves the uniformity of the HTL and avoids accumulation of Li salt. We also study degradation pathways by using FTIR (Fourier transform infrared spectroscopy) and APT (atom probe tomography) to investigate and visualize in 3-dimensions the moisture content associated with the Li salt. Long-term effects, over 1000 h, due to evaporation of tBP have also been studied. Based on our findings, a PSC failure mechanism associated with the morphological change of the HTL is proposed. tBP, the morphology controller in HTL, plays a key role in this process, and thus this study highlights the need for additive materials with higher boiling points for consistent long-term performance of PSCs. PMID:27547991

  12. Role of 4-tert-Butylpyridine as a Hole Transport Layer Morphological Controller in Perovskite Solar Cells.

    PubMed

    Wang, Shen; Sina, Mahsa; Parikh, Pritesh; Uekert, Taylor; Shahbazian, Brian; Devaraj, Arun; Meng, Ying Shirley

    2016-09-14

    Hybrid organic-inorganic materials for high-efficiency, low-cost photovoltaic devices have seen rapid progress since the introduction of lead based perovskites and solid-state hole transport layers. Although majority of the materials used for perovskite solar cells (PSC) are introduced from dye-sensitized solar cells (DSSCs), the presence of a perovskite capping layer as opposed to a single dye molecule (in DSSCs) changes the interactions between the various layers in perovskite solar cells. 4-tert-Butylpyridine (tBP), commonly used in PSCs, is assumed to function as a charge recombination inhibitor, similar to DSSCs. However, the presence of a perovskite capping layer calls for a re-evaluation of its function in PSCs. Using TEM (transmission electron microscopy), we first confirm the role of tBP as a HTL morphology controller in PSCs. Our observations suggest that tBP significantly improves the uniformity of the HTL and avoids accumulation of Li salt. We also study degradation pathways by using FTIR (Fourier transform infrared spectroscopy) and APT (atom probe tomography) to investigate and visualize in 3-dimensions the moisture content associated with the Li salt. Long-term effects, over 1000 h, due to evaporation of tBP have also been studied. Based on our findings, a PSC failure mechanism associated with the morphological change of the HTL is proposed. tBP, the morphology controller in HTL, plays a key role in this process, and thus this study highlights the need for additive materials with higher boiling points for consistent long-term performance of PSCs.

  13. Layered oxygen-deficient double perovskite as an efficient and stable anode for direct hydrocarbon solid oxide fuel cells.

    PubMed

    Sengodan, Sivaprakash; Choi, Sihyuk; Jun, Areum; Shin, Tae Ho; Ju, Young-Wan; Jeong, Hu Young; Shin, Jeeyoung; Irvine, John T S; Kim, Guntae

    2015-02-01

    Different layered perovskite-related oxides are known to exhibit important electronic, magnetic and electrochemical properties. Owing to their excellent mixed-ionic and electronic conductivity and fast oxygen kinetics, cation layered double perovskite oxides such as PrBaCo2O5 in particular have exhibited excellent properties as solid oxide fuel cell oxygen electrodes. Here, we show for the first time that related layered materials can be used as high-performance fuel electrodes. Good redox stability with tolerance to coking and sulphur contamination from hydrocarbon fuels is demonstrated for the layered perovskite anode PrBaMn2O5+δ (PBMO). The PBMO anode is fabricated by in situ annealing of Pr0.5Ba0.5MnO3-δ in fuel conditions and actual fuel cell operation is demonstrated. At 800 °C, layered PBMO shows high electrical conductivity of 8.16 S cm(-1) in 5% H2 and demonstrates peak power densities of 1.7 and 1.3 W cm(-2) at 850 °C using humidified hydrogen and propane fuels, respectively.

  14. Tackling pseudosymmetry problems in electron backscatter diffraction (EBSD) analyses of perovskite structures

    NASA Astrophysics Data System (ADS)

    Mariani, Elisabetta; Kaercher, Pamela; Mecklenburgh, Julian; Wheeler, John

    2016-04-01

    Perovskite minerals form an important mineral group that has applications in Earth science and emerging alternative energy technologies, however crystallographic quantification of these minerals with electron backscatter diffraction (EBSD) is not accurate due to pseudosymmetry problems. The silicate perovskite Bridgmanite, (Mg,Fe)SiO3, is understood to be the dominant phase in the Earth's lower mantle. Gaining insight into its physical and rheological properties is therefore vital to understand the dynamics of the Earth's deep interior. Rock deformation experiments on analogue perovskite phases, for example (Ca,Sr)TiO3, combined with quantitative microstructural analyses of the recovered samples by EBSD, yield datasets that can reveal what deformation mechanisms may dominate the flow of perovskite in the lower mantle. Additionally, perovskite structures have important technological applications as new, suitable cathodes for the operation of more efficient and environmentally-friendly solid oxide fuel cells (SOFC). In recent years they have also been recognised as a potential substitute for silicon in the next generation of photovoltaic cells for the construction of economic and energy efficient solar panels. EBSD has the potential to be a valuable tool for the study of crystal orientations achieved in perovskite substrates as crystal alignment has a direct control on the properties of these materials. However, perovskite structures currently present us with challenges during the automated indexing of Kikuchi bands in electron backscatter diffraction patterns (EBSPs). Such challenges are represented by the pseudosymmetric character of perovskites, where atoms are subtly displaced (0.005 nm to 0.05 nm) from their higher symmetry positions. In orthorhombic Pbnm perovskites, for example, pseudosymmetry may be evaluated from the c/a unit cell parameter ratio, which is very close to 1. Two main types of distortions from the higher symmetry structure are recognised: a

  15. Structure, Growth Process, and Growth Mechanism of Perovskite in High-Titanium-Bearing Blast Furnace Slag

    NASA Astrophysics Data System (ADS)

    Liu, Lu; Hu, Meilong; Xu, Yuzhou; Bai, Chenguang; Gan, Yunhua

    2015-08-01

    The isothermal crystallization of perovskite in TiO2-CaO-SiO2-Al2O3-MgO high-titanium-bearing blast furnace slag was observed in situ at 1698 K (1425 °C) using a confocal scanning laser microscope. The dendrite structure of perovskite (CaTiO3) thus obtained showed vividly the primary dendrite trunks and secondary dendrite arms. Furthermore, the dendritic growth of perovskite in liquid slag was clearly observed on line. The results showed that the dendrite arrays in which the primary dendrite trunks observed on slag surface were parallel with each other grew toward the same direction. The secondary dendrite arms grew in the perpendicular direction with the primary trucks and stopped growing when they encounter. The perovskite dendrites showed a linear growth at two stages. The dendrites grew faster at early stage at about 5 to 7 μm/s and grew with a lower growth rate at about 1 to 2 μm/s in later stage. Finally, the growth mechanism of perovskite in melt was analyzed with the solidification theory. Based on the theoretical calculation of equilibrium phases in slag, the initial slag could be considered as a binary component system. One component was perovskite and the other component was the sum of all the other species that did not attend the crystallization of perovskite (included SiO2, Al2O3, and MgO, as well as CaO and TiO2 that were not involved in the solid formation). The formation of perovskite required the diffusion of CaO and TiO2 to the solid/liquid interface and the rejection of the other species from the interface. The solid/liquid equilibrium schematic diagram was made based on the calculation.

  16. Artificial layered perovskite oxides A(B{sub 0.5}B′{sub 0.5})O{sub 3} as potential solar energy conversion materials

    SciTech Connect

    Chen, Hungru; Umezawa, Naoto

    2015-02-07

    Perovskite oxides with a d{sup 0} electronic configuration are promising photocatalysts and exhibit high electron mobilities. However, their band gaps are too large for efficient solar energy conversion. On the other hand, transition metal cations with partially filled d{sup n} electronic configurations give rise to visible light absorption. In this study, by using hybrid density functional theory calculations, it is demonstrated that the virtues of the two categories of materials can be combined in perovskite oxide A(B{sub 0.5}B′{sub 0.5})O{sub 3} with a layered B-site ordering along the [001] direction. The electronic structures of the four selected perovskite oxide compounds, La(Ti{sub 0.5}Ni{sub 0.5})O{sub 3}, La(Ti{sub 0.5}Zn{sub 0.5})O{sub 3}, Sr(Nb{sub 0.5}Cr{sub 0.5})O{sub 3}, and Sr(Nb{sub 0.5}Fe{sub 0.5})O{sub 3} are calculated and discussed.

  17. Structural and magnetic properties of perovskite Ca{sub 3}Fe{sub 2}WO{sub 9}

    SciTech Connect

    Ivanov, Sergey A. . E-mail: ivan@cc.nifhi.ac.ru; Eriksson, Sten Gunnar . E-mail: stene@inoc.chalmers.se; Tellgren, Roland . E-mail: rte@mkem.uu.se; Rundloef, Haekan

    2005-12-15

    A complex perovskite with composition Ca{sub 3}Fe{sub 2}WO{sub 9} has been synthesised, and the temperature evolution of nuclear and magnetic structures investigated by neutron powder diffraction. It was shown that at room temperature this compound adopts a monoclinic perovskite structure belonging to space group P12{sub 1}/n1 (a=5.4180(5)A, b=5.5093(5)A, c=7.7031(7)A), {beta}=90.04(2){sup o}). The partial B-site ordering, of the Fe{sup +3} and W{sup +6} cations, at (2c) and (2d) sites was determined. At low temperatures the magnetic diffraction peaks were registered and a possible model for the magnetic structure was proposed in accordance with the ferrimagnetic properties of the title compound. The magnetic structure is defined by a propagation vector k=(1/2,1/2,0) and can be described as an array of ferromagnetic (20-1) layers, which couple antiferromagnetically to each other. All the Fe moments within a layer are aligned parallel (or anti-parallel) to the c-axis. The structural and magnetic features of this compound are discussed and compared with those of some other quaternary oxides A{sub 3}Fe{sub 2}WO{sub 9} (A=Ba, Sr, Pb)

  18. Lattice instability and competing spin structures in the double perovskite insulator Sr2FeOsO6.

    PubMed

    Paul, Avijit Kumar; Reehuis, Manfred; Ksenofontov, Vadim; Yan, Binghai; Hoser, Andreas; Többens, Daniel M; Abdala, Paula M; Adler, Peter; Jansen, Martin; Felser, Claudia

    2013-10-18

    The semiconductor Sr2FeOsO6, depending on temperature, adopts two types of spin structures that differ in the spin sequence of ferrimagnetic iron-osmium layers along the tetragonal c axis. Neutron powder diffraction experiments, 57Fe Mössbauer spectra, and density functional theory calculations suggest that this behavior arises because a lattice instability resulting in alternating iron-osmium distances fine-tunes the balance of competing exchange interactions. Thus, Sr2FeOsO6 is an example of a double perovskite, in which the electronic phases are controlled by the interplay of spin, orbital, and lattice degrees of freedom. PMID:24182298

  19. Synthesis of freestanding single-crystal perovskite films and heterostructures by etching of sacrificial water-soluble layers

    DOE PAGES

    Lu, Di; Baek, David J.; Hong, Seung Sae; Kourkoutis, Lena F.; Hikita, Yasuyuki; Hwang, Harold Y.

    2016-09-12

    Here, the ability to create and manipulate materials in two-dimensional (2D) form has repeatedly had transformative impact on science and technology. In parallel with the exfoliation and stacking of intrinsically layered crystals1, 2, 3, 4, 5, atomic-scale thin film growth of complex materials has enabled the creation of artificial 2D heterostructures with novel functionality6, 7, 8, 9 and emergent phenomena, as seen in perovskite heterostructures10, 11, 12. However, separation of these layers from the growth substrate has proved challenging, limiting the manipulation capabilities of these heterostructures with respect to exfoliated materials. Here we present a general method to create freestandingmore » perovskite membranes. The key is the epitaxial growth of water-soluble Sr3Al2O6 on perovskite substrates, followed by in situ growth of films and heterostructures. Millimetre-size single-crystalline membranes are produced by etching the Sr3Al2O6 layer in water, providing the opportunity to transfer them to arbitrary substrates and integrate them with heterostructures of semiconductors and layered compounds13, 14.« less

  20. Perovskite Solar Cells Based on Low-Temperature Processed Indium Oxide Electron Selective Layers.

    PubMed

    Qin, Minchao; Ma, Junjie; Ke, Weijun; Qin, Pingli; Lei, Hongwei; Tao, Hong; Zheng, Xiaolu; Xiong, Liangbin; Liu, Qin; Chen, Zhiliang; Lu, Junzheng; Yang, Guang; Fang, Guojia

    2016-04-01

    Indium oxide (In2O3) as a promising n-type semiconductor material has been widely employed in optoelectronic applications. In this work, we applied low-temperature solution-processed In2O3 nanocrystalline film as an electron selective layer (ESL) in perovskite solar cells (PSCs) for the first time. By taking advantages of good optical and electrical properties of In2O3 such as high mobility, wide band gap, and high transmittance, we obtained In2O3-based PSCs with a good efficiency exceeding 13% after optimizing the concentration of the precursor solution and the annealing temperature. Furthermore, to enhance the performance of the In2O3-based PSCs, a phenyl-C61-butyric acid methyl ester (PCBM) layer was introduced to modify the surface of the In2O3 film. The PCBM film could fill up the pinholes or cracks along In2O3 grain boundaries to passivate the defects and make the ESL extremely compact and uniform, which is conducive to suppressing the charge recombination. As a result, the efficiency of the In2O3-based PSC was improved to 14.83% accompanied with V(OC), J(SC), and FF being 1.08 V, 20.06 mA cm(-2), and 0.685, respectively.

  1. Structure Investigation of CaSiO3 Perovskite at 91 GPa

    NASA Astrophysics Data System (ADS)

    Martin, C.; Prakapenka, V.; Parise, J. B.

    2007-12-01

    The crystallographic structure of CaSiO3 perovskite at 91(2) GPa is investigated using monochromatic X-ray diffraction and the laser-heated diamond anvil cell with a graphite gasket-insert to increase the volume of the sample under diffraction conditions. We report observations of weak X-ray reflections at d-spaces matching a perovskite super-structure, which appear in addition to splitting of diffraction from the cubic sub-structure. Considering this data in context with the space groups (SGs) of all perovskite structures observed experimentally and recorded in the Inorganic Crystal Structure Database, CaSiO3 perovskite adopts one of two possible tetragonal structures ( P4/ mbm, SG #127, rather than I4/ mcm, SG #123) after cooling from 2000(300) K at this pressure if an orthorhombic or monoclinic unit cell is discounted. When an orthorhombic perovskite structure is considered, reflections from the perovskite super-structure discount Imam (SG #74) and could favor Cmcm (SG #74) above Pbnm (SG #62). The raw diffraction data from CaSiO3 and our analysis are presented in addition to a detailed procedure for the construction of the graphite gasket-insert used during the high pressure experiment. In brief, graphite is machined from a monochromator by electronic discharge and placed within a conventional tungsten gasket. Oriented with its a-axis perpendicular to the direction of force in the diamond anvil cell, a sample chamber is machined within the graphite-insert after indenting with the diamond anvils.

  2. Preparation of ultra-thin and high-quality WO3 compact layers and comparision of WO3 and TiO2 compact layer thickness in planar perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Zhang, Jincheng; Shi, Chengwu; Chen, Junjun; Wang, Yanqing; Li, Mingqian

    2016-06-01

    In this paper, the ultra-thin and high-quality WO3 compact layers were successfully prepared by spin-coating-pyrolysis method using the tungsten isopropoxide solution in isopropanol. The influence of WO3 and TiO2 compact layer thickness on the photovoltaic performance of planar perovskite solar cells was systematically compared, and the interface charge transfer and recombination in planar perovskite solar cells with TiO2 compact layer was analyzed by electrochemical impedance spectroscopy. The results revealed that the optimum thickness of WO3 and TiO2 compact layer was 15 nm and 60 nm. The planar perovskite solar cell with 15 nm WO3 compact layer gave a 9.69% average and 10.14% maximum photoelectric conversion efficiency, whereas the planar perovskite solar cell with 60 nm TiO2 compact layer achieved a 11.79% average and 12.64% maximum photoelectric conversion efficiency.

  3. Planar heterojunction type perovskite solar cells based on TiOx compact layer fabricated by chemical bath deposition

    NASA Astrophysics Data System (ADS)

    Taima, Tetsuya; Shahiduzzaman, Md.; Yamamoto, Kouhei; Furumoto, Yoshikazu; Kuwabara, Takayuki; Takahashi, Kohshin

    2016-02-01

    Perovskite (CH3NH3PbI3) solar cell (PSC) have been recently emerged as a promising cost and energy efficient light absorber material for photovoltaic applications. In this paper, we fabricated planar heterojunction (PHJ) perovskite solar cells using chemical bath deposited low temperature titanium oxide (TiOx) compact layer as an electron collection layer. The devices modified by fullerene (C60) with the thickness of 7nm show very significant improvement in photovoltaic performances compared to without modified devices leading to efficiencies as high as 9.0%. This is due to enhanced electrons more efficiently at the CH3NH3PbI3 /compact-TiOx interface from the C60 leading to improved photocurrent densities and fill factors.

  4. Syntheses, structures, and ionic conductivities of perovskite-structured lithium–strontium–aluminum/gallium–tantalum-oxides

    SciTech Connect

    Phraewphiphat, Thanya; Iqbal, Muhammad; Suzuki, Kota; Matsuda, Yasuaki; Yonemura, Masao; Hirayama, Masaaki; Kanno, Ryoji

    2015-05-15

    The ionic conductivities of new perovskite-structured lithium–strontium–aluminum/gallium–tantalum oxides were investigated. Solid solutions of the new perovskite oxides, (Li{sub x}Sr{sub 1−x})(Al{sub (1−x)/2}Ta{sub (1+x)/2})O{sub 3} and (Li{sub x}Sr{sub 1−x})(Ga{sub (1−x)/2}Ta{sub (1+x)/2})O{sub 3}, were synthesized using a ball-milled-assisted solid-state method. The partial substitution of the smaller Ga{sup +3} for Ta{sup +5} resulted in new compositions, the structures of which were determined by neutron diffraction measurements using a cubic perovskite structural model with the Pm−3m space group. Vacancies were introduced into the Sr(Li) sites by the formation of solid solutions with compositions (Li{sub x}Sr{sub 1−x−y}☐{sub y})(Ga{sub [(1−x)/2]−y}Ta{sub [(1+x)/2]+y})O{sub 3}, where the composition range of 0≤y≤0.20 was examined for x=0.2 and 0.25. The highest conductivity, 1.85×10{sup −3} S cm{sup −1} at 250 °C, was obtained for (Li{sub 0.25}Sr{sub 0.625}☐{sub 0.125})(Ga{sub 0.25}Ta{sub 0.75})O{sub 3} (x=0.25, y=0.125). Enhanced ionic conductivities were achieved by the introduction of vacancies at the A-sites. - Graphical abstract: Novel lithium-conducting oxides with the cubic perovskite structure (Li{sub x}Sr{sub 1−x−y}☐{sub y})(Ga{sub [(1−x)/2]−y}Ta{sub [(1+x)/2]+y})O{sub 3} provide a specific solid-solution region with various x and y values, exhibiting the highest ionic conductivity (1.85 S cm{sup −1} at 250 °C) for (Li{sub 0.25}Sr{sub 0.625}☐{sub 0.125})(Ga{sub 0.25}Ta{sub 0.75})O{sub 3} (x=0.25, y=0.125 in (Li{sub x}Sr{sub 1−x−y}☐{sub y})(Ga{sub [(1−x)/2]−y}Ta{sub [(1+x)/2]+y})O{sub 3}). The vacancies (☐) introduced into the A-sites contribute to the enhancement of lithium diffusion in the perovskite structure because of the enlargement of the bottleneck size and suppression of the interaction between lithium and oxygen. - Highlights: • The perovskite-structured novel Li

  5. Moth-Eye TiO2 Layer for Improving Light Harvesting Efficiency in Perovskite Solar Cells.

    PubMed

    Kang, Seong Min; Jang, Segeun; Lee, Jong-Kwon; Yoon, Jungjin; Yoo, Dong-Eun; Lee, Jin-Wook; Choi, Mansoo; Park, Nam-Gyu

    2016-05-01

    A moth-eye nanostructured mp-TiO2 film using conventional lithography, nano-imprinting and polydimethyl-siloxane (PDMS) stamping methods is demonstrated for the first time. Power conversion efficiency of the moth-eye patterned perovskite solar cell is improved by ≈11%, which mainly results from increasing light harvesting efficiency by structural optical property.

  6. Single-Layer Light-Emitting Diodes Using Organometal Halide Perovskite/Poly(ethylene oxide) Composite Thin Films.

    PubMed

    Li, Junqiang; Bade, Sri Ganesh R; Shan, Xin; Yu, Zhibin

    2015-09-16

    Organometal halide perovskite and poly(ethylene oxide) composite thin films are studied. Single-layer light-emitting diodes using the composite thin film sandwiched between indium tin oxide and indium-gallium eutectic alloy exhibit a low turn-on voltage and high brightness because of the ionic conductivity of the composite film and the formation of a p-i-n homojunction. PMID:26247326

  7. Synthesis and thermal stability studies of a series of metastable Dion–Jacobson double-layered neodymium-niobate perovskites

    SciTech Connect

    Josepha, Elisha A.; Farooq, Sara; Mitchell, Cinnamon M.; Wiley, John B.

    2014-08-15

    The Dion–Jacobson double-layered perovskite, RbNdNb{sub 2}O{sub 7}, is used as a precursor to synthesize the series ANdNb{sub 2}O{sub 7} (A=H, Li, Na, K, NH{sub 4}, Ag), and (MCl)NdNb{sub 2}O{sub 7} (M=Mn, Fe, Cu) through ion-exchange reactions ≤400 °C. Thermal stability studies indicated that most of these compounds are metastable. A combination of X-ray powder diffraction and differential thermal analysis were used to determine various low temperature decomposition pathways; these pathways were very dependent on the interlayer species. Overall the ANdNb{sub 2}O{sub 7} series was found to be less stable than the corresponding lanthanides, ALaNb{sub 2}O{sub 7}. - Graphical abstract: A new series of topochemically-prepared metastable neodymium-containing layered perovskites are studied. - Highlights: • A series of new layered neodymium containing perovskites were synthesized by ion exchange. • Products were studied by variable temperature X-ray diffraction and thermal analysis. • Most of the series are metastable showing exothermic transitions on decomposition. • The Nd compounds are less stable due to the smaller size of the Nd relative to La.

  8. Magnetic and dielectric properties of layered perovskite Gd2Ti2O7 thin film epitaxially stabilized on a perovskite single crystal

    NASA Astrophysics Data System (ADS)

    Ukita, Takashi; Hirose, Yasushi; Ohno, Sawako; Hatabayashi, Kunitada; Fukumura, Tomoteru; Hasegawa, Tetsuya

    2012-04-01

    Layered perovskite (LP) titanates, Ln2Ti2O7 (Ln = lanthanoids), are ferroelectric materials containing magnetic Ln3+ ions at A-site. Metastable LP-Gd2Ti2O7 was fabricated in epitaxial thin film form on lattice-matched perovskite substrates and its dielectric and magnetic properties were investigated. The (100)-oriented LP-Gd2Ti2O7 films were epitaxially grown on (110) plane of (LaAlO3)0.3-(SrAl0.5Ta0.5O3)0.7 (LSAT) and Nb-doped SrTiO3 by using a pulsed laser deposition method. Piezoresponse force microscope measurements revealed that LP-Gd2Ti2O7 has spontaneous polarization along the b-axis at room temperature, strongly suggesting room temperature ferroelectricity. Magnetization measurements showed paramagnetic behavior with weak antiferromagnetic interaction around 2 K. Small positive magneto-dielectric effect (Δɛ/ɛ ˜ 10-5 order) was also confirmed at 10 K.

  9. Composition and crystal structure of perovskite films attained from electrodes of used car battery

    NASA Astrophysics Data System (ADS)

    Dhiaputra, Ilham; Permana, Bayu; Maulana, Yusep; Inayatie, Yuniar Dwi; Purba, Yonatan R.; Bahtiar, Ayi

    2016-02-01

    Perovskite solar cells have been intensively investigated for high performance and low-cost solid-state solar cells. Perovskite based-lead materials are commonly used as active material for high power conversion efficiency solar cells. Herein, we report our study on the development of used electrodes car battery as a cheap raw lead material to be converted into lead (II) iodide PbI2 by using simple chemical method. We have successfully obtained PbI2 material with purity higher than 85% and its crystal structure is comparable with that of commercial product. The perovskite CH3NH3PbI3 film was prepared by spin-coating of PbI2 solution and followed by spin-coating two-times of methylamonium iodide (MAI) solution. In this paper, the crystal structure of perovskite film attained from used car battery is shown and compared with that of prepared from commercial PbI2. By utilizing the used car battery into perovskite valuable material for high performance solar cells, we can not only improve the economical value (added-value) of wasted car battery but also we can simultaneously save the environment.

  10. Research Update: Challenges for high-efficiency hybrid lead-halide perovskite LEDs and the path towards electrically pumped lasing

    NASA Astrophysics Data System (ADS)

    Li, Guangru; Price, Michael; Deschler, Felix

    2016-09-01

    Hybrid lead-halide perovskites have emerged as promising solution-processed semiconductor materials for thin-film optoelectronics. In this review, we discuss current challenges in perovskite LED performance, using thin-film and nano-crystalline perovskite as emitter layers, and look at device performance and stability. Fabrication of electrically pumped, optical-feedback devices with hybrid lead halide perovskites as gain medium is a future challenge, initiated by the demonstration of optically pumped lasing structures with low gain thresholds. We explain the material parameters affecting optical gain in perovskites and discuss the challenges towards electrically pumped perovskite lasers.

  11. Exploring the Electronic Band Structure of Organometal Halide Perovskite via Photoluminescence Anisotropy of Individual Nanocrystals.

    PubMed

    Täuber, Daniela; Dobrovolsky, Alexander; Camacho, Rafael; Scheblykin, Ivan G

    2016-08-10

    Understanding electronic processes in organometal halide perovskites, flourishing photovoltaic, and emitting materials requires unraveling the origin of their electronic transitions. Light polarization studies can provide important information regarding transition dipole moment orientations. Investigating individual methylammonium lead triiodide perovskite nanocrystals enabled us to detect the polarization of photoluminescence intensity and photoluminescence excitation, hidden in bulk samples by ensemble averaging. Polarization properties of the crystals were correlated with their photoluminescence spectra and electron microscopy images. We propose that distortion of PbI6 octahedra leads to peculiarities of the electronic band structure close to the band-edge. Namely, the lowest band transition possesses a transition dipole moment along the apical Pb-I-Pb bond resulting in polarized photoluminescence. Excitation of photoluminescence above the bandgap is unpolarized because it involves molecular orbitals delocalized both in the apical and equatorial directions of the perovskite octahedron. Trap-assisted emission at 77 K, rather surprisingly, was polarized similar to the bandgap emission.

  12. The Electronic Structure of Iron in Aluminous (Mg,Fe)SiO3 Perovskite at High-Pressures and Temperatures

    NASA Astrophysics Data System (ADS)

    Jackson, J. M.; Sturhahn, W.; Lerche, M.; Li, J.

    2006-12-01

    Knowledge of iron valences and spin states in silicate perovskite is relevant to our understanding of the physical and chemical properties of Earth's lower mantle such as transport properties, mechanical behavior, and element partitioning. Recent studies have proposed that aluminous ferromagnesium silicate perovskite (Al- Pv) is the principle sink for ferric iron in Earth's lower mantle [e.g. 1]. Also of geophysical interest is the electronic spin state of Al-Pv under lower mantle conditions. To date, simultaneous high-pressure and high- temperature measurements of the hyperfine parameters to identify the valence and spin states of iron in Al-Pv have not been reported. In this study, we have measured the electronic structure of the iron component of an aluminous Fe-bearing silicate perovskite sample, (Mg0.88Fe0.09)(Si0.94Al0.10)O3, close to a pyrolite composition, using synchrotron Mössbauer spectroscopy (SMS) and laser heated diamond anvil cells. Recent developments in SMS have enabled in situ measurements of small samples (< 10 μm) with relatively low 57Fe contents (< 10 at.%) to Mbar pressures [e.g. 2,3]. The samples were first synthesized in a multi-anvil apparatus [3], and the perovskite structure was confirmed by X-ray diffraction. The sample was loaded into a diamond anvil cell sandwiched between NaCl insulating layers. Measurements were carried out to 65 GPa and up to 2000 K at beamline 3-ID of the Advanced Photon Source. Spectra were collected before, during, and after laser heating, at each pressure point. Synchrotron Mössbauer spectra were also collected on decreasing pressure. Evaluation of the spectra provided the isomer shift (relative to stainless steel) and the quadrupole splitting of the iron component in silicate perovskite, which gives information on valence and spin states under lower mantle conditions. This work is supported by NSF through COMPRES and the U.S. DOE-BES, Office of Science, under Contract No. W-31-109-ENG-38. [1] Mc

  13. Structural, Optical, and Electronic Properties of Wide Bandgap Perovskites: Experimental and Theoretical Investigations.

    PubMed

    Kumawat, Naresh K; Tripathi, Madhvendra Nath; Waghmare, Umesh; Kabra, Dinesh

    2016-06-01

    Wide bandgap hybrid halide perovskites based on bromine and chlorine halide anions have emerged as potential candidates for various optoelectronic devices. However, these materials are relatively less explored than the iodine-based perovskites for microscopic details. We present experiment and first-principles calculations to understand the structural, optical, and electronic structure of wide bandgap CH3NH3Pb(Br1-xClx)3 (x = 0, 0.33, 0.66, and 1) 3D hybrid perovskite materials. We substituted Br(-) with Cl(-) to tune the bandgap from 2.4 eV (green emissive) to 3.2 eV (blue (UV) emissive) of these materials. We correlate our experimental results with first-principles theory and provide an insight into important parameters like lattice constants, electronic structure, excitonic binding energy (EX), dielectric constant, and reduced effective mass (μr) of charge carriers in these perovskite semiconductors. Electronic structure calculations reveal that electronic properties are mainly governed by Pb 6p and halide p orbitals. Our estimates of EX within a hydrogen model suggest that an increase in EX by increasing the Cl(-) (chlorine) concentration is mainly due to a decrease in the dielectric constant with x and almost constant value of μr close to the range of 0.07me. PMID:27203800

  14. Perovskites: transforming photovoltaics, a mini-review

    DOE PAGES

    Chilvery, Ashwith Kumar; Batra, Ashok K.; Yang, Bin; Xiao, Kai; Guggilla, Padmaja; Aggarwal, Mohan D.; Surabhi, Raja; Lal, Ravi B.; Currie, James R.; Penn, Benjamin G.

    2015-01-06

    The recent power-packed advent of perovskite solar cells is transforming photovoltaics (PV) with their superior efficiencies, ease of fabrication, and cost. This perovskite solar cell further boasts of many unexplored features that can further enhance its PV properties and lead to it being branded as a successful commercial product. This paper provides a detailed insight of the organometal halide based perovskite structure, its unique stoichiometric design, and its underlying principles for PV applications. Finally, the compatibility of various PV layers and its fabrication methods is also discussed.

  15. Luminescence studies of perovskite structured titanates: A review

    NASA Astrophysics Data System (ADS)

    Nag Bhargavi, G.; Khare, Ayush

    2015-06-01

    Apart from widely known dielectric and ferroelectric properties, the perovskite type materials also constitute a class of materials, which are recently investigated for their optical properties. These materials are being used for fabrication of various microelectronics and optoelectronic devices. Photoluminescence (PL), mechanoluminescence (ML) and thermoluminescence (TL) are such phenomena offering numerous applications in different fields like electro-optics, flat panel displays, LED technology, sensors, dynamic visualization etc. This paper briefly reviews the status and new progress in luminescence studies of ferroelectric materials like barium titanate (BT), barium zirconate titanate (BZT), calcium titanate (CT), calcium zirconate titanate (CZT), lead titanate (PT), lead zirconate titanate (PZT), etc., prepared through various methods.

  16. Electroluminescence from perovskite LEDs with the structure of Ag/Spiro-OMeTAD/CH3NH3PbI3/TiO2/FTO

    NASA Astrophysics Data System (ADS)

    Wang, Minhuan; Shi, Yantao; Bian, Jiming; Dong, Qingshun; Sun, Hongjun; Liu, Hongzhu; Luo, Yingmin; Zhang, Yuzhi

    2016-10-01

    The perovskite light-emitting diodes (Pe-LEDs) with the structure of Ag/Spiro-OMeTAD/CH3NH3PbI3/TiO2/FTO were synthesized, where the CH3NH3PbI3 perovskite layer was deposited by a two-step spin-coating process. A dominant near-infrared electroluminescence (EL) at 773 nm was detected from the Pe-LEDs under forward bias at room temperature. The origin and mechanism of the EL were discussed in comparison with the photoluminescence (PL) spectra, and it was attributed to the radiative recombination of electrons and holes confined in the CH3NH3PbI3 emissive layer. Moreover, the corresponding energy band diagrams was proposed to illustrate the carrier transport mechanism in the Pe-LED device.

  17. Perovskite LaRhO{sub 3} as a p-type active layer in oxide photovoltaics

    SciTech Connect

    Nakamura, Masao Krockenberger, Yoshiharu; Fujioka, Jun; Kawasaki, Masashi; Tokura, Yoshinori

    2015-02-16

    Perovskite-type transition-metal oxides have a wide variety of physical properties and triggered intensive research on functional devices in the form of heteroepitaxial junctions. However, there is a missing component that is a p-type conventional band semiconductor. LaRhO{sub 3} (LRO) is one of very few promising candidates having its bandgap between filled t{sub 2g} and empty e{sub g} of Rh in low-spin state, but there has been no report on the synthesis of large-size single crystals or thin films. Here, we report on the junction properties of single-crystalline thin films of LRO grown on (110) oriented Nb-doped SrTiO{sub 3} substrates. The external quantum efficiency of the photo-electron conversion exceeds 1% in the visible-light region due to the wide depletion layer and long diffusion length of minority carriers in LRO. Clear indication of p-type band semiconducting character in a perovskite oxide of LRO will pave a way to explore oxide electronics of perovskite heterostructures.

  18. Graphene oxide/PEDOT:PSS composite hole transport layer for efficient and stable planar heterojunction perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Lee, Da-Young; Na, Seok-In; Kim, Seok-Soon

    2016-01-01

    We investigated a graphene oxide (GO)/poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) composite as a promising candidate for the practical application of a 2-D carbonaceous hole transport layer (HTL) to planar heterojunction perovskite solar cells (PeSCs) consisting of a transparent electrode/HTL/perovskite/fullerene/metal electrode. Both the insulating properties of GO and the non-uniform coating of the transparent electrode with GO cause the poor morphology of perovskite induced low power conversion efficiency (PCE) of 6.4%. On the other hand, PeSCs with a GO/PEDOT:PSS composite HTL, exhibited a higher PCE of 9.7% than that of a device fabricated with conventional PEDOT:PSS showing a PCE of 8.2%. The higher performance is attributed to the decreased series resistance (RS) and increased shunt resistance (RSh). The well-matched work-function between GO (4.9 eV) and PEDOT:PSS (5.1 eV) probably results in more efficient charge transport and an overall decrease in RS. The existence of GO with a large bandgap of ~3.6 eV might induce the effective blocking of electrons, leading to an increase of RSh. Moreover, improvement in the long-term stability under atmospheric conditions was observed.

  19. An efficient electron transport material of tin oxide for planar structure perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Murugadoss, Govindhasamy; Kanda, Hiroyuki; Tanaka, Soichiro; Nishino, Hitoshi; Ito, Seigo; Imahoric, Hiroshi; Umeyama, Tomokazu

    2016-03-01

    The photovoltaic performance of a perovskite solar cell based on a new electron conducting SnO2 film prepared at low temperature using different solvents was investigated. SnO2 was selected as an electron conducting medium due to its superior properties over TiO2, such as better antireflective properties, higher electron mobility, more suitable band edges and a wider band gap. A SnO2 layer was developed by spin-coating SnCl2 solution followed by annealing at 200 °C in air. The low-temperature (200 °C) annealed SnO2 layer exhibits enhanced crystallization, high transmittance, and uniform surface morphology using ethanol as a solvent rather than water. Solid state CuSCN hole conductor was used as HTM for reducing the device cost. A planar solar cell fabricated with CH3NH3PbI3 perovskite infiltrated SnO2 showed a power conversion efficiency of 8.38% with short-circuit current density of 18.99 mA cm-2, an open-circuit voltage of 0.96 mV and a fill factor of 45%. The devices were fabricated at >60% humidity level at room temperature. The results suggest that SnO2 is an effective charge collection system for CH3NH3PbI3 based planar perovskite solar cells. In addition, these results provide a new direction for the future improvement of perovskite solar cells using new electron conducting layers.

  20. Electronic structure and band alignment at an epitaxial spinel/perovskite heterojunction.

    PubMed

    Qiao, Liang; Li, Wei; Xiao, Haiyan; Meyer, Harry M; Liang, Xuelei; Nguyen, N V; Weber, William J; Biegalski, Michael D

    2014-08-27

    The electronic properties of solid-solid interfaces play critical roles in a variety of technological applications. Recent advances of film epitaxy and characterization techniques have demonstrated a wealth of exotic phenomena at interfaces of oxide materials, which are critically dependent on the alignment of their energy bands across the interface. Here we report a combined photoemission and electrical investigation of the electronic structures across a prototypical spinel/perovskite heterojunction. Energy-level band alignment at an epitaxial Co3O4/SrTiO3(001) heterointerface indicates a chemically abrupt, type I heterojunction without detectable band bending at both the film and substrate. The unexpected band alignment for this typical p-type semiconductor on SrTiO3 is attributed to its intrinsic d-d interband excitation, which significantly narrows the fundamental band gap between the top of the valence band and the bottom of the conduction band. The formation of the type I heterojunction with a flat-band state results in a simultaneous confinement of both electrons and holes inside the Co3O4 layer, thus rendering the epitaxial Co3O4/SrTiO3(001) heterostructure to be a very promising material for high-efficiency luminescence and optoelectronic device applications.

  1. Di-hydrogen contact induced lattice instabilities and structural dynamics in complex hydride perovskites.

    PubMed

    Schouwink, P; Hagemann, H; Embs, J P; D'Anna, V; Černý, R

    2015-07-01

    The structural phase transitions occurring in a series of perovskite-type complex hydrides based on the tetrahydroborate anion BH4(-) are investigated by means of in situ synchrotron x-ray powder diffraction, vibrational spectroscopy, thermal methods and ab initio calculations in the solid state. Structural dynamics of the BH4 anion are followed with quasi-elastic neutron scattering. We show that unexpected temperature-induced lattice instabilities in perovskite-type ACa(BH4)3 (A = K, Rb, Cs) have their origin in close hydridic di-hydrogen contacts. The rich lattice dynamics lead to coupling between internal B-H vibrations and phonons, resulting in distortions in the high-temperature polymorph that are identical in symmetry to well-known instabilities in oxide perovskites, generally condensing at lower temperatures. It is found that anion-substitution BH4(-) <-> (X = Halide) can relax distortions in ACa(BH4)3 by eliminating coulomb repulsive H(-)···H(-) effects. The interesting nature of phase transition in ACa(BH4)3 enters an unexplored field of weak interactions in ceramic-like host lattices and is the principal motivation for this study. Close di-hydrogen contacts suggest new concepts to tailor crystal symmetries in complex hydride perovskites in the future. PMID:26076047

  2. Excellent sun-light-driven photocatalytic activity by aurivillius layered perovskites, Bi₅-xLaxTi₃FeO₁₅ (x = 1, 2).

    PubMed

    Naresh, Gollapally; Mandal, Tapas Kumar

    2014-12-10

    Aurivillius phase layered perovskites, Bi5-xLaxTi3FeO15 (x = 1, 2) are synthesized by solid-state reaction. The compounds are characterized by powder X-ray diffraction (PXD), field-emission scanning electron microscopy (FE-SEM), energy-dispersive X-ray spectroscopy (EDS), UV-vis diffuse reflectance (UV-vis DRS), and photoluminescence (PL) spectroscopy. UV-vis DRS data revealed that the compounds are visible light absorbing semiconductors with band gaps ranging from ∼2.0-2.7 eV. Photocatalytic activity studies by Rhodamine B (RhB) degradation under sun-light irradiation showed that these layered oxides are very efficient photocatalysts in mild acidic medium. Scavenger test studies demonstrated that the photogenerated holes and superoxide radicals (O2(•-)) are the active species responsible for RhB degradation over the Aurivillius layered perovskites. Comparison of PL intensity, dye adsorption and ζ-potential suggested that a slow e(-)-h(+) recombination and effective dye adsorption are crucial for the degradation process over these photocatalysts. Moreover, relative positioning of the valence and conduction band edges of the semiconductors, O2/O2(•-), (•)OH/H2O potential and HOMO-LUMO levels of RhB appears to be responsible for making the degradation hole-specific. Photocatalytic cycle tests indicated high stability of the catalysts in the reaction medium without any observable loss of activity. This work shows great potential in developing novel photocatalysts with layered structures for sun-light-driven oxidation and degradation processes largely driven by holes and without any intervention of hydroxyl radicals, which is one of the most common reactive oxygen species (ROS) in many advanced oxidation processes.

  3. Using an airbrush pen for layer-by-layer growth of continuous perovskite thin films for hybrid solar cells.

    PubMed

    Ramesh, Mohan; Boopathi, Karunakara Moorthy; Huang, Tzu-Yen; Huang, Yu-Ching; Tsao, Cheng-Si; Chu, Chih-Wei

    2015-02-01

    In this manuscript we describe hybrid heterojunction solar cells, having the device architecture glass/indium tin oxide/poly(3,4-ethylenedioxythiopene)/poly(styrenesulfonic acid)/perovskite/[6,6]-phenyl-C61-butyric acid methyl ester/C60/2,9-dimethyl- 4,7-diphenyl-1,10-phenanthroline/Al, fabricated using lead halide perovskite obtained through spray-coating at a low precursor concentration. To study the relationship between the morphology and device performance, we recorded scanning electron microscopy images of perovskite films prepared at various precursor ratios, spray volumes, substrate temperatures, and postspray annealing temperatures. Optimization of the spray conditions ensured uniform film growth and high surface area coverage at low substrate temperatures. Lead halide perovskite solar cells prepared under the optimal conditions displayed an average power conversion efficiency (PCE) of approximately 9.2%, with 85% of such devices having efficiencies of greater than 8.3%. The best-performing device exhibited a short-circuit current density of 17.3 mA cm(-2), a fill factor of 0.63, and an open-circuit voltage of 0.93 V, resulting in a PCE of 10.2%. Because spray-coating technology allows large-area deposition, we also fabricated devices having areas of 60 and 342 mm(2), achieving PCEs with these devices of 6.88 and 4.66%, respectively. PMID:25562387

  4. Entropy-driven structural transition and kinetic trapping in formamidinium lead iodide perovskite

    PubMed Central

    Chen, Tianran; Foley, Benjamin J.; Park, Changwon; Brown, Craig M.; Harriger, Leland W.; Lee, Jooseop; Ruff, Jacob; Yoon, Mina; Choi, Joshua J.; Lee, Seung-Hun

    2016-01-01

    A challenge of hybrid perovskite solar cells is device instability, which calls for an understanding of the perovskite structural stability and phase transitions. Using neutron diffraction and first-principles calculations on formamidinium lead iodide (FAPbI3), we show that the entropy contribution to the Gibbs free energy caused by isotropic rotations of the FA+ cation plays a crucial role in the cubic-to-hexagonal structural phase transition. Furthermore, we observe that the cubic-to-hexagonal phase transition exhibits a large thermal hysteresis. Our first-principles calculations confirm the existence of a potential barrier between the cubic and hexagonal structures, which provides an explanation for the observed thermal hysteresis. By exploiting the potential barrier, we demonstrate kinetic trapping of the cubic phase, desirable for solar cells, even at 8.2 K by thermal quenching.

  5. Distribution change of oxygen vacancies in layered perovskite type(Sr, La){sub n+1}Fe{sub n}O{sub 3n+1} (n=3)

    SciTech Connect

    Kagomiya, Isao Jimbo, Keigo; Kakimoto, Ken-ichi

    2013-11-15

    To elucidate characteristic oxygen vacancy formation in layered perovskite (Sr, La){sub n+1}Fe{sub n}O{sub 3n+1} with the perovskite layer number: n=3, oxygen vacancy content δ of the (Sr{sub 0.775}La{sub 0.225}){sub 4}Fe{sub 3}O{sub 10−δ} (SLF4310) was investigated using a titration technique and a thermogravimetric analysis. The equilibrium constant K for the reduction reaction: Oo{sup ×}+2Fe{sub Fe}{sup ∙} (Fe{sup 4+})=1/2O{sub 2}+Vo{sup ∙∙}+2Fe{sub Fe}{sup ×}(Fe{sup 3+}) was estimated using the vacancy content δ. The Arrhenius plot of the K reveals slope change at approximately 775 °C. From the Rietveld analysis, the oxygen vacancies are the most remarkable at the O2 (O4) sites at lower (higher) temperatures than about 800 °C, which temperature is approximately comparable with that of slope change in the K. These facts mean that distribution of vacancy sites in the SLF4310 changes at approximately 775 °C, accompanying no structural phase transition. The vacancy distribution change affects to the ion conductivity of the SLF4310. - Graphical abstract: Crystal structure of (Sr{sub 0.775}La{sub 0.225}){sub 4}Fe{sub 3}O{sub 10−δ} (SLF4310) at 1000 °C. Display Omitted - Highlights: • Distribution change of oxygen vacancies is appeared at approximately 775 °C. • The distribution change with no structure phase transition is the first observation. • The vacancy distribution change affects the ion conductivity of the SLF4310.

  6. Cuprous Oxide as a Potential Low-Cost Hole-Transport Material for Stable Perovskite Solar Cells.

    PubMed

    Nejand, Bahram Abdollahi; Ahmadi, Vahid; Gharibzadeh, Saba; Shahverdi, Hamid Reza

    2016-02-01

    Inorganic hole-transport materials are commercially desired to decrease the fabrication cost of perovskite solar cells. Here, Cu2O is introduced as a potential hole-transport material for stable, low-cost devices. Considering that Cu2O formation is highly sensitive to the underlying mixture of perovskite precursors and their solvents, we proposed and engineered a technique for reactive magnetron sputtering. The rotational angular deposition of Cu2O yields high surface coverage of the perovskite layer for high rate of charge extraction. Deposition of this Cu2O layer on the pinhole-free perovskite layer produces devices with power conversion efficiency values of up to 8.93%. The engineered Cu2O layers showed uniform, compact, and crack-free surfaces on the perovskite layer without affecting the perovskite structure, which is desired for deposition of the top metal contact and for surface shielding against moisture and mechanical damages. PMID:26748959

  7. Efficiency Enhancement of Hybrid Perovskite Solar Cells with MEH-PPV Hole-Transporting Layers

    PubMed Central

    Chen, Hsin-Wei; Huang, Tzu-Yen; Chang, Ting-Hsiang; Sanehira, Yoshitaka; Kung, Chung-Wei; Chu, Chih-Wei; Ikegami, Masashi; Miyasaka, Tsutomu; Ho, Kuo-Chuan

    2016-01-01

    In this study, hybrid perovskite solar cells are fabricated using poly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene] (MEH-PPV) and poly(3-hexylthiophene-2,5-diyl) (P3HT) as dopant-free hole-transporting materials (HTMs), and two solution processes (one- and two-step methods, respectively) for preparing methylammonium lead iodide perovskite. By optimizing the concentrations and solvents of MEH-PPV solutions, a power conversion efficiency of 9.65% with hysteresis-less performance is achieved, while the device with 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenylamine)-9,9′spirobifluorene (Spiro-OMeTAD) doped with lithium salts and tert-butylpyridine (TBP) exhibits an efficiency of 13.38%. This result shows that non-doped MEH-PPV is a suitable, low-cost HTM for efficient polymer-based perovskite solar cells. The effect of different morphologies of methylammonium lead iodide perovskite on conversion efficiency is also investigated by incident photon-to-electron conversion efficiency (IPCE) curves and electrochemical impedance spectroscopy (EIS). PMID:27698464

  8. Efficiency Enhancement of Hybrid Perovskite Solar Cells with MEH-PPV Hole-Transporting Layers

    NASA Astrophysics Data System (ADS)

    Chen, Hsin-Wei; Huang, Tzu-Yen; Chang, Ting-Hsiang; Sanehira, Yoshitaka; Kung, Chung-Wei; Chu, Chih-Wei; Ikegami, Masashi; Miyasaka, Tsutomu; Ho, Kuo-Chuan

    2016-10-01

    In this study, hybrid perovskite solar cells are fabricated using poly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene] (MEH-PPV) and poly(3-hexylthiophene-2,5-diyl) (P3HT) as dopant-free hole-transporting materials (HTMs), and two solution processes (one- and two-step methods, respectively) for preparing methylammonium lead iodide perovskite. By optimizing the concentrations and solvents of MEH-PPV solutions, a power conversion efficiency of 9.65% with hysteresis-less performance is achieved, while the device with 2,2‧,7,7‧-tetrakis(N,N-di-p-methoxyphenylamine)-9,9‧spirobifluorene (Spiro-OMeTAD) doped with lithium salts and tert-butylpyridine (TBP) exhibits an efficiency of 13.38%. This result shows that non-doped MEH-PPV is a suitable, low-cost HTM for efficient polymer-based perovskite solar cells. The effect of different morphologies of methylammonium lead iodide perovskite on conversion efficiency is also investigated by incident photon-to-electron conversion efficiency (IPCE) curves and electrochemical impedance spectroscopy (EIS).

  9. Mechanism of biphasic charge recombination and accumulation in TiO2 mesoporous structured perovskite solar cells.

    PubMed

    Wang, Hao-Yi; Wang, Yi; Yu, Man; Han, Jun; Guo, Zhi-Xin; Ai, Xi-Cheng; Zhang, Jian-Ping; Qin, Yujun

    2016-04-28

    Organic-inorganic halide perovskite solar cells are becoming the next big thing in the photovoltaic field owing to their rapidly developing photoelectric conversion performance. Herein, mesoporous structured perovskite devices with various perovskite grain sizes are fabricated by a sequential dropping method, and the charge recombination dynamics is investigated by transient optical-electric measurements. All devices exhibit an overall power conversion efficiency around 15%. More importantly, a biphasic trap-limited charge recombination process is proposed and interpreted by taking into account the specific charge accumulation mechanism in perovskite solar cells. At low Fermi levels, photo-generated electrons predominately populate in the perovskite phase, while at high Fermi levels, most electrons occupy traps in mesoporous TiO2. As a result, the dynamics of charge recombination is, respectively, dominated by the perovskite phase and mesoporous TiO2 in these two cases. The present work would give a new perspective on the charge recombination process in meso-structured perovskite solar cells.

  10. Mechanism of biphasic charge recombination and accumulation in TiO2 mesoporous structured perovskite solar cells.

    PubMed

    Wang, Hao-Yi; Wang, Yi; Yu, Man; Han, Jun; Guo, Zhi-Xin; Ai, Xi-Cheng; Zhang, Jian-Ping; Qin, Yujun

    2016-04-28

    Organic-inorganic halide perovskite solar cells are becoming the next big thing in the photovoltaic field owing to their rapidly developing photoelectric conversion performance. Herein, mesoporous structured perovskite devices with various perovskite grain sizes are fabricated by a sequential dropping method, and the charge recombination dynamics is investigated by transient optical-electric measurements. All devices exhibit an overall power conversion efficiency around 15%. More importantly, a biphasic trap-limited charge recombination process is proposed and interpreted by taking into account the specific charge accumulation mechanism in perovskite solar cells. At low Fermi levels, photo-generated electrons predominately populate in the perovskite phase, while at high Fermi levels, most electrons occupy traps in mesoporous TiO2. As a result, the dynamics of charge recombination is, respectively, dominated by the perovskite phase and mesoporous TiO2 in these two cases. The present work would give a new perspective on the charge recombination process in meso-structured perovskite solar cells. PMID:27076212

  11. Highly efficient light management for perovskite solar cells

    PubMed Central

    Wang, Dong-Lin; Cui, Hui-Juan; Hou, Guo-Jiao; Zhu, Zhen-Gang; Yan, Qing-Bo; Su, Gang

    2016-01-01

    Organic-inorganic halide perovskite solar cells have enormous potential to impact the existing photovoltaic industry. As realizing a higher conversion efficiency of the solar cell is still the most crucial task, a great number of schemes were proposed to minimize the carrier loss by optimizing the electrical properties of the perovskite solar cells. Here, we focus on another significant aspect that is to minimize the light loss by optimizing the light management to gain a high efficiency for perovskite solar cells. In our scheme, the slotted and inverted prism structured SiO2 layers are adopted to trap more light into the solar cells, and a better transparent conducting oxide layer is employed to reduce the parasitic absorption. For such an implementation, the efficiency and the serviceable angle of the perovskite solar cell can be promoted impressively. This proposal would shed new light on developing the high-performance perovskite solar cells. PMID:26733112

  12. Highly efficient light management for perovskite solar cells.

    PubMed

    Wang, Dong-Lin; Cui, Hui-Juan; Hou, Guo-Jiao; Zhu, Zhen-Gang; Yan, Qing-Bo; Su, Gang

    2016-01-06

    Organic-inorganic halide perovskite solar cells have enormous potential to impact the existing photovoltaic industry. As realizing a higher conversion efficiency of the solar cell is still the most crucial task, a great number of schemes were proposed to minimize the carrier loss by optimizing the electrical properties of the perovskite solar cells. Here, we focus on another significant aspect that is to minimize the light loss by optimizing the light management to gain a high efficiency for perovskite solar cells. In our scheme, the slotted and inverted prism structured SiO2 layers are adopted to trap more light into the solar cells, and a better transparent conducting oxide layer is employed to reduce the parasitic absorption. For such an implementation, the efficiency and the serviceable angle of the perovskite solar cell can be promoted impressively. This proposal would shed new light on developing the high-performance perovskite solar cells.

  13. Two-Dimensional Layered Oxide Structures Tailored by Self-Assembled Layer Stacking via Interfacial Strain.

    PubMed

    Zhang, Wenrui; Li, Mingtao; Chen, Aiping; Li, Leigang; Zhu, Yuanyuan; Xia, Zhenhai; Lu, Ping; Boullay, Philippe; Wu, Lijun; Zhu, Yimei; MacManus-Driscoll, Judith L; Jia, Quanxi; Zhou, Honghui; Narayan, Jagdish; Zhang, Xinghang; Wang, Haiyan

    2016-07-01

    Study of layered complex oxides emerge as one of leading topics in fundamental materials science because of the strong interplay among intrinsic charge, spin, orbital, and lattice. As a fundamental basis of heteroepitaxial thin film growth, interfacial strain can be used to design materials that exhibit new phenomena beyond their conventional forms. Here, we report a strain-driven self-assembly of bismuth-based supercell (SC) with a two-dimensional (2D) layered structure. With combined experimental analysis and first-principles calculations, we investigated the full SC structure and elucidated the fundamental growth mechanism achieved by the strain-enabled self-assembled atomic layer stacking. The unique SC structure exhibits room-temperature ferroelectricity, enhanced magnetic responses, and a distinct optical bandgap from the conventional double perovskite structure. This study reveals the important role of interfacial strain modulation and atomic rearrangement in self-assembling a layered singe-phase multiferroic thin film, which opens up a promising avenue in the search for and design of novel 2D layered complex oxides with enormous promise. PMID:27295399

  14. Two-Dimensional Layered Oxide Structures Tailored by Self-Assembled Layer Stacking via Interfacial Strain.

    PubMed

    Zhang, Wenrui; Li, Mingtao; Chen, Aiping; Li, Leigang; Zhu, Yuanyuan; Xia, Zhenhai; Lu, Ping; Boullay, Philippe; Wu, Lijun; Zhu, Yimei; MacManus-Driscoll, Judith L; Jia, Quanxi; Zhou, Honghui; Narayan, Jagdish; Zhang, Xinghang; Wang, Haiyan

    2016-07-01

    Study of layered complex oxides emerge as one of leading topics in fundamental materials science because of the strong interplay among intrinsic charge, spin, orbital, and lattice. As a fundamental basis of heteroepitaxial thin film growth, interfacial strain can be used to design materials that exhibit new phenomena beyond their conventional forms. Here, we report a strain-driven self-assembly of bismuth-based supercell (SC) with a two-dimensional (2D) layered structure. With combined experimental analysis and first-principles calculations, we investigated the full SC structure and elucidated the fundamental growth mechanism achieved by the strain-enabled self-assembled atomic layer stacking. The unique SC structure exhibits room-temperature ferroelectricity, enhanced magnetic responses, and a distinct optical bandgap from the conventional double perovskite structure. This study reveals the important role of interfacial strain modulation and atomic rearrangement in self-assembling a layered singe-phase multiferroic thin film, which opens up a promising avenue in the search for and design of novel 2D layered complex oxides with enormous promise.

  15. Tunable room-temperature spin-selective optical Stark effect in solution-processed layered halide perovskites

    PubMed Central

    Giovanni, David; Chong, Wee Kiang; Dewi, Herlina Arianita; Thirumal, Krishnamoorthy; Neogi, Ishita; Ramesh, Ramamoorthy; Mhaisalkar, Subodh; Mathews, Nripan; Sum, Tze Chien

    2016-01-01

    Ultrafast spin manipulation for opto–spin logic applications requires material systems that have strong spin-selective light-matter interaction. Conventional inorganic semiconductor nanostructures [for example, epitaxial II to VI quantum dots and III to V multiple quantum wells (MQWs)] are considered forerunners but encounter challenges such as lattice matching and cryogenic cooling requirements. Two-dimensional halide perovskite semiconductors, combining intrinsic tunable MQW structures and large oscillator strengths with facile solution processability, can offer breakthroughs in this area. We demonstrate novel room-temperature, strong ultrafast spin-selective optical Stark effect in solution-processed (C6H4FC2H4NH3)2PbI4 perovskite thin films. Exciton spin states are selectively tuned by ~6.3 meV using circularly polarized optical pulses without any external photonic cavity (that is, corresponding to a Rabi energy of ~55 meV and equivalent to applying a 70 T magnetic field), which is much larger than any conventional system. The facile halide and organic replacement in these perovskites affords control of the dielectric confinement and thus presents a straightforward strategy for tuning light-matter coupling strength. PMID:27386583

  16. Tunable room-temperature spin-selective optical Stark effect in solution-processed layered halide perovskites.

    PubMed

    Giovanni, David; Chong, Wee Kiang; Dewi, Herlina Arianita; Thirumal, Krishnamoorthy; Neogi, Ishita; Ramesh, Ramamoorthy; Mhaisalkar, Subodh; Mathews, Nripan; Sum, Tze Chien

    2016-06-01

    Ultrafast spin manipulation for opto-spin logic applications requires material systems that have strong spin-selective light-matter interaction. Conventional inorganic semiconductor nanostructures [for example, epitaxial II to VI quantum dots and III to V multiple quantum wells (MQWs)] are considered forerunners but encounter challenges such as lattice matching and cryogenic cooling requirements. Two-dimensional halide perovskite semiconductors, combining intrinsic tunable MQW structures and large oscillator strengths with facile solution processability, can offer breakthroughs in this area. We demonstrate novel room-temperature, strong ultrafast spin-selective optical Stark effect in solution-processed (C6H4FC2H4NH3)2PbI4 perovskite thin films. Exciton spin states are selectively tuned by ~6.3 meV using circularly polarized optical pulses without any external photonic cavity (that is, corresponding to a Rabi energy of ~55 meV and equivalent to applying a 70 T magnetic field), which is much larger than any conventional system. The facile halide and organic replacement in these perovskites affords control of the dielectric confinement and thus presents a straightforward strategy for tuning light-matter coupling strength. PMID:27386583

  17. Effect of metal cation replacement on the electronic structure of metalorganic halide perovskites: Replacement of lead with alkaline-earth metals

    NASA Astrophysics Data System (ADS)

    Pazoki, Meysam; Jacobsson, T. Jesper; Hagfeldt, Anders; Boschloo, Gerrit; Edvinsson, Tomas

    2016-04-01

    Organic and inorganic lead halogen perovskites, and in particular, C H3N H3Pb I3 , have during the last years emerged as a class of highly efficient solar cell materials. Herein we introduce metalorganic halogen perovskite materials for energy-relevant applications based on alkaline-earth metals. Based on the classical notion of Goldschmidt's rules and quantum mechanical considerations, the three alkaline-earth metals, Ca, Sr, and Ba, are shown to be able to exchange lead in the perovskite structure. The three alkaline-earth perovskites, C H3N H3Ca I3,C H3N H3Sr I3 , and C H3N H3Ba I3 , as well as the reference compound, C H3N H3Pb I3 , are in this paper investigated with density functional theory (DFT) calculations, which predict these compounds to exist as stable perovskite materials, and their electronic properties are explored. A detailed analysis of the projected molecular orbital density of states and electronic band structure from DFT calculations were used for interpretation of the band-gap variations in these materials and for estimation of the effective masses of the electrons and holes. Neglecting spin-orbit effects, the band gap of MACa I3,MASr I3 , and MABa I3 were estimated to be 2.95, 3.6, and 3.3 eV, respectively, showing the relative change expected for metal cation exchange. The shifts in the conduction band (CB) edges for the alkaline-earth perovskites were quantified using scalar relativistic DFT calculations and tight-binding analysis, and were compared to the situation in the more extensively studied lead halide perovskite, C H3N H3Pb I3 , where the change in the work function of the metal is the single most important factor in tuning the CB edge and band gap. The results show that alkaline-earth-based organometallic perovskites will not work as an efficient light absorber in photovoltaic applications but instead could be applicable as charge-selective contact materials. The rather high CB edge and the wide band gap together with the large

  18. Computational Study of Structural and Electrical Properties of Methylammonium Lead Iodide Perovskite

    NASA Astrophysics Data System (ADS)

    Boinapally, Vamshidhar Rao

    Methyl ammonium lead iodide perovskite (CH3NH3PbI 3) plays an important role in light absorption in perovskite solar cells. The main aim of this thesis is to investigate the structural and electrical properties of cubic and tetragonal phases of CH3NH3PbI 3. The optimized structure and minimum energy lattice constants of relaxed cubic unit cells were initially computed. The most stable orientation of methylammonium cation was found to be in the [1 1 -1] direction. This directional preference is described by bonding analysis of the atomic cage of PbI3 with the C≡N dimer. The variation of c/a ratio with the distortion angle of PbI6 underlies the understanding of the transition from the cubic to the tetragonal phase. For the equilibrium structures band structures and effective masses were computed. The computed effective masses of both holes and electrons of CH 3NH3PbI3 are comparable to the widely used silicon in commercial inorganic solar cells. These results describe the light absorption nature of methylammonium lead iodide perovskite and its importance in future solar cell technology.

  19. Bifunctional Polymer Nanocomposites as Hole-Transport Layers for Efficient Light Harvesting: Application to Perovskite Solar Cells.

    PubMed

    Wang, Jhong-Yao; Hsu, Fang-Chi; Huang, Jeng-Yeh; Wang, Leeyih; Chen, Yang-Fang

    2015-12-23

    A new approach to largely enhancing light harvesting of solar cells by employing bifunctional polymer nanocomposites as hole-transport layers (HTLs) is proposed. To illustrate our working principle, CH3NH3PbI3-xClx perovskite solar cells are used as examples. Gold nanoparticles (Au-NPs) are added into a conjugated poly(3-hexylthiophene-2,5-diyl) (P3HT) matrix, resulting in a ∼4-fold enhancement in the electrical conductivity and carrier mobility of the native P3HT film. The improved electrical properties are attributed to enhanced polymer chain ordering caused by Au-NPs. By integration of those P3HT:Au-NP films with an optimum loading concentration of 20% into perovskite solar cells as HTLs, this leads to a more than 25% enhancement in the power conversion efficiency (PCE) compared with that of the NP-free one. In addition to the modulated electrical properties of the HTL, the improved performance can also be attributed to the scattering effect from the incorporated Au-NPs, which effectively extends the optical pathway to amplify photon absorption of the photoactive layer. The design principle shown here can be generalized to other organic materials as well, which should be very useful for the further development of high-performance optoelectronic devices.

  20. Solid oxide fuel cell composite cathodes based on perovskite and fluorite structures

    NASA Astrophysics Data System (ADS)

    Sadykov, Vladislav; Mezentseva, Natalia; Usoltsev, Vladimir; Sadovskaya, Ekaterina; Ishchenko, Arkady; Pavlova, Svetlana; Bespalko, Yulia; Kharlamova, Tamara; Zevak, Ekaterina; Salanov, Aleksei; Krieger, Tamara; Belyaev, Vladimir; Bobrenok, Oleg; Uvarov, Nikolai; Okhlupin, Yury; Smorygo, Oleg; Smirnova, Alevtina; Singh, Prabhakar; Vlasov, Aleksandr; Korobeynikov, Mikhail; Bryazgin, Aleksandr; Kalinin, Peter; Arzhannikov, Andrei

    This work presents the results related to the functionally graded fluorite (F)-perovskite (P) nanocomposite cathodes for IT SOFC. Nanocrystalline fluorites (GDC, ScCeSZ) and perovskites (LSrMn, LSrFNi) were synthesized by Pechini method. Nanocomposites were prepared by the ultrasonic dispersion of F and P powders in isopropanol with addition of polyvinyl butyral. Different techniques for deposition and sintering of functionally graded cathode materials were applied including traditional approaches as well as original methods, such as radiation-thermal sintering under electron beam or microwave radiation. Morphology, microstructure and elemental composition of nanocomposites was characterized by XRD and HRTEM/SEM with EDX. Even for dense composites, the sizes of perovskite and fluorite domains remain in the nanorange providing developed P-F interfaces. Oxygen isotope heteroexchange and conductivity/weight relaxation studies demonstrated that these interfaces provide a path for fast oxygen diffusion. The redistribution of the elements between P and F phases in nanocomposites occurs without formation of insulating zirconate phases. Button-size fuel cells with nanocomposite functionally graded cathodes, thin YSZ layers and anode Ni/YSZ cermet (either bulk or supported on Ni-Al foam substrates) were manufactured. For optimized composition and functionally graded design of P-F nanocomposite cathodes, a stable performance in the intermediate temperature range with maximum power density up to 0.5 W cm -2 at 700 °C in wet H 2/air feeds was demonstrated.

  1. Electro-spray deposition of a mesoporous TiO2 charge collection layer: toward large scale and continuous production of high efficiency perovskite solar cells.

    PubMed

    Kim, Min-cheol; Kim, Byeong Jo; Yoon, Jungjin; Lee, Jin-wook; Suh, Dongchul; Park, Nam-gyu; Choi, Mansoo; Jung, Hyun Suk

    2015-12-28

    The spin-coating method, which is widely used for thin film device fabrication, is incapable of large-area deposition or being performed continuously. In perovskite hybrid solar cells using CH(3)NH(3)PbI(3) (MAPbI(3)), large-area deposition is essential for their potential use in mass production. Prior to replacing all the spin-coating process for fabrication of perovskite solar cells, herein, a mesoporous TiO(2) electron-collection layer is fabricated by using the electro-spray deposition (ESD) system. Moreover, impedance spectroscopy and transient photocurrent and photovoltage measurements reveal that the electro-sprayed mesoscopic TiO(2) film facilitates charge collection from the perovskite. The series resistance of the perovskite solar cell is also reduced owing to the highly porous nature of, and the low density of point defects in, the film. An optimized power conversion efficiency of 15.11% is achieved under an illumination of 1 sun; this efficiency is higher than that (13.67%) of the perovskite solar cell with the conventional spin-coated TiO(2) films. Furthermore, the large-area coating capability of the ESD process is verified through the coating of uniform 10 × 10 cm(2) TiO(2) films. This study clearly shows that ESD constitutes therefore a viable alternative for the fabrication of high-throughput, large-area perovskite solar cells.

  2. Parameters Affecting I-V Hysteresis of CH3NH3PbI3 Perovskite Solar Cells: Effects of Perovskite Crystal Size and Mesoporous TiO2 Layer.

    PubMed

    Kim, Hui-Seon; Park, Nam-Gyu

    2014-09-01

    Current-voltage (I-V) characteristics of CH3NH3PbI3 perovskite solar cells are studied using a time-dependent current response with stepwise sweeping of the bias voltage. Compared with the crystalline Si solar cell showing time-independent current at a given bias voltage, the perovskite solar cells exhibit time-dependent current response. The current increases with time and becomes steady at forward scan from short-circuit to open-circuit, whereas it is decayed and saturated with time at reverse scan from open-circuit to short-circuit. Time-dependent current response eventually leads to I-V hysteresis depending on the scan direction and the scan rate. Crystal size of CH3NH3PbI3 and the mesoporous TiO2 (mp-TiO2) film are found to influence I-V hysteresis, where the I-V hysteresis is alleviated as crystal size increases and in the presence of mp-TiO2. The capacitance observed at low frequency (0.1 to 1 Hz), associated with dipole polarization, tends to diminish as size of perovskite and mp-TiO2 layer thickness increases, which suggests that the origin of hysteresis correlates to the capacitive characteristic of CH3NH3PbI3 and the degree of hysteresis depends strongly on perovskite crystal size and mesoporous TiO2 layer.

  3. Room-temperature, solution-processable organic electron extraction layer for high-performance planar heterojunction perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Kim, Jong H.; Chueh, Chu-Chen; Williams, Spencer T.; Jen, Alex K.-Y.

    2015-10-01

    In this work, we describe a room-temperature, solution-processable organic electron extraction layer (EEL) for high-performance planar heterojunction perovskite solar cells (PHJ PVSCs). This EEL is composed of a bilayered fulleropyrrolidinium iodide (FPI)-polyethyleneimine (PEIE) and PC61BM, which yields a promising power conversion efficiency (PCE) of 15.7% with insignificant hysteresis. We reveal that PC61BM can serve as a surface modifier of FPI-PEIE to simultaneously facilitate the crystallization of perovskite and the charge extraction at FPI-PEIE/CH3NH3PbI3 interface. Furthermore, the FPI-PEIE can also tune the work function of ITO and dope PC61BM to promote the efficient electron transport between ITO and PC61BM. Based on the advantages of room-temperature processability and decent electrical property of FPI-PEIE/PC61BM EEL, a high-performance flexible PVSC with a PCE ~10% is eventually demonstrated. This study shows the potential of low-temperature processed organic EEL to replace transition metal oxide-based interlayers for highly printing compatible PVSCs with high-performance.In this work, we describe a room-temperature, solution-processable organic electron extraction layer (EEL) for high-performance planar heterojunction perovskite solar cells (PHJ PVSCs). This EEL is composed of a bilayered fulleropyrrolidinium iodide (FPI)-polyethyleneimine (PEIE) and PC61BM, which yields a promising power conversion efficiency (PCE) of 15.7% with insignificant hysteresis. We reveal that PC61BM can serve as a surface modifier of FPI-PEIE to simultaneously facilitate the crystallization of perovskite and the charge extraction at FPI-PEIE/CH3NH3PbI3 interface. Furthermore, the FPI-PEIE can also tune the work function of ITO and dope PC61BM to promote the efficient electron transport between ITO and PC61BM. Based on the advantages of room-temperature processability and decent electrical property of FPI-PEIE/PC61BM EEL, a high-performance flexible PVSC with a PCE ~10% is

  4. K[sub 1[minus]x]La[sub x]Ca[sub 2[minus]x]Nb[sub 3]O[sub 10], a layered perovskite series with variable interlayer cation density, and LaCaNb[sub 3]O[sub 10], a novel layered perovskite oxide with no interlayer cations

    SciTech Connect

    Uma, S.; Gopalakrishnan, J. )

    1993-02-01

    A series of layered perovskite oxides of the formula K[sub 1[minus]x]La[sub x]Ca[sub 2[minus]x]Nb[sub 3]O[sub 10] for 0 < x [le] 1.0 have been prepared. All the members are isostructural, possessing the structure of KCa[sub 2]Nb[sub 3]O[sub 10]. The interlayer potassium ions in the new series can be ion-exchanged with protons to give H[sub 1[minus]x]La[sub x]Ca[sub 2[minus]x]Nb[sub 3]O[sub 10]. The latter readily forms intercalation compounds of the formula (C[sub n]H[sub 2n+1]NH[sub 3])[sub 1[minus]x]La[sub x]Ca[sub 2[minus]x]Nb[sub 3]O[sub 10], just as the parent solid acid HCa[sub 2]Nb[sub 3]O[sub 10]. The end member LaCaNb[sub 3]O[sub 10] containing no interlayer cations is a nove layered perovskite oxide, being a n = 3 member of the series A[sub n[minus]1]B[sub n]X[sub 3n+1]. 16 refs., 5 figs., 5 tabs.

  5. The Structural Disorder and Lattice Stability of (Ba,Sr)(Co,Fe)O3 Complex Perovskites

    SciTech Connect

    S.N.Rashkeev

    2011-05-01

    The structural disorder and lattice stability of complex perovskite (Ba,Sr)(Co,Fe)O3, a promising cathode material for solid oxide fuel cells and oxygen permeation membranes, is explored by means of first principles DFT calculations. It is predicted that Ba and Sr ions easily exchange their lattice positions (A-cation disorder) similarly to Co and Fe ions (B-cation disorder). The cation antisite defects (exchange of A- and B-type cations) have a relatively high formation energy. The BSCF is predicted to exist in an equilibrium mixture of several phases and can decompose exothermically into the Ba- and Co-rich hexagonal (Ba,Sr)CoO3 and Sr- and Fe-rich cubic (Ba,Sr)FeO3 perovskites.

  6. Lattice dynamics and the nature of structural transitions in organolead halide perovskites

    DOE PAGES

    Comin, Riccardo; Crawford, Michael K.; Said, Ayman H.; Herron, Norman; Guise, William E.; Wang, Xiaoping; Whitfield, Pamela S.; Jain, Ankit; Gong, Xiwen; McGaughey, Alan J. H.; et al

    2016-09-09

    Organolead halide perovskites are a family of hybrid organic-inorganic compounds whose remark- able optoelectronic properties have been under intensive scrutiny in recent years. Here we use inelastic X-ray scattering to study low-energy lattice excitations in single crystals of methylammonium lead iodide and bromide perovskites. Our ndings conrm the displacive nature of the cubic-to- tetragonal phase transition, which is further shown, using neutron and x-ray diraction, to be close to a tricritical point. The experimental sound speed, around 100-200 m/s, suggests that electron- phonon scattering is likely a limiting factor for further improvements in carrier mobility. Lastly, we detect quasistatic symmetry-breakingmore » nanodomains persisting well into the high-temperature cubic phase, possibly stabilized by local defects. These ndings reveal key structural properties of these materials, but also bear important implications for carrier dynamics across an extended temperature range relevant for photovoltaic applications.« less

  7. Highly Efficient, Reproducible, Uniform (CH3 NH3 )PbI3 Layer by Processing Additive Dripping for Solution-Processed Planar Heterojunction Perovskite Solar Cells.

    PubMed

    Kim, Hansol; Jeong, Hanbin; Lee, Jae Kwan

    2016-09-01

    A processing additive dripping (PAD) approach to forming highly efficient (CH3 NH3 )PbI3 (MAPbI3 ) perovskite layers was investigated. A MAPbI3 (CB/DIO) perovskite film fabricated by this approach, which included briefly dripping chlorobenzene incorporating a small amount of diiodooctane (DIO) during casting of a MAPbI3 perovskite precursor dissolved in dimethylformamide, exhibited superior smooth, uniform morphologies with high crystallinity and large grains and revealed completely homogeneous surface coverage. The surface coverage and morphology of the substrate significantly affected the photovoltaic performance of planar heterojunction (PHJ) perovskite solar cells (PrSCs), resulting in a power conversion efficiency of 11.45 % with high open-circuit voltage of 0.91 V and the highest fill factor of 80.87 %. Moreover, the PAD approach could effectively provide efficient MAPbI3 (CB/DIO) perovskite layers for highly efficient, reproducible, uniform PHJ PrSC devices without performance loss or variation even over larger active areas. PMID:27414840

  8. The Interface between FTO and the TiO2 Compact Layer Can Be One of the Origins to Hysteresis in Planar Heterojunction Perovskite Solar Cells.

    PubMed

    Jena, Ajay Kumar; Chen, Hsin-Wei; Kogo, Atsushi; Sanehira, Yoshitaka; Ikegami, Masashi; Miyasaka, Tsutomu

    2015-05-13

    Organometal halide perovskite solar cells have shown rapid rise in power conversion efficiency, and therefore, they have gained enormous attention in the past few years. However, hysteretic photovoltaic characteristics, found in these solid-state devices, have been a major problem. Although it is being proposed that the ferroelectric property of perovskite causes hysteresis in the device, we observed hysteresis in a device made of nonferroelectric PbI2 as a light absorber. This result evidently supports the fact that ferroelectric property cannot be the sole reason for hysteresis. The present study investigates the roles of some key interfaces in a planar heterojunction perovskite (CH3NH3PbI(3-x)Cl(x)) solar cell that can potentially cause hysteresis. The results confirm that the interface between fluorine doped tin oxide (FTO) substrate and the TiO2 compact layer has a definite contribution to hysteresis. Although this interface is one of the origins to hysteresis, we think that other interfaces, especially the interface of the TiO2 compact layer with perovskite, can also play major roles. Nevertheless, the results indicate that hysteresis in such devices can be reduced/eliminated by changing the interlayer between FTO and perovskite.

  9. Nano-structured CuO-Cu2O Complex Thin Film for Application in CH3NH3PbI3 Perovskite Solar Cells

    NASA Astrophysics Data System (ADS)

    Chen, Lung-Chieh; Chen, Cheng-Chiang; Liang, Kai-Chieh; Chang, Sheng Hsiung; Tseng, Zhong-Liang; Yeh, Shih-Chieh; Chen, Chin-Ti; Wu, Wen-Ti; Wu, Chun-Guey

    2016-09-01

    Nano-structured CuO-Cu2O complex thin film-based perovskite solar cells were fabricated on an indium tin oxide (ITO)-coated glass and studied. Copper (Cu) thin films with a purity of 99.995 % were deposited on an ITO-coated glass by magnetron reactive sputtering. To optimize the properties of the nano-structured CuO-Cu2O complex thin films, the deposited Cu thin films were thermally oxidized at various temperatures from 300 to 400 °C. A CH3NH3PbI3 perovskite absorber was fabricated on top of CuO-Cu2O complex thin film by a one-step spin-coating process with a toluene washing treatment. Following optimization, the maximum power conversion efficiency (PCE) exceeded 8.1 %. Therefore, the low-cost, solution-processed, stable nano-structured CuO-Cu2O complex thin film can be used as an alternative hole transport layer (HTL) in industrially produced perovskite solar cells.

  10. Nano-structured CuO-Cu2O Complex Thin Film for Application in CH3NH3PbI3 Perovskite Solar Cells.

    PubMed

    Chen, Lung-Chieh; Chen, Cheng-Chiang; Liang, Kai-Chieh; Chang, Sheng Hsiung; Tseng, Zhong-Liang; Yeh, Shih-Chieh; Chen, Chin-Ti; Wu, Wen-Ti; Wu, Chun-Guey

    2016-12-01

    Nano-structured CuO-Cu2O complex thin film-based perovskite solar cells were fabricated on an indium tin oxide (ITO)-coated glass and studied. Copper (Cu) thin films with a purity of 99.995 % were deposited on an ITO-coated glass by magnetron reactive sputtering. To optimize the properties of the nano-structured CuO-Cu2O complex thin films, the deposited Cu thin films were thermally oxidized at various temperatures from 300 to 400 °C. A CH3NH3PbI3 perovskite absorber was fabricated on top of CuO-Cu2O complex thin film by a one-step spin-coating process with a toluene washing treatment. Following optimization, the maximum power conversion efficiency (PCE) exceeded 8.1 %. Therefore, the low-cost, solution-processed, stable nano-structured CuO-Cu2O complex thin film can be used as an alternative hole transport layer (HTL) in industrially produced perovskite solar cells. PMID:27637894

  11. Thermal evolution of the crystal structure of the orthorhombic perovskite LaFeO{sub 3}

    SciTech Connect

    Dixon, Charlotte A.L.; Kavanagh, Christopher M.; Knight, Kevin S.; Kockelmann, Winfried; Morrison, Finlay D.; Lightfoot, Philip

    2015-10-15

    The thermal evolution of the crystal structure of the prototypical orthorhombic perovskite LaFeO{sub 3} has been studied in detail by powder neutron diffraction in the temperature range 25perovskite LaFeO{sub 3} is rationalized from a detailed powder neutron diffraction study. - Highlights: • Crystal structure of the perovskite LaFeO{sub 3} studied in detail by powder neutron diffraction. • Unusual thermal evolution of lattice metrics rationalized. • Contrasting behavior to Bi-doped LaFeO{sub 3}. • Octahedral distortion/tilt parameters explain unusual a and c lattice parameter behavior.

  12. CaTiO.sub.3 Interfacial template structure on semiconductor-based material and the growth of electroceramic thin-films in the perovskite class

    DOEpatents

    McKee, Rodney Allen; Walker, Frederick Joseph

    1998-01-01

    A structure including a film of a desired perovskite oxide which overlies and is fully commensurate with the material surface of a semiconductor-based substrate and an associated process for constructing the structure involves the build up of an interfacial template film of perovskite between the material surface and the desired perovskite film. The lattice parameters of the material surface and the perovskite of the template film are taken into account so that during the growth of the perovskite template film upon the material surface, the orientation of the perovskite of the template is rotated 45.degree. with respect to the orientation of the underlying material surface and thereby effects a transition in the lattice structure from fcc (of the semiconductor-based material) to the simple cubic lattice structure of perovskite while the fully commensurate periodicity between the perovskite template film and the underlying material surface is maintained. The film-growth techniques of the invention can be used to fabricate solid state electrical components wherein a perovskite film is built up upon a semiconductor-based material and the perovskite film is adapted to exhibit ferroelectric, piezoelectric, pyroelectric, electro-optic or large dielectric properties during use of the component.

  13. Synthesis, crystal structure and magnetic properties of a new pillared perovskite La{sub 5}Mo{sub 2.75}V{sub 1.25}O{sub 16}

    SciTech Connect

    Ramezanipour, Farshid; Derakhshan, Shahab; Greedan, John E. Cranswick, Lachlan M.D.

    2008-12-15

    A new pillared perovskite compound La{sub 5}Mo{sub 2.76(4)}V{sub 1.25(4)}O{sub 16}, has been synthesized by solid-state reaction and its crystal structure has been characterized using powder X-ray and neutron diffraction. The magnetic properties of this compound have been investigated using SQUID magnetometry, and the magnetic structure has been studied using neutron diffraction data. A theoretical calculation of relative strengths of spin interactions among different magnetic ions and through different pathways has been performed using extended Hueckel, spin dimer analysis. The crystal structure of this material contains perovskite-type layers that are connected through edge-sharing dimeric units of octahedra. The structure is described in space group C2/m with unit cell parameters a=7.931(2) A, b=7.913(2) A, c=10.346(5) A and {beta}=95.096(5){sup o}. The material shows both short-range ferrimagnetic correlations from {approx}200 to 110 K and long-range antiferromagnetic order below T{sub c}{approx}100 K. The magnetic structure was investigated by neutron diffraction and is described by k=(0 0 1/2 ) as for other pillared perovskites. It consists of a ferrimagnetic arrangement of Mo and V within the layers that are coupled antiferromagnetically between layers. This is the first magnetic structure determination for any Mo-based pillared perovskite. - Graphical abstract: Long-range magnetic order below 100 K in the pillared perovskite La{sub 5}Mo{sub 2.75}V{sub 1.25}O{sub 16}. The magnetic structure is shown in the inset.

  14. Molecularly Engineered Organic-Inorganic Hybrid Perovskite with Multiple Quantum Well Structure for Multicolored Light-Emitting Diodes.

    PubMed

    Hu, Hongwei; Salim, Teddy; Chen, Bingbing; Lam, Yeng Ming

    2016-01-01

    Organic-inorganic hybrid perovskites have the potential to be used as a new class of emitters with tunable emission, high color purity and good ease of fabrication. Recent studies have so far been focused on three-dimensional (3D) perovskites, such as CH3NH3PbBr3 and CH3NH3PbI3 for green and infrared emission. Here, we explore a new series of hybrid perovskite emitters with a general formula of (C4H9NH3)2(CH3NH3)n-1PbnI3n+1 (where n = 1, 2, 3), which possesses a multiple quantum well structure. The quantum well thickness of these materials is adjustable through simple molecular engineering which results in a continuously tunable bandgap and emission spectra. Deep saturated red emission was obtained with a peak external quantum efficiency of 2.29% and a maximum luminance of 214 cd/m(2). Green and blue LEDs were also demonstrated through halogen substitutions in these hybrid perovskites. We expect these results to open up the way towards high performance perovskite LEDs through molecular-structure engineering of these perovskite emitters. PMID:27633084

  15. Molecularly Engineered Organic-Inorganic Hybrid Perovskite with Multiple Quantum Well Structure for Multicolored Light-Emitting Diodes

    PubMed Central

    Hu, Hongwei; Salim, Teddy; Chen, Bingbing; Lam, Yeng Ming

    2016-01-01

    Organic-inorganic hybrid perovskites have the potential to be used as a new class of emitters with tunable emission, high color purity and good ease of fabrication. Recent studies have so far been focused on three-dimensional (3D) perovskites, such as CH3NH3PbBr3 and CH3NH3PbI3 for green and infrared emission. Here, we explore a new series of hybrid perovskite emitters with a general formula of (C4H9NH3)2(CH3NH3)n−1PbnI3n+1 (where n = 1, 2, 3), which possesses a multiple quantum well structure. The quantum well thickness of these materials is adjustable through simple molecular engineering which results in a continuously tunable bandgap and emission spectra. Deep saturated red emission was obtained with a peak external quantum efficiency of 2.29% and a maximum luminance of 214 cd/m2. Green and blue LEDs were also demonstrated through halogen substitutions in these hybrid perovskites. We expect these results to open up the way towards high performance perovskite LEDs through molecular-structure engineering of these perovskite emitters. PMID:27633084

  16. Molecularly Engineered Organic-Inorganic Hybrid Perovskite with Multiple Quantum Well Structure for Multicolored Light-Emitting Diodes

    NASA Astrophysics Data System (ADS)

    Hu, Hongwei; Salim, Teddy; Chen, Bingbing; Lam, Yeng Ming

    2016-09-01

    Organic-inorganic hybrid perovskites have the potential to be used as a new class of emitters with tunable emission, high color purity and good ease of fabrication. Recent studies have so far been focused on three-dimensional (3D) perovskites, such as CH3NH3PbBr3 and CH3NH3PbI3 for green and infrared emission. Here, we explore a new series of hybrid perovskite emitters with a general formula of (C4H9NH3)2(CH3NH3)n‑1PbnI3n+1 (where n = 1, 2, 3), which possesses a multiple quantum well structure. The quantum well thickness of these materials is adjustable through simple molecular engineering which results in a continuously tunable bandgap and emission spectra. Deep saturated red emission was obtained with a peak external quantum efficiency of 2.29% and a maximum luminance of 214 cd/m2. Green and blue LEDs were also demonstrated through halogen substitutions in these hybrid perovskites. We expect these results to open up the way towards high performance perovskite LEDs through molecular-structure engineering of these perovskite emitters.

  17. Molecularly Engineered Organic-Inorganic Hybrid Perovskite with Multiple Quantum Well Structure for Multicolored Light-Emitting Diodes.

    PubMed

    Hu, Hongwei; Salim, Teddy; Chen, Bingbing; Lam, Yeng Ming

    2016-09-16

    Organic-inorganic hybrid perovskites have the potential to be used as a new class of emitters with tunable emission, high color purity and good ease of fabrication. Recent studies have so far been focused on three-dimensional (3D) perovskites, such as CH3NH3PbBr3 and CH3NH3PbI3 for green and infrared emission. Here, we explore a new series of hybrid perovskite emitters with a general formula of (C4H9NH3)2(CH3NH3)n-1PbnI3n+1 (where n = 1, 2, 3), which possesses a multiple quantum well structure. The quantum well thickness of these materials is adjustable through simple molecular engineering which results in a continuously tunable bandgap and emission spectra. Deep saturated red emission was obtained with a peak external quantum efficiency of 2.29% and a maximum luminance of 214 cd/m(2). Green and blue LEDs were also demonstrated through halogen substitutions in these hybrid perovskites. We expect these results to open up the way towards high performance perovskite LEDs through molecular-structure engineering of these perovskite emitters.

  18. Topotactic synthesis of strontium cobalt oxyhydride thin film with perovskite structure

    SciTech Connect

    Katayama, Tsukasa; Chikamatsu, Akira Kamisaka, Hideyuki; Yokoyama, Yuichi; Hirata, Yasuyuki; Wadati, Hiroki; Fukumura, Tomoteru; Hasegawa, Tetsuya

    2015-10-15

    The substitution of hydride anions (H{sup −}) into transition metal oxides has recently become possible through topotactic reactions or high-pressure synthesis methods. However, the fabrication of oxyhydrides is still difficult because of their inherently less-stable frameworks. In this study, we successfully fabricated perovskite SrCoO{sub x}H{sub y} thin films via the topotactic hydride doping of brownmillerite SrCoO{sub 2.5} epitaxial thin films with CaH{sub 2}. The perovskite-type cation framework was maintained during the topotactic treatment owing to epitaxial stabilization. Structural and chemical analyses accompanied by X-ray absorption spectroscopy measurements revealed that the doped hydride ions form a two-dimensional network of Co-H{sup −}-Co bonds, in contrast to other reported perovskite oxyhydrides, SrMO{sub 3−x}H{sub x} (M = Cr, Ti, V). The SrCoO{sub x}H{sub y} thin film exhibited insulating behavior and had a direct band gap of 2.1 eV. Thus, topotactic hydride doping of transition-metal-oxide thin films on suitable substrates is a promising method for the synthesis of new transition metal oxyhydrides.

  19. Crystal structure of post-perovskite-type CaIrO3 reinvestigated: new insights into atomic thermal vibration behaviors

    PubMed Central

    Nakatsuka, Akihiko; Sugiyama, Kazumasa; Yoneda, Akira; Fujiwara, Keiko; Yoshiasa, Akira

    2015-01-01

    Single crystals of the title compound, the post-perovskite-type CaIrO3 [calcium iridium(IV) trioxide], have been grown from a CaCl2 flux at atmospheric pressure. The crystal structure consists of an alternate stacking of IrO6 octa­hedral layers and CaO8 hendeca­hedral layers along [010]. Chains formed by edge-sharing of IrO6 octa­hedra (point-group symmetry 2/m..) run along [100] and are inter­connected along [001] by sharing apical O atoms to build up the IrO6 octa­hedral layers. Chains formed by face-sharing of CaO8 hendeca­hedra (point-group symmetry m2m) run along [100] and are inter­connected along [001] by edge-sharing to build up the CaO8 hendeca­hedral layers. The IrO6 octa­hedral layers and CaO8 hendeca­hedral layers are inter­connected by sharing edges. The present structure refinement using a high-power X-ray source confirms the atomic positions determined by Hirai et al. (2009 ▸) [Z. Kristallogr. 224, 345–350], who had revised our previous report [Sugahara et al. (2008 ▸). Am. Mineral. 93, 1148–1152]. However, the displacement ellipsoids of the Ir and Ca atoms based on the present refinement can be approximated as uniaxial ellipsoids elongating along [100], unlike those reported by Hirai et al. (2009 ▸). This suggests that the thermal vibrations of the Ir and Ca atoms are mutually suppressed towards the Ir⋯Ca direction across the shared edge because of the dominant repulsion between the two atoms. PMID:26396860

  20. Crystal structure of post-perovskite-type CaIrO3 reinvestigated: new insights into atomic thermal vibration behaviors.

    PubMed

    Nakatsuka, Akihiko; Sugiyama, Kazumasa; Yoneda, Akira; Fujiwara, Keiko; Yoshiasa, Akira

    2015-09-01

    Single crystals of the title compound, the post-perovskite-type CaIrO3 [calcium iridium(IV) trioxide], have been grown from a CaCl2 flux at atmospheric pressure. The crystal structure consists of an alternate stacking of IrO6 octa-hedral layers and CaO8 hendeca-hedral layers along [010]. Chains formed by edge-sharing of IrO6 octa-hedra (point-group symmetry 2/m..) run along [100] and are inter-connected along [001] by sharing apical O atoms to build up the IrO6 octa-hedral layers. Chains formed by face-sharing of CaO8 hendeca-hedra (point-group symmetry m2m) run along [100] and are inter-connected along [001] by edge-sharing to build up the CaO8 hendeca-hedral layers. The IrO6 octa-hedral layers and CaO8 hendeca-hedral layers are inter-connected by sharing edges. The present structure refinement using a high-power X-ray source confirms the atomic positions determined by Hirai et al. (2009 ▸) [Z. Kristallogr. 224, 345-350], who had revised our previous report [Sugahara et al. (2008 ▸). Am. Mineral. 93, 1148-1152]. However, the displacement ellipsoids of the Ir and Ca atoms based on the present refinement can be approximated as uniaxial ellipsoids elongating along [100], unlike those reported by Hirai et al. (2009 ▸). This suggests that the thermal vibrations of the Ir and Ca atoms are mutually suppressed towards the Ir⋯Ca direction across the shared edge because of the dominant repulsion between the two atoms.

  1. Low-spin Fe[superscript 2+] in silicate perovskite and a possible layer at the base of the lower mantle

    SciTech Connect

    McCammon, C.; Dubrovinsky, L.; Narygina, O.; Kantor, I.; Wu, X.; Glazyrin, K.; Sergueev, I.; Chumakov, A.I.

    2010-08-04

    We investigated the spin state of iron in Mg{sub 0.82}Fe{sub 0.18}SiO{sub 3} silicate perovskite using Moessbauer spectroscopy and nuclear forward scattering (NFS) at pressures up to 130 GPa and temperatures up to 1000 K. Majorite starting material was loaded into diamond anvil cells in three separate experiments, and transformed to silicate perovskite through laser heating. We found, in agreement with previous work, the predominance of a component with high isomer shift ({approx}1 mm/s relative to {alpha}-Fe) and high-quadrupole splitting (QS) (>4 mm/s) in Moessbauer and NFS spectra up to 115 GPa at room temperature, and in accordance with previous work this component was assigned to intermediate-spin Fe{sup 2+}. At higher pressures, the intensity of the high QS component in the silicate perovskite spectrum decreased, while the intensity of a new component with low isomer shift ({approx}0 mm/s relative to {alpha}-Fe) and low quadrupole splitting (<0.5 mm/s) increased. This new component was assigned to low-spin Fe{sup 2+}, and its intensity increased with both increasing pressure and increasing temperature: at 120 GPa and 1000 K all Fe{sup 2+} was in the low-spin state. X-ray diffraction data showed well crystallized perovskite in all runs, and although the stable phase above 110 GPa is expected to be post-perovskite, sluggish transition kinetics likely preserved the perovskite phase in a metastable state. Our results combined with data in the literature and thermodynamic and topological considerations suggest that there may be a region where silicate perovskite containing low-spin Fe{sup 2+} is stable, which coincides with predicted pressure-temperature conditions near the D{double_prime} layer.

  2. Scalable fabrication of efficient organolead trihalide perovskite solar cells with doctor-bladed active layers

    SciTech Connect

    Deng, Yehao; Peng, Edwin; Shao, Yuchuan; Xiao, Zhengguo; Dong, Qingfeng; Huang, Jinsong

    2015-03-25

    Organolead trihalide perovskites (OTPs) are nature abundant materials with prospects as future low-cost renewable energy sources boosted by the solution process capability of these materials. Here we report the fabrication of efficient OTP devices by a simple, high throughput and low-cost doctor-blade coating process which can be compatible with the roll-to-roll fabrication process for the large scale production of perovskite solar cell panels. The formulation of appropriate precursor inks by removing impurities is shown to be critical in the formation of continuous, pin-hole free and phase-pure perovskite films on large area substrates, which is assisted by a high deposition temperature to guide the nucleation and grain growth process. The domain size reached 80–250 μm in 1.5–2 μm thick bladed films. By controlling the stoichiometry and thickness of the OTP films, highest device efficiencies of 12.8% and 15.1% are achieved in the devices fabricated on poly(3,4-ethylenedioxythiophene) polystyrene sulfonate and cross-linked N4,N4'-bis(4-(6-((3-ethyloxetan-3-yl)methoxy)hexyl)phenyl)–N4,N4'-diphenylbiphenyl-4,4'-diamine covered ITO substrates. Furthermore, the carrier diffusion length in doctor-bladed OTP films is beyond 3.5 μm which is significantly larger than in the spin-coated films, due to the formation of crystalline grains with a very large size by the doctor-blade coating method.

  3. Scalable fabrication of efficient organolead trihalide perovskite solar cells with doctor-bladed active layers

    DOE PAGES

    Deng, Yehao; Peng, Edwin; Shao, Yuchuan; Xiao, Zhengguo; Dong, Qingfeng; Huang, Jinsong

    2015-03-25

    Organolead trihalide perovskites (OTPs) are nature abundant materials with prospects as future low-cost renewable energy sources boosted by the solution process capability of these materials. Here we report the fabrication of efficient OTP devices by a simple, high throughput and low-cost doctor-blade coating process which can be compatible with the roll-to-roll fabrication process for the large scale production of perovskite solar cell panels. The formulation of appropriate precursor inks by removing impurities is shown to be critical in the formation of continuous, pin-hole free and phase-pure perovskite films on large area substrates, which is assisted by a high deposition temperaturemore » to guide the nucleation and grain growth process. The domain size reached 80–250 μm in 1.5–2 μm thick bladed films. By controlling the stoichiometry and thickness of the OTP films, highest device efficiencies of 12.8% and 15.1% are achieved in the devices fabricated on poly(3,4-ethylenedioxythiophene) polystyrene sulfonate and cross-linked N4,N4'-bis(4-(6-((3-ethyloxetan-3-yl)methoxy)hexyl)phenyl)–N4,N4'-diphenylbiphenyl-4,4'-diamine covered ITO substrates. Furthermore, the carrier diffusion length in doctor-bladed OTP films is beyond 3.5 μm which is significantly larger than in the spin-coated films, due to the formation of crystalline grains with a very large size by the doctor-blade coating method.« less

  4. Single step deposition of an interacting layer of a perovskite matrix with embedded quantum dots

    NASA Astrophysics Data System (ADS)

    Ngo, Thi Tuyen; Suarez, Isaac; Sanchez, Rafael S.; Martinez-Pastor, Juan P.; Mora-Sero, Ivan

    2016-07-01

    Hybrid lead halide perovskite (PS) derivatives have emerged as very promising materials for the development of optoelectronic devices in the last few years. At the same time, inorganic nanocrystals with quantum confinement (QDs) possess unique properties that make them suitable materials for the development of photovoltaics, imaging and lighting applications, among others. In this work, we report on a new methodology for the deposition of high quality, large grain size and pinhole free PS films (CH3NH3PbI3) with embedded PbS and PbS/CdS core/shell Quantum Dots (QDs). The strong interaction between both semiconductors is revealed by the formation of an exciplex state, which is monitored by photoluminescence and electroluminescence experiments. The radiative exciplex relaxation is centered in the near infrared region (NIR), ~1200 nm, which corresponds to lower energies than the corresponding band gap of both perovskite (PS) and QDs. Our approach allows the fabrication of multi-wavelength light emitting diodes (LEDs) based on a PS matrix with embedded QDs, which show considerably low turn-on potentials. The presence of the exciplex state of PS and QDs opens up a broad range of possibilities with important implications in both LEDs and solar cells.Hybrid lead halide perovskite (PS) derivatives have emerged as very promising materials for the development of optoelectronic devices in the last few years. At the same time, inorganic nanocrystals with quantum confinement (QDs) possess unique properties that make them suitable materials for the development of photovoltaics, imaging and lighting applications, among others. In this work, we report on a new methodology for the deposition of high quality, large grain size and pinhole free PS films (CH3NH3PbI3) with embedded PbS and PbS/CdS core/shell Quantum Dots (QDs). The strong interaction between both semiconductors is revealed by the formation of an exciplex state, which is monitored by photoluminescence and

  5. Identifying the Molecular Structures of Intermediates for Optimizing the Fabrication of High-Quality Perovskite Films.

    PubMed

    Cao, Jing; Jing, Xiaojing; Yan, Juanzhu; Hu, Chengyi; Chen, Ruihao; Yin, Jun; Li, Jing; Zheng, Nanfeng

    2016-08-10

    During the past two years, the introduction of DMSO has revolutionized the fabrication of high-quality pervoskite MAPbI3 (MA = CH3NH3) films for solar cell applications. In the developed DMSO process, the formation of (MA)2Pb3I8·2DMSO (shorted as Pb3I8) has well recognized as a critical factor to prepare high-quality pervoskite films and thus accomplish excellent performances in perovskite solar cells. However, Pb3I8 is an I-deficient intermediate and must further react with methylammonium iodide (MAI) to be fully converted into MAPbI3. By capturing and solving the molecular structures of several intermediates involved in the fabrication of perovskite films, we report in this work that the importance of DMSO is NOT due to the formation of Pb3I8. The use of different PbI2-DMSO ratios leads to two different structures of PbI2-DMSO precursors (PbI2·DMSO and PbI2·2DMSO), thus dramatically influencing the quality of fabricated perovskite films. However, such an influence can be minimized when the PbI2-DMSO precursor films are thermally treated to create mesoporous PbI2 films before reacting with MAI. Such a development makes the fabrication of high-quality pervoskite films highly reproducible without the need to precisely control the PbI2:DMSO ratio. Moreover, the formation of ionic compound (MA)4PbI6 is observed when excess MAI is used in the preparation of perovskite film. This I-rich phase heavily induces the hysteresis in PSCs, but is readily removed by isopropanol treatment. On the basis of all these findings, we develop a new effective protocol to fabricate high-performance PSCs. In the new protocol, high-quality perovskite films are prepared by simply treating the mesoporous PbI2 films (made from PbI2-DMSO precursors) with an isopropanol solution of MAI, followed by isopropanol washing. The best efficiency of fabricated MAPbI3 PSCs is up to 19.0%. As compared to the previously reported DMSO method, the devices fabricated by the method reported in this work

  6. Magnetization and magneto-transport staircaselike behavior in layered perovskite Sr2CoO4 at low temperature

    NASA Astrophysics Data System (ADS)

    Li, Qiuhang; Yuan, Xueping; Xing, Lei; Xu, Mingxiang

    2016-06-01

    Polycrystalline layered perovskite Sr2CoO4 sample was synthesized by high temperature and high pressure method. The staircaselike behavior has been observed in the magnetization and resistivity versus field curves of Sr2CoO4 at low temperature. The main features of the steps can be obtained from the measured results: (i) the positions of the external magnetic field at which steps occur are varying in different measurement runs, (ii) the steps only appear at low temperature and disappear with a slight increase of the temperature, (iii) the steps are dependent on the temperature and field sweep rate. Based on the features of the magnetization and magneto-transport staircaselike behavior in Sr2CoO4, the unusual phenomenon can be ascribed to an avalanche of flipping domains in terms of the random field theory.

  7. Magnetization and magneto-transport staircaselike behavior in layered perovskite Sr2CoO4 at low temperature.

    PubMed

    Li, Qiuhang; Yuan, Xueping; Xing, Lei; Xu, Mingxiang

    2016-06-13

    Polycrystalline layered perovskite Sr2CoO4 sample was synthesized by high temperature and high pressure method. The staircaselike behavior has been observed in the magnetization and resistivity versus field curves of Sr2CoO4 at low temperature. The main features of the steps can be obtained from the measured results: (i) the positions of the external magnetic field at which steps occur are varying in different measurement runs, (ii) the steps only appear at low temperature and disappear with a slight increase of the temperature, (iii) the steps are dependent on the temperature and field sweep rate. Based on the features of the magnetization and magneto-transport staircaselike behavior in Sr2CoO4, the unusual phenomenon can be ascribed to an avalanche of flipping domains in terms of the random field theory.

  8. Synthesis and thermal stability studies of a series of metastable Dion-Jacobson double-layered neodymium-niobate perovskites

    NASA Astrophysics Data System (ADS)

    Josepha, Elisha A.; Farooq, Sara; Mitchell, Cinnamon M.; Wiley, John B.

    2014-08-01

    The Dion-Jacobson double-layered perovskite, RbNdNb2O7, is used as a precursor to synthesize the series ANdNb2O7 (A=H, Li, Na, K, NH4, Ag), and (MCl)NdNb2O7 (M=Mn, Fe, Cu) through ion-exchange reactions ≤400 °C. Thermal stability studies indicated that most of these compounds are metastable. A combination of X-ray powder diffraction and differential thermal analysis were used to determine various low temperature decomposition pathways; these pathways were very dependent on the interlayer species. Overall the ANdNb2O7 series was found to be less stable than the corresponding lanthanides, ALaNb2O7.

  9. Magnetization and magneto-transport staircaselike behavior in layered perovskite Sr2CoO4 at low temperature

    PubMed Central

    Li, Qiuhang; Yuan, Xueping; Xing, Lei; Xu, Mingxiang

    2016-01-01

    Polycrystalline layered perovskite Sr2CoO4 sample was synthesized by high temperature and high pressure method. The staircaselike behavior has been observed in the magnetization and resistivity versus field curves of Sr2CoO4 at low temperature. The main features of the steps can be obtained from the measured results: (i) the positions of the external magnetic field at which steps occur are varying in different measurement runs, (ii) the steps only appear at low temperature and disappear with a slight increase of the temperature, (iii) the steps are dependent on the temperature and field sweep rate. Based on the features of the magnetization and magneto-transport staircaselike behavior in Sr2CoO4, the unusual phenomenon can be ascribed to an avalanche of flipping domains in terms of the random field theory. PMID:27293142

  10. Magnetization and magneto-transport staircaselike behavior in layered perovskite Sr2CoO4 at low temperature.

    PubMed

    Li, Qiuhang; Yuan, Xueping; Xing, Lei; Xu, Mingxiang

    2016-01-01

    Polycrystalline layered perovskite Sr2CoO4 sample was synthesized by high temperature and high pressure method. The staircaselike behavior has been observed in the magnetization and resistivity versus field curves of Sr2CoO4 at low temperature. The main features of the steps can be obtained from the measured results: (i) the positions of the external magnetic field at which steps occur are varying in different measurement runs, (ii) the steps only appear at low temperature and disappear with a slight increase of the temperature, (iii) the steps are dependent on the temperature and field sweep rate. Based on the features of the magnetization and magneto-transport staircaselike behavior in Sr2CoO4, the unusual phenomenon can be ascribed to an avalanche of flipping domains in terms of the random field theory. PMID:27293142

  11. The effect of ALD-Zno layers on the formation of CH₃NH₃PbI₃ with different perovskite precursors and sintering temperatures.

    PubMed

    Dong, Xu; Hu, Hongwei; Lin, Bencai; Ding, Jianning; Yuan, Ningyi

    2014-11-28

    ZnO films deposited by atomic layer deposition at 70 °C were used to fabricate perovskite solar cells, and a conversion efficiency of 13.1% was obtained. On the ZnO layer, CH3NH3PbI3 was formed at room temperature using CH3NH3I and PbCl2 precursors, which is in contrast to the reported results.

  12. Room-Temperature Solution-Processed NiOx:PbI2 Nanocomposite Structures for Realizing High-Performance Perovskite Photodetectors.

    PubMed

    Zhu, Hugh Lu; Cheng, Jiaqi; Zhang, Di; Liang, Chunjun; Reckmeier, Claas J; Huang, He; Rogach, Andrey L; Choy, Wallace C H

    2016-07-26

    While methylammonium lead iodide (MAPbI3) with interesting properties, such as a direct band gap, high and well-balanced electron/hole mobilities, as well as long electron/hole diffusion length, is a potential candidate to become the light absorbers in photodetectors, the challenges for realizing efficient perovskite photodetectors are to suppress dark current, to increase linear dynamic range, and to achieve high specific detectivity and fast response speed. Here, we demonstrate NiOx:PbI2 nanocomposite structures, which can offer dual roles of functioning as an efficient hole extraction layer and favoring the formation of high-quality MAPbI3 to address these challenges. We introduce a room-temperature solution process to form the NiOx:PbI2 nanocomposite structures. The nanocomposite structures facilitate the growth of the compact and ordered MAPbI3 crystalline films, which is essential for efficient photodetectors. Furthermore, the nanocomposite structures work as an effective hole extraction layer, which provides a large electron injection barrier and favorable hole extraction as well as passivates the surface of the perovskite, leading to suppressed dark current and enhanced photocurrent. By optimizing the NiOx:PbI2 nanocomposite structures, a low dark current density of 2 × 10(-10) A/cm(2) at -200 mV and a large linear dynamic range of 112 dB are achieved. Meanwhile, a high responsivity in the visible spectral range of 450-750 nm, a large measured specific detectivity approaching 10(13) Jones, and a fast fall time of 168 ns are demonstrated. The high-performance perovskite photodetectors demonstrated here offer a promising candidate for low-cost and high-performance near-ultraviolet-visible photodetection. PMID:27340899

  13. Single step deposition of an interacting layer of a perovskite matrix with embedded quantum dots.

    PubMed

    Ngo, Thi Tuyen; Suarez, Isaac; Sanchez, Rafael S; Martinez-Pastor, Juan P; Mora-Sero, Ivan

    2016-08-14

    Hybrid lead halide perovskite (PS) derivatives have emerged as very promising materials for the development of optoelectronic devices in the last few years. At the same time, inorganic nanocrystals with quantum confinement (QDs) possess unique properties that make them suitable materials for the development of photovoltaics, imaging and lighting applications, among others. In this work, we report on a new methodology for the deposition of high quality, large grain size and pinhole free PS films (CH3NH3PbI3) with embedded PbS and PbS/CdS core/shell Quantum Dots (QDs). The strong interaction between both semiconductors is revealed by the formation of an exciplex state, which is monitored by photoluminescence and electroluminescence experiments. The radiative exciplex relaxation is centered in the near infrared region (NIR), ≈1200 nm, which corresponds to lower energies than the corresponding band gap of both perovskite (PS) and QDs. Our approach allows the fabrication of multi-wavelength light emitting diodes (LEDs) based on a PS matrix with embedded QDs, which show considerably low turn-on potentials. The presence of the exciplex state of PS and QDs opens up a broad range of possibilities with important implications in both LEDs and solar cells. PMID:27437778

  14. The electronic structure of metal oxide/organo metal halide perovskite junctions in perovskite based solar cells

    PubMed Central

    Dymshits, Alex; Henning, Alex; Segev, Gideon; Rosenwaks, Yossi; Etgar, Lioz

    2015-01-01

    Cross-sections of a hole-conductor-free CH3NH3PbI3 perovskite solar cell were characterized with Kelvin probe force microscopy. A depletion region width of about 45 nm was determined from the measured potential profiles at the interface between CH3NH3PbI3 and nanocrystalline TiO2, whereas a negligible depletion was measured at the CH3NH3PbI3/Al2O3 interface. A complete solar cell can be realized with the CH3NH3PbI3 that functions both as light harvester and hole conductor in combination with a metal oxide. The band diagrams were estimated from the measured potential profile at the interfaces, and are critical findings for a better understanding and further improvement of perovskite based solar cells. PMID:25731963

  15. Application of mesoporous SiO2 layer as an insulating layer in high performance hole transport material free CH3NH3PbI3 perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Cheng, Nian; Liu, Pei; Bai, Sihang; Yu, Zhenhua; Liu, Wei; Guo, Shi-Shang; Zhao, Xing-Zhong

    2016-07-01

    A mesoporous SiO2 layer is successfully introduced into the hole transport material free perovskite solar cells by spin-coating a SiO2 paste onto the TiO2 scaffold layer. This SiO2 layer can act as an insulating layer and effectively inhibit the charge recombination between the TiO2 layer and carbon electrode. The variation of power conversion efficiencies with the thickness of SiO2 layer is studied here. Under optimized SiO2 thickness, perovskite solar cell fabricated on the TiO2/SiO2 film shows a superior power conversion efficiency of ∼12% and exhibits excellent long time stability for 30 days.

  16. Modeling of optical losses in perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Taghavi, M. Javad; Houshmand, Mohammad; Zandi, M. Hossein; Gorji, Nima E.

    2016-09-01

    The optical losses within the structure of hybrid perovskite solar cells are investigated using only the optical properties of each layer e.g. refractive index and extinction coefficient. This model allows calculating the transmission/reflection rates at the interfaces and absorption loss within any layer. Then, the short circuit current density and loss percentage are calculated versus the perovskite and TiO2 thicknesses from 50 nm to 150 nm. To make our calculations closer to reality, we extracted the optical properties of each device component from the literature reports on glass/TCO/TiO2/perovskite/metal. The simulations were fitted with the experimental results of some relevant references. Our simulations show that ITO transmits the light better than SnO2 as the TCO front electrode, and the light reflection at both sides of the perovskite layer, e.g. at TiO2/perovskite and perovskite/Spiro-OMeTAD, is lower than 25%. The light interference and multiple reflections have been accounted in our calculations and finally we showed that a thicker TiO2 and perovskite cause more optical loss in current density due to stronger absorption.

  17. Tetrastrontium-digalliumoxide (Sr{sub 4}Ga{sub 2}O{sub 7})-synthesis and crystal structure of a mixed anion strontium gallate related to perovskite

    SciTech Connect

    Kahlenberg, Volker . E-mail: volker.kahlenberg@uibk.ac.at; Lazic, Biljana; Krivovichev, Sergey V.

    2005-05-15

    Crystal growth experiments yielded single crystals of Sr{sub 4}Ga{sub 2}O{sub 7}. The title compound is monoclinic, space group P1c1, a=13.0822(7)A, b=15.7967(6)A, c=15.8586(8)A, {beta}=90.643(6){sup o}, V=3277.1(3)A{sup 3}, Z=16 (R1=0.041 for 7155 observed reflections and 660 parameters). The crystals showed twinning by pseudo-merohedry. Furthermore, the diffraction data exhibited the typical features of a superstructure. Sr{sub 4}Ga{sub 2}O{sub 7} can be classified as a mixed anion gallate comprising insular [GaO{sub 4}]-groups and [Ga{sub 3}O{sub 10}]-trimers. Both anion groups are located in layers perpendicular to [100]. 32 symmetrically independent Sr-cations crosslink between the tetrahedral anion groups. Alternatively, the compound can be described as a 3x4x4 superstructure of ABO{sub 3} perovskite, with 22.2% vacancies in the oxygen sublattice. The relationship with perovskite can be expressed in the following crystal chemical formula: Sr(Ga{sub 2/3}Sr{sub 1/3})(O{sub 7/9}-bar {sub 2/9}){sub 3}. A discussion of the structure in the context with other similar defect perovskites in presented.

  18. Stability limits of the perovskite structure in the Y-Ba-Cu-O system

    NASA Astrophysics Data System (ADS)

    Bormann, R.; Nölting, J.

    1989-05-01

    The equilibrium (molecular) oxygen partial pressure of the Y1Ba2Cu3O7-x phase has been measured by an electrochemical method. The investigations are focused on the low-temperature range between 560 and 750 °C and on oxygen stoichiometries close to the oxygen-poor phase boundary. In particular, the oxygen partial pressure has been determined below which the perovskite structure becomes thermodynamically unstable. This critical value should be considered during the preparation of high Tc Y1Ba2Cu3O7-x superconductors, especially in the case of an in situ preparation of thin films.

  19. An Ultrahigh-Performance Photodetector based on a Perovskite-Transition-Metal-Dichalcogenide Hybrid Structure.

    PubMed

    Kang, Dong-Ho; Pae, Seong Ryul; Shim, Jaewoo; Yoo, Gwangwe; Jeon, Jaeho; Leem, Jung Woo; Yu, Jae Su; Lee, Sungjoo; Shin, Byungha; Park, Jin-Hong

    2016-09-01

    An ultrahigh performance MoS2 photodetector with high photoresponsivity (1.94 × 10(6) A W(-1) ) and detectivity (1.29 × 10(12) Jones) under 520 nm and 4.63 pW laser exposure is demonstrated. This photodetector is based on a methyl-ammonium lead halide perovskite/MoS2 hybrid structure with (3-aminopropyl)triethoxysilane doping. The performance degradation caused by moisture is also minimized down to 20% by adopting a new encapsulation bilayer of octadecyltrichlorosilane/polymethyl methacrylate.

  20. Temperature and Pressure Sensors Based on Spin-Allowed Broadband Luminescence of Doped Orthorhombic Perovskite Structures

    NASA Technical Reports Server (NTRS)

    Eldridge, Jeffrey I. (Inventor); Chambers, Matthew D. (Inventor)

    2014-01-01

    Systems and methods that are capable of measuring pressure or temperature based on luminescence are discussed herein. These systems and methods are based on spin-allowed broadband luminescence of sensors with orthorhombic perovskite structures of rare earth aluminates doped with chromium or similar transition metals, such as chromium-doped gadolinium aluminate. Luminescence from these sensors can be measured to determine at least one of temperature or pressure, based on either the intense luminescence of these sensors, even at high temperatures, or low temperature techniques discussed herein.

  1. Revised structural phase transitions in the archetype KMnF3 perovskite crystal

    NASA Astrophysics Data System (ADS)

    Kapusta, Joanna; Daniel, Philippe; Ratuszna, Alicja

    1999-06-01

    Reinvestigation of the structural and vibrational properties of the typical perovskite KMnF3, exhibiting two antiferrodistortive structural phase transitions, was performed using x-ray powder diffraction and Raman spectroscopy in the range between 30 and 300 K. The x-ray-diffraction work has unambiguously shown that a monoclinic distortion (ra-b+c- tilt system P21/m space group) is observed at low temperature below TC2=91 K. This result corresponds with the Raman temperature study which shows that this transition, in spite of its first-order character, can be associated with a group-subgroup relation between tetragonal and monoclinic symmetries. Additionally, existence of a large structural disorder far above the cubic to tetragonal transition (TC1=186 K) is suggested by the two following experimental indications: (i) persistence of hard modes of the tetragonal phase in the cubic symmetry, and (ii) existence of Raman broad bands in normally inactive ideal cubic phase, which are interpreted by the folding of the whole phonons branches of the cubic Brillouin zone. This last observation allows us to follow the evolution of the cubic R'15 soft mode versus temperature, based only on the Raman-scattering data, in full agreement with previous inelastic neutron data. The results of Raman investigations into KMnF3 are discussed in more general framework of structural disorder in perovskite systems which exhibit anisotropic correlation between octahedra.

  2. "Ba6Nb4RuO18" and "LaBa4Nb3RuO15" - The structural consequences of substituting paramagnetic cations into AnBn-1O3n cation-deficient perovskite oxides

    NASA Astrophysics Data System (ADS)

    Kamil, Elynor L.; Morgan, Harry W. T.; Hayward, Michael A.

    2016-06-01

    The B-cation deficient perovskite phases Ba6Nb4RuO18 and LaBa4Nb3RuO15 were prepared by ceramic synthesis. Neutron powder diffraction analysis indicates that rather than the 6-layer and 5-layer cation-deficient perovskite structures expected for these phases (by analogy to the known structures of Ba6Nb4TiO18 and LaBa4Nb3TiO15) they adopt 5-layer and 4-layer B-cation deficient perovskite structures respectively, and are better described as Ba5Nb3.33Ru0.81O15 and Ba3.16La0.84Nb2.36Ru0.72O12. The factors that lead to the compositionally analogous Nb/Ru and Nb/Ti phases adopting different structures are discussed on the basis of the difference between d0 and non-d0 transition metal cations.

  3. Dielectric response of double layered perovskite Sr3MnTiO7

    NASA Astrophysics Data System (ADS)

    Chowki, S.; Sahu, B.; Singh, A. K.; Mohapatra, N.

    2016-05-01

    The results of dielectric and resistivity measurements on the Ruddlesden-Popper (RP) type compound Sr3MnTiO7 (SMTO) is presented here. The dielectric response of the compound was recorded in the temperature range 10-300 K with the probing frequency from 500 Hz-5 MHz. We observe a broad anomaly at ~ 200 K in the temperature dependence of dissipation factor (tanδ) and corresponding change in slope in the dielectric constant ɛr'(T) which may be attributed to a difference in the conduction mechanism below and above 200 K. The overall dielectric dispersion of SMTO resembles to that of the double perovskites Sr2MnTiO6 and La2NiMnO6 which follows the modified Debye relaxation equation. This indicates a relaxor type dielectric behavior of SMTO may be due to the contribution of grain boundary effects.

  4. Design of a dual-layer ceramic interconnect based on perovskite oxides for segmented-in-series solid oxide fuel cells

    NASA Astrophysics Data System (ADS)

    Park, Beom-Kyeong; Kim, Dae-Wi; Song, Rak-Hyun; Lee, Seung-Bok; Lim, Tak-Hyoung; Park, Seok-Joo; Park, Chong-Ook; Lee, Jong-Won

    2015-12-01

    A segmented-in series (SIS) SOFC consists of segmented unit cells connected in electrical series and shows improved stack efficiency over conventional SOFCs. In this design, a thin interconnect film provides both electrical contact and sealing between the anode of one cell and the cathode of the next; thus, it should have high conductivity and chemical/structural stability in both reducing and oxidizing atmospheres as well as impermeability to gases. Here, we report a dual-layer interconnect film for SIS-SOFCs comprising perovskite-type oxides, Sr0.7La0.2TiO3 (exposed to a reducing atmosphere) and La0.8Sr0.2FeO3 (exposed to an oxidizing atmosphere). The interconnect film is not only very dense but also highly conductive and stable under SOFC operating conditions; in particular, it shows an area-specific resistance of 19.6 mΩ cm2 at 800 °C, which is much lower than the generally accepted limit for SOFCs. A flat-tubular SIS-SOFC fabricated using these interconnect films exhibits a power density as high as 340 mW cm-2, which proves the feasibility of the dual-layer interconnect design.

  5. Structural and electric evidence of ferrielectric state in Pb₂MnWO₆ double perovskite system.

    PubMed

    Orlandi, Fabio; Righi, Lara; Cabassi, Riccardo; Delmonte, Davide; Pernechele, Chiara; Bolzoni, Fulvio; Mezzadri, Francesco; Solzi, Massimo; Merlini, Marco; Calestani, Gianluca

    2014-10-01

    In this paper we describe the new ferri-electric compound Pb2MnWO6 (PMW), a double perovskite that can be considered as a novel structural prototype showing complex nuclear structure and interesting electric properties. According to single-crystal synchrotron data, PMW crystallizes in the noncentrosymmetric polar group Pmc21, in which the two symmetry-independent lead atoms give rise to a ferrielectric arrangement. The accurate crystallographic characterization indicates the presence of a complex distortion of the perovskite lattice driven by the local instability induced by the 6s(2) lone pair of the lead atoms. These peculiar structural features are confirmed by the complete electrical characterization of the system. Dielectric and transport measurements indicate an insulating character of the sample, while pyroelectric measurements point out a ferrielectric state characterized by different contributions. The magnetic transition at 45 K is accompanied by a magnetostrictive effect indicating a probable spin-lattice coupling. The characterizations carried out on PMW, showing the evidence of a coexistence of antiferromagnetism and ferrielectricity at low temperature, could lead to the definition of a new class of multiferroic materials. PMID:25197959

  6. Enhanced photoelectrical performance of dye-sensitized solar cells with double-layer TiO2 on perovskite SrTiO3 substrate

    NASA Astrophysics Data System (ADS)

    Liu, Qiuhong; Sun, Qiong; Zhang, Min; Li, Yang; Zhao, Mei; Dong, Lifeng

    2016-04-01

    In this research, perovskite SrTiO3 particles are synthesized by a hydrothermal method, and TiO2 with a double-layer structure is grown on the SrTiO3 surface by a hydrolysis-condensation process. Structural characterizations reveal that TiO2 comprises of two phases: anatase film at the bottom and single-crystal rutile nanorods grown along the [110] direction on top. The TiO2-SrTiO3 composite film is investigated as photoanode material for dye-sensitized solar cells. In comparison with pure TiO2 and SrTiO3, the composite photoanode shows a much better performance in photoelectric conversion efficiency (1.35 %), which is about 2 and 100 times as efficient as pure TiO2 and SrTiO3, respectively. This indicates that the composite structure can facilitate charge carrier transfer and reduce electron-hole recombination to enhance photoelectrical properties of TiO2-based photoanode materials.

  7. Anion ordering, magnetic structure and properties of the vacancy ordered perovskite Ba3Fe3O7F

    NASA Astrophysics Data System (ADS)

    Clemens, Oliver; Reitz, Christian; Witte, Ralf; Kruk, Robert; Smith, Ronald I.

    2016-11-01

    This article describes a detailed investigation of the crystallographic and magnetic structure of perovskite type Ba3Fe3O7F by a combined analysis of X-ray and neutron powder diffraction data. Complete ordering of vacancies within the perovskite lattice could be confirmed. In addition, the structure of the anion sublattice was studied by means of the valence bond method, which suggested partial ordering of the fluoride ions on two of the six crystallographically different anion sites. Moreover, the compound was found to show G-type antiferromagnetic ordering of Fe moments, in agreement with magnetometric measurements as well as previously recorded 57Fe Mössbauer spectroscopy data.

  8. Tomographic reconstruction of layered tissue structures

    NASA Astrophysics Data System (ADS)

    Hielscher, Andreas H.; Azeez-Jan, Mohideen; Bartel, Sebastian

    2001-11-01

    In recent years the interest in the determination of optical properties of layered tissue structure has resurfaced. Applications include, for example, studies on layered skin tissue and underlying muscles, imaging of the brain underneath layers of skin, skull, and meninges, and imaging of the fetal head in utero beneath the layered structures of the maternal abdomen. In this work we approach the problem of layered structures in the framework of model-based iterative image reconstruction schemes. These schemes are currently developed to determine the optical properties inside tissue from measurement on the surface. If applied to layered structure these techniques yield substantial improvements over currently available semi-analytical approaches.

  9. Buffer layer for thin film structures

    DOEpatents

    Foltyn, Stephen R.; Jia, Quanxi; Arendt, Paul N.; Wang, Haiyan

    2010-06-15

    A composite structure including a base substrate and a layer of a mixture of strontium titanate and strontium ruthenate is provided. A superconducting article can include a composite structure including an outermost layer of magnesium oxide, a buffer layer of strontium titanate or a mixture of strontium titanate and strontium ruthenate and a top-layer of a superconducting material such as YBCO upon the buffer layer.

  10. Buffer layer for thin film structures

    DOEpatents

    Foltyn, Stephen R.; Jia, Quanxi; Arendt, Paul N.; Wang, Haiyan

    2006-10-31

    A composite structure including a base substrate and a layer of a mixture of strontium titanate and strontium ruthenate is provided. A superconducting article can include a composite structure including an outermost layer of magnesium oxide, a buffer layer of strontium titanate or a mixture of strontium titanate and strontium ruthenate and a top-layer of a superconducting material such as YBCO upon the buffer layer.

  11. Bright Visible-Infrared Light Emitting Diodes Based on Hybrid Halide Perovskite with Spiro-OMeTAD as a Hole-Injecting Layer.

    PubMed

    Jaramillo-Quintero, Oscar A; Sanchez, Rafael S; Rincon, Marina; Mora-Sero, Ivan

    2015-05-21

    Hybrid halide perovskites that are currently intensively studied for photovoltaic applications, also present outstanding properties for light emission. Here, we report on the preparation of bright solid state light emitting diodes (LEDs) based on a solution-processed hybrid lead halide perovskite (Pe). In particular, we have utilized the perovskite generally described with the formula CH3NH3PbI(3-x)Cl(x) and exploited a configuration without electron or hole blocking layer in addition to the injecting layers. Compact TiO2 and Spiro-OMeTAD were used as electron and hole injecting layers, respectively. We have demonstrated a bright combined visible-infrared radiance of 7.1 W·sr(-1)·m(-2) at a current density of 232 mA·cm(-2), and a maximum external quantum efficiency (EQE) of 0.48%. The devices prepared surpass the EQE values achieved in previous reports, considering devices with just an injecting layer without any additional blocking layer. Significantly, the maximum EQE value of our devices is obtained at applied voltages as low as 2 V, with a turn-on voltage as low as the Pe band gap (V(turn-on) = 1.45 ± 0.06 V). This outstanding performance, despite the simplicity of the approach, highlights the enormous potentiality of Pe-LEDs. In addition, we present a stability study of unsealed Pe-LEDs, which demonstrates a dramatic influence of the measurement atmosphere on the performance of the devices. The decrease of the electroluminescence (EL) under continuous operation can be attributed to an increase of the non-radiative recombination pathways, rather than a degradation of the perovskite material itself.

  12. Core/Shell Structured TiO2/CdS Electrode to Enhance the Light Stability of Perovskite Solar Cells.

    PubMed

    Hwang, Insung; Baek, Minki; Yong, Kijung

    2015-12-23

    In this work, enhanced light stability of perovskite solar cell (PSC) achieved by the introduction of a core/shell-structured CdS/TiO2 electrode and the related mechanism are reported. By a simple solution-based process (SILAR), a uniform CdS shell was coated onto the surface of a TiO2 layer, suppressing the activation of intrinsic trap sites originating from the oxygen vacancies of the TiO2 layer. As a result, the proposed CdS-PSC exhibited highly improved light stability, maintaining nearly 80% of the initial efficiency after 12 h of full sunlight illumination. From the X-ray diffraction analyses, it is suggested that the degradation of the efficiency of PSC during illumination occurs regardless of the decomposition of the perovskite absorber. Considering the light-soaking profiles of the encapsulated cells and the OCVD characteristics, it is likely that the CdS shell had efficiently suppressed the undesirable electron kinetics, such as trapping at the surface defects of the TiO2 and preventing the resultant charge losses by recombination. This study suggests that further complementary research on various effective methods for passivation of the TiO2 layer would be highly meaningful, leading to insight into the fabrication of PSCs stable to UV-light for a long time.

  13. Real-Space Imaging of the Atomic Structure of Organic-Inorganic Perovskite.

    PubMed

    Ohmann, Robin; Ono, Luis K; Kim, Hui-Seon; Lin, Haiping; Lee, Michael V; Li, Youyong; Park, Nam-Gyu; Qi, Yabing

    2015-12-30

    Organic-inorganic perovskite is a promising class of materials for photovoltaic applications and light emitting diodes. However, so far commercialization is still impeded by several drawbacks. Atomic-scale effects have been suggested to be possible causes, but an unequivocal experimental view at the atomic level is missing. Here, we present a low-temperature scanning tunneling microscopy study of single crystal methylammonium lead bromide CH3NH3PbBr3. Topographic images of the in situ cleaved perovskite surface reveal the real-space atomic structure. Compared to the bulk we observe modified arrangements of atoms and molecules on the surface. With the support of density functional theory we explain these by surface reconstruction and a substantial interplay of the orientation of the polar organic cations (CH3NH3)(+) with the position of the hosting anions. This leads to structurally and electronically distinct domains with ferroelectric and antiferroelectric character. We further demonstrate local probing of defects, which may also impact device performance.

  14. Structures of ordered tungsten- or molybdenum-containing quaternary perovskite oxides

    SciTech Connect

    Day, Bradley E.; Bley, Nicholas D.; Jones, Heather R.; McCullough, Ryan M.; Eng, Hank W.; Porter, Spencer H.; Woodward, Patrick M.; Barnes, Paris W.

    2012-01-15

    The room temperature crystal structures of six A{sub 2}MMoO{sub 6} and A{sub 2}MWO{sub 6} ordered double perovskites were determined from X-ray and neutron powder diffraction data. Ba{sub 2}MgWO{sub 6} and Ba{sub 2}CaMoO{sub 6} both adopt cubic symmetry (space group Fm3-bar m, tilt system a{sup 0}a{sup 0}a{sup 0}). Ba{sub 2}CaWO{sub 6} has nearly the same tolerance factor (t=0.972) as Ba{sub 2}CaMoO{sub 6} (t=0.974), yet it surprisingly crystallizes with I4/m symmetry indicative of out-of-phase rotations of the MO{sub 6} octahedra about the c-axis (a{sup 0}a{sup 0}c{sup -}). Sr{sub 2}ZnMoO{sub 6} (t=0.979) also adopts I4/m symmetry; whereas, Sr{sub 2}ZnWO{sub 6} (t=0.976) crystallizes with monoclinic symmetry (P2{sub 1}/n) with out-of-phase octahedral tilting distortions about the a- and b-axes, and in-phase tilting about the c-axis (a{sup -}a{sup -}c{sup +}). Ca{sub 2}CaWO{sub 6} (t=0.867) also has P2{sub 1}/n symmetry with large tilting distortions about all three crystallographic axes and distorted CaO{sub 6} octahedra. Analysis of 93 double perovskites and their crystal structures showed that while the type and magnitude of the octahedral tilting distortions are controlled primarily by the tolerance factor, the identity of the A-cation acts as the secondary structure directing factor. When A=Ba{sup 2+} the boundary between cubic and tetragonal symmetries falls near t=0.97, whereas when A=Sr{sup 2+} this boundary falls somewhere between t=1.018 and t=0.992. - Graphical abstract: A survey of the tolerance factor of 41 Mo/W- and 52 Nb/Ta-containing quaternary perovskites plotted as a function of the difference between the two six-coordinate M-cation ionic radii. Compounds with cubic symmetry are represented by diamonds, those with tetragonal symmetry are represented by squares, those with I2/m monoclinic symmetry are represented by Multiplication-Sign , and those with P2{sub 1}/n monoclinic symmetry are represented by triangles. White symbols represent

  15. The absence of ferroelectric polarization in layered and rock-salt ordered NaLnMnWO6 (Ln = La, Nd, Tb) perovskites.

    PubMed

    De, Chandan; Kim, Tai Hoon; Kim, Kee Hoon; Sundaresan, A

    2014-03-21

    The ordered perovskites, NaLnMnWO6 (Ln = La, Nd, Tb), are reported to exhibit simultaneous ordering of A-site cations (Na and Ln) in layered arrangement and B-site cations (Mn and W) in rock salt structure. They have been shown to crystallize in a monoclinic structure with the polar space group P21. Based on density functional calculations and group theoretical analysis, it has recently been proposed that NaLaMnWO6 should be ferroelectric with a relatively large polarization (16 μC cm(-2)). Contrary to this prediction, our electrical measurements such as conventional P-E loop, Positive-Up and Negative-Down (PUND), piezoelectric response and Second Harmonic Generation (SHG) reveal the absence of ferroelectric polarization in NaLnMnWO6 (Ln = La, Nd, Tb). A dielectric anomaly is observed just below room temperature (∼270 K) for all the three compounds, which is related to the change in conductivity as revealed by temperature dependent ac and dc resistivity. A pyrocurrent peak is also observed at the same temperature. However, its origin cannot be attributed to a ferroelectric transition. PMID:24503958

  16. Trace surface-clean palladium nanosheets as a conductivity enhancer in hole-transporting layers to improve the overall performances of perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Cao, Jing; Mo, Shiguang; Jing, Xiaojing; Yin, Jun; Li, Jing; Zheng, Nanfeng

    2016-02-01

    Surface-clean Pd nanosheets were synthesized and embedded in a hole transport material (HTM) matrix to improve the conductivity of the HTM layer. Applying only a trace amount of Pd nanosheets readily led to a remarkably enhanced performance of perovskite solar cells (PSCs). This finding provides an effective strategy to build efficient charge-transport materials for improving the overall performance of PSCs.Surface-clean Pd nanosheets were synthesized and embedded in a hole transport material (HTM) matrix to improve the conductivity of the HTM layer. Applying only a trace amount of Pd nanosheets readily led to a remarkably enhanced performance of perovskite solar cells (PSCs). This finding provides an effective strategy to build efficient charge-transport materials for improving the overall performance of PSCs. Electronic supplementary information (ESI) available: Details of the XRD, UV-vis spectra, cross-sectional SEM images and the EQE spectra of the cells. See DOI: 10.1039/c5nr07789c

  17. Enhanced performance of CH3NH3PbI3- x Cl x perovskite solar cells by CH3NH3I modification of TiO2-perovskite layer interface

    NASA Astrophysics Data System (ADS)

    Wang, Wen; Zhang, Zongbao; Cai, Yangyang; Chen, Jinshan; Wang, Jianming; Huang, Riyan; Lu, Xubing; Gao, Xingsen; Shui, Lingling; Wu, Sujuan; Liu, Jun-Ming

    2016-06-01

    In this work, perovskite solar cells (PSCs) with CH3NH3PbI3- x Cl x as active layer and spiro-OMeTAD as hole-transport media have been fabricated by one-step method. The methylammonium iodide (CH3NH3I) solution with different concentrations is used to modify the interface between mesoporous TiO2 (meso-TiO2) film and CH3NH3PbI3- x Cl x perovskite layer. Several techniques including X-ray diffraction, scanning electron microscopy, optical absorption, electrochemical impedance spectroscopy (EIS) and photoluminescence are used to investigate the effect of the interfacial modification. It is found that the interfacial modification by CH3NH3I enhance the crystallinity and increase the grain size of CH3NH3PbI3- x Cl x layer, and improve the surface wetting properties of perovskite precursor on meso-TiO2 film. The sunlight absorption and external quantum efficiency of PSCs in the visible region with wavelength less than 600 nm have been improved. The Nyquist plots obtained from the EIS suggest that the CH3NH3I modification can reduce the charge recombination rates. The photoluminescence measurement shows that the exciton dissociation in the modified devices is more effective than that in the control samples. The photovoltaic performance of the modified devices can be significantly improved with respect to the reference (control) devices. The CH3NH3I modified devices at the optimized concentration demonstrate the average power conversion efficiency of 12.27 % in comparison with the average efficiency of 9.68 % for the reference devices.

  18. Enhanced performance of CH3NH3PbI3-x Cl x perovskite solar cells by CH3NH3I modification of TiO2-perovskite layer interface.

    PubMed

    Wang, Wen; Zhang, Zongbao; Cai, Yangyang; Chen, Jinshan; Wang, Jianming; Huang, Riyan; Lu, Xubing; Gao, Xingsen; Shui, Lingling; Wu, Sujuan; Liu, Jun-Ming

    2016-12-01

    In this work, perovskite solar cells (PSCs) with CH3NH3PbI3-x Cl x as active layer and spiro-OMeTAD as hole-transport media have been fabricated by one-step method. The methylammonium iodide (CH3NH3I) solution with different concentrations is used to modify the interface between mesoporous TiO2 (meso-TiO2) film and CH3NH3PbI3-x Cl x perovskite layer. Several techniques including X-ray diffraction, scanning electron microscopy, optical absorption, electrochemical impedance spectroscopy (EIS) and photoluminescence are used to investigate the effect of the interfacial modification. It is found that the interfacial modification by CH3NH3I enhance the crystallinity and increase the grain size of CH3NH3PbI3-x Cl x layer, and improve the surface wetting properties of perovskite precursor on meso-TiO2 film. The sunlight absorption and external quantum efficiency of PSCs in the visible region with wavelength less than 600 nm have been improved. The Nyquist plots obtained from the EIS suggest that the CH3NH3I modification can reduce the charge recombination rates. The photoluminescence measurement shows that the exciton dissociation in the modified devices is more effective than that in the control samples. The photovoltaic performance of the modified devices can be significantly improved with respect to the reference (control) devices. The CH3NH3I modified devices at the optimized concentration demonstrate the average power conversion efficiency of 12.27 % in comparison with the average efficiency of 9.68 % for the reference devices.

  19. NaIrO{sub 3}-A pentavalent post-perovskite

    SciTech Connect

    Bremholm, M.; Dutton, S.E.; Stephens, P.W.; Cava, R.J.

    2011-03-15

    Sodium iridium (V) oxide, NaIrO{sub 3,} was synthesized by a high pressure solid state method and recovered to ambient conditions. It is found to be isostructural with CaIrO{sub 3}, the much-studied structural analog of the high-pressure post-perovskite phase of MgSiO{sub 3}. Among the oxide post-perovskites, NaIrO{sub 3} is the first example with a pentavalent cation. The structure consists of layers of corner- and edge-sharing IrO{sub 6} octahedra separated by layers of NaO{sub 8} bicapped trigonal prisms. NaIrO{sub 3} shows no magnetic ordering and resistivity measurements show non-metallic behavior. The crystal structure, electrical and magnetic properties are discussed and compared to known post-perovskites and pentavalent perovskite metal oxides. -- Graphical abstract: Sodium iridium(V) oxide, NaIrO{sub 3}, synthesized by a high pressure solid state method and recovered to ambient conditions is found to crystallize as the post-perovskite structure and is the first example of a pentavalent ABO{sub 3} post-perovskite. Research highlights: {yields} NaIrO{sub 3} post-perovskite stabilized by pressure. {yields} First example of a pentavalent oxide post-perovskite. {yields} Non-metallic and non-magnetic behavior of NaIrO{sub 3}.

  20. Hybrid functional band gap calculation of SnO{sub 6} containing perovskites and their derived structures

    SciTech Connect

    Lee, Hyewon; Cheong, S.W.; Kim, Bog G.

    2015-08-15

    We have studied the properties of SnO{sub 6} octahedra-containing perovskites and their derived structures using ab initio calculations with different density functionals. In order to predict the correct band gap of the materials, we have used B3LYP hybrid density functional, and the results of B3LYP were compared with those obtained using the local density approximation and generalized gradient approximation data. The calculations have been conducted for the orthorhombic ground state of the SnO{sub 6} containing perovskites. We also have expended the hybrid density functional calculation to the ASnO{sub 3}/A'SnO{sub 3} system with different cation orderings. We propose an empirical relationship between the tolerance factor and the band gap of SnO{sub 6} containing oxide materials based on first principles calculation. - Graphical abstract: (a) Structure of ASnO{sub 3} for orthorhombic ground state. The green ball is A (Ba, Sr, Ca) cation and the small (red) ball on edge is oxygen. SnO{sub 6} octahedrons are plotted as polyhedron. (b) Band gap of ASnO{sub 3} as a function of the tolerance factor for different density functionals. The experimental values of the band gap are marked as green pentagons. (c) ASnO{sub 3}/A'SnO{sub 3} superlattices with two types cation arrangement: [001] layered structure and [111] rocksalt structure, respectively. (d) B3LYP hybrid functional band gaps of ASnO{sub 3}, [001] ordered superlattices, and [111] ordered superlattices of ASnO{sub 3}/A'SnO{sub 3} as a function of the effective tolerance factor. Note the empirical linear relationship between the band gap and effective tolerance factor. - Highlights: • We report the hybrid functional band gap calculation of ASnO{sub 3} and ASnO{sub 3}/A'SnO{sub 3}. • The band gap of ASnO{sub 3} using B3LYP functional reproduces the experimental value. • We propose the linear relationship between the tolerance factor and the band gap.

  1. A First-Principles Study on the Structural and Electronic Properties of Sn-Based Organic-Inorganic Halide Perovskites

    NASA Astrophysics Data System (ADS)

    Ma, Zi-Qian; Pan, Hui; Wong, Pak Kin

    2016-11-01

    Organic-inorganic halide perovskites have attracted increasing interest on solar-energy harvesting because of their outstanding electronic properties. In this work, we systematically investigate the structural and electronic properties of Sn-based hybrid perovskites MASnX3 and FASnX3 (X = I, Br) based on density-functional-theory calculations. We find that their electronic properties strongly depend on the organic molecules, halide atoms, and structures. We show that there is a general rule to predict the band gap of the Sn-based hybrid perovskite: its band gap increases as the size of halide atom decreases as well as that of organic molecule increase. The band gap of high temperature phase (cubic structure) is smaller than that of low temperature phase (orthorhombic structure). The band gap of tetragonal structure (medium-temperature phase) may be larger or smaller than that of cubic phase, depending on the orientation of the molecule. Tunable band gap within a range of 0.73-1.53 eV can be achieved by choosing halide atom and organic molecule, and controlling structure. We further show that carrier effective mass also reduces as the size of halide atom increases and that of molecule decreases. By comparing with Pb-based hybrid perovskites, the Sn-based systems show enhanced visible-light absorption and carrier mobility due to narrowed band gap and reduced carrier effective mass. These Sn-based organic-inorganic halide perovskites may find applications in solar energy harvesting with improved performance.

  2. A First-Principles Study on the Structural and Electronic Properties of Sn-Based Organic-Inorganic Halide Perovskites

    NASA Astrophysics Data System (ADS)

    Ma, Zi-Qian; Pan, Hui; Wong, Pak Kin

    2016-08-01

    Organic-inorganic halide perovskites have attracted increasing interest on solar-energy harvesting because of their outstanding electronic properties. In this work, we systematically investigate the structural and electronic properties of Sn-based hybrid perovskites MASnX3 and FASnX3 (X = I, Br) based on density-functional-theory calculations. We find that their electronic properties strongly depend on the organic molecules, halide atoms, and structures. We show that there is a general rule to predict the band gap of the Sn-based hybrid perovskite: its band gap increases as the size of halide atom decreases as well as that of organic molecule increase. The band gap of high temperature phase (cubic structure) is smaller than that of low temperature phase (orthorhombic structure). The band gap of tetragonal structure (medium-temperature phase) may be larger or smaller than that of cubic phase, depending on the orientation of the molecule. Tunable band gap within a range of 0.73-1.53 eV can be achieved by choosing halide atom and organic molecule, and controlling structure. We further show that carrier effective mass also reduces as the size of halide atom increases and that of molecule decreases. By comparing with Pb-based hybrid perovskites, the Sn-based systems show enhanced visible-light absorption and carrier mobility due to narrowed band gap and reduced carrier effective mass. These Sn-based organic-inorganic halide perovskites may find applications in solar energy harvesting with improved performance.

  3. High Performance Perovskite Solar Cells

    PubMed Central

    Tong, Xin; Lin, Feng; Wu, Jiang

    2015-01-01

    Perovskite solar cells fabricated from organometal halide light harvesters have captured significant attention due to their tremendously low device costs as well as unprecedented rapid progress on power conversion efficiency (PCE). A certified PCE of 20.1% was achieved in late 2014 following the first study of long‐term stable all‐solid‐state perovskite solar cell with a PCE of 9.7% in 2012, showing their promising potential towards future cost‐effective and high performance solar cells. Here, notable achievements of primary device configuration involving perovskite layer, hole‐transporting materials (HTMs) and electron‐transporting materials (ETMs) are reviewed. Numerous strategies for enhancing photovoltaic parameters of perovskite solar cells, including morphology and crystallization control of perovskite layer, HTMs design and ETMs modifications are discussed in detail. In addition, perovskite solar cells outside of HTMs and ETMs are mentioned as well, providing guidelines for further simplification of device processing and hence cost reduction.

  4. Room temperature oxidative intercalation with chalcogen hydrides: Two-step method for the formation of alkali-metal chalcogenide arrays within layered perovskites

    SciTech Connect

    Ranmohotti, K.G. Sanjaya; Montasserasadi, M. Dariush; Choi, Jonglak; Yao, Yuan; Mohanty, Debasish; Josepha, Elisha A.; Adireddy, Shiva; Caruntu, Gabriel; Wiley, John B.

    2012-06-15

    Highlights: ► Topochemical reactions involving intercalation allow construction of metal chalcogenide arrays within perovskite hosts. ► Gaseous chalcogen hydrides serve as effect reactants for intercalation of sulfur and selenium. ► New compounds prepared by a two-step intercalation strategy are presented. -- Abstract: A two-step topochemical reaction strategy utilizing oxidative intercalation with gaseous chalcogen hydrides is presented. Initially, the Dion-Jacobson-type layered perovskite, RbLaNb{sub 2}O{sub 7}, is intercalated reductively with rubidium metal to make the Ruddlesden-Popper-type layered perovskite, Rb{sub 2}LaNb{sub 2}O{sub 7}. This compound is then reacted at room-temperature with in situ generated H{sub 2}S gas to create Rb-S layers within the perovskite host. Rietveld refinement of X-ray powder diffraction data (tetragonal, a = 3.8998(2) Å, c = 15.256(1) Å; space group P4/mmm) shows the compound to be isostructural with (Rb{sub 2}Cl)LaNb{sub 2}O{sub 7} where the sulfide resides on a cubic interlayer site surrounded by rubidium ions. The mass increase seen on sulfur intercalation and the refined S site occupation factor (∼0.8) of the product indicate a higher sulfur content than expected for S{sup 2−} alone. This combined with the Raman studies, which show evidence for an H-S stretch, indicate that a significant fraction of the intercalated sulfide exists as hydrogen sulfide ion. Intercalation reactions with H{sub 2}Se{sub (g)} were also carried out and appear to produce an isostructural selenide compound. The utilization of such gaseous hydride reagents could significantly expand multistep topochemistry to a larger number of intercalants.

  5. Influence of surface and finite size effects on the structural and magnetic properties of nanocrystalline lanthanum strontium perovskite manganites

    SciTech Connect

    Žvátora, Pavel; Veverka, Miroslav; Veverka, Pavel; Knížek, Karel; Závěta, Karel; Pollert, Emil; Goglio, Graziella; Duguet, Etienne; Kaman, Ondřej

    2013-08-15

    Syntheses of nanocrystalline perovskite phases of the general formula La{sub 1−x}Sr{sub x}MnO{sub 3+δ} were carried out employing sol–gel technique followed by thermal treatment at 700–900 °C under oxygen flow. The prepared samples exhibit a rhombohedral structure with space group R3{sup ¯}c in the whole investigated range of composition 0.20≤x≤0.45. The studies were aimed at the chemical composition including oxygen stoichiometry and extrinsic properties, i.e. size of the particles, both influencing the resulting structural and magnetic properties. The oxygen stoichiometry was determined by chemical analysis revealing oxygen excess in most of the studied phases. The excess was particularly high for the samples with the smallest crystallites (12–28 nm) while comparative bulk materials showed moderate non-stoichiometry. These differences are tentatively attributed to the surface effects in view of the volume fraction occupied by the upper layer whose atomic composition does not comply with the ideal bulk stoichiometry. - Graphical abstract: Evolution of the particle size with annealing temperature in the nanocrystalline La{sub 0.70}Sr{sub 0.30}MnO{sub 3+δ} phase. Display Omitted - Highlights: • The magnetic behaviour of nanocrystalline La{sub 1−x}Sr{sub x}MnO{sub 3+δ} phases was analyzed on the basis of their crystal structure, chemical composition and size of the particles. • Their Curie temperature and magnetization are markedly affected by finite size and surface effects. • The oxygen excess observed in the La{sub 1−x}Sr{sub x}MnO{sub 3+δ} nanoparticles might be generated by the surface layer with deviated oxygen stoichiometry.

  6. Thermoelectric properties of FeAs based superconductors, with thick perovskite- and Sm-O fluorite-type blocking layers

    NASA Astrophysics Data System (ADS)

    Singh, S. J.; Shimoyama, J.; Ogino, H.; Kishio, K.

    2015-11-01

    The transport properties (electrical resistivity, Hall and Seebeck coefficient, and thermal conductivity) of iron based superconductors with thick perovskite-type oxide blocking layers and fluorine-doped SmFeAsO were studied to explore their possible potential for thermoelectric applications. The thermal conductivity of former compounds depicts the dominated role of phonon and its value decreases rapidly below the Tc, suggesting the addition of scattering of phonons. Both the Seebeck coefficient (S) and Hall coefficient (RH) of all samples were negative in the whole temperature region below 300 K, indicating that the major contribution to the normal state conductivity is by electrons. In addition, the profile of S(T) and RH(T) of all samples have similar behaviours as would be expected for a multi-band superconductors. Although the estimated thermoelectric figure of merit (ZT) of these compounds was much lower than that of practically applicable thermoelectric materials, however its improvement can be expected by optimizing microstructure of the polycrystalline materials, such as densification and grain orientation.

  7. Low thermal budget, photonic-cured compact TiO2 layers for high-efficiency perovskite solar cells

    DOE PAGES

    Das, Sanjib; Gu, Gong; Joshi, Pooran C.; Yang, Bin; Aytug, Tolga; Rouleau, Christopher M.; Geohegan, David B.; Xiao, Kai

    2016-05-25

    Rapid advances in organometallic trihalide perovskite solar cells (PSCs) have positioned them to be one of the leading next generation photovoltaic technologies. However, most of the high-performance PSCs, particularly those using compact TiO2 as an electron transport layer, require a high-temperature sintering step, which is not compatible with flexible polymer-based substrates. Considering the materials of interest for PSCs and corresponding device configurations, it is technologically imperative to fabricate high-efficiency cells at low thermal budget so that they can be realized on low-temperature plastic substrates. In this paper, we report on a new photonic curing technique that produces crystalline anatase-phase TiO2more » films on indium tin oxide-coated glass and flexible polyethylene terephthalate (PET) substrates. Finally, the planar PSCs, using photonic-cured TiO2 films, exhibit PCEs as high as 15.0% and 11.2% on glass and flexible PET substrates, respectively, comparable to the device performance of PSCs incorporating furnace annealed TiO2 films.« less

  8. Low-Temperature and Solution-Processed Amorphous WO(x) as Electron-Selective Layer for Perovskite Solar Cells.

    PubMed

    Wang, Kai; Shi, Yantao; Dong, Qingshun; Li, Yu; Wang, Shufeng; Yu, Xufeng; Wu, Mengyao; Ma, Tingli

    2015-03-01

    The electron-selective layer (ESL) is an indispensable component of perovskite solar cells (PSCs) and is responsible for the collection of photogenerated electrons. Preparing ESL at a low temperature is significant for future fabrication of flexible PSCs. In this work, solution-processed amorphous WO(x) thin film was prepared facilely at low temperature and used as ESL in PSCs. Results indicated that a large quantity of nanocaves were observed in the WO(x) thin film. In comparison with the conventional TiO2 ESL, the WO(x) ESL exhibited comparable light transmittance but higher electrical conductivity. Compared with the TiO2-based PSCs, PSCs that use WO(x) ESL exhibited comparable photoelectric conversion efficiency, larger short-circuit current density, but lower open-circuit voltage. Electrochemical characterization indicated that the unsatisfied open-circuit voltage and fill factor were caused by the inherent charge recombination. This study demonstrated that this material is an excellent candidate for ESL.

  9. Low-Temperature and Solution-Processed Amorphous WO(x) as Electron-Selective Layer for Perovskite Solar Cells.

    PubMed

    Wang, Kai; Shi, Yantao; Dong, Qingshun; Li, Yu; Wang, Shufeng; Yu, Xufeng; Wu, Mengyao; Ma, Tingli

    2015-03-01

    The electron-selective layer (ESL) is an indispensable component of perovskite solar cells (PSCs) and is responsible for the collection of photogenerated electrons. Preparing ESL at a low temperature is significant for future fabrication of flexible PSCs. In this work, solution-processed amorphous WO(x) thin film was prepared facilely at low temperature and used as ESL in PSCs. Results indicated that a large quantity of nanocaves were observed in the WO(x) thin film. In comparison with the conventional TiO2 ESL, the WO(x) ESL exhibited comparable light transmittance but higher electrical conductivity. Compared with the TiO2-based PSCs, PSCs that use WO(x) ESL exhibited comparable photoelectric conversion efficiency, larger short-circuit current density, but lower open-circuit voltage. Electrochemical characterization indicated that the unsatisfied open-circuit voltage and fill factor were caused by the inherent charge recombination. This study demonstrated that this material is an excellent candidate for ESL. PMID:26262648

  10. Structural and Magnetic Phase Coexistence in Oxygen Deficient Perovskites (Sr,Ca)FeO 2 . 5 + δ

    NASA Astrophysics Data System (ADS)

    Carlo, J. P.; Evans, M. E.; Anczarski, J. A.; Ock, J.; Boyd, K.; Pollichemi, J. R.; Leahy, I. A.; Vogel, W.; Viescas, A. J.; Papaefthymiou, G. C.

    A variety of compounds crystallize into perovskite and similar structures, making them versatile laboratories for many phenomena and applications, including multiferroicity, superconductivity, and photovoltaics. Oxygen-deficient perovskites ABOx have attracted interest for use in fuel cells and related applications due to high oxygen mobility and the possibility of charge disproportionation. Vast chemical flexibility is obtained through reductions in lattice symmetry and rotation/distortion of the BO6 octahedra, as well as ordering of oxygen vacancies. We have synthesized and studied the structural and magnetic properties of oxygen-deficient perovskites (Sr,Ca)FeO2 . 5 + δ using x-ray diffraction and Mossbauer spectroscopy. While the ideal perovskite has δ = 0.5, this requires Fe4+, and hence strongly oxidizing environments. When grown in air, Fe3+ is favored, yielding δ ~ 0. SrFeO2 . 5 + δ exhibits cubic symmetry and paramagnetism at 300K, but CaFeO2 . 5 + δ crystallizes into the orthorhombic brownmillerite structure, and is magnetically ordered at 300K. In the doped intermediaries we find coexistence of cubic/paramagnetic and orthorhombic/magnetic phases over a wide range of Ca content. Financial support from the Villanova Undergraduate Research Fellowship program and the Research Corporation for Science Advancement.

  11. Synthesis, structure, and magnetism of BaVO[sub 2. 8]: A new perovskite-related vanadate with V[sup III]/V[sup IV] ordering

    SciTech Connect

    Chen, B.H.; Eichhorn, B.W.; Ju, H.L.; Greene, R.L. )

    1993-12-08

    A new barium vanadium oxide, BaVO[sub 2.8], was prepared from BaO and VO[sub 2] in an evacuated silica ampule at 1100[angstrom]C for 10 h with excess Zr getter. The compound consists of interleaving perovskite layers (two corner-sharing VO[sub 6] octahedra) and BaNiO[sub 3] type layers (three face-sharing CO[sub 6] octahedra) along the c-axis. Curie-Weiss magnetic behavior was observed with [mu][sub eff] = 1.96[mu][sub B]/ The structural and magnetic data reveal ordering of V[sup III] and V[sup IV] cations at the corner-sharing and face-shring octahedral holes, respectively. Qualitative molecular orbital analysis indicates M-M bonding in the face sharing [V[sub 3]O[sub 12

  12. Power Conversion Efficiency and Device Stability Improvement of Inverted Perovskite Solar Cells by Using a ZnO:PFN Composite Cathode Buffer Layer.

    PubMed

    Jia, Xiaorui; Zhang, Lianping; Luo, Qun; Lu, Hui; Li, Xueyuan; Xie, Zhongzhi; Yang, Yongzhen; Li, Yan-Qing; Liu, Xuguang; Ma, Chang-Qi

    2016-07-20

    We have demonstrated in this article that both power conversion efficiency (PCE) and performance stability of inverted planar heterojunction perovskite solar cells can be improved by using a ZnO:PFN nanocomposite (PFN: poly[(9,9-bis(3'-(N,N-dimethylamion)propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctyl)-fluorene]) as the cathode buffer layer (CBL). This nanocomposite could form a compact and defect-less CBL film on the perovskite/PC61BM surface (PC61BM: phenyl-C61-butyric acid methyl ester). In addition, the high conductivity of the nanocomposite layer makes it works well at a layer thickness of 150 nm. Both advantages of the composite layer are helpful in reducing interface charge recombination and improving device performance. The power conversion efficiency (PCE) of the best ZnO:PFN CBL based device was measured to be 12.76%, which is higher than that of device without CBL (9.00%), or device with ZnO (7.93%) or PFN (11.30%) as the cathode buffer layer. In addition, the long-term stability is improved by using ZnO:PFN composite cathode buffer layer when compare to that of the reference cells. Almost no degradation of open circuit voltage (VOC) and fill factor (FF) was found for the device having ZnO:PFN, suggesting that ZnO:PFN is able to stabilize the interface property and consequently improve the solar cell performance stability.

  13. Pyrolysis preparation of WO3 thin films using ammonium metatungstate DMF/water solution for efficient compact layers in planar perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Jincheng, Zhang; Chengwu, Shi; Junjun, Chen; Chao, Ying; Ni, Wu; Mao, Wang

    2016-03-01

    The tungsten trioxide (WO3) thin films were firstly prepared by spin-coating-pyrolysis methods using the ammonium metatungstate ((NH4)6H2W12O40) DMF/water solution, and successfully applied as the efficient compact layers for the planar perovskite solar cells. The influence of the WO3 film thickness and the rinsing treatment of CH3NH3PbI3 thin film with isopropanol on the photovoltaic performance of the corresponding perovskite solar cells was systematically investigated. The results revealed that the perovskite solar cell with a 62 nm thick WO3 compact layer achieved a photoelectric conversion efficiency of 5.72%, with a short circuit photocurrent density of 17.39 mA/cm2, an open circuit voltage of 0.58 V and a fill factor of 0.57. The photoelectric conversion efficiency was improved from 5.72% to 7.04% by the isopropanol rinsing treatment. Project supported by the National Natural Science Foundation of China (Nos. 51472071, 512720616, 51072043), and the National Basic Research Program of China (No. 2011CBA00700).

  14. Enhanced Efficiency and Stability of Inverted Perovskite Solar Cells Using Highly Crystalline SnO2 Nanocrystals as the Robust Electron-Transporting Layer.

    PubMed

    Zhu, Zonglong; Bai, Yang; Liu, Xiao; Chueh, Chu-Chen; Yang, Shihe; Jen, Alex K-Y

    2016-08-01

    Highly crystalline SnO2 is demonstrated to serve as a stable and robust electron-transporting layer for high-performance perovskite solar cells. Benefiting from its high crystallinity, the relatively thick SnO2 electron-transporting layer (≈120 nm) provides a respectable electron-transporting property to yield a promising power conversion efficiency (PCE)(18.8%) Over 90% of the initial PCE can be retained after 30 d storage in ambient with ≈70% relative humidity. PMID:27168338

  15. Structural phase transition in perovskite metal-formate frameworks: a Potts-type model with dipolar interactions.

    PubMed

    Šimėnas, Mantas; Balčiūnas, Sergejus; Ma Combining Cedilla Czka, Mirosław; Banys, Jūras; Tornau, Evaldas E

    2016-07-21

    We propose a combined experimental and numerical study to describe an order-disorder structural phase transition in perovskite-based [(CH3)2NH2][M(HCOO)3] (M = Zn(2+), Mn(2+), Fe(2+), Co(2+) and Ni(2+)) dense metal-organic frameworks (MOFs). The three-fold degenerate orientation of the molecular (CH3)2NH2(+) (DMA(+)) cation implies a selection of the statistical three-state model of the Potts type. It is constructed on a simple cubic lattice where each lattice point can be occupied by a DMA(+) cation in one of the available states. In our model the main interaction is the nearest-neighbor Potts-type interaction, which effectively accounts for the H-bonding between DMA(+) cations and M(HCOO)3(-) cages. The model is modified by accounting for the dipolar interactions which are evaluated for the real monoclinic lattice using density functional theory. We employ the Monte Carlo method to numerically study the model. The calculations are supplemented with the experimental measurements of electric polarization. The obtained results indicate that the three-state Potts model correctly describes the phase transition order in these MOFs, while dipolar interactions are necessary to obtain better agreement with the experimental polarization. We show that in our model with substantial dipolar interactions the ground state changes from uniform to the layers with alternating polarization directions. PMID:27341447

  16. The thermal equation of state of (Mg, Fe)SiO3 bridgmanite (perovskite) and implications for lower mantle structures

    NASA Astrophysics Data System (ADS)

    Wolf, Aaron S.; Jackson, Jennifer M.; Dera, Przemeslaw; Prakapenka, Vitali B.

    2015-11-01

    The high-pressure/high-temperature equation of state (EOS) of synthetic 13% Fe-bearing bridgmanite (Mg silicate perovskite) is measured using powder X-ray diffraction in a laser-heated diamond anvil cell with a quasi-hydrostatic neon pressure medium. We compare these results, which are consistent with previous 300 K sound speed and compression studies, with a reanalysis of Fe-free Mg end-member data from Tange et al. (2012) to determine the effect of iron on bridgmanite's thermoelastic properties. EOS parameters are incorporated into an ideal lattice mixing model to probe the behavior of bridgmanite at deep mantle conditions. With this model, a nearly pure bridgmanite mantle composition is shown to be inconsistent with density and compressibility profiles of the lower mantle. We also explore the buoyant stability of bridgmanite over a range of temperatures and compositions expected for Large Low-Shear Velocity Provinces, concluding that bridgmanite-dominated thermochemical piles are more likely to be passive dense layers externally supported by convection, rather than internally supported metastable domes. The metastable dome scenario is estimated to have a relative likelihood of only 4-7%, given the narrow range of compositions and temperatures consistent with seismic constraints. If buoyantly supported, such structures could not have remained stable with greater thermal contrast early in Earth's history, ruling out formation scenarios involving a large concentration of heat producing elements.

  17. Exploring a Lead-free Semiconducting Hybrid Ferroelectric with a Zero-Dimensional Perovskite-like Structure.

    PubMed

    Sun, Zhihua; Zeb, Aurang; Liu, Sijie; Ji, Chengmin; Khan, Tariq; Li, Lina; Hong, Maochun; Luo, Junhua

    2016-09-19

    Perovskite lead halides (CH3 NH3 PbI3 ) have recently taken a promising position in photovoltaics and optoelectronics because of remarkable semiconducting properties and possible ferroelectricity. However, the potential toxicity of lead arouses great environmental concern for widespread application. A new chemically tailored lead-free semiconducting hybrid ferroelectric is reported, N-methylpyrrolidinium)3 Sb2 Br9 (1), which consists of a zero-dimensional (0-D) perovskite-like anionic framework connected by corner- sharing SbBr6 coordinated octahedra. It presents a large ferroelectric spontaneous polarization of approximately 7.6 μC cm(-2) , as well as notable semiconducting properties, including positive temperature-dependent conductivity and ultraviolet-sensitive photoconductivity. Theoretical analysis of electronic structure and energy gap discloses a dominant contribution of the 0-D perovskite-like structure to the semiconducting properties of the material. This finding throws light on the rational design of new perovskite-like hybrids, especially lead-free semiconducting ferroelectrics.

  18. Optical and Structural Study of Organometal Halide Materials for Applications in Perovskite-Based Solar Cells

    NASA Astrophysics Data System (ADS)

    Nguyen, Minh Tu; Phan Vu, Thi Van; Bui, Bao Thoa; Luong, Thu Trang; Nguyen, Minh Hieu; Hoang Ngoc, Lam Huong; Bui, Van Diep; Truong, Thanh Tu; Nguyen-Tran, Thuat

    2016-05-01

    CH3NH3PbI3 and CH3NH3PbI2Br crystal powders and thin films with chemical formula CH3NH3PbI3- x Br x have been synthesized by reacting methylammonium bromide/iodide with lead iodide. The films were fabricated by a low-temperature solution process using the spin-coating method followed by thermal annealing, which is an effective means for controlling the composition and morphology of the CH3NH3PbI3- x Br x thin films. The resulting perovskite films exhibit good optical absorption and crystalline structure, being promising for potential application as light absorbers in future solar cells.

  19. Structural and optical characterization of DyAlO3 perovskite powders obtained by combustion synthesis

    NASA Astrophysics Data System (ADS)

    Saji S., K.; Raju, K.; Wariar, P. R. S.

    2016-05-01

    Phase pure Dysprosium monoaluminate has been prepared from Dysprosium oxide and Aluminium nitrate by auto-ignition citrate complex combustion process. The phase formation has been investigated using X-ray diffraction analysis (XRD), Thermo-Gravimetric/Differential Thermal Analysis (TGA/DTA) and Fourier Transform Infrared (FT-IR) spectroscopy analysis. X-ray diffraction analysis (XRD) revealed that DyAlO3 has an orthorhombic perovskite structure. From Transmission Electron Microscopy (TEM) studies, average particle-size has been found to be as low as 45 nm. The absorption spectrum of the DyAlO3 nanoparticles shows characteristic absorption bands of Dy atom. The optical band gap of the material was found to be 5.15eV, which corresponds to direct allowed transitions.

  20. Thermal evolution of the crystal structure of the orthorhombic perovskite LaFeO3

    NASA Astrophysics Data System (ADS)

    Dixon, Charlotte A. L.; Kavanagh, Christopher M.; Knight, Kevin S.; Kockelmann, Winfried; Morrison, Finlay D.; Lightfoot, Philip

    2015-10-01

    The thermal evolution of the crystal structure of the prototypical orthorhombic perovskite LaFeO3 has been studied in detail by powder neutron diffraction in the temperature range 25

  1. High-performance inverted planar heterojunction perovskite solar cells based on a solution-processed CuOx hole transport layer

    NASA Astrophysics Data System (ADS)

    Sun, Weihai; Li, Yunlong; Ye, Senyun; Rao, Haixia; Yan, Weibo; Peng, Haitao; Li, Yu; Liu, Zhiwei; Wang, Shufeng; Chen, Zhijian; Xiao, Lixin; Bian, Zuqiang; Huang, Chunhui

    2016-05-01

    During the past several years, methylammonium lead halide perovskites have been widely investigated as light absorbers for thin-film photovoltaic cells. Among the various device architectures, the inverted planar heterojunction perovskite solar cells have attracted special attention for their relatively simple fabrication and high efficiencies. Although promising efficiencies have been obtained in the inverted planar geometry based on poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) sulfonic acid (PEDOT:PSS) as the hole transport material (HTM), the hydrophilicity of the PEDOT:PSS is a critical factor for long-term stability. In this paper, a CuOx hole transport layer from a facile solution-processed method was introduced into the inverted planar heterojunction perovskite solar cells. After the optimization of the devices, a champion PCE of 17.1% was obtained with an open circuit voltage (Voc) of 0.99 V, a short-circuit current (Jsc) of 23.2 mA cm-2 and a fill factor (FF) of 74.4%. Furthermore, the unencapsulated device cooperating with the CuOx film exhibited superior performance in the stability test, compared to the device involving the PEDOT:PSS layer, indicating that CuOx could be a promising HTM for replacing PEDOT:PSS in inverted planar heterojunction perovskite solar cells.During the past several years, methylammonium lead halide perovskites have been widely investigated as light absorbers for thin-film photovoltaic cells. Among the various device architectures, the inverted planar heterojunction perovskite solar cells have attracted special attention for their relatively simple fabrication and high efficiencies. Although promising efficiencies have been obtained in the inverted planar geometry based on poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) sulfonic acid (PEDOT:PSS) as the hole transport material (HTM), the hydrophilicity of the PEDOT:PSS is a critical factor for long-term stability. In this paper, a CuOx hole transport layer from a

  2. An experimental study of perovskite-structured mixed ionic- electronic conducting oxides and membranes

    NASA Astrophysics Data System (ADS)

    Zeng, Pingying

    In recent decades, ceramic membranes based on mixed ionic and electronic conducting (MIEC) perovskite-structured oxides have received many attentions for their applications for air separation, or as a membrane reactor for methane oxidation. While numerous perovskite oxide materials have been explored over the past two decades; there are hardly any materials with sufficient practical economic value and performance for large scale applications, which justifies continuing the search for new materials. The main purposes of this thesis study are: (1) develop several novel SrCoO3-delta based MIEC oxides, SrCoCo1-xMxO3-delta, based on which membranes exhibit excellent oxygen permeability; (2) investigate the significant effects of the species and concentration of the dopants M (metal ions with fixed valences) on the various properties of these membranes; (3) investigate the significant effects of sintering temperature on the microstructures and performance of oxygen permeation membranes; and (4) study the performance of oxygen permeation membranes as a membrane reactor for methane combustion. To stabilize the cubic phase structure of the SrCoO3-delta oxide, various amounts of scandium was doped into the B-site of SrCoO 3-delta to form a series of new perovskite oxides, SrScxCoCo 1-xO3-delta (SSCx, x = 0-0.7). The significant effects of scandium-doping concentration on the phase structure, electrical conductivity, sintering performance, thermal and structural stability, cathode performance, and oxygen permeation performance of the SSCx membranes, were systematically studied. Also for a more in-depth understanding, the rate determination steps for the oxygen transport process through the membranes were clarified by theoretical and experimental investigation. It was found that only a minor amount of scandium (5 mol%) doping into the B-site of SrCoO3-delta can effectively stabilize the cubic phase structure, and thus significantly improve the electrical conductivity and

  3. Perovskite Materials for Light-Emitting Diodes and Lasers.

    PubMed

    Veldhuis, Sjoerd A; Boix, Pablo P; Yantara, Natalia; Li, Mingjie; Sum, Tze Chien; Mathews, Nripan; Mhaisalkar, Subodh G

    2016-08-01

    Organic-inorganic hybrid perovskites have cemented their position as an exceptional class of optoelectronic materials thanks to record photovoltaic efficiencies of 22.1%, as well as promising demonstrations of light-emitting diodes, lasers, and light-emitting transistors. Perovskite materials with photoluminescence quantum yields close to 100% and perovskite light-emitting diodes with external quantum efficiencies of 8% and current efficiencies of 43 cd A(-1) have been achieved. Although perovskite light-emitting devices are yet to become industrially relevant, in merely two years these devices have achieved the brightness and efficiencies that organic light-emitting diodes accomplished in two decades. Further advances will rely decisively on the multitude of compositional, structural variants that enable the formation of lower-dimensionality layered and three-dimensional perovskites, nanostructures, charge-transport materials, and device processing with architectural innovations. Here, the rapid advancements in perovskite light-emitting devices and lasers are reviewed. The key challenges in materials development, device fabrication, operational stability are addressed, and an outlook is presented that will address market viability of perovskite light-emitting devices.

  4. Perovskite Materials for Light-Emitting Diodes and Lasers.

    PubMed

    Veldhuis, Sjoerd A; Boix, Pablo P; Yantara, Natalia; Li, Mingjie; Sum, Tze Chien; Mathews, Nripan; Mhaisalkar, Subodh G

    2016-08-01

    Organic-inorganic hybrid perovskites have cemented their position as an exceptional class of optoelectronic materials thanks to record photovoltaic efficiencies of 22.1%, as well as promising demonstrations of light-emitting diodes, lasers, and light-emitting transistors. Perovskite materials with photoluminescence quantum yields close to 100% and perovskite light-emitting diodes with external quantum efficiencies of 8% and current efficiencies of 43 cd A(-1) have been achieved. Although perovskite light-emitting devices are yet to become industrially relevant, in merely two years these devices have achieved the brightness and efficiencies that organic light-emitting diodes accomplished in two decades. Further advances will rely decisively on the multitude of compositional, structural variants that enable the formation of lower-dimensionality layered and three-dimensional perovskites, nanostructures, charge-transport materials, and device processing with architectural innovations. Here, the rapid advancements in perovskite light-emitting devices and lasers are reviewed. The key challenges in materials development, device fabrication, operational stability are addressed, and an outlook is presented that will address market viability of perovskite light-emitting devices. PMID:27214091

  5. Crystal Structure of Pure and Aluminous Calcium Silicate Perovskites at Mantle Related Pressure and Temperature

    NASA Astrophysics Data System (ADS)

    Chen, H.; Shim, S. H.; Leinenweber, K. D.; Meng, Y.; Prakapenka, V.

    2015-12-01

    CaSiO3-perovskite (CaPv) is believed to be the third most abundant mineral (5 wt%) in the Earth's lower mantle (LM). Subducted slabs contain 23 wt% CaPv at the LM related pressure (P) and temperature (T), where Al2O3 could be incorporated into the crystal structure of CaPv (AlCaPv). However, there remains important discrepancy between computations and experiments on the crystal structure of CaPv at high P and low T. Some computations have predicted a tetragonal I4/mcm structure with a pseudo-cubic axial ratio (cp/ap) greater than 1, while X-ray diffraction (XRD) studies have suggested a tetragonal P4/mmm structure with cp/ap ~ 0.995. Using Ne as a pressure medium, we conducted in-situ XRD of CaSiO3 and 5 wt% Al-bearing CaSiO3 in the laser heated diamond anvil cell at the GSECARS and HPCAT sectors of the Advanced Photon Source. Rietveld refinements are performed on the diffraction patterns of CaPv at 300 K and 20-60 GPa. Similar to previous studies, we observed splitting of the 200 and 211 peaks after T-quench in pure CaPv. However, unlike previous experiments, diffraction patterns were more consistent with a tetragonal I4/mcm structure with cp/ap ~ 1.005 than P4/mmm. All the previous diffraction patterns have been measured with an Ar or MgO medium, or even without a medium, while we used more hydrostatic Ne medium. Considering the small free energy differences among different perovskite structures, the crystal structure of CaPv may be very sensitive to non-hydrostatic stresses. In runs with AlCaPv, asymmetrical 200 peaks are found up to 60 GPa and 2200 K, showing that non-cubic could be still stable at mantle geotherm temperatures in AlCaPv. The extreme sensitivity of CaPv on deviatoric stresses may have important implications for the elastic properties of the mantle regions with strong deformations, because the elastic anisotropy can change with the crystal structure of CaPv.

  6. Degradation of Methylammonium Lead Iodide Perovskite Structures through Light and Electron Beam Driven Ion Migration

    PubMed Central

    2016-01-01

    Organometal halide perovskites show promising features for cost-effective application in photovoltaics. The material instability remains a major obstacle to broad application because of the poorly understood degradation pathways. Here, we apply simultaneous luminescence and electron microscopy on perovskites for the first time, allowing us to monitor in situ morphology evolution and optical properties upon perovskite degradation. Interestingly, morphology, photoluminescence (PL), and cathodoluminescence of perovskite samples evolve differently upon degradation driven by electron beam (e-beam) or by light. A transversal electric current generated by a scanning electron beam leads to dramatic changes in PL and tunes the energy band gaps continuously alongside film thinning. In contrast, light-induced degradation results in material decomposition to scattered particles and shows little PL spectral shifts. The differences in degradation can be ascribed to different electric currents that drive ion migration. Moreover, solution-processed perovskite cuboids show heterogeneity in stability which is likely related to crystallinity and morphology. Our results reveal the essential role of ion migration in perovskite degradation and provide potential avenues to rationally enhance the stability of perovskite materials by reducing ion migration while improving morphology and crystallinity. It is worth noting that even moderate e-beam currents (86 pA) and acceleration voltages (10 kV) readily induce significant perovskite degradation and alter their optical properties. Therefore, attention has to be paid while characterizing such materials using scanning electron microscopy or transmission electron microscopy techniques. PMID:26804213

  7. Layered (Cu,Fe) oxides of double perovskite structure. II. Extension of solid solubility of copper in (Ba,La)Y(Cu0.5+xFe0.5-x)2O5+δ via high-pressure heat treatment

    NASA Astrophysics Data System (ADS)

    Nagase, M.; Lindén, J.; Suematsu, H.; Karppinen, M.; Yamauchi, H.

    1999-01-01

    In this paper, we report successful extension of the solid-solubility limit of copper at the transition element site in the (Ba,La)Y(Cu,Fe)2O5+δ phase of the double-perovskite ``0112'' structure. Upon the high-pressure heat treatment at 5 GPa and 1200 °C of the ambient-pressure synthesized samples that contained impurity phases, essentially single-phase samples were obtained for x up to 0.2 in the (Ba1-2xLa2x)Y(Cu0.5+xFe0.5-x)2O5+δ system. TEM observations and TEM energy dispersive x-ray analyses for the high-pressure synthesized (Ba0.6La0.4)Y(Cu0.7Fe0.3)2O5+δ material showed that the ratio of copper to iron varies in the sample with an average value of Cu:Fe=0.70:0.30, as measured for nine grains. It could thus be concluded that a 0112 phase in which the amount of copper is larger than that of iron in the oxygen pyramid was realized. In order to obtain the copper-rich 0112 phase, simultaneous substitution of the divalent barium site by trivalent lanthanum was found necessary. From 57Fe Mössbauer spectroscopy data, the relative intensities of five- and six-coordinated iron atoms were evaluated and the amount of excess oxygen in the structure could be estimated at δ~0.23. Furthermore, both Mössbauer and magnetic-susceptibility measurements of the x=0.2 sample showed that the Néel temperature of the copper-rich material is lower than the corresponding transition temperature observed for the material with the stoichiometric x=0 composition. Finally, conditions for the successful extension of the copper solubility are discussed and related to the tolerance factor of the 0112 structure.

  8. An ultra-thin, un-doped NiO hole transporting layer of highly efficient (16.4%) organic-inorganic hybrid perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Seo, Seongrok; Park, Ik Jae; Kim, Myungjun; Lee, Seonhee; Bae, Changdeuck; Jung, Hyun Suk; Park, Nam-Gyu; Kim, Jin Young; Shin, Hyunjung

    2016-06-01

    NiO is a wide band gap p-type oxide semiconductor and has potential for applications in solar energy conversion as a hole-transporting layer (HTL). It also has good optical transparency and high chemical stability, and the capability of aligning the band edges to the perovskite (CH3NH3PbI3) layers. Ultra-thin and un-doped NiO films with much less absorption loss were prepared by atomic layer deposition (ALD) with highly precise control over thickness without any pinholes. Thin enough (5-7.5 nm in thickness) NiO films with the thickness of few time the Debye length (LD = 1-2 nm for NiO) show enough conductivities achieved by overlapping space charge regions. The inverted planar perovskite solar cells with NiO films as HTLs exhibited the highest energy conversion efficiency of 16.40% with high open circuit voltage (1.04 V) and fill factor (0.72) with negligible current-voltage hysteresis.NiO is a wide band gap p-type oxide semiconductor and has potential for applications in solar energy conversion as a hole-transporting layer (HTL). It also has good optical transparency and high chemical stability, and the capability of aligning the band edges to the perovskite (CH3NH3PbI3) layers. Ultra-thin and un-doped NiO films with much less absorption loss were prepared by atomic layer deposition (ALD) with highly precise control over thickness without any pinholes. Thin enough (5-7.5 nm in thickness) NiO films with the thickness of few time the Debye length (LD = 1-2 nm for NiO) show enough conductivities achieved by overlapping space charge regions. The inverted planar perovskite solar cells with NiO films as HTLs exhibited the highest energy conversion efficiency of 16.40% with high open circuit voltage (1.04 V) and fill factor (0.72) with negligible current-voltage hysteresis. Electronic supplementary information (ESI) available. See DOI: 10.1039/c6nr01601d

  9. Niobium Doping Effects on TiO2 Mesoscopic Electron Transport Layer-Based Perovskite Solar Cells.

    PubMed

    Kim, Dong Hoe; Han, Gill Sang; Seong, Won Mo; Lee, Jin-Wook; Kim, Byeong Jo; Park, Nam-Gyu; Hong, Kug Sun; Lee, Sangwook; Jung, Hyun Suk

    2015-07-20

    Perovskite solar cells (PSCs) are the most promising candidates as next-generation solar energy conversion systems. To design a highly efficient PSC, understanding electronic properties of mesoporous metal oxides is essential. Herein, we explore the effect of Nb doping of TiO2 on electronic structure and photovoltaic properties of PSCs. Light Nb doping (0.5 and 1.0 at %) increased the optical band gap slightly, but heavy doping (5.0 at %) distinctively decreased it. The relative Fermi level position of the conduction band is similar for the lightly Nb-doped TiO2 (NTO) and the undoped TiO2 whereas that of the heavy doped NTO decreased by as much as ∼0.3 eV. The lightly doped NTO-based PSCs exhibit 10 % higher efficiency than PSCs based on undoped TiO2 (from 12.2 % to 13.4 %) and 52 % higher than the PSCs utilizing heavy doped NTO (from 8.8 % to 13.4 %), which is attributed to fast electron injection/transport and preserved electron lifetime, verified by transient photocurrent decay and impedance studies.

  10. Magnetic order and electronic structure of the 5 d3 double perovskite Sr2ScOsO6

    NASA Astrophysics Data System (ADS)

    Taylor, A. E.; Morrow, R.; Singh, D. J.; Calder, S.; Lumsden, M. D.; Woodward, P. M.; Christianson, A. D.

    2015-03-01

    The magnetic susceptibility, crystal and magnetic structures, and electronic structure of the double perovskite Sr2ScOsO6 are reported. Using both neutron and x-ray powder diffraction we find that the crystal structure is monoclinic P 21/n from 3.5 to 300 K. Magnetization measurements indicate an antiferromagnetic transition at TN=92 K , one of the highest transition temperatures of any double perovskite hosting only one magnetic ion. Type I antiferromagnetic order is determined by neutron powder diffraction, with an Os moment of only 1.6 (1 ) μB , close to half the spin-only value for a crystal field split 5 d electron state with a t2g 3 ground state. Density functional calculations show that this reduction is largely the result of strong Os-O hybridization, with spin-orbit coupling responsible for only a ˜0.1 μB reduction in the moment.

  11. Two layer structure for reinforcing pothole repair

    NASA Astrophysics Data System (ADS)

    Yuan, Wei; Yuan, Kuo-Yao; Zou, Linhua; Yang, Jenn-Ming; Ju, Jiann-Wen; Kao, Wei; Carlson, Larry

    2013-04-01

    We have applied dicyclopentadiene (DCPD) resin for reinforcing pothole patch materials due to its unique properties - low cost, low viscosity at beginning and ultra-toughness after curing, chemical compatibility with tar, tunable curing profile through catalyst design. In this paper, we have designed a two layer structure - well compacted base layer and DCPD reinforced 1-1.5" top layer - for pothole repair. By choosing two graded asphalt mixes, a porous top layer and fully compacted base layer was prepared after compaction and ready for DCPD resin infiltration. The DCPD curing and infiltration profile within this porous top layer was measured with thermocouples. The rutting resistance was tested with home-made wheel rutter. The cage effect due to the p-DCPD wrapping was characterized with wheel penetration test. The results showed that this two layer structure pothole repair has greatly improved properties and can be used for pothole repair to increase the service life.

  12. Simulation of Sintering of Layered Structures

    SciTech Connect

    OLEVSKY,EUGENE; TIKARE,VEENA; GARINO,TERRY J.; BRAGINSKY,MICHAEL V.

    2000-11-22

    An integrated approach, combining the continuum theory of sintering and Potts model based mesostructure evolution analysis, is used to solve the problem of bi-layered structure sintering. Two types of bi-layered structures are considered: layers of the same material with different initial porosity, and layers of two different materials. The effective sintering stress for the bi-layer powder sintering is derived, both at the meso- and the macroscopic levels. Macroscopic shape distortions and spatial distributions of porosity are determined as functions of the dimensionless specific time of sintering. The effect of the thickness of the layers on shrinkage, warpage, and pore-grain structure is studied. Ceramic ZnO powders are employed as a model experimental system to assess the model predictions.

  13. Unraveling the Role of Monovalent Halides in Mixed-Halide Organic-Inorganic Perovskites.

    PubMed

    Deepa, Melepurath; Ramos, F Javier; Shivaprasad, S M; Ahmad, Shahzada

    2016-03-16

    The performance of perovskite solar cells is strongly influenced by the composition and microstructure of the perovskite. A recent approach to improve the power conversion efficiencies utilized mixed-halide perovskites, but the halide ions and their roles were not directly studied. Unraveling their precise location in the perovskite layer is of paramount importance. Here, we investigated four different perovskites by using X-ray photoelectron spectroscopy, and found that among the three studied mixed-halide perovskites, CH3 NH3 Pb(I0.74 Br0.26 )3 and CH3 NH3 PbBr3-x Clx show peaks that unambiguously demonstrate the presence of iodide and bromide in the former, and bromide and chloride in the latter. The CH3 NH3 PbI3-x Clx perovskite shows anomalous behavior, the iodide content far outweighs that of the chloride; a small proportion of chloride, in all likelihood, resides deep within the TiO2 /absorber layer. Our study reveals that there are many distinguishable structural differences between these perovskites, and that these directly impact the photovoltaic performances. PMID:26717046

  14. Highly stable solution processed metal-halide perovskite lasers on nanoimprinted distributed feedback structures

    NASA Astrophysics Data System (ADS)

    Brenner, Philipp; Stulz, Mareike; Kapp, Dorothee; Abzieher, Tobias; Paetzold, Ulrich W.; Quintilla, Aina; Howard, Ian A.; Kalt, Heinz; Lemmer, Uli

    2016-10-01

    We report on the performance and stability of distributed feedback lasers based on the solution-processed methylammonium lead iodide perovskite (CH3NH3PbI3). The CH3NH3PbI3 layers are processed via solution-casting in ambient atmosphere onto nanoimprinted second order Bragg gratings. This way, we achieve highly polarized surface-emitted lasing at room temperature with a linewidth of less than 0.2 nm and a laser threshold of 120 kW/cm2. The lasing is stable; no change in the laser emission within 15 h of pulsed excitation with a repetition rate of 1 kHz (corresponding to >5 × 107 pulses) is observed, exceeding the stability achieved for solution processed organic semiconductor lasers. Furthermore, adjustment of the grating period allowed the lasing wavelength to be varied over the entire bandwidth of the amplified spontaneous emission (between 781 and 794 nm). The fabrication process of nanoimprinting followed by solution-casting of the gain material demonstrates that stable CH3NH3PbI3 lasers are compatible with scalable production technologies and offers a route towards electrically pumped diode architectures.

  15. Direct observation of the ferroelectric polarization in the layered perovskite Bi4Ti3O12

    NASA Astrophysics Data System (ADS)

    Urushihara, Daisuke; Komabuchi, Mai; Ishizawa, Nobuo; Iwata, Makoto; Fukuda, Koichiro; Asaka, Toru

    2016-10-01

    We investigated the crystal structure and ferroelectric domains of Bi4Ti3O12 (BTO) by means of transmission electron microscopy (TEM) and single-crystal X-ray diffractometry. From the extinction rule, we determined that the space group in the ferroelectric phase of BTO is P1a1 rather than B2cb and B1a1 which have been proposed previously. We successfully refined the crystal structure based on the space group P1a1. The 180° and 90° ferroelectric domain structures were observed by the [001]-zone dark-field TEM imaging. In the 180° domain structure, we determined that one component of the polarization vector is parallel to the a-axis. An annular bright-field scanning transmission electron microscopy (ABF-STEM) was performed for the direct observation of the crystal structures. The ABF-STEM images displayed the contrasts with respect to every atomic position in spite of the highly distorted structure of BTO. We could evaluate the tilting and distortion of the [TiO6] octahedra relatively. Therefore, we directly observed the ferroelectric displacements of Bi and Ti ions.

  16. NaIrO3—A Pentavalent Post-perovskite

    SciTech Connect

    M Bremholm; S Dutton; P Stephens; R Cava

    2011-12-31

    Sodium iridium (V) oxide, NaIrO{sub 3}, was synthesized by a high pressure solid state method and recovered to ambient conditions. It is found to be isostructural with CaIrO{sub 3}, the much-studied structural analog of the high-pressure post-perovskite phase of MgSiO{sub 3}. Among the oxide post-perovskites, NaIrO{sub 3} is the first example with a pentavalent cation. The structure consists of layers of corner- and edge-sharing IrO{sub 6} octahedra separated by layers of NaO{sub 8} bicapped trigonal prisms. NaIrO{sub 3} shows no magnetic ordering and resistivity measurements show non-metallic behavior. The crystal structure, electrical and magnetic properties are discussed and compared to known post-perovskites and pentavalent perovskite metal oxides.

  17. Structures, Phase Transitions and Tricritical Behavior of the Hybrid Perovskite Methyl Ammonium Lead Iodide

    PubMed Central

    Whitfield, P. S.; Herron, N.; Guise, W. E.; Page, K.; Cheng, Y. Q.; Milas, I.; Crawford, M. K.

    2016-01-01

    We have examined the crystal structures and structural phase transitions of the deuterated, partially deuterated and hydrogenous organic-inorganic hybrid perovskite methyl ammonium lead iodide (MAPbI3) using time-of-flight neutron and synchrotron X-ray powder diffraction. Near 330 K the high temperature cubic phases transformed to a body-centered tetragonal phase. The variation of the order parameter Q for this transition scaled with temperature T as Q ∼ (Tc−T)β, where Tc is the critical temperature and the exponent β was close to ¼, as predicted for a tricritical phase transition. However, we also observed coexistence of the cubic and tetragonal phases over a range of temperature in all cases, demonstrating that the phase transition was in fact first-order, although still very close to tricritical. Upon cooling further, all the tetragonal phases transformed into a low temperature orthorhombic phase around 160 K, again via a first-order phase transition. Based upon these results, we discuss the impact of the structural phase transitions upon photovoltaic performance of MAPbI3 based solar cells. PMID:27767049

  18. Local structure of the metal-organic perovskite dimethylammonium manganese(ii) formate.

    PubMed

    Duncan, Helen D; Dove, Martin T; Keen, David A; Phillips, Anthony E

    2016-03-14

    We report total neutron scattering measurements on the metal-organic perovskite analogue dimethylammonium manganese(ii) formate, (CD3)2ND2[Mn(DCO2)3]. Reverse Monte Carlo modelling shows that, in both the disordered high-temperature and ordered low-temperature phases, the ammonium moiety forms substantially shorter hydrogen bonds (N...O = 2.4 Å and 2.6 Å) than are visible in the average crystal structures. These bonds result from a pincer-like motion of two adjacent formate ions about the dimethylammonium ion in such a way that the framework can adjust independently to the positions of nearest-neighbour dimethylammonium ions. At low temperatures the shortest hydrogen bond is less favourable, apparently because it involves a greater distortion of the framework. Furthermore, in the high-temperature phase, in addition to the three disordered nitrogen positions expected from the average crystal structure, there appear to be also smaller probability maxima between these positions, corresponding to orientations in which the dimethylammonium is hydrogen-bonded to the two oxygen atoms of a single formate ion. The spontaneous strain across the phase transition reveals a contraction of the framework about the dimethylammonium cation, continuing as the material is cooled below the transition temperature. These results provide direct evidence of the local atomic structure of the guest-framework hydrogen bonding, and in particular the distortions of the framework responsible for the phase transition in this system. PMID:26763144

  19. Structures, Phase Transitions and Tricritical Behavior of the Hybrid Perovskite Methyl Ammonium Lead Iodide

    DOE PAGES

    Whitfield, P. S.; Herron, N.; Guise, W. E.; Page, K.; Cheng, Y. Q.; Milas, I.; Crawford, M. K.

    2016-10-21

    Here, we examine the crystal structures and structural phase transitions of the deuterated, partially deuterated and hydrogenous organic-inorganic hybrid perovskite methyl ammonium lead iodide (MAPbI3) using time-of-flight neutron and synchrotron X-ray powder diffraction. Near 330 K the high temperature cubic phases transformed to a body-centered tetragonal phase. The variation of the order parameter Q for this transition scaled with temperature T as Q (Tc-T) , where Tc is the critical temperature and the exponent was close to , as predicted for a tricritical phase transition. We also observed coexistence of the cubic and tetragonal phases over a range of temperaturemore » in all cases, demonstrating that the phase transition was in fact first-order, although still very close to tricritical. Upon cooling further, all the tetragonal phases transformed into a low temperature orthorhombic phase around 160 K, again via a first-order phase transition. Finally, based upon these results, we discuss the impact of the structural phase transitions upon photovoltaic performance of MAPbI3 based solar cells.« less

  20. Ultrathin efficient perovskite solar cells employing a periodic structure of a composite hole conductor for elevated plasmonic light harvesting and hole collection

    NASA Astrophysics Data System (ADS)

    Long, Mingzhu; Chen, Zefeng; Zhang, Tiankai; Xiao, Yubin; Zeng, Xiaoliang; Chen, Jian; Yan, Keyou; Xu, Jianbin

    2016-03-01

    We developed a molecule/polymer composite hole transporting material (HTM) with a periodic microstructure for morphology replication of a corrugated Au electrode, which in combination plays a dual role in the optical and electronic enhancement of high performance perovskite solar cells (PSCs). The electro-optics revealed that perovskite couldn't readily extinct the red light even though the thickness increased to 370 nm, but we found that the quasi periodic microstructure composite (PMC) HTM in combination with the conformal Au electrode could promote the absorption through the enhanced cavity effects, leading to comparable absorption even using much thinner perovskite (240 nm). We identified that the cavity was the combination of Fabry-Pérot interferometer and surface plasmonic resonance, with light harvesting enhancement through surface plasmon polariton or waveguide modes that propagate in the plane of the perovskite layer. On the other hand, the PMC HTM increased hole conductivity by one order of magnitude with respect to standard spiro-OMeTAD HTM due to molecular packing and self-assembly, embodying traceable hole mobility and density elevation up to 3 times, and thus the hysteresis was greatly avoided. Owing to dual optical and electronic enhancement, the PMC PSC afforded high efficiency PSC using as thin as 240 nm perovskite layer, delivering a Voc of 1.05 V, Jsc of 22.9 mA cm-2, FF of 0.736, and efficiency amounting to 17.7% PCE, the highest efficiency with ultrathin perovskite layer.We developed a molecule/polymer composite hole transporting material (HTM) with a periodic microstructure for morphology replication of a corrugated Au electrode, which in combination plays a dual role in the optical and electronic enhancement of high performance perovskite solar cells (PSCs). The electro-optics revealed that perovskite couldn't readily extinct the red light even though the thickness increased to 370 nm, but we found that the quasi periodic microstructure

  1. Stabilization of Organic-Inorganic Perovskite Layers by Partial Substitution of Iodide by Bromide in Methylammonium Lead Iodide.

    PubMed

    Ruess, Raffael; Benfer, Felix; Böcher, Felix; Stumpp, Martina; Schlettwein, Derck

    2016-05-18

    Thin films of the methylammonium lead halides CH3 NH3 Pb(I1-x Brx )3 are prepared on fluorine-doped tin oxide substrates and exposed to humid air in the dark and under illumination. To characterize the stability of the materials, UV/Vis spectra are acquired at fixed intervals, accompanied by XRD, energy-dispersive X-ray spectroscopy, SEM, and confocal laser scanning microscopy. Different degradation mechanisms are observed depending on the environmental conditions. It is found that bromide can successfully suppress the transformation of the perovskite into the monohydrate, presumably owing to stronger hydrogen-bonding interactions with the organic cation. However, under illumination in humid air, rather rapid decomposition of the perovskites was still observed, which is due to phase segregation. The use of increased bromide content in methylammonium lead halide absorbers is discussed in terms of their application in perovskite solar cells. PMID:26853438

  2. The effect of moisture on the structures and properties of lead halide perovskites: a first-principles theoretical investigation.

    PubMed

    Zhang, Lei; Ju, Ming-Gang; Liang, WanZhen

    2016-08-17

    With efficiencies exceeding 20% and low production costs, lead halide perovskite solar cells (PSCs) have become potential candidates for future commercial applications. However, there are serious concerns about their long-term stability and environmental friendliness, heavily related to their commercial viability. Herein, we present a theoretical investigation based on the ab initio molecular dynamics (AIMD) simulations and the first-principles density functional theory (DFT) calculations to investigate the effects of sunlight and moisture on the structures and properties of MAPbI3 perovskites. AIMD simulations have been performed to simulate the impact of a few water molecules on the structures of MAPbI3 surfaces terminated in three different ways. The evolution of geometric and electronic structures as well as the absorption spectra has been shown. It is found that the PbI2-terminated surface is the most stable while both the MAI-terminated and PbI2-defective surfaces undergo structural reconstruction, leading to the formation of hydrated compounds in a humid environment. The moisture-induced weakening of photoabsorption is closely related to the formation of hydrated species, and the hydrated crystals MAPbI3·H2O and MA4PbI6·2H2O scarcely absorb the visible light. The electronic excitation in the bare and water-absorbed MAPbI3 nanoparticles tends to weaken Pb-I bonds, especially those around water molecules, and the maximal decrease of photoexcitation-induced bond order can reach up to 20% in the excited state in which the water molecules are involved in the electronic excitation, indicating the accelerated decomposition of perovskites in the presence of sunlight and moisture. This work is valuable for understanding the mechanism of chemical or photochemical instability of MAPbI3 perovskites in the presence of moisture. PMID:27499005

  3. Boosting the power conversion efficiency of perovskite solar cells using self-organized polymeric hole extraction layers with high work function.

    PubMed

    Lim, Kyung-Geun; Kim, Hak-Beom; Jeong, Jaeki; Kim, Hobeom; Kim, Jin Young; Lee, Tae-Woo

    2014-10-01

    A self-organized hole extraction layer (SOHEL) with high work function (WF) is designed for energy level alignment with the ionization potential level of CH3 NH3 PbI3 . The SOHEL increases the built-in potential, photocurrent, and power conversion efficiency (PCE) of CH3 NH3 PbI3 perovskite solar cells. Thus, interface engineering of the positive electrode of solution-processed planar heterojunction solar cells using a high-WF SOHEL is a very effective way to achieve high device efficiency (PCE = 11.7% on glass).

  4. Perovskite Solar Cells with Large-Area CVD-Graphene for Tandem Solar Cells.

    PubMed

    Lang, Felix; Gluba, Marc A; Albrecht, Steve; Rappich, Jörg; Korte, Lars; Rech, Bernd; Nickel, Norbert H

    2015-07-16

    Perovskite solar cells with transparent contacts may be used to compensate for thermalization losses of silicon solar cells in tandem devices. This offers a way to outreach stagnating efficiencies. However, perovskite top cells in tandem structures require contact layers with high electrical conductivity and optimal transparency. We address this challenge by implementing large-area graphene grown by chemical vapor deposition as a highly transparent electrode in perovskite solar cells, leading to identical charge collection efficiencies. Electrical performance of solar cells with a graphene-based contact reached those of solar cells with standard gold contacts. The optical transmission by far exceeds that of reference devices and amounts to 64.3% below the perovskite band gap. Finally, we demonstrate a four-terminal tandem device combining a high band gap graphene-contacted perovskite top solar cell (Eg = 1.6 eV) with an amorphous/crystalline silicon bottom solar cell (Eg = 1.12 eV). PMID:26266857

  5. Perovskite Solar Cells with Large-Area CVD-Graphene for Tandem Solar Cells.

    PubMed

    Lang, Felix; Gluba, Marc A; Albrecht, Steve; Rappich, Jörg; Korte, Lars; Rech, Bernd; Nickel, Norbert H

    2015-07-16

    Perovskite solar cells with transparent contacts may be used to compensate for thermalization losses of silicon solar cells in tandem devices. This offers a way to outreach stagnating efficiencies. However, perovskite top cells in tandem structures require contact layers with high electrical conductivity and optimal transparency. We address this challenge by implementing large-area graphene grown by chemical vapor deposition as a highly transparent electrode in perovskite solar cells, leading to identical charge collection efficiencies. Electrical performance of solar cells with a graphene-based contact reached those of solar cells with standard gold contacts. The optical transmission by far exceeds that of reference devices and amounts to 64.3% below the perovskite band gap. Finally, we demonstrate a four-terminal tandem device combining a high band gap graphene-contacted perovskite top solar cell (Eg = 1.6 eV) with an amorphous/crystalline silicon bottom solar cell (Eg = 1.12 eV).

  6. An easy-to-fabricate low-temperature TiO{sub 2} electron collection layer for high efficiency planar heterojunction perovskite solar cells

    SciTech Connect

    Conings, B.; Baeten, L.; Jacobs, T.; Dera, R.; D’Haen, J.; Manca, J.; Boyen, H.-G.

    2014-08-01

    Organometal trihalide perovskite solar cells arguably represent the most auspicious new photovoltaic technology so far, as they possess an astonishing combination of properties. The impressive and brisk advances achieved so far bring forth highly efficient and solution processable solar cells, holding great promise to grow into a mature technology that is ready to be embedded on a large scale. However, the vast majority of state-of-the-art perovskite solar cells contains a dense TiO{sub 2} electron collection layer that requires a high temperature treatment (>450 °C), which obstructs the road towards roll-to-roll processing on flexible foils that can withstand no more than ∼150 °C. Furthermore, this high temperature treatment leads to an overall increased energy payback time and cumulative energy demand for this emerging photovoltaic technology. Here we present the implementation of an alternative TiO{sub 2} layer formed from an easily prepared nanoparticle dispersion, with annealing needs well within reach of roll-to-roll processing, making this technology also appealing from the energy payback aspect. Chemical and morphological analysis allows to understand and optimize the processing conditions of the TiO{sub 2} layer, finally resulting in a maximum obtained efficiency of 13.6% for a planar heterojunction solar cell within an ITO/TiO{sub 2}/CH{sub 3}NH{sub 3}PbI{sub 3-x}Cl{sub x}poly(3-hexylthiophene)/Ag architecture.

  7. High performance planar p-i-n perovskite solar cells with crown-ether functionalized fullerene and LiF as double cathode buffer layers

    SciTech Connect

    Liu, Xiaodong; Zhou, Yi E-mail: songbo@suda.edu.cn Song, Bo E-mail: songbo@suda.edu.cn; Lei, Ming; Li, Yongfang E-mail: songbo@suda.edu.cn

    2015-08-10

    Double cathode buffer layers (CBLs) composed of fullerene derivative functionalized with a crown-ether end group in its side chain (denoted as PCBC) and a LiF layer were introduced between the PCBM acceptor layer and the top cathode in planar p-i-n perovskite solar cells (pero-SCs) based on CH{sub 3}NH{sub 3}PbI{sub 3−X}Cl{sub X}. The devices with the PCBC/LiF double CBLs showed significant improvements in power conversion efficiency (PCE) and long-term stability when compared to the device with LiF single CBL. Through optimizing the spin-coating speed of PCBC, a maximum PCE of 15.53% has been achieved, which is approximately 15% higher than that of the device with single LiF CBL. The remarkable improvement in PCE can be attributed to the formation of a better ohmic contact in the CBL between PCBC and LiF/Al electrode arising from the dipole moment of PCBC, leading to the enhanced fill factor and short-circuit current density (J{sub sc}). Besides the PCE, the long-term stability of the devices with PCBC interlayer is also superior to that of the device with LiF single CBL, which is due to the more effective protection for the perovskite/PCBM interface.

  8. An ultra-thin, un-doped NiO hole transporting layer of highly efficient (16.4%) organic-inorganic hybrid perovskite solar cells.

    PubMed

    Seo, Seongrok; Park, Ik Jae; Kim, Myungjun; Lee, Seonhee; Bae, Changdeuck; Jung, Hyun Suk; Park, Nam-Gyu; Kim, Jin Young; Shin, Hyunjung

    2016-06-01

    NiO is a wide band gap p-type oxide semiconductor and has potential for applications in solar energy conversion as a hole-transporting layer (HTL). It also has good optical transparency and high chemical stability, and the capability of aligning the band edges to the perovskite (CH3NH3PbI3) layers. Ultra-thin and un-doped NiO films with much less absorption loss were prepared by atomic layer deposition (ALD) with highly precise control over thickness without any pinholes. Thin enough (5-7.5 nm in thickness) NiO films with the thickness of few time the Debye length (LD = 1-2 nm for NiO) show enough conductivities achieved by overlapping space charge regions. The inverted planar perovskite solar cells with NiO films as HTLs exhibited the highest energy conversion efficiency of 16.40% with high open circuit voltage (1.04 V) and fill factor (0.72) with negligible current-voltage hysteresis.

  9. An easy-to-fabricate low-temperature TiO2 electron collection layer for high efficiency planar heterojunction perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Conings, B.; Baeten, L.; Jacobs, T.; Dera, R.; D'Haen, J.; Manca, J.; Boyen, H.-G.

    2014-08-01

    Organometal trihalide perovskite solar cells arguably represent the most auspicious new photovoltaic technology so far, as they possess an astonishing combination of properties. The impressive and brisk advances achieved so far bring forth highly efficient and solution processable solar cells, holding great promise to grow into a mature technology that is ready to be embedded on a large scale. However, the vast majority of state-of-the-art perovskite solar cells contains a dense TiO2 electron collection layer that requires a high temperature treatment (>450 °C), which obstructs the road towards roll-to-roll processing on flexible foils that can withstand no more than ˜150 °C. Furthermore, this high temperature treatment leads to an overall increased energy payback time and cumulative energy demand for this emerging photovoltaic technology. Here we present the implementation of an alternative TiO2 layer formed from an easily prepared nanoparticle dispersion, with annealing needs well within reach of roll-to-roll processing, making this technology also appealing from the energy payback aspect. Chemical and morphological analysis allows to understand and optimize the processing conditions of the TiO2 layer, finally resulting in a maximum obtained efficiency of 13.6% for a planar heterojunction solar cell within an ITO/TiO2/CH3NH3PbI3-xClxpoly(3-hexylthiophene)/Ag architecture.

  10. An ultra-thin, un-doped NiO hole transporting layer of highly efficient (16.4%) organic-inorganic hybrid perovskite solar cells.

    PubMed

    Seo, Seongrok; Park, Ik Jae; Kim, Myungjun; Lee, Seonhee; Bae, Changdeuck; Jung, Hyun Suk; Park, Nam-Gyu; Kim, Jin Young; Shin, Hyunjung

    2016-06-01

    NiO is a wide band gap p-type oxide semiconductor and has potential for applications in solar energy conversion as a hole-transporting layer (HTL). It also has good optical transparency and high chemical stability, and the capability of aligning the band edges to the perovskite (CH3NH3PbI3) layers. Ultra-thin and un-doped NiO films with much less absorption loss were prepared by atomic layer deposition (ALD) with highly precise control over thickness without any pinholes. Thin enough (5-7.5 nm in thickness) NiO films with the thickness of few time the Debye length (LD = 1-2 nm for NiO) show enough conductivities achieved by overlapping space charge regions. The inverted planar perovskite solar cells with NiO films as HTLs exhibited the highest energy conversion efficiency of 16.40% with high open circuit voltage (1.04 V) and fill factor (0.72) with negligible current-voltage hysteresis. PMID:27216291

  11. Laser Crystallization of Organic-Inorganic Hybrid Perovskite Solar Cells.

    PubMed

    Jeon, Taewoo; Jin, Hyeong Min; Lee, Seung Hyun; Lee, Ju Min; Park, Hyung Il; Kim, Mi Kyung; Lee, Keon Jae; Shin, Byungha; Kim, Sang Ouk

    2016-08-23

    Organic-inorganic hybrid perovskites attract enormous research interest for next generation solar energy harvest. Synergistic crystalline structures comprising organic and inorganic components enable solution processing of perovskite films. A reliable crystallization method for perovskites, compatible with fast continuous process over large-area flexible substrates, is crucial for high performance solar cell production. Here, we present laser crystallization of hybrid perovskite solar cells using near-infrared (NIR) laser (λ = 1064 nm). Crystalline morphology of CH3NH3PbI3 (MAPbI3) perovskite films are widely controllable with laser irradiation condition while maintaining film uniformity. Photothermal heating effectively assisted by interfacial photoconversion layers is critical for phase transformation without beam damage of multilayered device structures. Notably, laser crystallization attains higher device performances than conventional thermal annealing. Fast laser crystallization with manufacture level scan rate (1 m min(-1)) demonstrates inverted-type perovskite solar cells with 11.3 and 8.0% efficiencies on typical glass and flexible polymer substrates, respectively, without rigorous device optimization.

  12. Laser Crystallization of Organic-Inorganic Hybrid Perovskite Solar Cells.

    PubMed

    Jeon, Taewoo; Jin, Hyeong Min; Lee, Seung Hyun; Lee, Ju Min; Park, Hyung Il; Kim, Mi Kyung; Lee, Keon Jae; Shin, Byungha; Kim, Sang Ouk

    2016-08-23

    Organic-inorganic hybrid perovskites attract enormous research interest for next generation solar energy harvest. Synergistic crystalline structures comprising organic and inorganic components enable solution processing of perovskite films. A reliable crystallization method for perovskites, compatible with fast continuous process over large-area flexible substrates, is crucial for high performance solar cell production. Here, we present laser crystallization of hybrid perovskite solar cells using near-infrared (NIR) laser (λ = 1064 nm). Crystalline morphology of CH3NH3PbI3 (MAPbI3) perovskite films are widely controllable with laser irradiation condition while maintaining film uniformity. Photothermal heating effectively assisted by interfacial photoconversion layers is critical for phase transformation without beam damage of multilayered device structures. Notably, laser crystallization attains higher device performances than conventional thermal annealing. Fast laser crystallization with manufacture level scan rate (1 m min(-1)) demonstrates inverted-type perovskite solar cells with 11.3 and 8.0% efficiencies on typical glass and flexible polymer substrates, respectively, without rigorous device optimization. PMID:27377145

  13. Correlating structure and electronic band-edge properties in organolead halide perovskites nanoparticles.

    PubMed

    Zhu, Qiushi; Zheng, Kaibo; Abdellah, Mohamed; Generalov, Alexander; Haase, Dörthe; Carlson, Stefan; Niu, Yuran; Heimdal, Jimmy; Engdahl, Anders; Messing, Maria E; Pullerits, Tonu; Canton, Sophie E

    2016-06-01

    After having emerged as primary contenders in the race for highly efficient optoelectronics materials, organolead halide perovskites (OHLP) are now being investigated in the nanoscale regime as promising building blocks with unique properties. For example, unlike their bulk counterpart, quantum dots of OHLP are brightly luminescent, owing to large exciton binding energies that cannot be rationalized solely on the basis of quantum confinement. Here, we establish the direct correlation between the structure and the electronic band-edge properties of CH3NH3PbBr3 nanoparticles. Complementary structural and spectroscopic measurements probing long-range and local order reveal that lattice strain influences the nature of the valence band and modifies the subtle stereochemical activity of the Pb(2+) lone-pair. More generally, this work demonstrates that the stereochemical activity of the lone-pair at the metal site is a specific physicochemical parameter coupled to composition, size and strain, which can be employed to engineer novel functionalities in OHLP nanomaterials. PMID:27189431

  14. Structural and magnetic properties of double perovskite oxide Ba2CeSbO6

    NASA Astrophysics Data System (ADS)

    Dutta, Alo; Mukhopadhyay, P. K.; Sinha, T. P.; Das, Dipankar; Shannigrahi, Santiranjan

    2016-08-01

    The structural and magnetic properties of a double perovskite oxide Ba2CeSbO6 (BCSO) synthesized by solid state reaction technique have been investigated. The Rietveld refinement of the X-ray diffraction pattern of BCSO suggests the monoclinic crystal structure at room temperature with P21/n space group. The vibrational properties of BCSO are investigated by the Fourier transform Infrared and Raman spectroscopy. The Raman spectrum confirms the B-site ordering of cations in BCSO. The temperature dependent magnetic susceptibility data in the field cooled mode show the anti-ferromagnetic behaviour of BCSO below 59 K. The core level X-ray photoemission (XPS) spectrum of Ce-3d and Sb-3d states confirms the presence of multiple oxidation states of these cations. The presence of both the Ce3+ and Ce4+ ions in BCSO gives the 4f4-δ intermediate valence state which may reduce the effective magnetic moment with respect to the system having single valence Ce3+ ion.

  15. Pressure-Induced Structural and Optical Properties of Organometal Halide Perovskite-Based Formamidinium Lead Bromide.

    PubMed

    Wang, Lingrui; Wang, Kai; Zou, Bo

    2016-07-01

    Organometal halide perovskites (OMHPs) are attracting an ever-growing scientific interest as photovoltaic materials with moderate cost and compelling properties. In this Letter, pressure-induced optical and structural changes of OMHP-based formamidinium lead bromide (FAPbBr3) were systematically investigated. We studied the pressure dependence of optical absorption and photoluminescence, both of which showed piezochromism. Synchrotron X-ray diffraction indicated that FAPbBr3 underwent two phase transitions and subsequent amorphization, leading directly to the bandgap evolution with redshift followed by blueshift during compression. Raman experiments illustrated the high pressure behavior of organic cation and the surrounding inorganic octahedra. Additionally, the effect of cation size and the different intermolecular interactions between organic cation and inorganic octahedra result in the fact that FAPbBr3 is less compressible than the reported methylammonium lead bromide (MAPbBr3). High pressure studies of the structural evolution and optical properties of OMHPs provide important clues in optimizing photovoltaic performance and help to design novel OMHPs with higher stimuli-resistant ability. PMID:27321024

  16. Power Conversion Efficiency and Device Stability Improvement of Inverted Perovskite Solar Cells by Using a ZnO:PFN Composite Cathode Buffer Layer.

    PubMed

    Jia, Xiaorui; Zhang, Lianping; Luo, Qun; Lu, Hui; Li, Xueyuan; Xie, Zhongzhi; Yang, Yongzhen; Li, Yan-Qing; Liu, Xuguang; Ma, Chang-Qi

    2016-07-20

    We have demonstrated in this article that both power conversion efficiency (PCE) and performance stability of inverted planar heterojunction perovskite solar cells can be improved by using a ZnO:PFN nanocomposite (PFN: poly[(9,9-bis(3'-(N,N-dimethylamion)propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctyl)-fluorene]) as the cathode buffer layer (CBL). This nanocomposite could form a compact and defect-less CBL film on the perovskite/PC61BM surface (PC61BM: phenyl-C61-butyric acid methyl ester). In addition, the high conductivity of the nanocomposite layer makes it works well at a layer thickness of 150 nm. Both advantages of the composite layer are helpful in reducing interface charge recombination and improving device performance. The power conversion efficiency (PCE) of the best ZnO:PFN CBL based device was measured to be 12.76%, which is higher than that of device without CBL (9.00%), or device with ZnO (7.93%) or PFN (11.30%) as the cathode buffer layer. In addition, the long-term stability is improved by using ZnO:PFN composite cathode buffer layer when compare to that of the reference cells. Almost no degradation of open circuit voltage (VOC) and fill factor (FF) was found for the device having ZnO:PFN, suggesting that ZnO:PFN is able to stabilize the interface property and consequently improve the solar cell performance stability. PMID:27349330

  17. The Kinematics of Turbulent Boundary Layer Structure

    NASA Technical Reports Server (NTRS)

    Robinson, Stephen Kern

    1991-01-01

    The long history of research into the internal structure of turbulent boundary layers has not provided a unified picture of the physics responsible for turbulence production and dissipation. The goals of the present research are to: (1) define the current state of boundary layer structure knowledge; and (2) utilize direct numerical simulation results to help close the unresolved issues identified in part A and to unify the fragmented knowledge of various coherent motions into a consistent kinematic model of boundary layer structure. The results of the current study show that all classes of coherent motion in the low Reynolds number turbulent boundary layer may be related to vortical structures, but that no single form of vortex is representative of the wide variety of vortical structures observed. In particular, ejection and sweep motions, as well as entrainment from the free-streem are shown to have strong spatial and temporal relationships with vortical structures. Disturbances of vortex size, location, and intensity show that quasi-streamwise vortices dominate the buffer region, while transverse vortices and vortical arches dominate the wake region. Both types of vortical structure are common in the log region. The interrelationships between the various structures and the population distributions of vortices are combined into a conceptual kinematic model for the boundary layer. Aspects of vortical structure dynamics are also postulated, based on time-sequence animations of the numerically simulated flow.

  18. Structure and properties of epitaxial perovskite Pb(Zr0.52Ti0.48)O3/La0.7Sr0.3MnO3 heterostructures

    NASA Astrophysics Data System (ADS)

    Zou, Cheng; Chen, Yuan-Fu; Li, Ping-Jian; Fan, Rui; Peng, Bing; Zhang, Wen-Xu; Wang, Ze-Gao; Hao, Xin; Liu, Jing-Bo; Zhang, Wan-Li; Li, Yan-Rong; Li, Run-Wei

    2012-04-01

    The morphology, crystalline structure of epitaxial heterostructures of Pb(Zr0.52Ti0.48)O3/La0.7Sr0.3MnO3 (PZT/LSMO) grown on single crystalline SrTiO3 substrates by pulse laser deposition (PLD), have been investigated. The morphology results show that the LSMO layers and PZT layers are smooth and homogenous. The crystalline structure measurements indicate that good epitaxial relationships between LSMO and PZT and STO were obtained. The effects of applied electric and magnetic fields on the physical properties of epitaxial perovskite ferroelectric/ferromagnetic heterostructures were investigated. The results show that the polarized electric field has a very significant influence on the transport properties of LSMO layers while has little influence on the magnetization, and the magnetic field has an obvious influence on the ferroelectric behavior of the PZT layer.

  19. Efficient light-emitting diodes based on nanocrystalline perovskite in a dielectric polymer matrix.

    PubMed

    Li, Guangru; Tan, Zhi-Kuang; Di, Dawei; Lai, May Ling; Jiang, Lang; Lim, Jonathan Hua-Wei; Friend, Richard H; Greenham, Neil C

    2015-04-01

    Electroluminescence in light-emitting devices relies on the encounter and radiative recombination of electrons and holes in the emissive layer. In organometal halide perovskite light-emitting diodes, poor film formation creates electrical shunting paths, where injected charge carriers bypass the perovskite emitter, leading to a loss in electroluminescence yield. Here, we report a solution-processing method to block electrical shunts and thereby enhance electroluminescence quantum efficiency in perovskite devices. In this method, a blend of perovskite and a polyimide precursor dielectric (PIP) is solution-deposited to form perovskite nanocrystals in a thin-film matrix of PIP. The PIP forms a pinhole-free charge-blocking layer, while still allowing the embedded perovskite crystals to form electrical contact with the electron- and hole-injection layers. This modified structure reduces nonradiative current losses and improves quantum efficiency by 2 orders of magnitude, giving an external quantum efficiency of 1.2%. This simple technique provides an alternative route to circumvent film formation problems in perovskite optoelectronics and offers the possibility of flexible and high-performance light-emitting displays.

  20. Structure of the low latitude boundary layer

    NASA Technical Reports Server (NTRS)

    Sckopke, N.; Paschmann, G.; Haerendel, G.; Sonnerup, B. U. O.; Bame, S. J.; Forbes, T. G.; Hones, E. W., Jr.; Russell, C. T.

    1980-01-01

    Observations at high temporal resolution of the frontside magnetopause and plasma boundary layer, made with the LASL/MPE fast plasma analyzer onboard the ISEE 1 and 2 spacecraft, revealed a complex quasiperiodic structure of some of the observed boundary layers. A cool tailward streaming boundary layer plasma was seen intermittently, with intervening periods of hot tenuous plasma which has properties similar to the magnetospheric population. While individual encounters with the boundary layer plasma last only a few minutes, the total observation time may extend over one hour or more.

  1. Multilayer Transparent Top Electrode for Solution Processed Perovskite/Cu(In,Ga)(Se,S)2 Four Terminal Tandem Solar Cells.

    PubMed

    Yang, Yang Michael; Chen, Qi; Hsieh, Yao-Tsung; Song, Tze-Bin; Marco, Nicholas De; Zhou, Huanping; Yang, Yang

    2015-07-28

    Halide perovskites (PVSK) have attracted much attention in recent years due to their high potential as a next generation solar cell material. To further improve perovskites progress toward a state-of-the-art technology, it is desirable to create a tandem structure in which perovskite may be stacked with a current prevailing solar cell such as silicon (Si) or Cu(In,Ga)(Se,S)2 (CIGS). The transparent top electrode is one of the key components as well as challenges to realize such tandem structure. Herein, we develop a multilayer transparent top electrode for perovskite photovoltaic devices delivering an 11.5% efficiency in top illumination mode. The transparent electrode is based on a dielectric/metal/dielectric structure, featuring an ultrathin gold seeded silver layer. A four terminal tandem solar cell employing solution processed CIGS and perovskite cells is also demonstrated with over 15% efficiency.

  2. Aluminum in magnesium silicate perovskite: Formation, structure, and energetics of magnesium-rich defect solid solutions

    NASA Astrophysics Data System (ADS)

    Navrotsky, Alexandra; Schoenitz, Mirko; Kojitani, Hiroshi; Xu, Hongwu; Zhang, Jianzhong; Weidner, Donald J.; Jeanloz, Raymond

    2003-07-01

    MgSiO3-rich perovskite is expected to dominate Earth's lower mantle (pressures >25 GPa) with iron and aluminum as significant substituents. The incorporation of trivalent ions, M3+, may occur by two competing mechanisms: MgA + SiB = MA + MB and SiB = AlB + 0.5 (vacancy)O. Phase synthesis studies show that both substitutions do occur and the nonstoichiometric or defect substitution is prevalent along the MgSiO3-MgAlO2.5 join. Lattice parameters associated with the first substitution (stoichiometric) show more rapid increases with increasing Al content than those for the second substitution (nonstoichiometric), consistent with the differences in size of substituting ions. Oxide melt solution calorimetry has been used to compare the energetics of both substitutions. The stoichiometric substitution, represented by the reaction 0.95 MgSiO3 (perovskite) + 0.05 Al2O3 (corundum) = Mg0.95Al0.10Si0.95O3 (perovskite), has an enthalpy of -0.8 ± 2.2 kJ/mol. The nonstoichiometric reaction, 0.90 MgSiO3 (perovskite) + 0.10 MgO (rocksalt) + 0.05 Al2O3 (corundum) = MgSi0.9Al0.1O2.95 (perovskite) has a small positive enthalpy of 8.5 ± 4.6 kJ/mol. Configurational T ΔS terms play a role in both substitutions. The defect substitution is not prohibitive in enthalpy, entropy, or volume, is favored in perovskite coexisting with magnesiowüstite and may significantly affect the elasticity, rheology, and water retention of silicate perovskite in Earth.

  3. Self-formed grain boundary healing layer for highly efficient CH3 NH3 PbI3 perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Son, Dae-Yong; Lee, Jin-Wook; Choi, Yung Ji; Jang, In-Hyuk; Lee, Seonhee; Yoo, Pil J.; Shin, Hyunjung; Ahn, Namyoung; Choi, Mansoo; Kim, Dongho; Park, Nam-Gyu

    2016-07-01

    Perovskite solar cells have attracted significant research efforts due to their remarkable performance, with certified power conversion efficiency now reaching 22%. Solution-processed perovskite thin films are polycrystalline, and grain boundaries are thought to be responsible for causing recombination and trapping of charge carriers. Here we report an effective and reproducible way of treating grain boundaries in CH3NH3PbI3 films deposited by means of a Lewis acid-base adduct approach. We show by high-resolution transmission electron microscopy lattice images that adding 6 mol% excess CH3NH3I to the precursor solution resulted in a CH3NH3I layer forming at the grain boundaries. This layer is responsible for suppressing non-radiative recombination and improving hole and electron extraction at the grain boundaries by forming highly ionic-conducting pathways. We report an average power conversion efficiency of 20.1% over 50 cells (best cell at 20.4%) together with significantly reduced current-voltage hysteresis achieved by this grain boundary healing process.

  4. Self-formed grain boundary healing layer for highly efficient CH3 NH3 PbI3 perovskite solar cells

    NASA Astrophysics Data System (ADS)

    Son, Dae-Yong; Lee, Jin-Wook; Choi, Yung Ji; Jang, In-Hyuk; Lee, Seonhee; Yoo, Pil J.; Shin, Hyunjung; Ahn, Namyoung; Choi, Mansoo; Kim, Dongho; Park, Nam-Gyu

    2016-07-01

    Perovskite solar cells have attracted significant research efforts due to their remarkable performance, with certified power conversion efficiency now reaching 22%. Solution-processed perovskite thin films are polycrystalline, and grain boundaries are thought to be responsible for causing recombination and trapping of charge carriers. Here we report an effective and reproducible way of treating grain boundaries in CH3NH3PbI3 films deposited by means of a Lewis acid–base adduct approach. We show by high-resolution transmission electron microscopy lattice images that adding 6 mol% excess CH3NH3I to the precursor solution resulted in a CH3NH3I layer forming at the grain boundaries. This layer is responsible for suppressing non-radiative recombination and improving hole and electron extraction at the grain boundaries by forming highly ionic-conducting pathways. We report an average power conversion efficiency of 20.1% over 50 cells (best cell at 20.4%) together with significantly reduced current–voltage hysteresis achieved by this grain boundary healing process.

  5. Perovskites: transforming photovoltaics, a mini-review

    NASA Astrophysics Data System (ADS)

    Chilvery, Ashwith Kumar; Batra, Ashok K.; Yang, Bin; Xiao, Kai; Guggilla, Padmaja; Aggarwal, Mohan D.; Surabhi, Raja; Lal, Ravi B.; Currie, James R.; Penn, Benjamin G.

    2015-01-01

    The recent power-packed advent of perovskite solar cells is transforming photovoltaics (PV) with their superior efficiencies, ease of fabrication, and cost. This perovskite solar cell further boasts of many unexplored features that can further enhance its PV properties and lead to it being branded as a successful commercial product. This article provides a detailed insight of the organometal halide based perovskite structure, its unique stoichiometric design, and its underlying principles for PV applications. The compatibility of various PV layers and its fabrication methods is also discussed.

  6. Selective Precipitation and Concentrating of Perovskite Crystals from Titanium-Bearing Slag Melt in Supergravity Field

    NASA Astrophysics Data System (ADS)

    Gao, Jintao; Zhong, Yiwei; Guo, Zhancheng

    2016-08-01

    Selective precipitation and concentrating of perovskite crystals from titanium-bearing slag melt in the supergravity field was investigated in this study. Since perovskite was the first precipitated phase from the slag melt during the cooling process, and a greater precipitation quantity and larger crystal sizes of perovskite were obtained at 1593 K to 1563 K (1320 °C to 1290 °C), concentrating of perovskite crystals from the slag melt was carried out at this temperature range in the supergravity field, at which the perovskite transforms into solid particles while the other minerals remain in the liquid melt. The layered structures appeared significantly in the sample obtained by supergravity treatment, and all the perovskite crystals moved along the supergravity direction and concentrated as the perovskite-rich phase in the bottom area, whereas the molten slag concentrated in the upper area along the opposite direction, in which it was impossible to find any perovskite crystals. With the gravity coefficient of G = 750, the mass fraction of TiO2 in the perovskite-rich phase was up to 34.65 wt pct, whereas that of the slag phase was decreased to 12.23 wt pct, and the recovery ratio of Ti in the perovskite-rich phase was up to 75.28 pct. On this basis, an amplification experimental centrifugal apparatus was exploited and the continuous experiment with larger scale was further carried out, the results confirming that selective precipitation and concentrating of perovskite crystals from the titanium-bearing slag melt by supergravity was a feasible method.

  7. Device modeling of perovskite solar cells based on structural similarity with thin film inorganic semiconductor solar cells

    NASA Astrophysics Data System (ADS)

    Minemoto, Takashi; Murata, Masashi

    2014-08-01

    Device modeling of CH3NH3PbI3-xCl3 perovskite-based solar cells was performed. The perovskite solar cells employ a similar structure with inorganic semiconductor solar cells, such as Cu(In,Ga)Se2, and the exciton in the perovskite is Wannier-type. We, therefore, applied one-dimensional device simulator widely used in the Cu(In,Ga)Se2 solar cells. A high open-circuit voltage of 1.0 V reported experimentally was successfully reproduced in the simulation, and also other solar cell parameters well consistent with real devices were obtained. In addition, the effect of carrier diffusion length of the absorber and interface defect densities at front and back sides and the optimum thickness of the absorber were analyzed. The results revealed that the diffusion length experimentally reported is long enough for high efficiency, and the defect density at the front interface is critical for high efficiency. Also, the optimum absorber thickness well consistent with the thickness range of real devices was derived.

  8. Atomic Layer Deposition of TiO2 for a High-Efficiency Hole-Blocking Layer in Hole-Conductor-Free Perovskite Solar Cells Processed in Ambient Air.

    PubMed

    Hu, Hang; Dong, Binghai; Hu, Huating; Chen, Fengxiang; Kong, Mengqin; Zhang, Qiuping; Luo, Tianyue; Zhao, Li; Guo, Zhiguang; Li, Jing; Xu, Zuxun; Wang, Shimin; Eder, Dominik; Wan, Li

    2016-07-20

    In this study we design and construct high-efficiency, low-cost, highly stable, hole-conductor-free, solid-state perovskite solar cells, with TiO2 as the electron transport layer (ETL) and carbon as the hole collection layer, in ambient air. First, uniform, pinhole-free TiO2 films of various thicknesses were deposited on fluorine-doped tin oxide (FTO) electrodes by atomic layer deposition (ALD) technology. Based on these TiO2 films, a series of hole-conductor-free perovskite solar cells (PSCs) with carbon as the counter electrode were fabricated in ambient air, and the effect of thickness of TiO2 compact film on the device performance was investigated in detail. It was found that the performance of PSCs depends on the thickness of the compact layer due to the difference in surface roughness, transmittance, charge transport resistance, electron-hole recombination rate, and the charge lifetime. The best-performance devices based on optimized TiO2 compact film (by 2000 cycles ALD) can achieve power conversion efficiencies (PCEs) of as high as 7.82%. Furthermore, they can maintain over 96% of their initial PCE after 651 h (about 1 month) storage in ambient air, thus exhibiting excellent long-term stability.

  9. Atomic Layer Deposition of TiO2 for a High-Efficiency Hole-Blocking Layer in Hole-Conductor-Free Perovskite Solar Cells Processed in Ambient Air.

    PubMed

    Hu, Hang; Dong, Binghai; Hu, Huating; Chen, Fengxiang; Kong, Mengqin; Zhang, Qiuping; Luo, Tianyue; Zhao, Li; Guo, Zhiguang; Li, Jing; Xu, Zuxun; Wang, Shimin; Eder, Dominik; Wan, Li

    2016-07-20

    In this study we design and construct high-efficiency, low-cost, highly stable, hole-conductor-free, solid-state perovskite solar cells, with TiO2 as the electron transport layer (ETL) and carbon as the hole collection layer, in ambient air. First, uniform, pinhole-free TiO2 films of various thicknesses were deposited on fluorine-doped tin oxide (FTO) electrodes by atomic layer deposition (ALD) technology. Based on these TiO2 films, a series of hole-conductor-free perovskite solar cells (PSCs) with carbon as the counter electrode were fabricated in ambient air, and the effect of thickness of TiO2 compact film on the device performance was investigated in detail. It was found that the performance of PSCs depends on the thickness of the compact layer due to the difference in surface roughness, transmittance, charge transport resistance, electron-hole recombination rate, and the charge lifetime. The best-performance devices based on optimized TiO2 compact film (by 2000 cycles ALD) can achieve power conversion efficiencies (PCEs) of as high as 7.82%. Furthermore, they can maintain over 96% of their initial PCE after 651 h (about 1 month) storage in ambient air, thus exhibiting excellent long-term stability. PMID:27340730

  10. Hexagonal β-NaYF4:Yb(3+), Er(3+) Nanoprism-Incorporated Upconverting Layer in Perovskite Solar Cells for Near-Infrared Sunlight Harvesting.

    PubMed

    Roh, Jongmin; Yu, Haejun; Jang, Jyongsik

    2016-08-10

    Hexagonal β-NaYF4:Yb(3+), Er(3+) nanoprisms, successfully prepared using a hydrothermal method, were incorporated into CH3NH3PbI3 perovskite solar cells (PSCs) as an upconverting mesoporous layer. Due to their near-infrared (NIR) sunlight harvesting, the PSCs based on the upconverting mesoporous layer exhibited a power conversion efficiency of 16.0%, an increase of 13.7% compared with conventional TiO2 nanoparticle-based PSCs (14.1%). This result suggests that the hexagonal β-NaYF4:Yb(3+), Er(3+) nanoprisms expand the absorption range of the PSC via upconversion photoluminescence, leading to an enhancement of the photocurrent. PMID:27472304

  11. Structure of relaminarizing turbulent boundary layers

    NASA Astrophysics Data System (ADS)

    Ramesh, O.; Patwardhan, Saurabh

    2014-11-01

    Relaminarization of a turbulent boundary layer in a strongly accelerated flow has received a great attention in recent times. It has been found that such relaminarization is a general and regularly occurring phenomenon in the leading-edge region of a swept wing of an airplane (van Dam et al., 1993). In this work, we investigate the effect of initial Reynolds number on the process of relaminarization in turbulent boundary layers. The experimental and numerical investigation of relaminarizing turbulent boundary layers undergoing same history reveals that the boundary layer with higher initial Reynolds number relaminarizes at a lower pressure gradient value compared to the one with lower Reynolds number. This effect can be explained on the inviscid theory proposed earlier in the literature. Further, various parameter criteria proposed to predict relaminarization, are assessed and the structure of relaminarizing boundary layers is investigated. A mechanism for stabilization of near-wall low speed streaks is proposed.

  12. Temperature structure in the atmospheric boundary layer

    NASA Astrophysics Data System (ADS)

    Smedman, Ann-Sofi

    2010-05-01

    Temperature structure in the atmospheric boundary layer It is well established from experimental and theoretical studies that the temperature structure in the atmospheric boundary layer is depends on stability. During free convection conditions the flow is dominated by circular thermals but when stratification is becoming slightly unstable longitudinal roll structures that extend vertically throughout the entire boundary layer will be present. In close to neutral conditions on the unstable side (the UVCN regime) when the Obukhov length is much greater than the surface layer depth, it is observed that the structure of the surface layer turbulence does not accord with standard similarity theory. In particular the efficiency of the turbulent exchange of sensible and latent heat is observed to be more strongly enhanced than is consistent with the standard model. Also the profiles of dissipation of turbulent kinetic energy and temperature fluctuation variance are found to depend on the structure of the whole boundary layer (i.e. are non-local), indicating that a large-scale transport process is at work. At the same time, co-spectral analysis shows how the large scale eddy motions that determine the heat transport process near the surface are typically 1/5 of the surface layer depth. All these features are found to be similar in measurements at two marine sites, in the Baltic Sea and in Lake Ontario respectively and at several flat land sites ( around Uppsala and at the Island of Gotland), indicating that they are determined by the dynamics of the whole boundary layer rather than being simply dependent on the surface boundary conditions. The observed structures can also be interpreted as possible manifestations of a bifurcation of the large scale eddy structure towards a state in which there are quasi-steady longitudinal rolls and, on a smaller scale, unsteady detached eddies. Our interpretation of the results from the measurements is that, in the UVCN regime, the latter

  13. Ultrathin efficient perovskite solar cells employing a periodic structure of a composite hole conductor for elevated plasmonic light harvesting and hole collection.

    PubMed

    Long, Mingzhu; Chen, Zefeng; Zhang, Tiankai; Xiao, Yubin; Zeng, Xiaoliang; Chen, Jian; Yan, Keyou; Xu, Jianbin

    2016-03-28

    We developed a molecule/polymer composite hole transporting material (HTM) with a periodic microstructure for morphology replication of a corrugated Au electrode, which in combination plays a dual role in the optical and electronic enhancement of high performance perovskite solar cells (PSCs). The electro-optics revealed that perovskite couldn't readily extinct the red light even though the thickness increased to 370 nm, but we found that the quasi periodic microstructure composite (PMC) HTM in combination with the conformal Au electrode could promote the absorption through the enhanced cavity effects, leading to comparable absorption even using much thinner perovskite (240 nm). We identified that the cavity was the combination of Fabry-Pérot interferometer and surface plasmonic resonance, with light harvesting enhancement through surface plasmon polariton or waveguide modes that propagate in the plane of the perovskite layer. On the other hand, the PMC HTM increased hole conductivity by one order of magnitude with respect to standard spiro-OMeTAD HTM due to molecular packing and self-assembly, embodying traceable hole mobility and density elevation up to 3 times, and thus the hysteresis was greatly avoided. Owing to dual optical and electronic enhancement, the PMC PSC afforded high efficiency PSC using as thin as 240 nm perovskite layer, delivering a V(oc) of 1.05 V, J(sc) of 22.9 mA cm(-2), FF of 0.736, and efficiency amounting to 17.7% PCE, the highest efficiency with ultrathin perovskite layer. PMID:26377231

  14. Cobalt based layered perovskites as cathode material for intermediate temperature Solid Oxide Fuel Cells: A brief review

    NASA Astrophysics Data System (ADS)

    Pelosato, Renato; Cordaro, Giulio; Stucchi, Davide; Cristiani, Cinzia; Dotelli, Giovanni

    2015-12-01

    Nowadays, the cathode is the most studied component in Intermediate Temperature-Solid Oxide Fuel Cells (IT-SOFCs). Decreasing SOFCs operating temperature implies slow oxygen reduction kinetics and large polarization losses. Double perovskites with general formula REBaCo2O5+δ are promising mixed ionic-electronic conductors, offering a remarkable enhancement of the oxygen diffusivity and surface exchange respect to disordered perovskites. In this review, more than 250 compositions investigated in the literature were analyzed. The evaluation was performed in terms of electrical conductivity, Area Specific Resistance (ASR), chemical compatibility with electrolytes and Thermal Expansion Coefficient (TEC). The most promising materials have been identified as those bearing the mid-sized rare earths (Pr, Nd, Sm, Gd). Doping strategies have been analyzed: Sr doping on A site promotes higher electrical conductivity, but worsen ASR and TECs; B-site doping (Fe, Ni, Mn) helps lowering TECs, but is detrimental for the electrochemical properties. A promising boost of the electrochemical activity is obtained by simply introducing a slight Ba under-stoichiometry. Still, the high sensitivity of the electrochemical properties against slight changes in the stoichiometry hamper a conclusive comparison of all the investigated compounds. Opportunities for an improvement of double perovskite cathodes performance is tentatively foreseen in combining together the diverse effective doping strategies.

  15. Employing PEDOT as the p-Type Charge Collection Layer in Regular Organic-Inorganic Perovskite Solar Cells.

    PubMed

    Liu, Jiewei; Pathak, Sandeep; Stergiopoulos, Thomas; Leijtens, Tomas; Wojciechowski, Konrad; Schumann, Stefan; Kausch-Busies, Nina; Snaith, Henry J

    2015-05-01

    Organic-inorganic halide perovskite solar cells have recently emerged as high-performance photovoltaic devices with low cost, promising for affordable large-scale energy production, with laboratory cells already exceeding 20% power conversion efficiency (PCE). To date, a relatively expensive organic hole-conducting molecule with low conductivity, namely spiro-OMeTAD (2,2',7,7'-tetrakis(N,N-di-p-methoxyphenyl-amine) 9,9'- spirobifluorene), is employed widely to achieve highly efficient perovskite solar cells. Here, we report that by replacing spiro-OMeTAD with much cheaper and highly conductive poly(3,4-ethylenedioxythiophene) (PEDOT) we can achieve PCE of up to 14.5%, with PEDOT cast from a toluene based ink. However, the stabilized power output of the PEDOT-based devices is only 6.6%, in comparison to 9.4% for the spiro-OMeTAD-based cells. We deduce that accelerated recombination is the cause for this lower stabilized power output and postulate that reduced levels of p-doping are required to match the stabilized performance of Spiro-OMeTAD. The entirely of the materials employed in the perovskite solar cell are now available at commodity scale and extremely inexpensive.

  16. Investigations of the magnetic properties and structures of the pillared perovskites, La{sub 5}Re{sub 3}MO{sub 16} (M=Co, Ni)

    SciTech Connect

    Cuthbert, Heather L. . E-mail: cuthbehl@mcmaster.ca; Greedan, John E.; Cranswick, Lachlan

    2006-07-15

    La{sub 5}Re{sub 3}CoO{sub 16} and La{sub 5}Re{sub 3}NiO{sub 16} were synthesized by solid-state reaction and studied by SQUID magnetometry, heat capacity and powder neutron diffraction measurements. These two compounds belong to a series of isostructural Re-based pillared perovskites [Chi et al. J. Solid State Chem. 170 (2003) 165]. Magnetic susceptibility measurements indicate apparent short-range ferri or ferromagnetic correlations and possible long-range antiferromagnetic order for La{sub 5}Re{sub 3}CoO{sub 16} at 35K, and at 38 and 14K for La{sub 5}Re{sub 3}NiO{sub 16}. Heat capacity measurements of the Co compound show a lambda anomaly, typical of long-range magnetic order, at 32K. In contrast, the Ni compound displays a broader, more symmetric feature at 12K in the heat capacity data, indicative of short-range magnetic order. Low-temperature powder neutron diffraction revealed contrasting magnetic structures. While both show an ordering wave vector, k=(0,0,1/2), in La{sub 5}Re{sub 3}CoO{sub 16}, the Co{sup 2+} and Re{sup 5+} moments are ordered ferrimagnetically within the corner-shared octahedral layers, while the layers themselves are coupled antiferromagnetically along the c-axis, as also found in La{sub 5}Re{sub 3}MnO{sub 16} and La{sub 5}Re{sub 3}FeO{sub 16}. In the case of the Ni material, the Re{sup 5+} and Ni{sup 2+} moments in the perovskite layers couple ferromagnetically and are canted 30 deg. away from the c-axis, angled 45 deg. in the ab-plane. The layers then couple antiferromagnetically at low temperature, a unique magnetic structure for this series. The properties of the La{sub 5}Re{sub 3}MO{sub 16} series, with M=Mn, Fe, Co, Ni and Mg are also reviewed.

  17. From Morphology to Interfaces to Tandem Geometries: Enhancing the Performance of Perovskite/Polymer Solar Cells

    NASA Astrophysics Data System (ADS)

    Russell, Thomas

    We have taken a new approach to develop mesoporous lead iodide scaffolds, using the nucleation and growth of lead iodide crystallites in a wet film. A simple time-dependent growth control enabled the manipulation of the mesoporous lead iodide layer quality in a continuous manner. The morphology of lead iodide is shown to influence the subsequent crystallization of methyamoniumleadiodide film by using angle-dependent grazing incidence x-ray scattering. The morphology of lead iodide film can be fine-tuned, and thus the methyamoniumleadiodide film quality can be effectively controlled, leading to an optimization of the perovskite active layer. Using this strategy, perovskite solar cells with inverted PHJ structure showed a PCE of 15.7 per cent with little hysteresis. Interface engineering is critical for achieving efficient solar cells, yet a comprehensive understanding of the interface between metal electrode and electron transport layer (ETL) is lacking. A significant power conversion efficiency (PCE) improvement of fullerene/perovskite planar heterojunction solar cells was achieved by inserting a fulleropyrrolidine interlayer between the silver electrode and electron transport layer. The interlayer was found to enhance recombination resistance, increases electron extraction rate and prolongs free carrier lifetime. We also uncovered a facile solution-based fabrication of high performance tandem perovskite/polymer solar cells where the front sub-cell consists of perovskite and the back sub-cell is a polymer-based layer. A record maximum PCE of 15.96 per cent was achieved, demonstrating the synergy between the perovskite and semiconducting polymers. This design balances the absorption of the perovskite and the polymer, eliminates the adverse impact of thermal annealing during perovskite fabrication, and affords devices with no hysteresis. This work was performed in collaboration with Y. Liu, Z. Page, D. Venkataraman and T. Emrick (UMASS), F. Liu (LBNL) and Q. Hu and R

  18. Scaling Effects in Perovskite Ferroelectrics: Fundamental Limits and Process-Structure-Property Relations

    DOE PAGES

    Ihlefeld, Jon F.; Harris, David T.; Keech, Ryan; Jones, Jacob L.; Maria, Jon-Paul; Trolier-McKinstry, Susan

    2016-07-05

    Ferroelectric materials are well-suited for a variety of applications because they can offer a combination of high performance and scaled integration. Examples of note include piezoelectrics to transform between electrical and mechanical energies, capacitors used to store charge, electro-optic devices, and non-volatile memory storage. Accordingly, they are widely used as sensors, actuators, energy storage, and memory components, ultrasonic devices, and in consumer electronics products. Because these functional properties arise from a non-centrosymmetric crystal structure with spontaneous strain and a permanent electric dipole, the properties depend upon physical and electrical boundary conditions, and consequently, physical dimension. The change of properties withmore » decreasing physical dimension is commonly referred to as a size effect. In thin films, size effects are widely observed, while in bulk ceramics, changes in properties from the values of large-grained specimens is most notable in samples with grain sizes below several microns. It is important to note that ferroelectricity typically persists to length scales of about 10 nm, but below this point is often absent. Despite the stability of ferroelectricity for dimensions greater than ~10 nm, the dielectric and piezoelectric coefficients of scaled ferroelectrics are suppressed relative to their bulk counterparts, in some cases by changes up to 80%. The loss of extrinsic contributions (domain and phase boundary motion) to the electromechanical response accounts for much of this suppression. In this article the current understanding of the underlying mechanisms for this behavior in perovskite ferroelectrics are reviewed. We focus on the intrinsic limits of ferroelectric response, the roles of electrical and mechanical boundary conditions, grain size and thickness effects, and extraneous effects related to processing. Ultimately, in many cases, multiple mechanisms combine to produce the observed scaling

  19. Nanomanufacturing : nano-structured materials made layer-by-layer.

    SciTech Connect

    Cox, James V.; Cheng, Shengfeng; Grest, Gary Stephen; Tjiptowidjojo, Kristianto; Reedy, Earl David, Jr.; Fan, Hongyou; Schunk, Peter Randall; Chandross, Michael Evan; Roberts, Scott A.

    2011-10-01

    Large-scale, high-throughput production of nano-structured materials (i.e. nanomanufacturing) is a strategic area in manufacturing, with markets projected to exceed $1T by 2015. Nanomanufacturing is still in its infancy; process/product developments are costly and only touch on potential opportunities enabled by growing nanoscience discoveries. The greatest promise for high-volume manufacturing lies in age-old coating and imprinting operations. For materials with tailored nm-scale structure, imprinting/embossing must be achieved at high speeds (roll-to-roll) and/or over large areas (batch operation) with feature sizes less than 100 nm. Dispersion coatings with nanoparticles can also tailor structure through self- or directed-assembly. Layering films structured with these processes have tremendous potential for efficient manufacturing of microelectronics, photovoltaics and other topical nano-structured devices. This project is designed to perform the requisite R and D to bring Sandia's technology base in computational mechanics to bear on this scale-up problem. Project focus is enforced by addressing a promising imprinting process currently being commercialized.

  20. Goldstone-like states in a layered perovskite with frustrated polarization : a first-principles investigation of PbSr{sub 2}Ti{sub 2}o{sub 7}.

    SciTech Connect

    Nakhmanson, S. M.; Naumov, I.; Materials Science Division; Hewlett-Packard Info. and Quantum Systems Lab.

    2010-03-05

    With the help of first-principles-based computational techniques, we demonstrate that Goldstone-like states can be artificially induced in a layered-perovskite ferroelectric compound with frustrated polarization, resulting in the emergence of a variety of interesting physical properties that include large, tunable dielectric constants and an ability to easily form vortex polar states in a nanodot geometry. In a similar fashion to the well-known perovskite materials with morphotropic phase boundaries (MPBs), these states manifest themselves as polarization rotations with almost no energy penalty, suggesting that the existence of an MPB is actually yet another manifestation of the Goldstone theorem in solids.

  1. TiO2 quantum dots as superb compact block layers for high-performance CH3NH3PbI3 perovskite solar cells with an efficiency of 16.97%

    NASA Astrophysics Data System (ADS)

    Tu, Yongguang; Wu, Jihuai; Zheng, Min; Huo, Jinghao; Zhou, Pei; Lan, Zhang; Lin, Jianming; Huang, Miaoliang

    2015-12-01

    A compact TiO2 layer is crucial to achieve high-efficiency perovskite solar cells. In this study, we developed a facile, low-cost and efficient method to fabricate a pinhole-free and ultrathin blocking layer based on highly crystallized TiO2 quantum dots (QDs) with an average diameter of 3.6 nm. The surface morphology of the blocking layer and the photoelectric performance of the perovskite solar cells were investigated by spin-coating with three different materials: colloidal TiO2 QDs, titanium precursor solution, and aqueous TiCl4. Among these three treatments, the perovskite solar cell based on the TiO2 QD compact layer offered the highest power conversion efficiency (PCE) of 16.97% with a photocurrent density of 22.48 mA cm-2, a photovoltage of 1.063 V and a fill factor of 0.71. The enhancement of PCE mainly stems from the small series resistance and the large shunt resistance of the TiO2 QD layer.A compact TiO2 layer is crucial to achieve high-efficiency perovskite solar cells. In this study, we developed a facile, low-cost and efficient method to fabricate a pinhole-free and ultrathin blocking layer based on highly crystallized TiO2 quantum dots (QDs) with an average diameter of 3.6 nm. The surface morphology of the blocking layer and the photoelectric performance of the perovskite solar cells were investigated by spin-coating with three different materials: colloidal TiO2 QDs, titanium precursor solution, and aqueous TiCl4. Among these three treatments, the perovskite solar cell based on the TiO2 QD compact layer offered the highest power conversion efficiency (PCE) of 16.97% with a photocurrent density of 22.48 mA cm-2, a photovoltage of 1.063 V and a fill factor of 0.71. The enhancement of PCE mainly stems from the small series resistance and the large shunt resistance of the TiO2 QD layer. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr05563f

  2. Electronic band structure trends of perovskite halides: Beyond Pb and Sn to Ge and Si

    NASA Astrophysics Data System (ADS)

    Huang, Ling-yi; Lambrecht, Walter R. L.

    2016-05-01

    The trends in electronic band structure are studied in the cubic A B X3 halide perovskites for A =Cs ; B =Pb , Sn, Ge, Si; and X =I , Br, Cl. The gaps are found to decrease from Pb to Sn and from Ge to Si, but increase from Sn to Ge. The trend is explained in terms of the atom s levels of the group-IV element and the atomic sizes which changes the amount of hybridization with X -p and hence the valence bandwidth. Along the same series spin-orbit coupling also decreases and this tends to increase the gap because of the smaller splitting of the conduction band minimum. Both effects compensate each other to a certain degree. The trend with halogens is to reduce the gap from Cl to I, i.e., with decreasing electronegativity. The role of the tolerance factor in avoiding octahedron rotations and octahedron edge sharing is discussed. The Ge containing compounds have tolerance factor t >1 and hence do not show the series of octahedral rotation distortions and the existence of edge-sharing octahedral phases known for Pb and Sn-based compounds, but rather a rhombohedral distortion. CsGeI3 is found to have a suitable gap for photovoltaics both in its cubic (high-temperature) and rhombohedral (low-temperature) phases. The structural stability of the materials in the different phases is also discussed. We find the rhombohedral phase to have lower total energy and slightly larger gaps but to present a less significant distortion of the band structure than the edge-sharing octahedral phases, such as the yellow phase in CsSnI3. The corresponding silicon based compounds have not yet been synthesized and therefore our estimates are less certain but indicate a small gap for cubic CsSiI3 and CsSiBr3 of about 0.2 ±0.2 eV and 0.8 ±0.6 eV for CsSiCl3. The intrinsic stability of the Si compounds is discussed.

  3. First-principles study of crystal structure, electronic structure, and second-harmonic generation in a polar double perovskite Bi2ZnTiO6.

    PubMed

    Ju, Sheng; Guo, Guang-Yu

    2008-11-21

    Within the density functional theory with the generalized gradient approximation, we present a systematic ab initio investigation of crystal structure, electronic structure, and linear and nonlinear optical responses in a polar double perovskite Bi(2)ZnTiO(6). The effect of B-site ordering is explored by comparing three possible configurations: A-type with alternative Zn and Ti layers stacking along the c axis; C-type with Zn and Ti c axis chains; and G-type with every Zn(Ti) atoms is surrounded by its nearby six Ti(Zn) atoms. It is found that the system with G-type B-site ordering is energetically favorable, which is lower in the total energies of 0.055 and 0.133 eV/formula unit than C-type and A-type, respectively. Optical calculations indicate that all the three configurations show large second-harmonic generation (SHG) coefficients, and the largest static SHG observed in the C-type system reaches 123 (10(-9) esu), the value of which is much larger than ever known polar oxides, e.g., 72 (10(-9) esu) in LiNbO(3). The predicted significant nonlinear optical properties are consistent with the calculated high tetragonality as well as the large off-center displacement of Zn, Ti, and Bi atoms. In particular, a large off-center displacement greater than 0.5 A in Zn atoms is revealed for the first time. A further microscopic picture is presented via the successful connection of the prominent feature of SHG in Bi(2)ZnTiO(6) with that of the linear optical dielectric function in terms of single-photon and double-photon resonances. Our calculations demonstrate the promising application of Bi(2)ZnTiO(6) in optoelectronics.

  4. Magnetic order and electronic structure of 5d3 double perovskite Sr2ScOsO6

    DOE PAGES

    Taylor, A. E.; Morrow, R.; Singh, D. J.; Calder, S.; Lumsden, M. D.; Woodward, P. M.; Christianson, A. D.

    2015-03-01

    The magnetic susceptibility, crystal and magnetic structures, and electronic structure of double perovskite Sr2ScOsO6 are reported. Using both neutron and x-ray powder diffraction we find that the crystal structure is monoclinic P21/n from 3.5 to 300 K. Magnetization measurements indicate an antiferromagnetic transition at TN=92 K, one of the highest transition temperatures of any double perovskite hosting only one magnetic ion. Type I antiferromagnetic order is determined by neutron powder diffraction, with an Os moment of only 1.6(1) muB, close to half the spin-only value for a crystal field split 5d electron state with t2g^3 ground state. Density functional calculationsmore » show that this reduction is largely the result of strong Os-O hybridization, with spin-orbit coupling responsible for only a ~0.1 muB reduction in the moment.« less

  5. Structural and transport properties of double perovskite Dy{sub 2}NiMnO{sub 6}

    SciTech Connect

    Chanda, Sadhan Saha, Sujoy; Dutta, Alo; Sinha, T.P.

    2015-02-15

    Highlights: • Sol–gel citrate method is used to prepare the double perovskite Dy{sub 2}NiMnO{sub 6}. • Structure and dielectric relaxation of the sample are studied for nano and bulk phases. • The relaxation mechanism of the sample is modeled by Cole–Cole equation. • With increasing sintering temperature conductivity increases. • Electronic structures and magnetic properties have been studied by DFT calculations. - Abstract: The double perovskite oxide Dy{sub 2}NiMnO{sub 6} (DNMO) is synthesized in nano and bulk phase by the sol–gel citrate method. The Rietveld refinement of X-ray diffraction pattern of the sample at room temperature shows the monoclinic P2{sub 1}/n phase. Dielectric relaxation of the sample is investigated in the impedance and electric modulus formalisms in the frequency range from 50 Hz to 1 MHz and in the temperature range from 253 to 415 K. The Cole–Cole model is used to explain the relaxation mechanism in DNMO. The frequency-dependent maxima in the imaginary part of impedance are found to obey an Arrhenius law with activation energy of 0.346 and 0.344 eV for nano and bulk DNMO, respectively. A significant increase in conductivity of bulk DNMO has been observed than that of the nanoceramic. Electronic structures and magnetic properties of DNMO have been studied by performing first principles calculation based on density functional theory.

  6. Synthesis of novel perovskite crystal structure phase of strontium doped rare earth manganites using sol gel method

    NASA Astrophysics Data System (ADS)

    Abdel-Latif, I. A.; Ismail, Adel A.; Bouzid, Houcine; Al-Hajry, A.

    2015-11-01

    In the present work, polycrystalline perovskites of R0.6Sr0.4MnO3 nanocomposites (R=La, Nd, or Sm) were synthesized using the sol-gel method in the presence of citric acid and polyethylene glycol as chelating and structure directing agents respectively. The synthesized gel was calcined at 800 °C for 5 h. The XRD revealed that the obtained nanocrystalline R0.6Sr0.4MnO3 is monoclinic crystal structure of space group (I2/a). TEM images showed that the prepared perovskites are homogeneous and uniform with particle sizes in a range 20-40 nm and the HR-TEM images and lattice fringes displayed the monoclinic structure. IV measurements showed that Nd0.6Sr0.4MnO3 has semiconducting properties at room temperature. With applying low magnetic field, a transition from semiconductor behavior to Ohmic resistivity was observed. The static resistance of Nd0.6Sr0.4MnO3 was calculated to be ~2.985 TΩ for semiconductor phase and the resistance increased 1000 times that gives rise to negative magnetoresistance (MR). The value of MR of Nd0.6Sr0.4MnO3 equals to 99.84%, which leads to the use of these materials in fabrication of magnetic devices in the industrial scale.

  7. Quasiparticle band gap of organic-inorganic hybrid perovskites: Crystal structure, spin-orbit coupling, and self-energy effects

    NASA Astrophysics Data System (ADS)

    Gao, Weiwei; Gao, Xiang; Abtew, Tesfaye; Sun, Yiyang; Zhang, Shengbai; Zhang, Peihong

    The quasiparticle band gaps of organic-inorganic hybrid perovskites are often determined (and can be controlled) by various factors, complicating predictive materials optimization. Here we report a comprehensive investigation on the band gap formation mechanism in CH3NH3PbI3 by decoupling various contributing factors which ultimately determine their electronic structure and quasiparticle band gap. Four major factors, namely, quasiparticle self-energy, spin-orbit coupling, volume (lattice constant) effects, and structural distortions due to the presence of organic molecules, and their influences on the quasiparticle band structure of organometal hybrid perovskites are illustrated. We find that although methylammonium cations do not contribute directly to the electronic states near band edges, they play an important role in defining the band gap through a lattice distortion mechanism and by controlling the overall lattice constants (thus the chemical bonding of the optically active PbI3-). The spin-orbit coupling effects drastically reduce the electron and hole effective masses in these systems, which is beneficial for high carrier mobilities and small exciton binding energies. This work is supported by the National Natural Science Foundation of China (Grant No. 11328401), NSF (Grant No. DMR-0946404 and DMR-1506669), and the SUNY Networks of Excellence.

  8. Electronic structure of ferromagnetic semiconductor material on the monoclinic and rhombohedral ordered double perovskites La{sub 2}FeCoO{sub 6}

    SciTech Connect

    Fuh, Huei-Ru; Chang, Ching-Ray; Weng, Ke-Chuan; Wang, Yin-Kuo

    2015-05-07

    Double perovskite La{sub 2}FeCoO{sub 6} with monoclinic structure and rhombohedra structure show as ferromagnetic semiconductor based on density functional theory calculation. The ferromagnetic semiconductor state can be well explained by the superexchange interaction. Moreover, the ferromagnetic semiconductor state remains under the generalized gradient approximation (GGA) and GGA plus onsite Coulomb interaction calculation.

  9. Electronic structure of bacterial surface protein layers

    SciTech Connect

    Maslyuk, Volodymyr V.; Mertig, Ingrid; Bredow, Thomas; Mertig, Michael; Vyalikh, Denis V.; Molodtsov, Serguei L.

    2008-01-15

    We report an approach for the calculation of the electronic density of states of the dried two-dimensional crystalline surface protein layer (S layer) of the bacterium Bacillus sphaericus NCTC 9602. The proposed model is based on the consideration of individual amino acids in the corresponding conformation of the peptide chain which additively contribute to the electronic structure of the entire protein complex. The derived results agree well with the experimental data obtained by means of photoemission (PE), resonant PE, and near-edge x-ray absorption spectroscopy.

  10. Identifying layers in random multiphase structures

    NASA Astrophysics Data System (ADS)

    Mader, Kevin; Stampanoni, Marco

    2016-01-01

    X-Ray microscopic methods, benefiting from the large penetration depth of X-rays in many materials, enable 3D investigation of a wide variety of samples. This allows for a wide variety of physical, chemical, and biological structures to be seen and explored, in some cases even in real time. Such measurements have lead to insights into paleontology, vulcanology, genetics, and material science. The ability to see and visualize complex systems can provide otherwise unobtainable information on structure, interactions, mechanical behavior, and evolution. The field has, however, led to a massive amount of new, heterogenous, difficult to process data. We present a general, model-free approach for characterizing multiphase 3D systems and show how the method can be applied to experimental X-ray microscopy data to better understand and quantify layer structure in two typical systems: investigation of layered fibers and clay samples.

  11. Mechanism of charge recombination in meso-structured organic-inorganic hybrid perovskite solar cells: A macroscopic perspective

    NASA Astrophysics Data System (ADS)

    Yang, Wenchao; Yao, Yao; Wu, Chang-Qin

    2015-04-01

    In the currently popular organic-inorganic hybrid perovskite solar cells, the slowness of the charge recombination processes is found to be a key factor for contributing to their high efficiencies and high open circuit voltages, but the underlying recombination mechanism remains unclear. In this work, we investigate the bimolecular recombination (BR) and the trap-assisted monomolecular recombination (MR) in meso-structured perovskite solar cells under steady state working condition, and try to reveal their roles on determining the device performance. Some interfacial effects such as the injection barriers at the selective contacts are examined as well. Based on the macroscopic device modeling, the recombination resistance-voltage (Rrec-V) and the current density-voltage (J-V) curves are calculated to characterize the recombination mechanism and describe the device performance, respectively. Through comparison with the impedance spectroscopy extracted Rrec data, it is found that under the typical BR reduction factor and deep trap densities observed in experiments, the MR dominates the charge recombination in the low voltage regime, while the BR dominates in the high voltage regime. The short circuit current and the fill factor could be reduced by the significant MR but the open circuit voltage is generally determined by the BR. The different electron injection barriers at the contact can change the BR rate and induce different patterns for the Rrec-V characteristics. For the perovskites of increased band gaps, the Rrec's are significantly enhanced, corresponding to the high open circuit voltages. Finally, it is revealed that the reduced effective charge mobility due to the transport in electron and hole transporting material makes the Rrec decrease slowly with the increasing voltage, which leads to increased open circuit voltage.

  12. Mechanism of charge recombination in meso-structured organic-inorganic hybrid perovskite solar cells: A macroscopic perspective

    SciTech Connect

    Yang, Wenchao; Yao, Yao Wu, Chang-Qin

    2015-04-21

    In the currently popular organic-inorganic hybrid perovskite solar cells, the slowness of the charge recombination processes is found to be a key factor for contributing to their high efficiencies and high open circuit voltages, but the underlying recombination mechanism remains unclear. In this work, we investigate the bimolecular recombination (BR) and the trap-assisted monomolecular recombination (MR) in meso-structured perovskite solar cells under steady state working condition, and try to reveal their roles on determining the device performance. Some interfacial effects such as the injection barriers at the selective contacts are examined as well. Based on the macroscopic device modeling, the recombination resistance-voltage (R{sub rec}−V) and the current density-voltage (J–V) curves are calculated to characterize the recombination mechanism and describe the device performance, respectively. Through comparison with the impedance spectroscopy extracted R{sub rec} data, it is found that under the typical BR reduction factor and deep trap densities observed in experiments, the MR dominates the charge recombination in the low voltage regime, while the BR dominates in the high voltage regime. The short circuit current and the fill factor could be reduced by the significant MR but the open circuit voltage is generally determined by the BR. The different electron injection barriers at the contact can change the BR rate and induce different patterns for the R{sub rec}–V characteristics. For the perovskites of increased band gaps, the R{sub rec}'s are significantly enhanced, corresponding to the high open circuit voltages. Finally, it is revealed that the reduced effective charge mobility due to the transport in electron and hole transporting material makes the R{sub rec} decrease slowly with the increasing voltage, which leads to increased open circuit voltage.

  13. Surface coverage enhancement of a mixed halide perovskite film by using an UV-ozone treatment

    NASA Astrophysics Data System (ADS)

    Lee, Hyunho; Rhee, Seunghyun; Kim, Jaeyoul; Lee, Changhee; Kim, Hyeok

    2016-08-01

    Recently, a significant breakthrough in emerging photovoltaics occurred. Now, perovskite solar cells, hybrid types of organic and inorganic solar cells, are considered as reliable next-generation solar cells due to their outstanding photovoltaic performance. Records of the National Renewable Energy Laboratory (NREL) on cell efficiency research indicates a prominent growth in the power conversion efficiency (PCE) of a perovskite solar cells which is now approaching 20.1%. Perovskite solar cells are, in general, classified into three types based on their structures; the mesoporous type with TiO2 nanoparticles, the meso-superstructure type with Al2O3 and the planar hetero-junction type. Among them, planar-structured perovskite solar cells have strong advantages due to their easy processibility and flexibility. We can replace the materials in the electron transport layer (ETL) and the hole transport layer (HTL) with common materials that are available in organic solar cells. However, a great challenge is to fabricate a high-quality perovskite film because the perovskite morphology is highly sensitive to its fabrication conditions. For control of the film's morphology, some experiments, such as changing the annealing temperature or time and adding some additives, have been done to increase the surface coverage of perovskite films. In this work, we introduce normal, planar, perovskite solar cells with a hetero-junction structure based on compact TiO2 and a mixed halide perovskite (CH3NH3PbI3- x Cl x ). To enlarge the surface coverage of perovskite film, we used an UV-ozone treatment on top of the compact TiO2, which made the surface of TiO2 hydrophilic. Because a perovskite precursor is hydrophilic, an UV-ozone treatment is expected to improve the wettability between the compact TiO2 and the perovskite film. Here, we present the photovoltaic performance, along with the surface coverage difference, for various UV-ozone treatment time. In addition, the effect of the UV

  14. Structural chemistry and magnetic properties of the perovskite Sr3Fe2TeO9

    NASA Astrophysics Data System (ADS)

    Tang, Yawei; Hunter, Emily C.; Battle, Peter D.; Sena, Robert Paria; Hadermann, Joke; Avdeev, Maxim; Cadogan, J. M.

    2016-10-01

    A polycrystalline sample of perovskite-like Sr3Fe2TeO9 has been prepared in a solid-state reaction and studied by a combination of electron microscopy, Mössbauer spectroscopy, magnetometry, X-ray diffraction and neutron diffraction. The majority of the reaction product is shown to be a trigonal phase with a 2:1 ordered arrangement of Fe3+ and Te6+ cations. However, the sample is prone to nano-twinning and tetragonal domains with a different pattern of cation ordering exist within many crystallites. Antiferromagnetic ordering exists in the trigonal phase at 300 K and Sr3Fe2TeO9 is thus the first example of a perovskite with 2:1 trigonal cation ordering to show long-range magnetic order. At 300 K the antiferromagnetic phase coexists with two paramagnetic phases which show spin-glass behaviour below ~80 K.

  15. Structural properties of PbVO3 perovskites under hydrostatic pressure conditions up to 10.6 GPa.

    PubMed

    Zhou, Wei; Tan, Dayong; Xiao, Wansheng; Song, Maoshuang; Chen, Ming; Xiong, Xiaolin; Xu, Jian

    2012-10-31

    High-pressure synchrotron x-ray powder diffraction experiments were performed on PbVO(3) tetragonal perovskite in a diamond anvil cell under hydrostatic pressures of up to 10.6 GPa at room temperature. The compression behavior of the PbVO(3) tetragonal phase is highly anisotropic, with the c-axis being the soft direction. A reversible tetragonal to cubic perovskite structural phase transition was observed between 2.7 and 6.4 GPa in compression and below 2.2 GPa in decompression. This transition was accompanied by a large volume collapse of 10.6% at 2.7 GPa, which was mainly due to electronic structural changes of the V(4+) ion. The polar pyramidal coordination of the V(4+) ion in the tetragonal phase changed to an isotropic octahedral coordination in the cubic phase. Fitting the observed P-V data using the Birch-Murnaghan equation of state with a fixed [Formula: see text] of 4 yielded a bulk modulus K(0) = 61(2) GPa and a volume V(0) = 67.4(1) Å(3) for the tetragonal phase, and the values of K(0) = 155(3) GPa and V(0) = 58.67(4) Å(3) for the cubic phase. The first-principles calculated results were in good agreement with our experiments. PMID:23041755

  16. Sputtered lead scandium tantalate thin films: Pb{sup 4+} in B sites in the perovskite structure

    SciTech Connect

    Whatmore, R.W.; Huang, Z.; Todd, M.

    1997-12-01

    Perovskite lead scandium tantalate (PST){emdash}PbSc{sub 1/2}Ta{sub 1/2}O{sub 3}{emdash}thin films have been prepared from lead-rich targets by rf magnetron sputtering onto a variety of substrates (e.g., MgO-on-sapphire and platinized silicon). Detailed microstructural chemical analysis of the films using transmission electron microscopy and energy dispersive x-ray spectroscopy techniques showed that they contained large amounts of excess lead, ranging from 7 to over 70 at.{percent} and that this was located within the crystallite grains making up the films rather than solely at grain boundaries. Measurement of the lattice parameters of the films using x-ray diffraction and using the underlying materials as internal standards have shown that the lattice parameters of the films are consistently larger than those for bulk PST. Comparison of the film lattice parameters with composition and with the lattice parameter/composition trend of a large number of lead containing perovskites strongly suggests that the excess lead is present on the B sites of the structure as Pb{sup 4+}. The consequences for this on the structural and electrical properties of these films and PST films deposited by other workers are discussed. {copyright} {ital 1997 American Institute of Physics.}

  17. Novel Carbazole-Based Hole-Transporting Materials with Star-Shaped Chemical Structures for Perovskite-Sensitized Solar Cells.

    PubMed

    Kang, Min Soo; Sung, Sang Do; Choi, In Taek; Kim, Hyoungjin; Hong, MunPyo; Kim, Jeongho; Lee, Wan In; Kim, Hwan Kyu

    2015-10-14

    Novel carbazole-based hole-transporting materials (HTMs), including extended π-conjugated central core units such as 1,4-phenyl, 4,4'-biphenyl, or 1,3,5-trisphenylbenzene for promoting effective π-π stacking as well as the hexyloxy flexible group for enhancing solubility in organic solvent, have been synthesized as HTM of perovskite-sensitized solar cells. A HTM with 1,3,5-trisphenylbenzene core, coded as SGT-411, exhibited the highest charge conductivity caused by its intrinsic property to form crystallized structure. The perovskite-sensitized solar cells with SGT-411 exhibited the highest PCE of 13.00%, which is 94% of that of the device derived from spiro-OMeTAD (13.76%). Time-resolved photoluminescence spectra indicate that SGT-411 shows the shortest decay time constant, which is in agreement with the trends of conductivity data, indicating it having fastest charge regeneration. In this regard, a carbazole-based HTM with star-shaped chemical structure is considered to be a promising candidate HTM.

  18. Structural properties of PbVO3 perovskites under hydrostatic pressure conditions up to 10.6 GPa.

    PubMed

    Zhou, Wei; Tan, Dayong; Xiao, Wansheng; Song, Maoshuang; Chen, Ming; Xiong, Xiaolin; Xu, Jian

    2012-10-31

    High-pressure synchrotron x-ray powder diffraction experiments were performed on PbVO(3) tetragonal perovskite in a diamond anvil cell under hydrostatic pressures of up to 10.6 GPa at room temperature. The compression behavior of the PbVO(3) tetragonal phase is highly anisotropic, with the c-axis being the soft direction. A reversible tetragonal to cubic perovskite structural phase transition was observed between 2.7 and 6.4 GPa in compression and below 2.2 GPa in decompression. This transition was accompanied by a large volume collapse of 10.6% at 2.7 GPa, which was mainly due to electronic structural changes of the V(4+) ion. The polar pyramidal coordination of the V(4+) ion in the tetragonal phase changed to an isotropic octahedral coordination in the cubic phase. Fitting the observed P-V data using the Birch-Murnaghan equation of state with a fixed [Formula: see text] of 4 yielded a bulk modulus K(0) = 61(2) GPa and a volume V(0) = 67.4(1) Å(3) for the tetragonal phase, and the values of K(0) = 155(3) GPa and V(0) = 58.67(4) Å(3) for the cubic phase. The first-principles calculated results were in good agreement with our experiments.

  19. Efficient conversion from UV light to near-IR emission in Yb{sup 3+}-doped triple-layered perovskite CaLaNb{sub 3}O{sub 10}

    SciTech Connect

    Lu, Yuting; Li, Yuze; Qin, Lin; Huang, Yanlin; Qin, Chuanxiang; Tsuboi, Taiju; Huang, Wei

    2015-04-15

    Graphical abstract: CaRNb{sub 3}O{sub 10} is a self-activated oxide due to charge transfer transition in octahedral NbO{sub 6} groups. CaLaNb{sub 3}O{sub 10}:Yb{sup 3+} presents intense IR emission due to the cooperative energy transfer from host (NbO{sub 6}) to Yb{sup 3+} is responsible. It could be expected to be potentially applicable for enhancing photovoltaic conversion efficiency of Si-based solar cells. - Abstract: Yb{sup 3+}-doped triple-layered perovskite CaLaNb{sub 3}O{sub 10} micro-particles were synthesized via the solid-state reaction method. The crystal structure and morphology of the polycrystalline samples were investigated by X-ray powder diffraction (XRD) and scanning electron microscopy (SEM) measurements, respectively. The reflectance spectra, photoluminescence (PL) excitation and emission spectra, the decay curves, and the absolute quantum efficiency (QE) of the near-infrared (NIR) emission (910–1100 nm) were measured. Under excitation of UV light, Yb{sup 3+}-doped perovskite shows an intense NIR emission attributed to the {sup 2}F{sub 5/2} → {sup 2}F{sub 7/2} transitions of Yb{sup 3+} ions, which could match maximum spectral response of a Si-based solar cell. This is beneficial for its possible application in an enhancement of the photovoltaic conversion efficiency of solar energy utilization. The efficient energy transfer in Yb{sup 3+}-doped CaLaNb{sub 3}O{sub 10} from NbO{sub 6} groups into Yb{sup 3+} ions was confirmed by the spectra and fluorescent decay measurements. Cooperative energy transfer (CET) was supposed to be the NIR emission mechanism.

  20. Coupling and electrical control of structural, orbital and magnetic orders in perovskites

    PubMed Central

    Varignon, Julien; Bristowe, Nicholas C.; Bousquet, Eric; Ghosez, Philippe

    2015-01-01

    Perovskite oxides are already widely used in industry and have huge potential for novel device applications thanks to the rich physical behaviour displayed in these materials. The key to the functional electronic properties exhibited by perovskites is often the so-called Jahn-Teller distortion. For applications, an electrical control of the Jahn-Teller distortions, which is so far out of reach, would therefore be highly desirable. Based on universal symmetry arguments, we determine new lattice mode couplings that can provide exactly this paradigm, and exemplify the effect from first-principles calculations. The proposed mechanism is completely general, however for illustrative purposes, we demonstrate the concept on vanadium based perovskites where we reveal an unprecedented orbital ordering and Jahn-Teller induced ferroelectricity. Thanks to the intimate coupling between Jahn-Teller distortions and electronic degrees of freedom, the electric field control of Jahn-Teller distortions is of general relevance and may find broad interest in various functional devices. PMID:26482414

  1. Normal mode determination of perovskite crystal structures with octahedral rotations: theory and applications.

    PubMed

    Islam, Mohammad A; Rondinelli, James M; Spanier, Jonathan E

    2013-05-01

    Nuclear site analysis methods are used to enumerate the normal modes of ABX3 perovskite polymorphs with octahedral rotations. We provide the modes of the 14 subgroups of the cubic aristotype describing the Glazer octahedral tilt patterns, which are obtained from rotations of the BX6 octahedra with different sense and amplitude about high-symmetry axes. We tabulate all normal modes of each tilt system and specify the contribution of each atomic species to the mode displacement pattern, elucidating the physical meaning of the symmetry unique modes. We have systematically generated 705 schematic atomic displacement patterns for the normal modes of all 15 (14 rotated + 1 unrotated) Glazer tilt systems. We show through some illustrative examples how to use these tables to identify the octahedral rotations, symmetric breathing, and first-order Jahn-Teller anti-symmetric breathing distortions of the BX6 octahedra, and the associated Raman selection rules. We anticipate that these tables and schematics will be useful in understanding the lattice dynamics of bulk perovskites and could serve as a reference point in elucidating the atomic origins of a wide range of physical properties of synthetic perovskite thin films and superlattices. PMID:23567868

  2. Femtosecond time-resolved transient absorption spectroscopy of CH3NH3PbI3 perovskite films: evidence for passivation effect of PbI2.

    PubMed

    Wang, Lili; McCleese, Christopher; Kovalsky, Anton; Zhao, Yixin; Burda, Clemens

    2014-09-01

    CH3NH3PbI3 perovskite layered films deposited on substrates with and without a titania support structure have been prepared and studied using time-resolved femtosecond transient absorption (fs-TA) spectroscopy in the visible light range (450-800 nm). The electron injection dynamics from the photoexcited perovskite layers to the neighboring film structures could be directly monitored via the transient bleaching dynamics of the perovskite at ∼750 nm and thus systematically studied as a function of the layer-by-layer architecture. In addition, for the first time we could spectrally distinguish transient bleaching at ∼750 nm from laser-induced fluorescence that occurs red-shifted at ∼780 nm. We show that an additional bleach feature at ∼510 nm appears when PbI2 is present in the perovskite film. The amplitudes of the PbI2 and perovskite TA peaks were compared to estimate relative amounts of PbI2 in the samples. Kinetic analysis reveals that perovskite films with less PbI2 show faster relaxation rates than those containing more PbI2. These fast dynamics are attributed to charge carrier trapping at perovskite grain boundaries, and the slower dynamics in samples containing PbI2 are due to a passivation effect, in line with other recently reported work.

  3. Plane mixing layer vortical structure kinematics

    NASA Technical Reports Server (NTRS)

    Leboeuf, Richard L.

    1993-01-01

    The objective of the current project was to experimentally investigate the structure and dynamics of the streamwise vorticity in a plane mixing layer. The first part of this research program was intended to clarify whether the observed decrease in mean streamwise vorticity in the far-field of mixing layers is due primarily to the 'smearing' caused by vortex meander or to diffusion. Two-point velocity correlation measurements have been used to show that there is little spanwise meander of the large-scale streamwise vortical structure. The correlation measurements also indicate a large degree of transverse meander of the streamwise vorticity which is not surprising since the streamwise vorticity exists in the inclined braid region between the spanwise vortex core regions. The streamwise convection of the braid region thereby introduces an apparent transverse meander into measurements using stationary probes. These results corroborated with estimated secondary velocity profiles in which the streamwise vorticity produces a signature which was tracked in time.

  4. Structural and Optoelectronic Properties of X3ZN (X = Ca, Sr, Ba; Z = As, Sb, Bi) Anti-Perovskite Compounds

    NASA Astrophysics Data System (ADS)

    Ullah, Imran; Murtaza, G.; Khenata, R.; Mahmood, Asif; Muzzamil, M.; Amin, N.; Saleh, M.

    2016-06-01

    We employed first-principles calculations to predict the structural and optoelectronic properties of X3ZN (X = Ca, Sr, Ba; Z = As, Sb, Bi) anti-perovskite compounds using an all-electron full-potential linearized augmented plane-wave method. Optimized structural parameters are found to be in good agreement with the available experimental measurements. The electronic band structure is calculated using different exchange-correlation potentials which reveal that the investigated compounds are narrow direct band gap semiconductors. A direct narrow band gap at the center of the Brillouin zone emphasises the optical activity of these compounds. Prediction of the optical properties, such as the real and imaginary parts of the dielectric function and refractive index along with reflectivity and optical conductivity, reveals the importance of these compounds in the visible and near UV optoelectronic devices industry.

  5. Depletion region effect of highly efficient hole conductor free CH3NH3PbI3 perovskite solar cells.

    PubMed

    Aharon, Sigalit; Gamliel, Shany; El Cohen, Bat; Etgar, Lioz

    2014-06-14

    The inorganic-organic perovskite is currently attracting a lot of attention due to its use as a light harvester in solar cells. The large absorption coefficients, high carrier mobility and good stability of organo-lead halide perovskites present good potential for their use as light harvesters in mesoscopic heterojunction solar cells. This work concentrated on a unique property of the lead halide perovskite, its function simultaneously as a light harvester and a hole conductor in the solar cell. A two-step deposition technique was used to optimize the perovskite deposition and to enhance the solar cell efficiency. It was revealed that the photovoltaic performance of the hole conductor free perovskite solar cell is strongly dependent on the depletion layer width which was created at the TiO2-CH3NH3PbI3 junction. X-ray diffraction measurements indicate that there were no changes in the crystallographic structure of the CH3NH3PbI3 perovskite over time, which supports the high stability of these hole conductor free perovskite solar cells. Furthermore, the power conversion efficiency of the best cells reached 10.85% with a fill factor of 68%, a Voc of 0.84 V, and a Jsc of 19 mA cm(-2), the highest efficiency to date of a hole conductor free perovskite solar cell.

  6. Advances in Perovskite Solar Cells

    PubMed Central

    Zuo, Chuantian; Bolink, Henk J.; Han, Hongwei; Huang, Jinsong

    2016-01-01

    Organolead halide perovskite materials possess a combination of remarkable optoelectronic properties, such as steep optical absorption edge and high absorption coefficients, long charge carrier diffusion lengths and lifetimes. Taken together with the ability for low temperature preparation, also from solution, perovskite‐based devices, especially photovoltaic (PV) cells have been studied intensively, with remarkable progress in performance, over the past few years. The combination of high efficiency, low cost and additional (non‐PV) applications provides great potential for commercialization. Performance and applications of perovskite solar cells often correlate with their device structures. Many innovative device structures were developed, aiming at large‐scale fabrication, reducing fabrication cost, enhancing the power conversion efficiency and thus broadening potential future applications. This review summarizes typical structures of perovskite solar cells and comments on novel device structures. The applications of perovskite solar cells are discussed. PMID:27812475

  7. Interface and Composition Analysis on Perovskite Solar Cells.

    PubMed

    Matteocci, Fabio; Busby, Yan; Pireaux, Jean-Jacques; Divitini, Giorgio; Cacovich, Stefania; Ducati, Caterina; Di Carlo, Aldo

    2015-12-01

    Organometal halide (hybrid) perovskite solar cells have been fabricated following four different deposition procedures and investigated in order to find correlations between the solar cell characteristics/performance and their structure and composition as determined by combining depth-resolved imaging with time-of-flight secondary ion mass spectrometry (ToF-SIMS), X-ray photoelectron spectroscopy (XPS), and analytical scanning transmission electron microscopy (STEM). The interface quality is found to be strongly affected by the perovskite deposition procedure, and in particular from the environment where the conversion of the starting precursors into the final perovskite is performed (air, nitrogen, or vacuum). The conversion efficiency of the precursors into the hybrid perovskite layer is compared between the different solar cells by looking at the ToF-SIMS intensities of the characteristic molecular fragments from the perovskite and the precursor materials. Energy dispersive X-ray spectroscopy in the STEM confirms the macroscopic ToF-SIMS findings and allows elemental mapping with nanometer resolution. Clear evidence for iodine diffusion has been observed and related to the fabrication procedure.

  8. Interface and Composition Analysis on Perovskite Solar Cells.

    PubMed

    Matteocci, Fabio; Busby, Yan; Pireaux, Jean-Jacques; Divitini, Giorgio; Cacovich, Stefania; Ducati, Caterina; Di Carlo, Aldo

    2015-12-01

    Organometal halide (hybrid) perovskite solar cells have been fabricated following four different deposition procedures and investigated in order to find correlations between the solar cell characteristics/performance and their structure and composition as determined by combining depth-resolved imaging with time-of-flight secondary ion mass spectrometry (ToF-SIMS), X-ray photoelectron spectroscopy (XPS), and analytical scanning transmission electron microscopy (STEM). The interface quality is found to be strongly affected by the perovskite deposition procedure, and in particular from the environment where the conversion of the starting precursors into the final perovskite is performed (air, nitrogen, or vacuum). The conversion efficiency of the precursors into the hybrid perovskite layer is compared between the different solar cells by looking at the ToF-SIMS intensities of the characteristic molecular fragments from the perovskite and the precursor materials. Energy dispersive X-ray spectroscopy in the STEM confirms the macroscopic ToF-SIMS findings and allows elemental mapping with nanometer resolution. Clear evidence for iodine diffusion has been observed and related to the fabrication procedure. PMID:26523427

  9. TiO2 quantum dots as superb compact block layers for high-performance CH3NH3PbI3 perovskite solar cells with an efficiency of 16.97.

    PubMed

    Tu, Yongguang; Wu, Jihuai; Zheng, Min; Huo, Jinghao; Zhou, Pei; Lan, Zhang; Lin, Jianming; Huang, Miaoliang

    2015-12-28

    A compact TiO(2) layer is crucial to achieve high-efficiency perovskite solar cells. In this study, we developed a facile, low-cost and efficient method to fabricate a pinhole-free and ultrathin blocking layer based on highly crystallized TiO(2) quantum dots (QDs) with an average diameter of 3.6 nm. The surface morphology of the blocking layer and the photoelectric performance of the perovskite solar cells were investigated by spin-coating with three different materials: colloidal TiO(2) QDs, titanium precursor solution, and aqueous TiCl(4). Among these three treatments, the perovskite solar cell based on the TiO(2) QD compact layer offered the highest power conversion efficiency (PCE) of 16.97% with a photocurrent density of 22.48 mA cm(-2), a photovoltage of 1.063 V and a fill factor of 0.71. The enhancement of PCE mainly stems from the small series resistance and the large shunt resistance of the TiO(2) QD layer.

  10. TiO2 quantum dots as superb compact block layers for high-performance CH3NH3PbI3 perovskite solar cells with an efficiency of 16.97.

    PubMed

    Tu, Yongguang; Wu, Jihuai; Zheng, Min; Huo, Jinghao; Zhou, Pei; Lan, Zhang; Lin, Jianming; Huang, Miaoliang

    2015-12-28

    A compact TiO(2) layer is crucial to achieve high-efficiency perovskite solar cells. In this study, we developed a facile, low-cost and efficient method to fabricate a pinhole-free and ultrathin blocking layer based on highly crystallized TiO(2) quantum dots (QDs) with an average diameter of 3.6 nm. The surface morphology of the blocking layer and the photoelectric performance of the perovskite solar cells were investigated by spin-coating with three different materials: colloidal TiO(2) QDs, titanium precursor solution, and aqueous TiCl(4). Among these three treatments, the perovskite solar cell based on the TiO(2) QD compact layer offered the highest power conversion efficiency (PCE) of 16.97% with a photocurrent density of 22.48 mA cm(-2), a photovoltage of 1.063 V and a fill factor of 0.71. The enhancement of PCE mainly stems from the small series resistance and the large shunt resistance of the TiO(2) QD layer. PMID:26585357

  11. Impact of Film Stoichiometry on the Ionization Energy and Electronic Structure of CH3 NH3 PbI3 Perovskites.

    PubMed

    Emara, Jennifer; Schnier, Tobias; Pourdavoud, Neda; Riedl, Thomas; Meerholz, Klaus; Olthof, Selina

    2016-01-20

    The electronic structure of a large sample set of CH3 NH3 PbI3 -based perovskites is studied. Combined investigations by UV/X-ray photoelectron spectroscopy and X-ray diffraction reveal that interstitials present in the film lead to changes in the occupied density of states close to the valence band, which in turn influences the performance of solar cells. Changes in elemental composition tune the ionization energy of the perovskite film by almost 1 eV without introducing significant amounts of gap states.

  12. Local structural distortion and electrical transport properties of Bi(Ni1/2Ti1/2)O3 perovskite under high pressure

    DOE PAGES

    Zhu, Jinlong; Yang, Liuxiang; Wang, Hsiu -Wen; Zhang, Jianzhong; Yang, Wenge; Hong, Xinguo; Jin, Changqing; Zhao, Yusheng

    2015-12-16

    Perovskite-structure materials generally exhibit local structural distortions that are distinct from long-range, average crystal structure. The characterization of such distortion is critical to understanding the structural and physical properties of materials. In this work, we combined Pair Distribution Function (PDF) technique with Raman spectroscopy and electrical resistivity measurement to study Bi(Ni1/2Ti1/2)O3 perovskite under high pressure. PDF analysis reveals strong local structural distortion at ambient conditions. As pressure increases, the local structure distortions are substantially suppressed and eventually vanish around 4 GPa, leading to concurrent changes in the electronic band structure and anomalies in the electrical resistivity. We find, consistent withmore » PDF analysis, Raman spectroscopy data suggest that the local structure changes to a higher ordered state at pressures above 4 GPa.« less

  13. Local structural distortion and electrical transport properties of Bi(Ni1/2Ti1/2)O3 perovskite under high pressure.

    PubMed

    Zhu, Jinlong; Yang, Liuxiang; Wang, Hsiu-Wen; Zhang, Jianzhong; Yang, Wenge; Hong, Xinguo; Jin, Changqing; Zhao, Yusheng

    2015-01-01

    Perovskite-structure materials generally exhibit local structural distortions that are distinct from long-range, average crystal structure. The characterization of such distortion is critical to understanding the structural and physical properties of materials. In this work, we combined Pair Distribution Function (PDF) technique with Raman spectroscopy and electrical resistivity measurement to study Bi(Ni1/2Ti1/2)O3 perovskite under high pressure. PDF analysis reveals strong local structural distortion at ambient conditions. As pressure increases, the local structure distortions are substantially suppressed and eventually vanish around 4 GPa, leading to concurrent changes in the electronic band structure and anomalies in the electrical resistivity. Consistent with PDF analysis, Raman spectroscopy data suggest that the local structure changes to a higher ordered state at pressures above 4 GPa. PMID:26671171

  14. Local structural distortion and electrical transport properties of Bi(Ni1/2Ti1/2)O3 perovskite under high pressure

    PubMed Central

    Zhu, Jinlong; Yang, Liuxiang; Wang, Hsiu-Wen; Zhang, Jianzhong; Yang, Wenge; Hong, Xinguo; Jin, Changqing; Zhao, Yusheng

    2015-01-01

    Perovskite-structure materials generally exhibit local structural distortions that are distinct from long-range, average crystal structure. The characterization of such distortion is critical to understanding the structural and physical properties of materials. In this work, we combined Pair Distribution Function (PDF) technique with Raman spectroscopy and electrical resistivity measurement to study Bi(Ni1/2Ti1/2)O3 perovskite under high pressure. PDF analysis reveals strong local structural distortion at ambient conditions. As pressure increases, the local structure distortions are substantially suppressed and eventually vanish around 4 GPa, leading to concurrent changes in the electronic band structure and anomalies in the electrical resistivity. Consistent with PDF analysis, Raman spectroscopy data suggest that the local structure changes to a higher ordered state at pressures above 4 GPa. PMID:26671171

  15. Local structural distortion and electrical transport properties of Bi(Ni1/2Ti1/2)O3 perovskite under high pressure

    NASA Astrophysics Data System (ADS)

    Zhu, Jinlong; Yang, Liuxiang; Wang, Hsiu-Wen; Zhang, Jianzhong; Yang, Wenge; Hong, Xinguo; Jin, Changqing; Zhao, Yusheng

    2015-12-01

    Perovskite-structure materials generally exhibit local structural distortions that are distinct from long-range, average crystal structure. The characterization of such distortion is critical to understanding the structural and physical properties of materials. In this work, we combined Pair Distribution Function (PDF) technique with Raman spectroscopy and electrical resistivity measurement to study Bi(Ni1/2Ti1/2)O3 perovskite under high pressure. PDF analysis reveals strong local structural distortion at ambient conditions. As pressure increases, the local structure distortions are substantially suppressed and eventually vanish around 4 GPa, leading to concurrent changes in the electronic band structure and anomalies in the electrical resistivity. Consistent with PDF analysis, Raman spectroscopy data suggest that the local structure changes to a higher ordered state at pressures above 4 GPa.

  16. The Impact of the Crystallization Processes on the Structural and Optical Properties of Hybrid Perovskite Films for Photovoltaics.

    PubMed

    Grancini, Giulia; Marras, Sergio; Prato, Mirko; Giannini, Cinzia; Quarti, Claudio; De Angelis, Filippo; De Bastiani, Michele; Eperon, Giles E; Snaith, Henry J; Manna, Liberato; Petrozza, Annamaria

    2014-11-01

    We investigate the relationship between structural and optical properties of organo-lead mixed halide perovskite films as a function of the crystallization mechanism. For methylammonium lead tri-iodide, the organic cations rearrange within the inorganic cage, moving from crystals grown in a mesoporous scaffold to larger, oriented crystals grown on a flat substrate. This reduces the strain felt by the bonds forming the cage and affects the motion of the organic cation in it, influencing the electronic transition at the onset of the optical absorption spectrum of the semiconductor. Moreover, we demonstrate that in mixed-halide perovskite, though Cl(-) ions are not present in a detectable concentration in the unit cell, they drive the crystallization dynamics. This induces a preferential order during crystallization, from a molecular, i.e., organic-inorganic moieties arrangement, to a nano-mesoscopic level, i.e., larger crystals with anisotropic shape. Finally, we show that while Cl is mainly expelled from flat films made of large crystals, in the presence of an oxide mesoporous scaffold they are partially retained in the composite.

  17. Flow visualization of turbulent boundary layer structure

    NASA Astrophysics Data System (ADS)

    Head, M. R.; Bandyopadhyay, P.

    1980-01-01

    The results from flow visualization experiments performed using an argon-ion laser to illuminate longitudinal and transverse sections of the smoke filled boundary layer in zero pressure gradient are discussed. Most of the experiments were confined to the range 600 Re sub theta 10,000. Results indicate that the boundary layer consists almost exclusively of vortex loops or hairpins, some of which may extend through the complete boundary layer thickness and all of which are inclined at a more or less constant characteristic angle of approximately 45 deg to the wall. Since the cross-stream dimensions of the hairpins appear to scale roughly with the wall variables U sub tau and nu, while their length is limited only by the boundary layer thickness, there are very large scale effects on the turbulence structure. At high Reynolds numbers (Re sub theta = 10,000) there is little evidence of large-scale coherent motions, other than a slow overturning of random agglomerations of the hairpins just mentioned.

  18. Flexible Hybrid Organic-Inorganic Perovskite Memory.

    PubMed

    Gu, Chungwan; Lee, Jang-Sik

    2016-05-24

    Active research has been done on hybrid organic-inorganic perovskite materials for application to solar cells with high power conversion efficiency. However, this material often shows hysteresis, which is undesirable, shift in the current-voltage curve. The hysteresis may come from formation of defects and their movement in perovskite materials. Here, we utilize the defects in perovskite materials to be used in memory operations. We demonstrate flexible nonvolatile memory devices based on hybrid organic-inorganic perovskite as the resistive switching layer on a plastic substrate. A uniform perovskite layer is formed on a transparent electrode-coated plastic substrate by solvent engineering. Flexible nonvolatile memory based on the perovskite layer shows reproducible and reliable memory characteristics in terms of program/erase operations, data retention, and endurance properties. The memory devices also show good mechanical flexibility. It is suggested that resistive switching is done by migration of vacancy defects and formation of conducting filaments under the electric field in the perovskite layer. It is believed that organic-inorganic perovskite materials have great potential to be used in high-performance, flexible memory devices. PMID:27093096

  19. New structure and spin state of iron-rich (Mg,Fe)SiO[subscript 3] post-perovskite

    SciTech Connect

    Yamanaka, T.; Mao, W.L.; Mao, H.-K.; Hemley, R.J.; Shen, G.

    2010-05-24

    There was a discrepancy between the seismic tomography and the elastic property of MgSiO{sub 3} perovskite at near the D{double_prime} zone and core boundary. Since a discovery of post-perovskite (ppv) of MgSiO{sub 3}, many investigations have made to explain the presence of low seismic velocity of the lower mantle and D{double_prime} zone. However, precise experimental structure analysis of ppv-(Mg{sub 1-x}Fe{sub x})SiO{sub 3} has never been reported because of the experimental difficulty. Fe and Mg cation distribution and ordering in ppv-(Mg,Fe)SiO{sub 3} in consideration of spins states are significant subject in lower mantle electronic and magnetic states. The present experiment aims X-ray emission study and structure analysis by Rietveld profile fitting of ppv-(Mg{sub 0.6},Fe{sub 0.4})SiO{sub 3} by the precise powder diffraction measurement. Monte Carlo calculation proposed the reliable structures of iron-rich phase of ppv-(Mg,Fe)SiO{sub 3}: Pmmn, Pmma, and Cm2m and Cmcm proposed by. The best-fit structure model with the highest reliability in the Rietveld fitting of ppv-(Mg{sub 0.6}Fe{sub 0.4})SiO{sub 3} is the structure of space group Pmma, in which Fe and Mg occupy two different sites of M1 and M2: the site occupancies are (Fe{sub 0.25}Mg{sub 0.75}) in the larger M1 site and (Fe{sub 0.55}, Mg{sub 0.45}) in the smaller M2 site. The two-site model is consistence with the previous results of X-ray emission and X-ray Moessbauer experiments.

  20. Efficient Visible Quasi-2D Perovskite Light-Emitting Diodes.

    PubMed

    Byun, Jinwoo; Cho, Himchan; Wolf, Christoph; Jang, Mi; Sadhanala, Aditya; Friend, Richard H; Yang, Hoichang; Lee, Tae-Woo

    2016-09-01

    Efficient quasi-2D-structure perovskite light-emitting diodes (4.90 cd A(-1) ) are demonstrated by mixing a 3D-structured perovskite material (methyl ammonium lead bromide) and a 2D-structured perovskite material (phenylethyl ammonium lead bromide), which can be ascribed to better film uniformity, enhanced exciton confinement, and reduced trap density. PMID:27334788

  1. Efficient Visible Quasi-2D Perovskite Light-Emitting Diodes.

    PubMed

    Byun, Jinwoo; Cho, Himchan; Wolf, Christoph; Jang, Mi; Sadhanala, Aditya; Friend, Richard H; Yang, Hoichang; Lee, Tae-Woo

    2016-09-01

    Efficient quasi-2D-structure perovskite light-emitting diodes (4.90 cd A(-1) ) are demonstrated by mixing a 3D-structured perovskite material (methyl ammonium lead bromide) and a 2D-structured perovskite material (phenylethyl ammonium lead bromide), which can be ascribed to better film uniformity, enhanced exciton confinement, and reduced trap density.

  2. Single Cesium Lead Halide Perovskite Nanocrystals at Low Temperature: Fast Single-Photon Emission, Reduced Blinking, and Exciton Fine Structure

    PubMed Central

    2016-01-01

    Metal-halide semiconductors with perovskite crystal structure are attractive due to their facile solution processability, and have recently been harnessed very successfully for high-efficiency photovoltaics and bright light sources. Here, we show that at low temperature single colloidal cesium lead halide (CsPbX3, where X = Cl/Br) nanocrystals exhibit stable, narrow-band emission with suppressed blinking and small spectral diffusion. Photon antibunching demonstrates unambiguously nonclassical single-photon emission with radiative decay on the order of 250 ps, representing a significant acceleration compared to other common quantum emitters. High-resolution spectroscopy provides insight into the complex nature of the emission process such as the fine structure and charged exciton dynamics. PMID:26771336

  3. Tunable Photonic Devices in Ferroelectric-Based Layered Structures

    NASA Astrophysics Data System (ADS)

    Xin, Jianzhuo

    This thesis presents the studies on the optical properties of perovskite ferroelectric thin films, as well as the preparation and applications of ferroelectrics in tunable photonic devices. Ba(Zr,Ti)O3 (BZT) thin films with different Zr concentration were grown on MgO substrates by pulsed laser deposition, and their structural and optical properties in the visible range were systematically characterized, including the out-of-plane lattice constant, grain size, refractive index, optical band gap energy, electro-optic coefficient, optical loss and absorption coefficient. The obtained results provide information for the design of BZT thin film-based optical devices. One-dimensional photonic crystal filter working in the terahertz (THz) range was studied. The transmission properties of SrTiO3 (STO) crystals were first characterized by THz time-domain spectroscopy. Si/STO multilayers with different STO defect thicknesses were designed by the transfer matrix method and then constructed by polishing and stacking. The shift of defect mode was observed and comparable with the calculations. Two-dimensional photonic structures in the optical and infra-red range were then attempted. A combination of nanoimprint lithography and inductively coupled plasma etching were investigated on (Ba,Sr)TiO3 thin films. Then, in order to simplify the nanoimprint process and allow thick metal sacrificial layer deposition for high aspect-ratio etching, a transfer imprint lithography technique was developed. Finally, surface plasmon resonance (SPR) tuning via thermally-induced refractive index changes in ferroelectrics was investigated. Ag stripes with periodicity 750 nm were fabricated on flat BST surface by nanoimprint lithography and subsequent lift-off. (-1), (2) and (-2) SP modes from Ag/BST interface were observed in visible range. Red shift of the modes up to 3.9 nm was obtained with increasing temperature. Then continuous Au film on corrugated BST surface with periodicity of 1 mum was

  4. Correlations of Optical Absorption, Charge Trapping, and Surface Roughness of TiO2 Photoanode Layer Loaded with Neat Ag-NPs for Efficient Perovskite Solar Cells.

    PubMed

    Yang, Dongwook; Jang, Jae Gyu; Lim, Joohyun; Lee, Jin-Kyu; Kim, Sung Hyun; Hong, Jong-In

    2016-08-24

    We systematically investigated the effect of silver nanoparticles (Ag-NPs) on the power conversion efficiency (PCE) of perovskite solar cells (PSCs). Neat, spherical Ag-NPs at loading levels of 0.0, 0.5, 1.0, and 2.0 wt % were embedded into the titanium dioxide (TiO2) photoanode layer. The plasmonic effect of the Ag-NPs strongly enhanced the incident light absorption over a wide range of the visible wavelength region in addition to the inherent absorbance of the perovskite sensitizer. The low conduction energy level of the Ag-NPs compared to that of TiO2 provides trap sites for free charge carriers. Thus, the correlation between the enhancement of the optical absorption and the number of charge traps provided by the Ag-NPs is critical to determine the device performance, especially current density (Jsc) and PCE. This is confirmed by the quantitative comparison of the incident light absorption and the time-resolved photoluminescence decay according to the loading levels of the Ag-NPs in the TiO2 layer. The absorption enhancement from 380 to 750 nm in the UV-visible spectrum is proportional to the increase in the loading levels of the Ag-NPs. However, the Jsc increases with the device with 0.5 wt % Ag-NPs and gradually decreases with increases in the loading level above 0.5 wt % because of the different contributions to the absorbance and the charge trapping by different Ag-NP loading levels. In addition, the suppression of the surface roughness with dense packing by the Ag-NPs helps to improve the Jsc and the following PCE. Consequently, the PCE of the PSC with 0.5 wt % Ag-NPs is increased to 11.96%. These results are attributed to the balance between increased absorbance by the localized surface plasmon resonance and the decreased charge trapping as well as the decreased surface roughness of the TiO2 layer with the Ag-NPs. PMID:27471777

  5. Effect of sintering time on structural, microstructural and chemical composition of Ni-doped lanthanum gallate perovskites

    SciTech Connect

    Colomer, M.T.

    2015-08-15

    This work reports the effect of two different sintering times, 6 and 48 h on the structural, microstructural, and chemical features of Ni-doped La{sub 0.90}Sr{sub 0.10}GaO{sub 3.00−δ}. Independently of the sintering time, La{sub 0.90}Sr{sub 0.10}Ga{sub 1−x}Ni{sub x}O{sub 3.00−δ} (where x=0.10, and 0.20 (mol)) presents a rhombohedral symmetry with a lattice volume that decreases when NiO dopant increases. Besides the perovskite, LaSrGa{sub 3.00}O{sub 7.00} (nominal composition) is present as second phase in all cases. When the samples are doped with NiO, the peaks of this second phase are shifted with respect to the peaks of the pure phase. These shifts suggest that this second phase could admit some Ni ions in its structure. According to the XRD patterns, the amount of the latter phase is larger when sintering time is increased. Electron probe microanalysis (EPMA) indicated that the matrix of the samples sintered for 6 h is constituted by a perovskite with an experimental composition very close to the nominal one. However, when the samples are sintered for 48 h the matrix of each sample is constituted by two perovskites; both with compositional deviations with respect to their nominal one. In particular, a significant Sr depletion compensated by a La increment in the A site is observed. Those compositional deviations could be mainly due to the diffusion of the cations in the bulk and/or from the bulk to the surface of the samples. That diffusion can favour the formation, not only, of a second perovskite with a different composition in relation with the first one formed, but also, the formation of second phases. In addition, a very slight broadening of Bragg peaks of the perovskites sintered for 48 h is observed by XRD and can be related to the presence of two different perovskites in each sample according to EPMA results. By BSEM and EPMA analyses La{sub 4.00}Ga{sub 2.00}O{sub 9.00} (nominal composition) is also observed as second phase when samples are

  6. Synthesis, structural and dielectric properties of double perovskite Ho2FeMnO6

    NASA Astrophysics Data System (ADS)

    Chakraborty, Tirthankar; Elizabeth, Suja

    2016-05-01

    A new double perovskite Ho2FeMnO6 was grown by nitrate route. Temperature dependent dielectric response was recorded at different frequencies. Relaxor-like-behavior is observed whose activation energy was calculated using Arrhenius equation. The dispersion is very small at room temperature. The Nyquist plot over a broad frequency range at room temperature provides evidence for the presence of three relaxations from sample electrode interface, grain boundary and grain. The corresponding values of resistance and capacitance were calculated from the equivalent circuit model analysis of the Nyquist plot.

  7. Damage modes in dental layer structures.

    PubMed

    Jung, Y G; Wuttiphan, S; Peterson, I M; Lawn, B R

    1999-04-01

    Natural teeth (enamel/dentin) and most restorations are essentially layered structures. This study examines the hypothesis that coating thickness and coating/substrate mismatch are key factors in the determination of contact-induced damage in clinically relevant bilayer composites. Accordingly, we study crack patterns in two model "coating/substrate" bilayer systems conceived to simulate crown and tooth structures, at opposite extremes of elastic/plastic mismatch: porcelain on glass-infiltrated alumina ("soft/hard"); and glass-ceramic on resin composite ("hard/soft"). Hertzian contacts are used to investigate the evolution of fracture damage in the coating layers, as functions of contact load and coating thickness. The crack patterns differ radically in the two bilayer systems: In the porcelain coatings, cone cracks initiate at the coating top surface; in the glass-ceramic coatings, cone cracks again initiate at the top surface, but additional, upward-extending transverse cracks initiate at the internal coating/substrate interface, with the latter dominant. The substrate is thereby shown to have a profound influence on the damage evolution to ultimate failure in the bilayer systems. However, the cracks are highly stabilized in both systems, with wide ranges between the loads to initiate first cracking and to cause final failure, implying damage-tolerant structures. Finite element modeling is used to evaluate the tensile stresses responsible for the different crack types. The clinical relevance of these observations is considered. PMID:10326733

  8. Enhancing stability and efficiency of perovskite solar cells with crosslinkable silane-functionalized and doped fullerene

    PubMed Central

    Bai, Yang; Dong, Qingfeng; Shao, Yuchuan; Deng, Yehao; Wang, Qi; Shen, Liang; Wang, Dong; Wei, Wei; Huang, Jinsong

    2016-01-01

    The instability of hybrid perovskite materials due to water and moisture arises as one major challenge to be addressed before any practical application of the demonstrated high efficiency perovskite solar cells. Here we report a facile strategy that can simultaneously enhance the stability and efficiency of p–i–n planar heterojunction-structure perovskite devices. Crosslinkable silane molecules with hydrophobic functional groups are bonded onto fullerene to make the fullerene layer highly water-resistant. Methylammonium iodide is introduced in the fullerene layer for n-doping via anion-induced electron transfer, resulting in dramatically increased conductivity over 100-fold. With crosslinkable silane-functionalized and doped fullerene electron transport layer, the perovskite devices deliver an efficiency of 19.5% with a high fill factor of 80.6%. A crosslinked silane-modified fullerene layer also enhances the water and moisture stability of the non-sealed perovskite devices by retaining nearly 90% of their original efficiencies after 30 days' exposure in an ambient environment. PMID:27703136

  9. Enhancing stability and efficiency of perovskite solar cells with crosslinkable silane-functionalized and doped fullerene

    NASA Astrophysics Data System (ADS)

    Bai, Yang; Dong, Qingfeng; Shao, Yuchuan; Deng, Yehao; Wang, Qi; Shen, Liang; Wang, Dong; Wei, Wei; Huang, Jinsong

    2016-10-01

    The instability of hybrid perovskite materials due to water and moisture arises as one major challenge to be addressed before any practical application of the demonstrated high efficiency perovskite solar cells. Here we report a facile strategy that can simultaneously enhance the stability and efficiency of p-i-n planar heterojunction-structure perovskite devices. Crosslinkable silane molecules with hydrophobic functional groups are bonded onto fullerene to make the fullerene layer highly water-resistant. Methylammonium iodide is introduced in the fullerene layer for n-doping via anion-induced electron transfer, resulting in dramatically increased conductivity over 100-fold. With crosslinkable silane-functionalized and doped fullerene electron transport layer, the perovskite devices deliver an efficiency of 19.5% with a high fill factor of 80.6%. A crosslinked silane-modified fullerene layer also enhances the water and moisture stability of the non-sealed perovskite devices by retaining nearly 90% of their original efficiencies after 30 days' exposure in an ambient environment.

  10. PbnI4n+2(2n+2)- ribbons (n = 3, 5) as dimensional reductions of 2D perovskite layers in cystamine cation based hybrids, also incorporating iodine molecules or reversible guest water molecules.

    PubMed

    Louvain, Nicolas; Bi, Wenhua; Mercier, Nicolas; Buzaré, Jean-Yves; Legein, Christophe; Corbel, Gwenaël

    2007-03-01

    Pb(n)I(4n+2)((2n+2)-) (n = 3, 5) ribbons, which can be regarded as dimensional reductions of 2D perovskite layers, are stabilized by diprotonated cystamine cations in (NH(3)(CH(2))(2)SS(CH(2))(2)NH(3))(4)Pb(3)I(14),I(2) (1) and (NH(3)(CH(2))(2)SS(CH(2))(2)NH(3))(6)Pb(5)I(22).4H(2)O (2). Both 1 and 2 have interesting structural characteristics; it is unprecedented that the ribbons are linked via I(2) molecules incorporated in the lattice of 1, while tetrameric water clusters are trapped in the structure of 2. 2 undergoes a (reversible) water desorption process at 310 K leading to (NH(3)(CH(2))(2)SS(CH(2))(2)NH(3))(6)Pb(5)I(22).2H(2)O (3). The electrical behavior of 2 and 3 has been investigated in the ranges 293-310 K and 310-358 K respectively. Above 310 K, the electronic contribution remains constant while the ionic transference number tends towards unity showing almost pure ionic transport at 360 K (6 x 10(-7) S cm(-1) at 330 K) originating probably from the migration of protons through the hydrogen bonds connecting the water molecules to the cystamine counter cations.

  11. Solution-processed flexible planar perovskite solar cells: A strategy to enhance efficiency by controlling the ZnO electron transfer layer, PbI2 phase, and CH3NH3PbI3 morphologies

    NASA Astrophysics Data System (ADS)

    Jung, Kyungeun; Lee, Jeongwon; Kim, Joosun; Chae, Weon-Sik; Lee, Man-Jong

    2016-08-01

    This paper reports a synergistic strategy to enhance the power conversion efficiency (PCE) of flexible planar perovskite solar cells (PSCs) by controlling the thickness of the ZnO electron transport layer (ETL), PbI2 phase, and size/morphology of the perovskite (MAPbI3) absorber layer. To optimize the size/morphology of MAPbI3 via a two-step spin coating process, various volumes of CH3NH3I precursor solutions with a constant concentration were continuously coated, which greatly affected the grain growth condition of the MAPbI3. In addition, the remnant PbI2 phase in the MAPbI3, which acted as a recombination barrier, was simultaneously controlled. This strategic method to synergistically combine the major factors affecting the final PCE resulted in the best efficiency of 12.3%, which is the highest efficiency among ZnO-ETL-based flexible planar PSCs to date.

  12. Cycling Performance of a Columnar-Structured Complex Perovskite in a Temperature Gradient Test

    NASA Astrophysics Data System (ADS)

    Schlegel, N.; Sebold, D.; Sohn, Y. J.; Mauer, G.; Vaßen, R.

    2015-10-01

    To increase the efficiency of turbines for the power generation and the aircraft industry, advanced thermal barrier coatings (TBCs) are required. They need to be long-term stable at temperatures higher than 1200 °C. Nowadays, yttria partially stabilized zirconia (YSZ) is applied as standard TBC material. But its long-term application at temperatures higher than 1200 °C leads to detrimental phase changes and sintering effects. Therefore, new materials have to be investigated, for example, complex perovskites. They provide high melting points, high thermal expansion coefficients and thermal conductivities of approx. 2.0 W/(m K). In this work, the complex perovskite La(Al1/4Mg1/2Ta1/4)O3 (LAMT) was investigated. It was deposited by the suspension plasma spraying (SPS) process, resulting in a columnar microstructure of the coating. The coatings were tested in thermal cycling gradient tests and they show excellent results, even though some phase decomposition was found.

  13. The electronic structure of the high-symmetry perovskite iridate Ba2IrO4

    NASA Astrophysics Data System (ADS)

    Moser, S.; Moreschini, L.; Ebrahimi, A.; Dalla Piazza, B.; Isobe, M.; Okabe, H.; Akimitsu, J.; Mazurenko, V. V.; Kim, K. S.; Bostwick, A.; Rotenberg, E.; Chang, J.; Rønnow, H. M.; Grioni, M.

    2014-01-01

    We report angle-resolved photoemission (ARPES) measurements, density functional and model tight-binding calculations on Ba2IrO4 (Ba-214), an antiferromagnetic (TN = 230 K) insulator. Ba-214 does not exhibit the rotational distortion of the IrO6 octahedra that is present in its sister compound Sr2IrO4 (Sr-214), and is therefore an attractive reference material to study the electronic structure of layered iridates. We find that the band structures of Ba-214 and Sr-214 are qualitatively similar, hinting at the predominant role of the spin-orbit interaction in these materials. Temperature-dependent ARPES data show that the energy gap persists well above TN, and favor a Mott over a Slater scenario for this compound.

  14. High-Pressure Single-Crystal Structures of 3D Lead-Halide Hybrid Perovskites and Pressure Effects on their Electronic and Optical Properties.

    PubMed

    Jaffe, Adam; Lin, Yu; Beavers, Christine M; Voss, Johannes; Mao, Wendy L; Karunadasa, Hemamala I

    2016-04-27

    We report the first high-pressure single-crystal structures of hybrid perovskites. The crystalline semiconductors (MA)PbX3 (MA = CH3NH3 (+), X = Br(-) or I(-)) afford us the rare opportunity of understanding how compression modulates their structures and thereby their optoelectronic properties. Using atomic coordinates obtained from high-pressure single-crystal X-ray diffraction we track the perovskites' precise structural evolution upon compression. These structural changes correlate well with pressure-dependent single-crystal photoluminescence (PL) spectra and high-pressure bandgaps derived from density functional theory. We further observe dramatic piezochromism where the solids become lighter in color and then transition to opaque black with compression. Indeed, electronic conductivity measurements of (MA)PbI3 obtained within a diamond-anvil cell show that the material's resistivity decreases by 3 orders of magnitude between 0 and 51 GPa. The activation energy for conduction at 51 GPa is only 13.2(3) meV, suggesting that the perovskite is approaching a metallic state. Furthermore, the pressure response of mixed-halide perovskites shows new luminescent states that emerge at elevated pressures. We recently reported that the perovskites (MA)Pb(Br x I1-x )3 (0.2 < x < 1) reversibly form light-induced trap states, which pin their PL to a low energy. This may explain the low voltages obtained from solar cells employing these absorbers. Our high-pressure PL data indicate that compression can mitigate this PL redshift and may afford higher steady-state voltages from these absorbers. These studies show that pressure can significantly alter the transport and thermodynamic properties of these technologically important semiconductors. PMID:27163050

  15. High-Pressure Single-Crystal Structures of 3D Lead-Halide Hybrid Perovskites and Pressure Effects on their Electronic and Optical Properties.

    PubMed

    Jaffe, Adam; Lin, Yu; Beavers, Christine M; Voss, Johannes; Mao, Wendy L; Karunadasa, Hemamala I

    2016-04-27

    We report the first high-pressure single-crystal structures of hybrid perovskites. The crystalline semiconductors (MA)PbX3 (MA = CH3NH3 (+), X = Br(-) or I(-)) afford us the rare opportunity of understanding how compression modulates their structures and thereby their optoelectronic properties. Using atomic coordinates obtained from high-pressure single-crystal X-ray diffraction we track the perovskites' precise structural evolution upon compression. These structural changes correlate well with pressure-dependent single-crystal photoluminescence (PL) spectra and high-pressure bandgaps derived from density functional theory. We further observe dramatic piezochromism where the solids become lighter in color and then transition to opaque black with compression. Indeed, electronic conductivity measurements of (MA)PbI3 obtained within a diamond-anvil cell show that the material's resistivity decreases by 3 orders of magnitude between 0 and 51 GPa. The activation energy for conduction at 51 GPa is only 13.2(3) meV, suggesting that the perovskite is approaching a metallic state. Furthermore, the pressure response of mixed-halide perovskites shows new luminescent states that emerge at elevated pressures. We recently reported that the perovskites (MA)Pb(Br x I1-x )3 (0.2 < x < 1) reversibly form light-induced trap states, which pin their PL to a low energy. This may explain the low voltages obtained from solar cells employing these absorbers. Our high-pressure PL data indicate that compression can mitigate this PL redshift and may afford higher steady-state voltages from these absorbers. These studies show that pressure can significantly alter the transport and thermodynamic properties of these technologically important semiconductors.

  16. Investigation on structural, optical and magnetic properties of double perovskite Gd{sub 2}NiMnO{sub 6}

    SciTech Connect

    Mohapatra, S. R.; Sahu, B.; Raut, S.; Singh, A. K.; Kaushik, S. D.

    2015-06-24

    Single phase double perovskite Gd{sub 2}NiMnO{sub 6} was prepared by conventional solid state reaction route. X-ray diffraction (XRD) result reveals that the compound possess monoclinic structure with space group P2{sub 1}/n. Optical characterization performed at room temperature via UV-visible spectroscopy confirms Gd{sub 2}NiMnO{sub 6} as a direct band-gap material with band gap of ∼1.5 eV. Magnetization measurement in Zero field cooled (ZFC) condition at H = 100 Oe shows magnetic transition at ∼ 125 K. Due to competing interactions between magnetic ions (Ni{sup 2+} and Mn{sup 4+}), we could observe two magnetic transition below 40 K.

  17. Structure and magnetic properties of spinel-perovskite nanocomposite thin films on SrTiO3 (111) substrates

    NASA Astrophysics Data System (ADS)

    Kim, Dong Hun; Yang, Junho; Kim, Min Seok; Kim, Tae Cheol

    2016-09-01

    Epitaxial CoFe2O4-BiFeO3 nanocomposite thin films were synthesized on perovskite structured SrTiO3 (001) and (111) substrates by combinatorial pulsed laser deposition and characterized using scanning electron microscopy, x-ray diffraction, and vibrating sample magnetometer. Triangular BiFeO3 nanopillars were formed in a CoFe2O4 matrix on (111) oriented SrTiO3 substrates, while CoFe2O4 nanopillars with rectangular or square top surfaces grew in a BiFeO3 matrix on (001) substrates. The magnetic hysteresis loops of nanocomposites on (111) oriented SrTiO3 substrates showed isotropic properties due to the strain relaxation while those of films on SrTiO3 (001) substrates exhibited a strong out-of-plane anisotropy originated from shape and strain effects.

  18. Dominance of interface chemistry over the bulk properties in determining the electronic structure of epitaxial metal/perovskite oxide heterojunctions

    SciTech Connect

    Chambers, Scott A.; Du, Yingge; Gu, Meng; Droubay, Timothy C.; Hepplestone, Steven; Sushko, Petr

    2015-06-09

    We show that despite very similar crystallographic properties and work function values in the bulk, epitaxial Fe and Cr metallizations on Nb:SrTiO3(001) generate completely different heterojunction electronic properties. Cr is Ohmic whereas Fe forms a Schottky barrier with a barrier height of 0.50 eV. This contrast arises because of differences in interface chemistry. In contrast to Cr [Chambers, S. A. et al., Adv. Mater. 2013, 25, 4001.], Fe exhibits a +2 oxidation state and occupies Ti sites in the perovskite lattice, resulting in negligible charge transfer to Ti, upward band bending, and Schottky barrier formation. The differences between Cr and Fe are understood by performing first-principles calculations of the energetics of defect formation which corroborate the observed interface chemistry and structure.

  19. Layered graphene structure of a hexagonal carbon

    NASA Astrophysics Data System (ADS)

    Zhang, Bin

    2013-06-01

    Experiments show that there is a novel hexagonal carbon polymorph restricted to the space group of P-62c, but the detailed atomic structure is not determined. Here we set carbon atoms occupying P-62c 4f or P-62c 2c and 2d Wyckoff positions, and calculate the total energy of the different cell structures changing the internal parameter by first-principles calculations, which demonstrates that the stable structures in energy (at local minima) are hexagonal carbon (P-62c 2c and 2d) and hexagonal diamond (P-62c 4f, z=1/16). The calculated bulk modulus 437±16 GPa and interlayer distance 2.062 Å of the layered graphene structure P-62c 2c and 2d are in good agreement with those of the proposed new carbon, which indicates that P-62c 2c and 2d is a possible precursor or intermediate hard phase during the structural transformation of carbon.

  20. Structured Water Layers Adjacent to Biological Membranes

    PubMed Central

    Higgins, Michael J.; Polcik, Martin; Fukuma, Takeshi; Sader, John E.; Nakayama, Yoshikazu; Jarvis, Suzanne P.

    2006-01-01

    Water amid the restricted space of crowded biological macromolecules and at membrane interfaces is essential for cell function, though the structure and function of this “biological water” itself remains poorly defined. The force required to remove strongly bound water is referred to as the hydration force and due to its widespread importance, it has been studied in numerous systems. Here, by using a highly sensitive dynamic atomic force microscope technique in conjunction with a carbon nanotube probe, we reveal a hydration force with an oscillatory profile that reflects the removal of up to five structured water layers from between the probe and biological membrane surface. Further, we find that the hydration force can be modified by changing the membrane fluidity. For 1,2-dipalmitoyl-sn-glycero-3-phosphocholine gel (Lβ) phase bilayers, each oscillation in the force profile indicates the force required to displace a single layer of water molecules from between the probe and bilayer. In contrast, 1,2-dipalmitoyl-sn-glycero-3-phosphocholine fluid (Lα) phase bilayers at 60°C and 1,2-dioleoyl-sn-glycero-3-phosphocholine fluid (Lα) phase bilayers at 24°C seriously disrupt the molecular ordering of the water and result predominantly in a monotonic force profile. PMID:16798815

  1. Improving the efficiency of perovskite solar cells through optimization of the CH3NH3PbI3 film growth in solution process method

    NASA Astrophysics Data System (ADS)

    Zhao, Ying; Liu, Jian; Lu, Xinrong; Gao, Yandong; You, Xiaozeng; Xu, Xiangxing

    2015-12-01

    Perovskite-structured organic-inorganic materials such as CH3NH3PbI3 are attracting much interest in the scientific community because of their abilities to function as revolutionary light harvesters and charge transfer materials for solar cells. To achieve high power conversion efficiency (PCE), it is critical to optimize the perovskite film layer. This paper reports the temperature and concentration controls on the two-step solution process. A diffusion-controlled growth mechanism is proposed for this process in tuning the morphology and purity of the perovskite film, which are proven to be important factors contributing to the photovoltaic performance. The highest PCE of 11.92% is achieved with an optimized perovskite crystal size of ∼150 nm and an appropriate amount of residual PbI2. This study sheds light on the design and fabrication of highly efficient, low-cost, solution-processed perovskite solar cells.

  2. Krypton irradiation damage in Nd-doped zirconolite and perovskite

    NASA Astrophysics Data System (ADS)

    Davoisne, C.; Stennett, M. C.; Hyatt, N. C.; Peng, N.; Jeynes, C.; Lee, W. E.

    2011-08-01

    Understanding the effect of radiation damage and noble gas accommodation in potential ceramic hosts for plutonium disposition is necessary to evaluate their long-term behaviour during geological disposal. Polycrystalline samples of Nd-doped zirconolite and Nd-doped perovskite were irradiated ex situ with 2 MeV Kr + at a dose of 5 × 10 15 ions cm -2 to simulate recoil of Pu nuclei during alpha decay. The feasibility of thin section preparation of both pristine and irradiated samples by Focused Ion Beam sectioning was demonstrated. After irradiation, the Nd-doped zirconolite revealed a well defined amorphous region separated from the pristine material by a thin (40-60 nm) damaged interface. The zirconolite lattice was lost in the damaged interface, but the fluorite sublattice was retained. The Nd-doped perovskite contained a defined irradiated layer composed of an amorphous region surrounded by damaged but still crystalline layers. The structural evolution of the damaged regions is consistent with a change from orthorhombic to cubic symmetry. In addition in Nd-doped perovskite, the amorphisation dose depended on crystallographic orientation and possibly sample configuration (thin section or bulk). Electron Energy Loss Spectroscopy revealed Ti remained in the 4+ oxidation state but there was a change in Ti coordination in both Nd-doped perovskite and Nd-doped zirconolite associated with the crystalline to amorphous transition.

  3. Synthesis of LaYbO3 perovskite through modified Pechini method: Structural, electric and magnetic characterization

    NASA Astrophysics Data System (ADS)

    Jaramillo P, J. A.; Landínez Téllez, D. A.; Roa-Rojas, J.; Parra Vargas, C. A.; Barrera, E. W.

    2015-10-01

    Single phase LaYbO3 lanthanide-based perovskite powder was synthesized by modified Pechini method, which is based on polyesterification of metal-citrate complexes in aqueous solution. Complexes were formed in aqueous solution and after polyalcohol addition and slow water evaporation, bond formation is allowed and a macroscopic polymeric network was produced, where cations are embedded and uniformly distributed. Finally, through several pyrolysis steps, microcrystalline oxide particles were obtained. Structural characterization was performed by means the powder X-ray diffraction (XRD) technique. The obtained patterns were indexed and refined to reveal that the LaYbO3 simple perovskite crystallizes in an orthorhombic structure, belonging to the Pnma (#62) space group, with lattice constants a = 6.0327 Å, b = 8.4138 Å and c = 5.8307 Å. Studies of electron dispersive X-ray spectroscopy show that the LaYbO3 is free of impurities. Electric response was evaluated by electric polarization measurements as a function of applied electric fields. Obtained curves show evidence of a hysteretic behavior related with dielectric losses which are characteristics of insulator materials. From the saturation values of electric charge, the relative dielectric constant was determined to be 22.6. The magnetic behavior was examined by means of the curves of magnetic susceptibility as a function of temperature. The fit with the Curie equation is in agreement with a typical paramagnetic feature with effective magnetic moment μ = 4.9 μB, which is close to the theoretical expected value from the Hund’s rules.

  4. Emergence of Hysteresis and Transient Ferroelectric Response in Organo-Lead Halide Perovskite Solar Cells.

    PubMed

    Chen, Hsin-Wei; Sakai, Nobuya; Ikegami, Masashi; Miyasaka, Tsutomu

    2015-01-01

    Although there has been rapid progress in the efficiency of perovskite-based solar cells, hysteresis in the current-voltage performance is not yet completely understood. Owing to its complex structure, it is not easy to attribute the hysteretic behavior to any one of different components, such as the bulk of the perovskite or different heterojunction interfaces. Among organo-lead halide perovskites, methylammonium lead iodide perovskite (CH3NH3PbI3) is known to have a ferroelectric property. The present investigation reveals a strong correlation between transient ferroelectric polarization of CH3NH3PbI3 induced by an external bias in the dark and hysteresis enhancement in photovoltaic characteristics. Our results demonstrate that the reverse bias poling (-0.3 to -1.1 V) of CH3NH3PbI3 photovoltaic layers prior to the photocurrent-voltage measurement generates stronger hysteresis whose extent changes significantly by the cell architecture. The phenomenon is interpreted as the effect of remanent polarization in the perovskite film on the photocurrent, which is most enhanced in planar perovskite structures without mesoporous scaffolds.

  5. Impact failure mechanisms of layered structures

    NASA Astrophysics Data System (ADS)

    Choi, Seung-Woo

    The response of layered materials to impact is extensively investigated. This study provides a demonstration of failure mechanisms of structures that undergo elastic and plastic deformation and sustain damage ranging in severity from surface plastic deformation and cracks at low velocity, variously developed conical, lateral and radial cracking at intermediate speeds, to catastrophic fragmentation and erosion that cause penetration at sufficiently high velocity. In order to demonstrate cracking fragmentation and penetration during impact in a structure, the cohesive element modeling and element erosion scheme are used, which is based on nonlinear dynamics using corotational scheme that is particularly effective method for handling relatively large deflection and rotations. It will provide a means of design of structure to moderate in impact loading from foreign object to protect safety zone by identifying the failure modes of structures for a wide range of impact. The assessment of the protection efficiency to impact is presented by computer simulation. Extensive results from a parametric study of the effects of confinement on residual strength and effects of interactions between phenomena that are essentially accompanied by impact, are also provided to supplement the statement.

  6. Mixed metallic Ba(Co,Fe)X(0.2)O(3-δ) (X = F, Cl) hexagonal perovskites: drastic effect of Fe-incorporation on structural and electronic features.

    PubMed

    Iorgulescu, Mihaela; Roussel, Pascal; Tancret, Nathalie; Renault, Nicolas; Porcher, Florence; André, Gilles; Kabbour, Houria; Mentré, Olivier

    2012-07-16

    Starting from the parent 10H-Ba(5)Co(5)X(1-x)O(13-δ) (trimeric strings of face-sharing CoO(6) octahedra with terminal CoO(4) tetrahedra, stacking sequence (chhch')(2)) and 6H-Ba(6)Co(6)X(1-x)O(16-δ) (similar with tetrameric strings, stacking sequence chhhch') hexagonal perovskites forms (X = F, Cl; c, h = [BaO(3)] layers ; h' = [BaOX(1-y)] layers), we show here that the Fe incorporation leads to large domains of solid solutions for both X = F and Cl but exclusively stabilizes the 10H-form independently of the synthesis method. In this form, the lowest concentration of h-layers is stabilized by a sensitive metal reduction with increasing the Fe ratio. In a more general context of competition between several hexagonal perovskite polymorphs available for most of the transition metals, this redox change is most probably the key factor driving 1D (face-sharing chains) to 3D (corner-sharing) connectivities. Strikingly, ND data evidence the location of oxygen deficiencies in the tetrahedral (Co/Fe) coordination. This effect is exaggerated at high temperature, while (Co/Fe)O(4-δ) coordinations are completed by the displacement of X(-) anions toward the (Co/Fe) sphere of coordination following a "push-and-pull" mechanism within h'-[BaOX(1-y)] layers. The Fe-incorporation is also accompanied by increasing conduction gaps with predominant 1D variable range hopping. The full series show antiferromagnetic behavior with increasing T(N) as [Fe] increases. For Fe-rich compounds T(N) is estimated about 600 K, as rarely observed for hexagonal perovskite compounds. Finally, magnetic structures of all iron-doped compounds show a site-to-site AFM ordering, different of the magnetic structure of Co-only parent compounds. Here, DFT calculations predict low-spin octahedral Co configurations, but high-spin Fe species in the same sites.

  7. On the Role of Interfaces in Planar-Structured HC(NH2 )2 PbI3 Perovskite Solar Cells.

    PubMed

    Seol, Dong-Jin; Lee, Jin-Wook; Park, Nam-Gyu

    2015-07-20

    Planar-structured HC(NH2 )2 PbI3 (FAPbI3 ) perovskite solar cells were prepared via a two-step deposition process. To investigate the role of interface, the perovskite morphology was intentionally modified by varying HC(NH2 )2 I concentration. Surface and grain sizes of the deposited FAPbI3 became rougher and larger as the HC(NH2 )2 I concentration decreased from 58.2 to 40.7 mM. Average photocurrent was improved but photovoltage deteriorated slightly with decreasing concentration. Consequently, the average efficiency was improved from 7.82 % to 10.70 % and the best efficiency of 12.17 % was obtained at 40.7 mM. Photoluminescence (PL) at TiO2 /FAPbI3 interface was reduced with decreasing concentration, which was, however, reversed at FAPbI3 /spiro-MeOTAD one. By correlating PL data and the photovoltaic performance, we concluded that the TiO2 /perovskite interface plays a crucial role in determining photocurrent while the perovskite/spiro-MeOTAD interface is important in governing photovoltage.

  8. Functionalization of perovskite thin films with moisture-tolerant molecules

    NASA Astrophysics Data System (ADS)

    Yang, Shuang; Wang, Yun; Liu, Porun; Cheng, Yi-Bing; Zhao, Hui Jun; Yang, Hua Gui

    2016-02-01

    Organic-inorganic hybrid perovskites are particularly suited as light-harvesting materials in photovoltaic devices. The power conversion efficiency of perovskite solar cells has reached certified values of over 20% in just a few years. However, one of the major hindrances for application of these materials in real-world devices is the performance degradation in humid conditions, leading to a rapid loss of photovoltaic response. Here, we demonstrate that hydrophobic tertiary and quaternary alkyl ammonium cations can be successfully assembled on the perovskite surface as efficient water-resisting layers via a facile surface functionalization technique. Such layers can protect the perovskite film under high relative humidity (90 ± 5%) over 30 days. More importantly, devices based on such films can retain the photovoltaic capacities of bulk perovskites, with power conversion efficiencies over 15%. Improving the humidity tolerance of perovskite materials is a necessary step towards large-scale production of high-performance perovskite-based devices under ambient humidity.

  9. Performance enhancement of perovskite solar cells with Mg-doped TiO{sub 2} compact film as the hole-blocking layer

    SciTech Connect

    Wang, Jing; Qin, Minchao; Tao, Hong; Ke, Weijun; Chen, Zhao; Wan, Jiawei; Qin, Pingli; Lei, Hongwei; Fang, Guojia; Xiong, Liangbin; Yu, Huaqing

    2015-03-23

    In this letter, we report perovskite solar cells with thin dense Mg-doped TiO{sub 2} as hole-blocking layers (HBLs), which outperform cells using TiO{sub 2} HBLs in several ways: higher open-circuit voltage (V{sub oc}) (1.08 V), power conversion efficiency (12.28%), short-circuit current, and fill factor. These properties improvements are attributed to the better properties of Mg-modulated TiO{sub 2} as compared to TiO{sub 2} such as better optical transmission properties, upshifted conduction band minimum (CBM) and downshifted valence band maximum (VBM), better hole-blocking effect, and higher electron life time. The higher-lying CBM due to the modulation with wider band gap MgO and the formation of magnesium oxide and magnesium hydroxides together resulted in an increment of V{sub oc}. In addition, the Mg-modulated TiO{sub 2} with lower VBM played a better role in the hole-blocking. The HBL with modulated band position provided better electron transport and hole blocking effects within the device.

  10. Solid State Structure-Reactivity Studies on Bixbyites, Fluorites and Perovskites Belonging to the Vanadate, Titanate and Cerate Families

    NASA Astrophysics Data System (ADS)

    Shafi, Shahid P.

    This thesis primarily focuses on the systematic understanding of structure-reactivity relationships in two representative systems: bixbyite and related structures as well as indium doped CeO2. Topotactic reaction routes have gained significant attention over the past two decades due to their potential to access kinetically controlled metastable materials. This has contributed substantially to the understanding of solid state reaction pathways and provided first insights into mechanisms. Contrary to the widely used ex-situ methods, in-situ techniques including powder x-ray diffraction and thermogravimetric-differential thermal analysis have been employed extensively throughout this work in order to follow the reaction pathways in real time. Detailed analysis of the AVO3 (A = In, Sc) bixbyite reactivity under oxidative conditions has been carried out and a variety of novel metastable oxygen defect phases have been identified and characterized. The novel metastable materials have oxygen deficient fluorite structures and consequently are potential ion conductors. Structural aspects of the topotactic vs. reconstructive transformations are illustrated with this model system. The structure-reactivity study of AVO3 phases was extended to AVO3 perovskite family. Based on the research methodologies and results from AVO3 bixbyite reactivity studies a generalized mechanistic oxidation pathway has been established with a non-vanadium phase, ScTiO3 bixbyite. However, there is stark contrast in terms of structural stability and features beyond this stability limit during AVO3 and ScTiO3 bixbyite reaction pathways. A series of complex reaction sequences including phase separation and phase transitions were identified during the investigation of ScTiO3 reactivity. The two-step formation pathway for the fluorite-type oxide ion conductor Ce1-xInxO2-delta (0 ≤ x ≤ 0.3) is being reported. The formation of the BaCe1-xInxO 3-delta perovskites and the subsequent CO2-capture reaction

  11. Structural manipulation and tailoring of dielectric properties in SrTi1−xFexTaxO3 perovskites: Design of new lead free relaxors

    PubMed Central

    Shukla, R.; Patwe, S. J.; Deshpande, S. K.; Achary, S. N.; Krishna, P. S. R.; Shinde, A. B.; Gopalakrishnan, J.; Tyagi, A. K.

    2016-01-01

    We report composition dependent structure evolution from SrTiO3 to SrFe0.5Ta0.5O3 by powder X-ray and neutron diffraction studies of SrTi1−2xFexTaxO3 (0.00 ≤ × ≤ 0.50) compositions. Structural studies reveal cubic (Pm3m) perovskite-type structure of the parent SrTiO3 for x up to 0.075 and cation disordered orthorhombic (Pbnm) perovskite-type structure for x ≥ 0.33. A biphasic region consisting of a mixture of cubic and orthorhombic structures is found in the range for 0.10 ≤ × ≤ 0.25. Dielectric studies reveal transformation from a normal dielectric to relaxor like properties with increasing Fe3+ and Ta5+ concentration. Dielectric response is maximum at x = 0.33 in the series. The results establish a protocol for designing new lead-free relaxor materials based on the co-substitution of Fe3+ and Ta5+ for Ti4+ in SrTiO3. A complex interplay of strain effects arising from distribution of cations at the octahedral sites of the perovskite structure controls the dielectric properties. PMID:27514668

  12. Structural manipulation and tailoring of dielectric properties in SrTi1‑xFexTaxO3 perovskites: Design of new lead free relaxors

    NASA Astrophysics Data System (ADS)

    Shukla, R.; Patwe, S. J.; Deshpande, S. K.; Achary, S. N.; Krishna, P. S. R.; Shinde, A. B.; Gopalakrishnan, J.; Tyagi, A. K.

    2016-08-01

    We report composition dependent structure evolution from SrTiO3 to SrFe0.5Ta0.5O3 by powder X-ray and neutron diffraction studies of SrTi1‑2xFexTaxO3 (0.00 ≤ × ≤ 0.50) compositions. Structural studies reveal cubic (Pm3m) perovskite-type structure of the parent SrTiO3 for x up to 0.075 and cation disordered orthorhombic (Pbnm) perovskite-type structure for x ≥ 0.33. A biphasic region consisting of a mixture of cubic and orthorhombic structures is found in the range for 0.10 ≤ × ≤ 0.25. Dielectric studies reveal transformation from a normal dielectric to relaxor like properties with increasing Fe3+ and Ta5+ concentration. Dielectric response is maximum at x = 0.33 in the series. The results establish a protocol for designing new lead-free relaxor materials based on the co-substitution of Fe3+ and Ta5+ for Ti4+ in SrTiO3. A complex interplay of strain effects arising from distribution of cations at the octahedral sites of the perovskite structure controls the dielectric properties.

  13. Structural manipulation and tailoring of dielectric properties in SrTi1-xFexTaxO3 perovskites: Design of new lead free relaxors.

    PubMed

    Shukla, R; Patwe, S J; Deshpande, S K; Achary, S N; Krishna, P S R; Shinde, A B; Gopalakrishnan, J; Tyagi, A K

    2016-01-01

    We report composition dependent structure evolution from SrTiO3 to SrFe0.5Ta0.5O3 by powder X-ray and neutron diffraction studies of SrTi1-2xFexTaxO3 (0.00 ≤ × ≤ 0.50) compositions. Structural studies reveal cubic (Pm3m) perovskite-type structure of the parent SrTiO3 for x up to 0.075 and cation disordered orthorhombic (Pbnm) perovskite-type structure for x ≥ 0.33. A biphasic region consisting of a mixture of cubic and orthorhombic structures is found in the range for 0.10 ≤ × ≤ 0.25. Dielectric studies reveal transformation from a normal dielectric to relaxor like properties with increasing Fe(3+) and Ta(5+) concentration. Dielectric response is maximum at x = 0.33 in the series. The results establish a protocol for designing new lead-free relaxor materials based on the co-substitution of Fe(3+) and Ta(5+) for Ti(4+) in SrTiO3. A complex interplay of strain effects arising from distribution of cations at the octahedral sites of the perovskite structure controls the dielectric properties. PMID:27514668

  14. Structural manipulation and tailoring of dielectric properties in SrTi1-xFexTaxO3 perovskites: Design of new lead free relaxors.

    PubMed

    Shukla, R; Patwe, S J; Deshpande, S K; Achary, S N; Krishna, P S R; Shinde, A B; Gopalakrishnan, J; Tyagi, A K

    2016-08-12

    We report composition dependent structure evolution from SrTiO3 to SrFe0.5Ta0.5O3 by powder X-ray and neutron diffraction studies of SrTi1-2xFexTaxO3 (0.00 ≤ × ≤ 0.50) compositions. Structural studies reveal cubic (Pm3m) perovskite-type structure of the parent SrTiO3 for x up to 0.075 and cation disordered orthorhombic (Pbnm) perovskite-type structure for x ≥ 0.33. A biphasic region consisting of a mixture of cubic and orthorhombic structures is found in the range for 0.10 ≤ × ≤ 0.25. Dielectric studies reveal transformation from a normal dielectric to relaxor like properties with increasing Fe(3+) and Ta(5+) concentration. Dielectric response is maximum at x = 0.33 in the series. The results establish a protocol for designing new lead-free relaxor materials based on the co-substitution of Fe(3+) and Ta(5+) for Ti(4+) in SrTiO3. A complex interplay of strain effects arising from distribution of cations at the octahedral sites of the perovskite structure controls the dielectric properties.

  15. Magnetic order and electronic structure of 5d3 double perovskite Sr2ScOsO6

    SciTech Connect

    Taylor, A. E.; Morrow, R.; Singh, D. J.; Calder, S.; Lumsden, M. D.; Woodward, P. M.; Christianson, A. D.

    2015-03-01

    The magnetic susceptibility, crystal and magnetic structures, and electronic structure of double perovskite Sr2ScOsO6 are reported. Using both neutron and x-ray powder diffraction we find that the crystal structure is monoclinic P21/n from 3.5 to 300 K. Magnetization measurements indicate an antiferromagnetic transition at TN=92 K, one of the highest transition temperatures of any double perovskite hosting only one magnetic ion. Type I antiferromagnetic order is determined by neutron powder diffraction, with an Os moment of only 1.6(1) muB, close to half the spin-only value for a crystal field split 5d electron state with t2g^3 ground state. Density functional calculations show that this reduction is largely the result of strong Os-O hybridization, with spin-orbit coupling responsible for only a ~0.1 muB reduction in the moment.

  16. Using Low Temperature Photoluminescence Spectroscopy to Investigate CH₃NH₃PbI₃ Hybrid Perovskite Degradation.

    PubMed

    Jemli, Khaoula; Diab, Hiba; Lédée, Ferdinand; Trippé-Allard, Gaelle; Garrot, Damien; Geffroy, Bernard; Lauret, Jean-Sébastien; Audebert, Pierre; Deleporte, Emmanuelle

    2016-01-01

    Investigating the stability and evaluating the quality of the CH₃NH₃PbI₃ perovskite structures is quite critical both to the design and fabrication of high-performance perovskite devices and to fundamental studies of the photophysics of the excitons. In particular, it is known that, under ambient conditions, CH₃NH₃PbI₃ degrades producing some PbI₂. We show here that low temperature Photoluminescence (PL) spectroscopy is a powerful tool to detect PbI₂ traces in hybrid perovskite layers and single crystals. Because PL spectroscopy is a signal detection method on a black background, small PbI₂ traces can be detected, when other methods currently used at room temperature fail. Our study highlights the extremely high stability of the single crystals compared to the thin layers and defects and grain boundaries are thought to play an important role in the degradation mechanism. PMID:27399669

  17. High-performance perovskite photoanode enabled by Ni passivation and catalysis.

    PubMed

    Da, Peimei; Cha, Mingyang; Sun, Lu; Wu, Yizheng; Wang, Zhong-Sheng; Zheng, Gengfeng

    2015-05-13

    Lead halide perovskites have achieved phenomenal successes in photovoltaics due to their suitable bandgaps, long diffusion lengths, and balanced charge transport. However, the extreme susceptibility of perovskites to water or air has imposed a seemingly insurmountable barrier for leveraging these unique materials into solar-to-fuel applications such as photoelectrochemical conversion. Here we developed a CH3NH3PbI3-based photoanode with an ultrathin Ni surface layer, which functions as both a physical passivation barrier and a hole-transferring catalyst. Remarkably, a much enhanced photocurrent density, an unassisted photoelectrochemical conversion capability, and a substantially better stability against water have been achieved, which are exceeding most of the previously reported photoanodes as well as a similar CH3NH3PbI3-based device structure but without the Ni surface layer. Our study suggests many exciting opportunities of developing perovskite-based solar-to-fuel conversion.

  18. Defect structure of the high-dielectric-constant perovskite Ca Cu3 Ti4 O12

    NASA Astrophysics Data System (ADS)

    Wu, L.; Zhu, Y.; Park, S.; Shapiro, S.; Shirane, G.; Tafto, J.

    2005-01-01

    Using transmission electron microscopy (TEM) we studied CaCu3Ti4O12 , an intriguing material that exhibits a huge dielectric response, up to kilohertz frequencies, over a wide range of temperature. Neither in single crystals, nor in polycrystalline samples, including sintered bulk and thin films, did we observe the twin domains suggested in the literature. Nevertheless, in the single crystals, we saw a very high density of dislocations with a Burger vector of [110], as well as regions with cation disorder and planar defects with a displacement vector (1)/(4)[110] . In the polycrystalline samples, we observed many grain boundaries with oxygen deficiency, in comparison with the grain interior. The defect-related structural disorders and inhomogeneity, serving as an internal barrier layer capacitance in a semiconducting matrix, might explain the very large dielectric response of the material. Our TEM study of the structure defects in CaCu3Ti4O12 supports a recently proposed morphological model with percolating conducting regions and blocking regions.

  19. High-pressure synthesis, crystal structure and magnetic properties of double perovskite oxide Ba{sub 2}CuOsO{sub 6}

    SciTech Connect

    Feng, Hai L.; Arai, Masao; Matsushita, Yoshitaka; Tsujimoto, Yoshihiro; Yuan, Yahua; Sathish, Clastin I.; He, Jianfeng; Tanaka, Masahiko; Yamaura, Kazunari

    2014-09-15

    A new compositional double perovskite oxide Ba{sub 2}CuOsO{sub 6} was synthesized under high-pressure (6 GPa) and high-temperature (1500 °C) conditions. The polycrystalline Ba{sub 2}CuOsO{sub 6} was characterized by synchrotron X-ray diffraction, thermogravimetric analysis, and magnetic susceptibility, isothermal magnetization, and specific heat measurements. The oxide crystallizes in a double-perovskite structure with an I4/m space group, in which Os(VI) and Cu(II) are ordered in the perovskite B-site. Ba{sub 2}CuOsO{sub 6} is electrically insulating with an activation energy of 0.813(2) eV and shows antiferromagnetic-like characteristics at temperatures of ∼55 K and ∼70 K. The results of the first-principle calculation suggested that the spin–orbit interaction of Os(VI) plays a substantial role in the insulating state. The Jahn–Teller distortion of CuO{sub 6} octahedra influences the magnetic characteristics with regard to possible two-dimensional magnetic correlations. - Graphical abstract: A new compositional double perovskite oxide Ba{sub 2}CuOsO{sub 6} synthesized by a high-pressure (6 GPa) and high-temperature (1500 °C) method. - Highlights: • A new compositional double perovskite oxide Ba{sub 2}CuOsO{sub 6} was synthesized. • Ba{sub 2}CuOsO{sub 6} is electrically insulating and antiferromagnetic below ∼70 K. • The Jahn–Teller distortion of CuO{sub 6} has relevance to possible magnetic anisotropy.

  20. Elucidating the Reaction Pathways in the Synthesis of Organolead Trihalide Perovskite for High-Performance Solar Cells

    PubMed Central

    Wang, Baohua; Young Wong, King; Xiao, Xudong; Chen, Tao

    2015-01-01

    The past two years have witnessed unprecedentedly rapid development of organic–inorganic halide perovskite–based solar cells. The solution–processability and high efficiency make this technology extraordinarily attractive. The intensive investigations have accumulated rich experiences in the perovskite fabrication; while the mechanism of the chemical synthesis still remains unresolved. Here, we set up the chemical equation of the synthesis and elucidate the reactions from both thermodynamic and kinetic perspectives. Our study shows that gaseous products thermodynamically favour the reaction, while the activation energy and “collision” probability synergistically determine the reaction rate. These understandings enable us to finely tune the crystal size for high-quality perovskite film, leading to a record fill factor among similar device structures in the literature. This investigation provides a general strategy to explore the mechanism of perovskite synthesis and benefits the fabrication of high–efficiency perovskite photoactive layer. PMID:26020476

  1. Monolayer and Few-Layer All-Inorganic Perovskites as a New Family of Two-Dimensional Semiconductors for Printable Optoelectronic Devices.

    PubMed

    Song, Jizhong; Xu, Leimeng; Li, Jianhai; Xue, Jie; Dong, Yuhui; Li, Xiaoming; Zeng, Haibo

    2016-06-01

    Printed flexible photodetectors based on 2D inorganic perovskites with atomic thickness show excellent photosensing with fast rise and decay response times. As-synthesized nanosheets can easily be dispersed in various solvents, leading to large-area, crack-free, low-roughness, flexible films after printing. This study demonstrates that all-inorganic perovskite CsPbX3 nanosheets as a new class of 2D semiconductors have huge potential for flexible optoelectronic applications. PMID:27110705

  2. Structural Characterization of Layered Morphologies in Precise Copolymers

    NASA Astrophysics Data System (ADS)

    Trigg, Edward; Gaines, Taylor; Wagener, Kenneth; Winey, Karen

    2015-03-01

    Layered morphologies have been observed in precise polyethylene-based copolymers that contain acid, charged, or polar functional groups precisely spaced along a linear alkane chain. Sufficiently long alkane segments form structures resembling orthorhombic polyethylene crystals, while the functional groups form 2-D layers that disrupt the alkane crystal structure to varying degrees. Here, layered morphologies in precise copolymers containing acrylic acid, phosphonic acid, imidazolium bromide, and sulfone groups are studied via X-ray scattering. Specifically, the composition profiles of the layered structures are obtained by Fourier synthesis, and the coherence length is investigated using peak width analysis. This analysis indicates that the layers of functional groups are frequently bordered by two crystallites, which suggests different dynamics relative to layers bordered by one crystalline and one amorphous microdomain. Detailed understanding of the structure of the layered morphologies will allow for a systematic investigation of proton and ion conductivity mechanisms, which are expected to occur through the high-dielectric layers.

  3. Low temperature thermoelastic and structural properties of LaGaO3 perovskite in the Pbnm phase

    NASA Astrophysics Data System (ADS)

    Knight, Kevin S.

    2012-10-01

    The thermoelastic and structural properties of LaGaO3 perovskite have been studied using high resolution neutron diffractometry at 158 temperatures between 11 K and 548 K. Data collected in 2 K intervals between 410 K and 430 K show no evidence for an intermediate phase between the low temperature phase in space group Pbnm and the high temperature phase in space group F3¯2/n. From a simultaneous fit of the unit cell volume and the isochoric heat capacity, the phonon density of states in the Pbnm phase is shown to be approximated by a two-term Debye model, with characteristic temperatures 294(1) K and 831(1) K. Vibrational Debye temperatures, determined from fitting the temperature variation of the atomic displacement parameters, show the cations to be more associated with the lower characteristic temperature, whilst that for the anions, is closer to the higher characteristic temperature. Structural parameters are presented as the amplitudes of the seven symmetry-adapted basis-vectors of the aristotype phase, and a structural basis for the temperature-dependence of the bond lengths is outlined. The phase transition in both temperature and pressure arises when a non-bonded La-O distance approaches the La coordination sphere.

  4. Post-perovskite transitions in CaB4+O3 at high pressure

    NASA Astrophysics Data System (ADS)

    Akaogi, M.; Shirako, Y.; Kojitani, H.; Takamori, S.; Yamaura, K.; Takayama-Muromachi, E.

    2010-03-01

    High-pressure phase transitions in CaRhO3 were examined using a multianvil apparatus up to 27 GPa and 1930 oC. CaRhO3 perovskite transforms to post-perovskite via a monoclinic intermediate phase with increasing pressure. Volume changes for the transitions of perovskite - intermediate phase and of intermediate phase - post-perovskite are -1.1 and -0.7 %, respectively. CaRhO3 post-perovskite is the fourth quenchable post-perovskite oxide found so far. By high-temperature calorimetric experiments, enthalpy of the perovskite - post-perovskite transition in CaRuO3 was measured as 15.2±3.3 kJ/mol. Combining the datum with those of CaIrO3, it is shown that CaIrO3 perovskite is energetically less stable than CaRuO3 perovskite. This is consistent with the fact that orthorhombic distortion of CaIrO3 perovskite is larger than CaRuO3, as indicated with the tilt-angle of octahedral framework of perovskite structure. The transition pressure from perovskite to post-perovskite in CaBO3 (B = Ru, Rh, Ir) increases almost linearly with decreasing the tilt-angle, suggesting that the perovskite - post-perovskite transition may result from instability of the perovskite structure with pressure.

  5. Perovskite-Type LaSrMnO Electrocatalyst with Uniform Porous Structure for an Efficient Li-O2 Battery Cathode.

    PubMed

    Yang, Yanbing; Yin, Wei; Wu, Shiting; Yang, Xiangdong; Xia, Wei; Shen, Yue; Huang, Yunhui; Cao, Anyuan; Yuan, Quan

    2016-01-26

    Perovskite is an excellent candidate as low cost catalyst for Li-O2 cells. However, the limited porosity, which impedes molecular transport, and the inherent low electronic conductivity are the main barriers toward production of high-performance electrodes. Here, we designed a hierarchical porous flexible architecture by coating thin mesoporous yet crystalline LaSrMnO layers throughout a graphene foam to form graphene/meso-LaSrMnO sandwich-like nanosheets. In this well-designed system, the macropore between nanosheets facilitates O2 and Li(+) diffusion, the mesopore provides large surface area for electrolyte immersion and discharge products deposition, the perovskite phase catalyst decreases reactive overpotential, and the graphene serves as conductive network for electrons transport. When used as a freestanding electrode of Li-O2 cell, it shows high specific capacity, superior rate capability, and cyclic stability. Combination of mesoporous perovskites with conductive graphene networks represents an effective strategy for developing efficient electrodes in various energy storage systems. PMID:26679735

  6. Perovskite-Type LaSrMnO Electrocatalyst with Uniform Porous Structure for an Efficient Li-O2 Battery Cathode.

    PubMed

    Yang, Yanbing; Yin, Wei; Wu, Shiting; Yang, Xiangdong; Xia, Wei; Shen, Yue; Huang, Yunhui; Cao, Anyuan; Yuan, Quan

    2016-01-26

    Perovskite is an excellent candidate as low cost catalyst for Li-O2 cells. However, the limited porosity, which impedes molecular transport, and the inherent low electronic conductivity are the main barriers toward production of high-performance electrodes. Here, we designed a hierarchical porous flexible architecture by coating thin mesoporous yet crystalline LaSrMnO layers throughout a graphene foam to form graphene/meso-LaSrMnO sandwich-like nanosheets. In this well-designed system, the macropore between nanosheets facilitates O2 and Li(+) diffusion, the mesopore provides large surface area for electrolyte immersion and discharge products deposition, the perovskite phase catalyst decreases reactive overpotential, and the graphene serves as conductive network for electrons transport. When used as a freestanding electrode of Li-O2 cell, it shows high specific capacity, superior rate capability, and cyclic stability. Combination of mesoporous perovskites with conductive graphene networks represents an effective strategy for developing efficient electrodes in various energy storage systems.

  7. Electronic structure and exchange interactions of insulating double perovskite La2CuRuO6

    NASA Astrophysics Data System (ADS)

    Panda, S. K.; Kvashnin, Y. O.; Sanyal, B.; Dasgupta, I.; Eriksson, O.

    2016-08-01

    We have performed first-principles calculations of the electronic and magnetic properties of insulating double perovskite compound La2CuRuO6 (LCRO) which has recently been reported to exhibit intriguing magnetic properties. We derived a tight-binding Hamiltonian for LCRO based on the N th -order muffin-tin orbital (NMTO) downfolding technique. The computed on-site energies and hopping integrals are used to estimate the dominant exchange interactions employing an extended Kugel-Khomskii model. This way the dominant exchange paths were identified and a low-energy spin model was proposed. The Green function method based on the magnetic force theorem has also been used to extract the exchange interactions to provide a more accurate estimation and to justify the model calculations. Our results show that the nearest neighbor (NN) Cu-Ru magnetic interactions are very much direction dependent and a strong antiferromagnetic next nearest neighbor Ru-Ru interaction along the crystallographic b axis is responsible for the magnetic frustration observed experimentally in this system. We argue that due to the broken symmetry, NN Cu-Ru interaction becomes stronger along one direction than the other, which essentially reduces the amount of frustration and helps the system to achieve an antiferromagnetic ground state at low temperature. A detailed microscopic explanation of the exchange mechanism is discussed. We also find that spin-orbit coupling effect is significant and causes a canting of the Ru spin with respect to the Cu moments.

  8. High-Pressure Single-Crystal Structures of 3D Lead-Halide Hybrid Perovskites and Pressure Effects on their Electronic and Optical Properties

    PubMed Central

    2016-01-01

    We report the first high-pressure single-crystal structures of hybrid perovskites. The crystalline semiconductors (MA)PbX3 (MA = CH3NH3+, X = Br– or I–) afford us the rare opportunity of understanding how compression modulates their structures and thereby their optoelectronic properties. Using atomic coordinates obtained from high-pressure single-crystal X-ray diffraction we track the perovskites’ precise structural evolution upon compression. These structural changes correlate well with pressure-dependent single-crystal photoluminescence (PL) spectra and high-pressure bandgaps derived from density functional theory. We further observe dramatic piezochromism where the solids become lighter in color and then transition to opaque black with compression. Indeed, electronic conductivity measurements of (MA)PbI3 obtained within a diamond-anvil cell show that the material’s resistivity decreases by 3 orders of magnitude between 0 and 51 GPa. The activation energy for conduction at 51 GPa is only 13.2(3) meV, suggesting that the perovskite is approaching a metallic state. Furthermore, the pressure response of mixed-halide perovskites shows new luminescent states that emerge at elevated pressures. We recently reported that the perovskites (MA)Pb(BrxI1–x)3 (0.2 < x < 1) reversibly form light-induced trap states, which pin their PL to a low energy. This may explain the low voltages obtained from solar cells employing these absorbers. Our high-pressure PL data indicate that compression can mitigate this PL redshift and may afford higher steady-state voltages from these absorbers. These studies show that pressure can significantly alter the transport and thermodynamic properties of these technologically important semiconductors. PMID:27163050

  9. Bloch oscillations in chirped layered structures with metamaterials.

    PubMed

    Davoyan, Arthur R; Shadrivov, Ilya V; Sukhorukov, Andrey A; Kivshar, Yuri S

    2008-03-01

    We analyze the Bloch oscillations of electromagnetic waves in chirped layered structures with alternating layers of negative-index metamaterial and conventional dielectric under the condition of the zero average refractive index. We consider the case when the chirp is introduced by varying the thickness of the layers linearly across the structure. We demonstrate that such structures can support three different types of the Bloch oscillations for electromagnetic waves associated with either propagating or evanescent guided modes. In particular, we predict a novel type of the Bloch oscillations associated with coupling between surface waves excited at the interfaces separating the layers of negative-index metamaterial and the layers of the conventional dielectric.

  10. Hydrogen in magnesium palladium thin layer structures

    NASA Astrophysics Data System (ADS)

    Kruijtzer, G. L.

    2008-02-01

    In this thesis, the study of hydrogen storage, absorption and desorption in magnesium layers is described. The magnesium layers have a thickness of 50-500 nm and are covered by a palladium layer which acts as a hydrogen dissociation/association catalyst. The study was preformed under ultra high vacuum conditions to avoid oxygen contamination. The main analysis techniques were RBS, ERD and TDS.

  11. Structural and magnetic properties of RTiNO{sub 2} (R=Ce, Pr, Nd) perovskite nitride oxides

    SciTech Connect

    Porter, Spencer H.; Huang, Zhenguo; Cheng, Zhenxiang; Avdeev, Maxim; Chen, Zhixin; Dou, Shixue; Woodward, Patrick M.

    2015-03-15

    Neutron powder diffraction indicates that CeTiNO{sub 2} and PrTiNO{sub 2} crystallize with orthorhombic Pnma symmetry (Ce: a=5.5580(5), b=7.8369(7), and c=5.5830(4) Å; Pr: a=5.5468(5), b=7.8142(5), and c=5.5514(5) Å) as a result of a{sup –}b{sup +}a{sup –} tilting of the titanium-centered octahedra. Careful examination of the NPD data, confirms the absence of long range anion order in both compounds, while apparent superstructure reflections seen in electron diffraction patterns provide evidence for short range anion order. Inverse magnetic susceptibility plots reveal that the RTiNO{sub 2} (R=Ce, Pr, Nd) compounds are paramagnetic with Weiss constants that vary from −28 to −42 K. Effective magnetic moments for RTiNO{sub 2} (R=Ce, Pr, Nd) are 2.43 μ{sub B}, 3.63 μ{sub B}, and 3.47 μ{sub B}, respectively, in line with values expected for free rare-earth ions. Deviations from Curie–Weiss behavior that occur below 150 K for CeTiNO{sub 2} and below 30 K for NdTiNO{sub 2} are driven by magnetic anisotropy, spin–orbit coupling, and crystal field effects. - Graphical abstract: The structure and magnetism of the oxide nitride perovskites RTiNO{sub 2} (R=Ce, Pr, Nd) have been explored. The average symmetry is shown to be Pnma with a random distribution of oxide and nitride ions and a{sup −}b{sup +}a{sup −} tilting of the titanium-centered octahedra, but electron diffraction shows evidence for short range anion order. All three compounds are paramagnetic but deviations from the Curie Weiss law are seen below 150 K for R=Ce and below 30 K for R=Nd. - Highlights: • The oxide nitride perovskites RTiNO{sub 2} (R=Ce, Pr) have been prepared and their structures determined. • Diffraction measurements indicate short range cis-order of O and N, but no long range order. • Compounds are paramagnetic with Weiss constants that vary from −28 to −42 K. • CeTiO{sub 2}N and NdTiO{sub 2}N deviate from Curie–Weiss behavior below 150 and 30 K, respectively.

  12. Effects of Bi doping on structural and magnetic properties of double perovskite oxides Sr2FeMoO6

    NASA Astrophysics Data System (ADS)

    Lan, Yaohai; Feng, Xiaomei; Zhang, Xin; Shen, Yifu; Wang, Ding

    2016-08-01

    A new series of double perovskite compounds Sr2 - δBixFeMoO6 have been synthesized by solid-state reaction. δ refers to the nominal doping content of Bi (δ = 0, 0.1, 0.2, 0.3, 0.4, 0.5), while the Bi content obtained by the Rietveld refinement is x = 0, 0.01, 0.05, 0.08, 0.10 and 0.12. Their crystal structure and magnetic properties are investigated. Rietveld analysis of the room temperature XRD data shows all the samples crystallize in the cubic crystal structure with the space group Fm 3 ‾ m and have no phase transition. SEM images show that substituted samples present a denser microstructure and bigger grains than Sr2FeMoO6, which is caused by a liquid sintering process due to the effumability of Bi. The unit cell volume increases with augment of Bi3+ concentration despite the smaller ionic radius Bi3+ compared with the Sr2+, which is attributed to the electronic effect. The degree of Fe/Mo order (η) increases first and then decreases to almost disappearance with augment of Bi doping, which is the result of contribution from electronic effect. Calculated saturation magnetization Ms(3) according to our phase separation likeness model matches well with the experimental ones. The observed variations of magnetoresistance (MR) are consistent with the Fe/Mo order (η) due to the internal connection with anti-site defect (ASD).

  13. Ab initio study of structural, mechanical, thermal and electronic properties of perovskites Sr(Li,Pd)H3

    NASA Astrophysics Data System (ADS)

    Benlamari, S.; Amara Korba, S.; Lakel, S.; Meradji, H.; Ghemid, S.; El Haj Hassan, F.

    2016-01-01

    The structural, elastic, thermal and electronic properties of perovskite hydrides SrLiH3 and SrPdH3 have been investigated using the all-electron full-potential linear augmented plane wave (FP-LAPW) method based on the density functional theory (DFT). For the exchange-correlation potential, local-density approximation (LDA) and generalized gradient approximation (GGA) have been used to calculate theoretical lattice parameters, bulk modulus, and its pressure derivative. The present results are in good agreement with available theoretical and experimental data. The three independent elastic constants (C11, C12 and C44) are also reported. From electronic band structure and density of states (DOSs), it is found that SrLiH3 is an insulator characterized by an indirect gap of 3.48 eV, while SrPdH3 is metallic with a calculated DOSs at Fermi energy of 0.745 states/eV-unit cell. Poisson’s ratio (σ), Young’s modulus (E), shear modulus (G), anisotropy factor (A), average sound velocities (vm) and density (ρ) of these compounds are also estimated for the first time. The Debye temperature is deduced from the average sound velocity. Variation of elastic constants and bulk modulus of these compounds as a function of pressure is also reported. Pressure and thermal effects on some macroscopic properties are predicted using the quasi-harmonic Debye model.

  14. PrBa0.5Sr0.5Co2O5+δ layered perovskite cathode for intermediate temperature solid oxide fuel cells

    SciTech Connect

    Ding, Hanping; Xue, Xingjian

    2010-02-06

    Layered perovskite oxides have ordered A-cations localizing oxygen vacancies, and may potentially improve oxygen ion diffusivity and surface exchange coefficient. The A-site-ordered layered perovskite PrBa0.5Sr0.5Co2O5+δ (PBSC) was evaluated as new cathode material for intermediate temperature solid oxide fuel cells (IT-SOFCs). The material was characterized using electrochemical impedance spectroscopy in a symmetrical cell system (PBSC/Ce0.9Sm0.1O1.9 (SDC)/PBSC), exhibiting excellent performance in the intermediate temperature range of 500–700 °C. An area-specific-resistance (ASR) of 0.23 Ω cm2 was achieved at 650 °C for cathode polarization. The low activation energy (Ea) 124 kJ mol-1 is comparable to that of La0.8Sr0.2CoO3-δ. A laboratory-scaled SDC-based tri-layer cell of Ni-SDC/SDC/PBSC was tested in intermediate temperature conditions of 550 to 700 °C. A maximum power density of 1045 mW cm-2 was achieved at 700 °C. The interfacial polarization resistance is as low as 0.285, 0.145, 0.09 and 0.05 Ω cm2 at 550, 600, 650 and 700 °C, respectively. Layered perovskite PBSC shows promising performance as cathode material for IT-SOFCs.

  15. Molecular dynamics of MgSiO 3 perovskite at high pressures: Equation of state, structure, and melting transition

    NASA Astrophysics Data System (ADS)

    Belonoshko, Anatoly B.

    1994-10-01

    Molecular dynamics (MD) simulations of MgSiO 3-perovskite and melt with the MATSUI (1988) interatomic potential are used to resolve the problem of inconsistency between modeled and experimental melting curves. Equations of state for solid and liquid MgSiO 3-perovskite are in agreement with experimental data and are useful for calculating densities at experimentally inaccessible temperatures and pressures. Comparison with the Preliminary Earth Model ( DZIEWONSKI and ANDERSON, 1981) shows that the equation of state of MgSiO 3-perovskite is consistent with seismic parameter for lower mantle. Two-phase MD simulations at constant pressure were also performed to calculate a melting curve of MgSiO 3-perovskite in agreement with the recent experiments. Overheating does not exceed 400 K in accord with the theoretical estimate for finite systems. Extrapolation of meltings temperature to the coremantle boundary pressure (134 GPa) with the Simon equation gives temperature of ≈6400 K for MgSiO 3-perovskite and shows that, according to accepted estimates of temperature at core-mantle boundary, MgSiO 3-perovskite remains solid.

  16. Large Grained Perovskite Solar Cells Derived from Single-Crystal Perovskite Powders with Enhanced Ambient Stability.

    PubMed

    Yen, Hung-Ju; Liang, Po-Wei; Chueh, Chu-Chen; Yang, Zhibin; Jen, Alex K-Y; Wang, Hsing-Lin

    2016-06-15

    In this study, we demonstrate the large grained perovskite solar cells prepared from precursor solution comprising single-crystal perovskite powders for the first time. The resultant large grained perovskite thin film possesses a negligible physical (structural) gap between each large grain and is highly crystalline as evidenced by its fan-shaped birefringence observed under polarized light, which is very different from the thin film prepared from the typical precursor route (MAI + PbI2).

  17. The performance of La0.6Sr1.4MnO4 layered perovskite electrode material for intermediate temperature symmetrical solid oxide fuel cells

    NASA Astrophysics Data System (ADS)

    Zhou, Jun; Chen, Gang; Wu, Kai; Cheng, Yonghong

    2014-12-01

    A layered perovskite electrode material, La0.6Sr1.4MnO4+δ (LSMO4), has been studied for intermediate temperature symmetrical solid oxide fuel cells (IT-SSOFCs) on La0.9Sr0.1Ga0.8Mg0.2O3-δ (LSGM) electrolyte. The chemical compatibility tests indicate that no reaction occurred between LSMO4 oxide and LSGM electrolyte at temperature up to 1000 °C both in air and 5% H2. The lower conductivity in 5% H2 and higher conduction activation energy than those in air would be caused by poorer overlap of both σ and π bonds. DFT + U calculations also show that oxygen vacancies which formed in reducing atmosphere may block the 3D hopping path for electrons or holes through Mn-O-Mn chains. For LSMO4 electrode, SEM results indicate that the electrode formed good contact with the electrolyte after being sintered at 900 °C for 2 h. At 800 °C, the polarization resistance of the LSMO4 cathode is about 0.87 Ω cm2 in air, while the polarization resistance of the LSMO4 anode is about 2.07 Ω cm2 in 5% H2. LSMO4 exhibits better electrochemical activity for oxygen reduction than that for hydrogen oxidation. A cell with LSGM electrolyte, LSMO4-LSGM mixture as anode and cathode simultaneously displays a maximum power density of 59 mW cm-2 at 800 °C.

  18. Cation ordering and effect of biaxial strain in double perovskite CsRbCaZnCl6

    DOE PAGES

    Pilania, G.; Uberuaga, B. P.

    2015-03-19

    Here, we investigate the electronic structure, energetics of cation ordering, and effect of biaxial strain on double perovskite CsRbCaZnCl6 using first-principles calculations based on density functional theory. The two constituents (i.e., CsCaCl3 and RbZnCl3) forming the double perovskite exhibit a stark contrast. While CsCaCl3 is known to exist in a cubic perovskite structure and does not show any epitaxial strain induced phase transitions within an experimentally accessible range of compressive strains, RbZnCl3 is thermodynamically unstable in the perovskite phase and exhibits ultra-sensitive response at small epitaxial strains if constrained in the perovskite phase. We show that combining the two compositionsmore » in a double perovskite structure not only improves overall stability but also the strain-polarization coupling of the material. Our calculations predict a ground state with P4/nmm space group for the double perovskite, where A-site cations (i.e., Cs and Rb) are layer-ordered and B-site cations (i.e., Ca and Zn) prefer a rocksalt type ordering. The electronic structure and bandgap in this system are shown to be quite sensitive to the B-site cation ordering and is minimally affected by the ordering of A-site cations. We find that at experimentally accessible compressive strains CsRbCaZnCl6 can be phase transformed from its paraelectric ground state to an antiferroelectric state, where Zn atoms contribute predominantly to the polarization. Furthermore, both energy difference and activation barrier for a transformation between this antiferroelectric state and the corresponding ferroelectric configuration are predicted to be small. As a result, the computational approach presented here opens a new pathway towards a rational design of novel double perovskites with improved strain response and functionalities.« less

  19. Cation ordering and effect of biaxial strain in double perovskite CsRbCaZnCl6

    SciTech Connect

    Pilania, G.; Uberuaga, B. P.

    2015-03-19

    Here, we investigate the electronic structure, energetics of cation ordering, and effect of biaxial strain on double perovskite CsRbCaZnCl6 using first-principles calculations based on density functional theory. The two constituents (i.e., CsCaCl3 and RbZnCl3) forming the double perovskite exhibit a stark contrast. While CsCaCl3 is known to exist in a cubic perovskite structure and does not show any epitaxial strain induced phase transitions within an experimentally accessible range of compressive strains, RbZnCl3 is thermodynamically unstable in the perovskite phase and exhibits ultra-sensitive response at small epitaxial strains if constrained in the perovskite phase. We show that combining the two compositions in a double perovskite structure not only improves overall stability but also the strain-polarization coupling of the material. Our calculations predict a ground state with P4/nmm space group for the double perovskite, where A-site cations (i.e., Cs and Rb) are layer-ordered and B-site cations (i.e., Ca and Zn) prefer a rocksalt type ordering. The electronic structure and bandgap in this system are shown to be quite sensitive to the B-site cation ordering and is minimally affected by the ordering of A-site cations. We find that at experimentally accessible compressive strains CsRbCaZnCl6 can be phase transformed from its paraelectric ground state to an antiferroelectric state, where Zn atoms contribute predominantly to the polarization. Furthermore, both energy difference and activation barrier for a transformation between this antiferroelectric state and the corresponding ferroelectric configuration are predicted to be small. As a result, the computational approach presented here opens a new pathway towards a rational design of novel double perovskites with improved strain response and functionalities.

  20. Cation ordering and effect of biaxial strain in double perovskite CsRbCaZnCl{sub 6}

    SciTech Connect

    Pilania, G. Uberuaga, B. P.

    2015-03-21

    Here, we investigate the electronic structure, energetics of cation ordering, and effect of biaxial strain on double perovskite CsRbCaZnCl{sub 6} using first-principles calculations based on density functional theory. The two constituents (i.e., CsCaCl{sub 3} and RbZnCl{sub 3}) forming the double perovskite exhibit a stark contrast. While CsCaCl{sub 3} is known to exist in a cubic perovskite structure and does not show any epitaxial strain induced phase transitions within an experimentally accessible range of compressive strains, RbZnCl{sub 3} is thermodynamically unstable in the perovskite phase and exhibits ultra-sensitive response at small epitaxial strains if constrained in the perovskite phase. We show that combining the two compositions in a double perovskite structure not only improves overall stability but also the strain-polarization coupling of the material. Our calculations predict a ground state with P4/nmm space group for the double perovskite, where A-site cations (i.e., Cs and Rb) are layer-ordered and B-site cations (i.e., Ca and Zn) prefer a rocksalt type ordering. The electronic structure and bandgap in this system are shown to be quite sensitive to the B-site cation ordering and is minimally affected by the ordering of A-site cations. We find that at experimentally accessible compressive strains CsRbCaZnCl{sub 6} can be phase transformed from its paraelectric ground state to an antiferroelectric state, where Zn atoms contribute predominantly to the polarization. Furthermore, both energy difference and activation barrier for a transformation between this antiferroelectric state and the corresponding ferroelectric configuration are predicted to be small. The computational approach presented here opens a new pathway towards a rational design of novel double perovskites with improved strain response and functionalities.

  1. Reduced ultraviolet light induced degradation and enhanced light harvesting using YVO{sub 4}:Eu{sup 3+} down-shifting nano-phosphor layer in organometal halide perovskite solar cells

    SciTech Connect

    Chander, Nikhil; Chandrasekhar, P. S.; Thouti, Eshwar; Swami, Sanjay Kumar; Dutta, Viresh; Komarala, Vamsi K.; Khan, A. F.

    2014-07-21

    We report a simple method to mitigate ultra-violet (UV) degradation in TiO{sub 2} based perovskite solar cells (PSC) using a transparent luminescent down-shifting (DS) YVO{sub 4}:Eu{sup 3+} nano-phosphor layer. The PSC coated with DS phosphor showed an improvement in stability under prolonged illumination retaining more than 50% of its initial efficiency, whereas PSC without the phosphor layer degraded to ∼35% of its initial value. The phosphor layer also provided ∼8.5% enhancement in photocurrent due to DS of incident UV photons into additional red photons. YVO{sub 4}:Eu{sup 3+} layer thus served a bi-functional role in PSC by reducing photo-degradation as well as enhancing energy conversion efficiency.

  2. Compositional and Structural Versatility in an Unusual Family of anti-Perovskite Fluorides: [Cu(H2O)4]3[(MF6)(M'F6)].

    PubMed

    Felder, Justin B; Yeon, Jeongho; Smith, Mark D; Zur Loye, Hans-Conrad

    2016-07-18

    A series of six anti-perovskite fluorides of the type [Cu(H2O)4]3(M1-xM'xF6)2 (where M and M' = V, Cr, Mn, Fe as well as M = Fe and M' = V and Cr) was synthesized as high-quality single crystals via a mild hydrothermal route. These materials belong to a class of perovskite-based structures in which the anions and cations of the regular ABX3 perovskite structure have exchanged positions. Two complex anions, MF6(3-) and M'F6(3-), occupy the normal A and B cation positions, while three complex cations, [Cu(H2O)4](2+), occupy the normally anionic X positions. As in the ABX3 compositions, the A and B positions can be occupied by different complex anions, allowing for the preparation of a wide range of compositions. Magnetic property measurements were performed on all six phases, and complex magnetic behavior was observed at low temperatures in the Mn, Fe, and bimetallic Fe/V and Fe/Cr phases. PMID:27367900

  3. Stability of organometal perovskites with organic overlayers

    SciTech Connect

    Tran, Catherine D. T.; Liu, Yi; Thibau, Emmanuel S.; Llanos, Adrian; Lu, Zheng-Hong

    2015-08-15

    The air-stability of vapour-phase-deposited methylammonium lead triiodide (CH{sub 3}NH{sub 3}PbI{sub 3}) perovskite thin films has been studied using X-ray diffraction. It is found that the perovskite structure without organic coating decomposes completely within a short period of time (∼two days) upon exposure to ambient environment. The degradation of the perovskite structure is drastically reduced when the perovskite films are capped with thin N,N′-Di(1-naphthyl)-N,N′-diphenyl-(1,1′-biphenyl)-4,4′-diamine (NPB) films. We discovered that the amount of lead iodide (PbI{sub 2}), a product of the degradation, grows as a function of time in a sigmoidal manner. Further mathematical modeling analysis shows that the perovskite degradation follows the Avrami equation, a kinetics theory developed for quantifying phase transformations in solid-state materials.

  4. Atomic structure of metal-halide perovskites from first principles: The chicken-and-egg paradox of the organic-inorganic interaction

    NASA Astrophysics Data System (ADS)

    Li, Jingrui; Rinke, Patrick

    2016-07-01

    We have studied the prototype hybrid organic-inorganic perovskite CH3NH3PbI3 and its three close relatives, CH3NH3SnI3 ,CH3NH3PbCl3 , and CsPbI3, using relativistic density function theory. The long-range van der Waals (vdW) interactions were incorporated into the Perdew-Burke-Ernzerhof (PBE) exchange-correlation functional using the Tkatchenko-Scheffler pairwise scheme. Our results reveal that hydrogen bonding, which is well described by the PBE functional, plays a decisive role for the structural parameters of these systems, including the position and orientation of the organic cation as well as the deformation of the inorganic framework. The magnitude of the inorganic-framework deformation depends sensitively on the orientation of the organic cation, and directly influences the stability of the hybrid perovskites. Our results suggest that the organic and the inorganic components complement each other; the low symmetry of the organic cation is the origin of the inorganic-framework deformation, which then aids the overall stabilization of the hybrid perovskite structure. This stabilization is indirectly affected by vdW interactions, which lead to smaller unit-cell volumes than in PBE and therefore modulate the interaction between the organic cation and the inorganic framework. The vdW-induced lattice-constant corrections are system dependent and lead to PBE+vdW lattice constants in good agreement with experiment. Further insight is gained by analyzing the vdW contributions. In all iodide-based hybrid perovskites, the interaction between the organic cation and the iodide anions provides the largest lattice-constant change, followed by iodine-iodine and the organic cation—heavy-metal cation interaction. These corrections follow an almost linear dependence on the lattice constant within the range considered in our study and are therefore approximately additive.

  5. Elucidating the band structure and free charge carrier dynamics of pure and impurities doped CH3NH3PbI(3-x)Cl(x) perovskite thin films.

    PubMed

    Zhang, Zhen-Yu; Chen, Xin; Wang, Hai-Yu; Xu, Ming; Gao, Bing-Rong; Chen, Qi-Dai; Sun, Hong-Bo

    2015-11-28

    CH3NH3PbI3-xClx perovskite material has been commonly used as the free charge generator and reservoir in highly efficient perovskite-based solid-state solar photovoltaic devices. However, many of the underlying fundamental photophysical mechanisms in this material such as the perovskite transition band structure as well as the dependent relationship between the carrier properties and lattice properties still lack sufficient understanding. Here, we elucidated the fundamental band structure of the pure CH3NH3PbI3-xClx pervoskite lattice, and then reported about the dependent relationship between the free charge carrier characteristic and the different CH3NH3PbI3-xClx pervoskite lattice thin films utilizing femtosecond time-resolved pump-probe technologies. The data demonstrated that the pure perovskite crystal band structure should only have one conduction and one valence band rather than dual valences, and the pure perovskite lattice could trigger more free charge carriers with a slower recombination rate under an identical pump intensity compared with the impurities doped perovskite crystal. We also investigated the perovskite film performance when exposed to moisture and water, the corresponding results gave us a dip in the optimization of the performance of perovskite based devices, and so as a priority this material should be isolated from moisture (water). This work may propose a deeper perspective on the comprehension for this material and it is useful for future optimization of applications in photovoltaic and light emission devices. PMID:26497219

  6. Nanocrystalline rutile electron extraction layer enables low-temperature solution processed perovskite photovoltaics with 13.7% efficiency.

    PubMed

    Yella, Aswani; Heiniger, Leo-Philipp; Gao, Peng; Nazeeruddin, Mohammad Khaja; Grätzel, Michael

    2014-05-14

    We demonstrate low-temperature (70 °C) solution processing of TiO2/CH3NH3PbI3 based solar cells, resulting in impressive power conversion efficiency (PCE) of 13.7%. Along with the high efficiency, a strikingly high open circuit potential (VOC) of 1110 mV was realized using this low-temperature chemical bath deposition approach. To the best of our knowledge, this is so far the highest VOC value for solution-processed TiO2/CH3NH3PbI3 solar cells. We deposited a nanocrystalline TiO2 (rutile) hole-blocking layer on a fluorine-doped tin oxide (FTO) conducting glass substrate via hydrolysis of TiCl4 at 70 °C, forming the electron selective contact with the photoactive CH3NH3PbI3 film. We find that the nanocrystalline rutile TiO2 achieves a much better performance than a planar TiO2 (anatase) film prepared by high-temperature spin coating of TiCl4, which produces a much lower PCE of 3.7%. We attribute this to the formation of an intimate junction of large interfacial area between the nanocrystalline rutile TiO2 and the CH3NH3PbI3 layer, which is much more effective in extracting photogenerated electrons than the planar anatase film. Since the complete fabrication of the solar cell is carried out below 100 °C, this method can be easily extended to plastic substrates.

  7. Low temperature thermoelastic and structural properties of LaGaO{sub 3} perovskite in the Pbnm phase

    SciTech Connect

    Knight, Kevin S.

    2012-10-15

    The thermoelastic and structural properties of LaGaO{sub 3} perovskite have been studied using high resolution neutron diffractometry at 158 temperatures between 11 K and 548 K. Data collected in 2 K intervals between 410 K and 430 K show no evidence for an intermediate phase between the low temperature phase in space group Pbnm and the high temperature phase in space group F3{sup Macron }2/n. From a simultaneous fit of the unit cell volume and the isochoric heat capacity, the phonon density of states in the Pbnm phase is shown to be approximated by a two-term Debye model, with characteristic temperatures 294(1) K and 831(1) K. Vibrational Debye temperatures, determined from fitting the temperature variation of the atomic displacement parameters, show the cations to be more associated with the lower characteristic temperature, whilst that for the anions, is closer to the higher characteristic temperature. Structural parameters are presented as the amplitudes of the seven symmetry-adapted basis-vectors of the aristotype phase, and a structural basis for the temperature-dependence of the bond lengths is outlined. The phase transition in both temperature and pressure arises when a non-bonded La-O distance approaches the La coordination sphere. - Graphical abstract: The weight fraction of the rhombohedral phase of LaGaO{sub 3} from the onset of the phase transition at 408 K to its completion at 430 K. Highlights: Black-Right-Pointing-Pointer Thermoelastic properties of LaGaO{sub 3} analyzed as a two-term Debye model. Black-Right-Pointing-Pointer Crystal structure and bonding analyzed in terms of symmetry-adapted basis-vectors. Black-Right-Pointing-Pointer Consistency between calorimetric and crystallographic measurements.

  8. Structural chemistry and magnetic properties of the perovskite SrLa2Ni2TeO9

    NASA Astrophysics Data System (ADS)

    Paria Sena, Robert; Hadermann, Joke; Chin, Chun-Mann; Hunter, Emily C.; Battle, Peter D.

    2016-11-01

    A polycrystalline sample of SrLa2Ni2TeO9 has been synthesized using a standard ceramic method and characterized by neutron diffraction, magnetometry and electron microscopy. The compound adopts a monoclinic, perovskite-like structure with space group P21/n and unit cell parameters a=5.6008(1), b=5.5872(1), c=7.9018(2) Å, β=90.021(6)° at room temperature. The two crystallographically-distinct B sites are occupied by Ni2+ and Te6+ in ratios of 83:17 and 50:50. Both ac and dc magnetometry suggest that the compound is a spin glass below 35 K but the neutron diffraction data show that some regions of the sample are antiferromagnetic. Electron microscopy revealed twinning on a nanoscale and local variations in composition. These defects are thought to be responsible for the presence of two distinct types of antiferromagnetic ordering. The magnetic properties of SrLa2Ni2TeO9 are discussed in terms of cation ordering in the microstructure.

  9. Structures, magnetic and dielectric properties of the ordered double perovskites LnPbNiSbO6 (Ln = La, Pr)

    NASA Astrophysics Data System (ADS)

    Han, Lin; Bai, Yijia; Liu, Xiaojuan; Yao, Chuangang; Meng, Junling; Liang, Qingshuang; Wu, Xiaojie; Meng, Jian

    2014-09-01

    The crystal structures, magnetic and dielectric properties for the ordered double perovskites LnPbNiSbO6 (Ln = La, Pr) have been investigated. Rietveld refinements of x-ray diffraction data have been indexed for the monoclinic symmetry in space group P21/n (No. 14) and a highly rock-salt ordered arrangement of NiO6 and SbO6 octahedra. The B-site lattices are distorted strongly due to the substitution of rare Earth ions at the A-site. The magnetization measurements show an antiferromagnetic ordering. The effective magnetic moments μ eff are larger than the spin-only values, suggesting that the orbital component for Ni2+ is significant. The maximum values of isothermal magnetization increase due to the lattice distortion of BO6 octahedra, which may weaken the antiferromagnetic interaction via Ni2+-O-Sb5+-O-Ni2+ paths. The dielectric constants for LaPbNiSbO6 present frequency dependence and the tan δ curves exhibit relaxor-like dielectric response. The ɛ‧ decreases with the reduction of the magnetic moments of B-site transition metal ions, which reveals a relationship between the dielectric and magnetic properties.

  10. X-ray Absorption Fine Structure Studies of Mn Coordination in Doped Perovskite SrTiO3

    SciTech Connect

    Levin, I.; Krayzman, V; Woicik, J; Tkach, A; Vilarinho, P

    2010-01-01

    The coordination of Mn in doped SrTiO{sub 3} ceramics having nominal compositions SrTi{sub 0.98}Mn{sub 0.02}O{sub 3} and Sr{sub 0.98}Mn{sub 0.02}TiO{sub 3} was analyzed using x-ray absorption fine structure (XAFS) measurements. As expected, Mn{sup 4+} substitution for Ti{sup 4+} leads to Mn occupancy of the octahedral B-sites of ABO{sub 3} perovskite lattice with a Mn-O bond distance of 1.902 {angstrom} (compared to 1.953 {angstrom} for Ti-O) and no significant local distortions around the Mn atoms. In contrast, for the composition Sr{sub 0.98}Mn{sup 0.02}TiO{sub 3}, Mn segregates to both the A-sites (as Mn{sup 2+}) and the B-sites (predominantly as Mn{sup 4+}). Extended XAFS confirms strong ({approx} 0.77 {angstrom}) displacements of Mn{sup 2+} cations off the ideal A-site positions along <001> directions with a significant distortion of several coordination shells around the dopant atoms.

  11. Spectroscopy and structural characteristics of Eu3+-activated perovskite tungstate Ba2La2ZnW2O12

    NASA Astrophysics Data System (ADS)

    Yang, Li; Huang, Yanlin; Cheng, Han; Seo, Hyo Jin

    2015-11-01

    Eu3+-doped tungstate Ba2La2ZnW2O12 was prepared by the high-temperature solid-state reaction method. The x-ray powder diffraction (XRD) patterns indicate that the matrix has a perovskite structure. The samples were characterized by the scanning electron microscope (SEM), by optical diffuse reflection, photoluminescence (PL) spectra and by their decay curves. Eu3+-activated Ba2La2ZnW2O12 shows red luminescence under the excitation of near-ultraviolet and blue light. Laser site-selective excitation and emission spectroscopy technology was applied to investigate the spectroscopic and microstructural properties. The excitation spectra were tested by monitoring the emission from 5D0  →  7F0-4 transitions. Accordingly the emission spectra and decay curves (lifetime) were measured by the excitation in the 5D0  →  7F0 wavelength region using a pulsed, tunable, and narrow-band dye laser. We have detected two Eu3+ sites in Ba2La2ZnW2O12 with the temperature region ranging from 10 K to below 300 K. On the spectra data of the site-selective emission and decay, the Stark energy levels of Eu3+ at two different sites were determined. The lifetimes of Eu3+ ions at the two sites were compared. The energy transfer and crystallographic assignments for the Eu3+ sites were discussed.

  12. Composite S-layer lipid structures

    PubMed Central

    Schuster, Bernhard; Sleytr, Uwe B.

    2010-01-01

    Designing and utilization of biomimetic membrane systems generated by bottom-up processes is a rapidly growing scientific and engineering field. Elucidation of the supramolecular construction principle of archaeal cell envelopes composed of S-layer stabilized lipid membranes led to new strategies for generating highly stable functional lipid membranes at meso- and macroscopic scale. In this review, we provide a state of the art survey how S-layer proteins, lipids, and polysaccharides may be used as basic building blocks for the assembly of S-layer supported lipid membranes. These biomimetic membrane systems are distinguished by a nanopatterned fluidity, enhanced stability and longevity and thus, provide a dedicated reconstitution matrix for membrane-active peptides and transmembrane proteins. Exciting areas for application of composite S-layer membrane systems concern sensor systems involving specific membrane functions. PMID:19303933

  13. Preservation of Archaeal Surface Layer Structure During Mineralization

    PubMed Central

    Kish, Adrienne; Miot, Jennyfer; Lombard, Carine; Guigner, Jean-Michel; Bernard, Sylvain; Zirah, Séverine; Guyot, François

    2016-01-01

    Proteinaceous surface layers (S-layers) are highly ordered, crystalline structures commonly found in prokaryotic cell envelopes that augment their structural stability and modify interactions with metals in the environment. While mineral formation associated with S-layers has previously been noted, the mechanisms were unconstrained. Using Sulfolobus acidocaldarius a hyperthermophilic archaeon native to metal-enriched environments and possessing a cell envelope composed only of a S-layer and a lipid cell membrane, we describe a passive process of iron phosphate nucleation and growth within the S-layer of cells and cell-free S-layer “ghosts” during incubation in a Fe-rich medium, independently of metabolic activity. This process followed five steps: (1) initial formation of mineral patches associated with S-layer; (2) patch expansion; (3) patch connection; (4) formation of a continuous mineral encrusted layer at the cell surface; (5) early stages of S-layer fossilization via growth of the extracellular mineralized layer and the mineralization of cytosolic face of the cell membrane. At more advanced stages of encrustation, encrusted outer membrane vesicles are formed, likely in an attempt to remove damaged S-layer proteins. The S-layer structure remains strikingly well preserved even upon the final step of encrustation, offering potential biosignatures to be looked for in the fossil record. PMID:27221593

  14. Doubly slanted layer structures in holographic gelatin emulsions: solar concentrators

    NASA Astrophysics Data System (ADS)

    Hung, Jenny; Chan, Po Shan; Sun, Caiming; Wing Ho, Choi; Tam, Wing Yim

    2010-04-01

    We have fabricated doubly slanted layer structures in holographic gelatin emulsions using a double-exposure two-beam interference from two light sources with different wavelengths. The doubly slanted layers, with different spacings and overlapping with each other, are fabricated such that they are slanted in opposite directions making a 30° angle with the holographic plate. The doubly slanted layer structures exhibit photonic stop bands corresponding to the two layered structures. More importantly, diffracted light beams from the slanted layers travel in different directions and emerge, through internal reflections, at the opposite edges of the gelatin plate. The doubly slanted layer structures could be used as solar concentrators such that sunlight is separated into different components and steered directly to photovoltaics with the corresponding wavelength sensitivities to enhance energy conversion efficiency.

  15. Shear-layer structures in near-wall turbulence

    NASA Technical Reports Server (NTRS)

    Johansson, A. V.; Alfredsson, P. H.; Kim, J.

    1987-01-01

    The structure of internal shear layer observed in the near-wall region of turbulent flows is investigated by analyzing flow fields obtained from numerical simulations of channel and boundary-layer flows. It is found that the shear layer is an important contributor to the turbulence production. The conditionally averaged production at the center of the structure was almost twice as large as the long-time mean value. The shear-layer structure is also found to retain its coherence over streamwise distances on the order of a thousand viscous length units, and propagates with a constant velocity of about 10.6 u sub rho throughout the near wall region.

  16. Synthesis and Characterization of Complex Metal Oxides with Perovskite-Related Structure

    NASA Astrophysics Data System (ADS)

    Liu, Chia-Jyi

    localization of carriers at low temperatures. Metal-like temperature dependence sustains to x = 0.36 and y = 0.2 with localization of carriers at low temperatures. In contrast to the system rm La_{1.85}Sr_{0.15 }Cu_{1-y}Ni_ yO_{4 -delta}, metal-nonmetal transition can be tuned by varying the Sr content with a given Ni content. For the nonmetallic samples and those materials which show localization of carriers at low temperature, their conductivities nicely follow the form exp ((T_0/T) ^{rm v}) with v = {1over4} or {1 over2} (VRH law), indicating that localization of carriers is caused by disorder. Comparison between the systems rm La_{2-x}Sr_ x CuO_{4 -delta} and rm La_ {1.85}Sr_{0.15}Cu_{1 -y}Ni_ yO_{4-delta} in terms of their transport properties and magnetism together with the structural consideration of random distribution of Ni within the - (CuO_2) - planes and of Sr within the - (LaO) - layers, it is concluded that disorder has a profound effect on the transport properties in the system rm La_{2-x}Sr _ xCu_{1-y}Ni_ yO_ {4-delta}.

  17. Experimentally excellent beaming in a two-layer dielectric structure

    DOE PAGES

    Tasolamprou, Anna C.; Zhang, Lei; Kafesaki, Maria; Koschny, Thomas; Soukoulis, Costas M.

    2014-09-15

    We demonstrate both experimentally and theoretically that a two-layer dielectric structure can provide collimation and enhanced transmission of a Gaussian beam passing through it. This is due to formation of surface localized states along the layered structure and the coupling of these states to outgoing propagating waves. As a result, a system of multiple cascading two-layers can sustain the beaming for large propagation distances.

  18. Multi-layer laminate structure and manufacturing method

    DOEpatents

    Keenihan, James R.; Cleereman, Robert J.; Eurich, Gerald; Graham, Andrew T.; Langmaid, Joe A.

    2012-04-24

    The present invention is premised upon a multi-layer laminate structure and method of manufacture, more particularly to a method of constructing the multi-layer laminate structure utilizing a laminate frame and at least one energy activated flowable polymer.

  19. Multi-layer laminate structure and manufacturing method

    DOEpatents

    Keenihan, James R.; Cleereman, Robert J.; Eurich, Gerald; Graham, Andrew T.; Langmaid, Joe A.

    2013-01-29

    The present invention is premised upon a multi-layer laminate structure and method of manufacture, more particularly to a method of constructing the multi-layer laminate structure utilizing a laminate frame and at least one energy activated flowable polymer.

  20. Electroluminescent apparatus having a structured luminescence conversion layer

    DOEpatents

    Krummacher, Benjamin Claus

    2008-09-02

    An apparatus such as a light source is disclosed which has an OLED device and a structured luminescence conversion layer disposed on the substrate or transparent electrode of said OLED device and on the exterior of said OLED device. The structured luminescence conversion layer contains color-changing and non-color-changing regions arranged in a particular pattern.

  1. Recent Advances in Interface Engineering for Planar Heterojunction Perovskite Solar Cells.

    PubMed

    Yin, Wei; Pan, Lijia; Yang, Tingbin; Liang, Yongye

    2016-06-25

    Organic-inorganic hybrid perovskite solar cells are considered as one of the most promising next-generation solar cells due to their advantages of low-cost precursors, high power conversion efficiency (PCE) and easy of processing. In the past few years, the PCEs have climbed from a few to over 20% for perovskite solar cells. Recent developments demonstrate that perovskite exhibits ambipolar semiconducting characteristics, which allows for the construction of planar heterojunction (PHJ) perovskite solar cells. PHJ perovskite solar cells can avoid the use of high-temperature sintered mesoporous metal oxides, enabling simple processing and the fabrication of flexible and tandem perovskite solar cells. In planar heterojunction materials, hole/electron transport layers are introduced between a perovskite film and the anode/cathode. The hole and electron transporting layers are expected to enhance exciton separation, charge transportation and collection. Further, the supporting layer for the perovskite film not only plays an important role in energy-level alignment, but also affects perovskite film morphology, which have a great effect on device performance. In addition, interfacial layers also affect device stability. In this review, recent progress in interfacial engineering for PHJ perovskite solar cells will be reviewed, especially with the molecular interfacial materials. The supporting interfacial layers for the optimization of perovskite films will be systematically reviewed. Finally, the challenges remaining in perovskite solar cells research will be discussed.

  2. Photovoltaic Performance of Perovskite Solar Cells with Different Grain Sizes.

    PubMed

    Kim, Hyung Do; Ohkita, Hideo; Benten, Hiroaki; Ito, Shinzaburo

    2016-02-01

    Perovskite solar cells exhibit improved photovoltaic parameters with increasing perovskite grain size. The larger photocurrent is due to the enhanced absorption efficiency for thicker perovskite layers. The larger open-circuit voltage (VOC ) is ascribed to the reduced trap-assisted recombination for the larger grains. As a result, the power conversion efficiency exceeds 19% at best. Further improvement in VOC would be possible if the trap density were reduced.

  3. Non-collinear magnetism in multiferroic perovskites.

    PubMed

    Bousquet, Eric; Cano, Andrés

    2016-03-31

    We present an overview of the current interest in non-collinear magnetism in multiferroic perovskite crystals. We first describe the different microscopic mechanisms giving rise to the non-collinearity of spins in this class of materials. We discuss, in particular, the interplay between non-collinear magnetism and ferroelectric and antiferrodistortive distortions of the perovskite structure, and how this can promote magnetoelectric responses. We then provide a literature survey on non-collinear multiferroic perovskites. We discuss numerous examples of spin cantings driving weak ferromagnetism in transition metal perovskites, and of spin-induced ferroelectricity as observed in the rare-earth based perovskites. These examples are chosen to best illustrate the fundamental role of non-collinear magnetism in the design of multiferroicity.

  4. Structural responses of the supersonic turbulent boundary layer to expansions

    NASA Astrophysics Data System (ADS)

    Wang, Qian-cheng; Wang, Zhen-guo; Zhao, Yu-xin

    2016-09-01

    Structural responses of the supersonic turbulent boundary layer to the expansions induced by a convex wall and a ramp are experimentally investigated. Relaminarization of part of the turbulent boundary layer in the near wall region is clearly visualized, which has been seldom presented before. The relaminarized layers formed over two test models are different. While a thicker relaminarized layer is observed for the ramp, a longer lasting layer is noticed for the convex wall. The structure angle is found to be increased by the expansions. Increases of turbulence scale and boundary layer thickness are observed. The contribution of the bulk dilatation to the boundary layer growth is stronger than that of the centrifugal force.

  5. Disproportionation of (Mg,Fe)SiO₃ perovskite in Earth's deep lower mantle.

    PubMed

    Zhang, Li; Meng, Yue; Yang, Wenge; Wang, Lin; Mao, Wendy L; Zeng, Qiao-Shi; Jeong, Jong Seok; Wagner, Andrew J; Mkhoyan, K Andre; Liu, Wenjun; Xu, Ruqing; Mao, Ho-kwang

    2014-05-23

    The mineralogical constitution of the Earth's mantle dictates the geophysical and geochemical properties of this region. Previous models of a perovskite-dominant lower mantle have been built on the assumption that the entire lower mantle down to the top of the D″ layer contains ferromagnesian silicate [(Mg,Fe)SiO3] with nominally 10 mole percent Fe. On the basis of experiments in laser-heated diamond anvil cells, at pressures of 95 to 101 gigapascals and temperatures of 2200 to 2400 kelvin, we found that such perovskite is unstable; it loses its Fe and disproportionates to a nearly Fe-free MgSiO3 perovskite phase and an Fe-rich phase with a hexagonal structure. This observation has implications for enigmatic seismic features beyond ~2000 kilometers depth and suggests that the lower mantle may contain previously unidentified major phases. PMID:24855264

  6. Numerical simulation: Toward the design of high-efficiency planar perovskite solar cells

    SciTech Connect

    Liu, Feng; Zhu, Jun E-mail: sydai@ipp.ac.cn; Wei, Junfeng; Li, Yi; Lv, Mei; Yang, Shangfeng; Zhang, Bing; Yao, Jianxi; Dai, Songyuan E-mail: sydai@ipp.ac.cn

    2014-06-23

    Organo-metal halide perovskite solar cells based on planar architecture have been reported to achieve remarkably high power conversion efficiency (PCE, >16%), rendering them highly competitive to the conventional silicon based solar cells. A thorough understanding of the role of each component in solar cells and their effects as a whole is still required for further improvement in PCE. In this work, the planar heterojunction-based perovskite solar cells were simulated with the program AMPS (analysis of microelectronic and photonic structures)-1D. Simulation results revealed a great dependence of PCE on the thickness and defect density of the perovskite layer. Meanwhile, parameters including the work function of the back contact as well as the hole mobility and acceptor density in hole transport materials were identified to significantly influence the performance of the device. Strikingly, an efficiency over 20% was obtained under the moderate simulation conditions.

  7. Fabrication of Planar Heterojunction Perovskite Solar Cells by Controlled Low-Pressure Vapor Annealing.

    PubMed

    Li, Yanbo; Cooper, Jason K; Buonsanti, Raffaella; Giannini, Cinzia; Liu, Yi; Toma, Francesca M; Sharp, Ian D

    2015-02-01

    A new method for achieving high efficiency planar CH3NH3I3-xClx perovskite photovoltaics, based on a low pressure, reduced temperature vapor annealing is demonstrated. Heterojunction devices based on this hybrid halide perovskite exhibit a top PCE of 16.8%, reduced J-V hysteresis, and highly repeatable performance without need for a mesoporous or nanocrystalline metal oxide layer. Our findings demonstrate that large hysteresis is not an inherent feature of planar heterojunctions, and that efficient charge extraction can be achieved with uniform halide perovskite materials with desired composition. X-ray diffraction, valence band spectroscopy, and transient absorption measurements of these thin films reveal that structural modifications induced by chlorine clearly dominate over chemical and electronic doping effects, without affecting the Fermi level or photocarrier lifetime in the material.

  8. Calculated high-pressure structural properties, lattice dynamics and quasi particle band structures of perovskite fluorides KZnF3, CsCaF3 and BaLiF3

    NASA Astrophysics Data System (ADS)

    Vaitheeswaran, G.; Kanchana, V.; Zhang, Xinxin; Ma, Yanming; Svane, A.; Christensen, N. E.

    2016-08-01

    A detailed study of the high-pressure structural properties, lattice dynamics and band structures of perovskite structured fluorides KZnF3, CsCaF3 and BaLiF3 has been carried out by means of density functional theory. The calculated structural properties including elastic constants and equation of state agree well with available experimental information. The phonon dispersion curves are in good agreement with available experimental inelastic neutron scattering data. The electronic structures of these fluorides have been calculated using the quasi particle self-consistent GW approximation. The GW calculations reveal that all the fluorides studied are wide band gap insulators, and the band gaps are significantly larger than those obtained by the standard local density approximation, thus emphasizing the importance of quasi particle corrections in perovskite fluorides.

  9. Calculated high-pressure structural properties, lattice dynamics and quasi particle band structures of perovskite fluorides KZnF3, CsCaF3 and BaLiF3.

    PubMed

    Vaitheeswaran, G; Kanchana, V; Zhang, Xinxin; Ma, Yanming; Svane, A; Christensen, N E

    2016-08-10

    A detailed study of the high-pressure structural properties, lattice dynamics and band structures of perovskite structured fluorides KZnF3, CsCaF3 and BaLiF3 has been carried out by means of density functional theory. The calculated structural properties including elastic constants and equation of state agree well with available experimental information. The phonon dispersion curves are in good agreement with available experimental inelastic neutron scattering data. The electronic structures of these fluorides have been calculated using the quasi particle self-consistent [Formula: see text] approximation. The [Formula: see text] calculations reveal that all the fluorides studied are wide band gap insulators, and the band gaps are significantly larger than those obtained by the standard local density approximation, thus emphasizing the importance of quasi particle corrections in perovskite fluorides. PMID:27300494

  10. Hybrid inorganic–organic superlattice structures with atomic layer deposition/molecular layer deposition

    SciTech Connect

    Tynell, Tommi; Yamauchi, Hisao; Karppinen, Maarit

    2014-01-15

    A combination of the atomic layer deposition (ALD) and molecular layer deposition (MLD) techniques is successfully employed to fabricate thin films incorporating superlattice structures that consist of single layers of organic molecules between thicker layers of ZnO. Diethyl zinc and water are used as precursors for the deposition of ZnO by ALD, while three different organic precursors are investigated for the MLD part: hydroquinone, 4-aminophenol and 4,4′-oxydianiline. The successful superlattice formation with all the organic precursors is verified through x-ray reflectivity studies. The effects of the interspersed organic layers/superlattice structure on the electrical and thermoelectric properties of ZnO are investigated through resistivity and Seebeck coefficient measurements at room temperature. The results suggest an increase in carrier concentration for small concentrations of organic layers, while higher concentrations seem to lead to rather large reductions in carrier concentration.

  11. Phonon localization in ultrathin layered structures

    NASA Astrophysics Data System (ADS)

    Döring, F.; Eberl, C.; Schlenkrich, S.; Schlenkrich, F.; Hoffmann, S.; Liese, T.; Krebs, H. U.; Pisana, S.; Santos, T.; Schuhmann, H.; Seibt, M.; Mansurova, M.; Ulrichs, H.; Zbarsky, V.; Münzenberg, M.

    2015-04-01

    An efficient way for minimizing phonon thermal conductivity in solids is to nanostructure them by means of reduced phonon mean free path, phonon scattering and phonon reflection at interfaces. A sophisticated approach toward this lies in the fabrication of thin multilayer films of different materials. In this paper, we show by femtosecond-pump-probe reflectivity measurements that in different multilayer systems with varying acoustic mismatch (consisting of metals, semiconductors, oxides and polymers), oscillations due to phonon localization can be observed. For the growth of multilayer films with well-defined layer thicknesses, we used magnetron sputtering, evaporation and pulsed laser deposition. By altering the material combinations and reducing the layer thicknesses down to 3 nm, we observed different mechanisms of phonon blocking, reaching in the frequency regime up to 360 GHz.

  12. Formation and structural characterization of 1:1 ordered perovskites in the Ba(Zn{sub 1/3}Ta{sub 2/3})O{sub 3}-BaZrO{sub 3} system

    SciTech Connect

    Chai, L.; Davies, P.K.

    1997-12-01

    The phase stabilities in the (1{minus}x)Ba(Zn{sub 1/3}Ta{sub 2/3})O{sub 3} (BZT)-xBaZrO{sub 3} (BZ) system have been investigated using samples prepared by the mixed-oxide method. The substitution of Zr{sup 4+} destabilizes the 1:2 cation ordering in BZT and promotes the formation of a cubic, 1:1 ordered structure with a doubled perovskite repeat. The homogeneity range of the 1:1 phase extends from x = 0.04 to approximately x = 0.25; substitutions beyond this range stabilize a disordered perovskite. The limits of stability of the 1:1 ordering coincide with compositions previously found to exhibit anomalies in their dielectric loss. The range of homogeneity is consistent with a random layer model for the 1:1 ordered Ba{l_brace}{beta}{prime}{sub 1/2}{beta}{double_prime}{sub 1/2}{r_brace}O{sub 3} structure. In this model the {beta}{double_prime} positions are assumed to be occupied exclusively by Ta{sup 5+}, and the {beta}{prime} sites by a random distribution of Zn{sup 2+}, Zr{sup 4+}, and the remaining Ta{sup 5+} cations. The validity of the model, where the ordered solid solutions can be represented by Ba{l_brace}[Zn{sub (2{minus}y)/3}Ta{sub (1{minus}2y)/3}Zr{sub y}]{sub 1/2}[Ta]{sub 1/2}{r_brace}O{sub 3} (y = 2x) was confirmed by Rietveld refinements conducted using data collected with a synchrotron X-ray source.

  13. Synthesis, crystal structure and characterization of new 12H hexagonal perovskite-related oxides Ba 6M2Na 2X2O 17 ( M=Ru, Nb, Ta, Sb; X=V, Cr, Mn, P, As)

    NASA Astrophysics Data System (ADS)

    Quarez, Eric; Abraham, Francis; Mentré, Olivier

    2003-11-01

    The new Ba 6Ru 2Na 2X2O 17 ( X=V, Mn) compounds have been prepared by electrosynthesis in molten NaOH and their crystal structures have been refined from single crystals X-ray diffraction, space group P6 3/ mmc, Z=2, for X=V: a =5.8506(1) Å, c =29.6241(4) Å, R1=4.76%, for X=Mn : a =5.8323(1) Å, c =29.5299(3) Å, R1=3.48%. The crystal structure is a 12H-type perovskite with a ( c' cchcc) 2 stacking sequence of [BaO 3] c, [BaO 3] h and [BaO 2] c' layers. The tridimensional edifice is formed by blocks of Ru 2O 9 dimers that share corners with NaO 6 octahedra. These blocks sandwich double sheets of X5+O 4 tetrahedra. Several isotypic Ba 6M5+2Na 2X5+2O 17 materials ( X=V, Cr, Mn, P, As) and ( M=Ru, Nb, Ta, Sb) have been prepared by solid state reaction and characterized by Rietveld analysis. The magnetic and electric properties have been investigated and show besides the Ru 5+2O 9 typical intradimer antiferromagnetic couplings, discrepancies of both χ and ρ versus T at 50 and 100 K for Ba 6Ru 2Na 2X2O 17 ( X=V, As). In this work, a review of the identified Ru-hexagonal perovskite materials is also reported in order to overview the wide variety of possibilities in the field of new compounds synthesis.

  14. Classification of structures in the stable boundary layer

    NASA Astrophysics Data System (ADS)

    Belusic, Danijel

    2015-04-01

    Ubiquitous but generally unknown flow structures populate the stable boundary layer at scales larger than turbulence. They introduce nonstationarity, affect the generation of turbulence and induce fluxes. Classification of the structures into clusters based on a similarity measure could reduce their apparent complexity and lead to better understanding of their characteristics and mechanisms. Here we explore different approaches to detect and classify structures, the usefulness of those approaches, and their potential to provide better understanding of the stable boundary layer.

  15. Selective dissolution of halide perovskites as a step towards recycling solar cells

    NASA Astrophysics Data System (ADS)

    Kim, Byeong Jo; Kim, Dong Hoe; Kwon, Seung Lee; Park, So Yeon; Li, Zhen; Zhu, Kai; Jung, Hyun Suk

    2016-05-01

    Most research on perovskite solar cells has focused on improving power-conversion efficiency and stability. However, if one could refurbish perovskite solar cells, their stability might not be a critical issue. From the perspective of cost effectiveness, if failed, perovskite solar cells could be collected and recycled; reuse of their gold electrodes and transparent conducting glasses could reduce the price per watt of perovskite photovoltaic modules. Herein, we present a simple and effective method for removing the perovskite layer and reusing the mesoporous TiO2-coated transparent conducting glass substrate via selective dissolution. We find that the perovskite layer can be easily decomposed in polar aprotic solvents because of the reaction between polar aprotic solvents and Pb2+ cations. After 10 cycles of recycling, a mesoporous TiO2-coated transparent conducting glass substrate-based perovskite solar cell still shows a constant power-conversion efficiency, thereby demonstrating the possibility of recycling perovskite solar cells.

  16. Selective dissolution of halide perovskites as a step towards recycling solar cells

    PubMed Central

    Kim, Byeong Jo; Kim, Dong Hoe; Kwon, Seung Lee; Park, So Yeon; Li, Zhen; Zhu, Kai; Jung, Hyun Suk

    2016-01-01

    Most research on perovskite solar cells has focused on improving power-conversion efficiency and stability. However, if one could refurbish perovskite solar cells, their stability might not be a critical issue. From the perspective of cost effectiveness, if failed, perovskite solar cells could be collected and recycled; reuse of their gold electrodes and transparent conducting glasses could reduce the price per watt of perovskite photovoltaic modules. Herein, we present a simple and effective method for removing the perovskite layer and reusing the mesoporous TiO2-coated transparent conducting glass substrate via selective dissolution. We find that the perovskite layer can be easily decomposed in polar aprotic solvents because of the reaction between polar aprotic solvents and Pb2+ cations. After 10 cycles of recycling, a mesoporous TiO2-coated transparent conducting glass substrate-based perovskite solar cell still shows a constant power-conversion efficiency, thereby demonstrating the possibility of recycling perovskite solar cells. PMID:27211006

  17. Perovskite catalysts for oxidative coupling

    DOEpatents

    Campbell, K.D.

    1991-06-25

    Perovskites of the structure A[sub 2]B[sub 2]C[sub 3]O[sub 10] are useful as catalysts for the oxidative coupling of lower alkane to heavier hydrocarbons. A is alkali metal; B is lanthanide or lanthanum, cerium, neodymium, samarium, praseodymium, gadolinium or dysprosium; and C is titanium.

  18. Perovskite catalysts for oxidative coupling

    DOEpatents

    Campbell, Kenneth D.

    1991-01-01

    Perovskites of the structure A.sub.2 B.sub.2 C.sub.3 O.sub.10 are useful as catalysts for the oxidative coupling of lower alkane to heavier hydrocarbons. A is alkali metal; B is lanthanide or lanthanum, cerium, neodymium, samarium, praseodymium, gadolinium or dysprosium; and C is titanium.

  19. Improper Ferroelectric Contributions in the Double Perovskite Pb2Mn0.6Co0.4WO6 System with a Collinear Magnetic Structure.

    PubMed

    Orlandi, Fabio; Righi, Lara; Mezzadri, Francesco; Manuel, Pascal; Khalyavin, Dmitry D; Delmonte, Davide; Pernechele, Chiara; Cabassi, Riccardo; Bolzoni, Fulvio; Solzi, Massimo; Calestani, Gianluca

    2016-05-01

    The physical characterization and the extended crystallographic study of the double perovskite system Pb2Mn0.6Co0.4WO6 indicate an improper ferroelectric contribution to the polarization induced by the magnetic ordering. In the paramagnetic phase, the compound displays a centrosymmetric orthorhombic double perovskite structure with the Pmcn1' symmetry. The structure is strongly distorted by the lead stereoactivity. Magnetization measurements show two magnetic transitions at 188 and 9 K, but the time-of-flight neutron diffraction data provide evidence for a long-range magnetic ordering only below the second transition. Quantitative structure refinements combined with a comprehensive symmetry analysis indicate the Pm'c21' magnetic space group to be the adequate symmetry to describe the structural distortions and spin ordering in the ground state of the system. The symmetry implies a coexistence of a spontaneous ferromagnetic moment and a ferroelectric polarization along the orthogonal b- and c-axes, respectively, in the long-range ordered structure. Macroscopic measurements confirm the presence of the spontaneous polarization also below the first transition at 188 K, where only short-range magnetic correlations are evidenced by diffuse scattering in neutron diffraction. PMID:27078522

  20. Heterojunction modification for highly efficient organic-inorganic perovskite solar cells.

    PubMed

    Wojciechowski, Konrad; Stranks, Samuel D; Abate, Antonio; Sadoughi, Golnaz; Sadhanala, Aditya; Kopidakis, Nikos; Rumbles, Garry; Li, Chang-Zhi; Friend, Richard H; Jen, Alex K-Y; Snaith, Henry J

    2014-12-23

    Organic-inorganic perovskites, such as CH3NH3PbX3 (X=I, Br, Cl), have emerged as attractive absorber materials for the fabrication of low cost high efficiency solar cells. Over the last 3 years, there has been an exceptional rise in power conversion efficiencies (PCEs), demonstrating the outstanding potential of these perovskite materials. However, in most device architectures, including the simplest thin-film planar structure, a current-voltage response displays an "anomalous hysteresis", whereby the power output of the cell varies with measurement time, direction and light exposure or bias history. Here we provide insight into the physical processes occurring at the interface between the n-type charge collection layer and the perovskite absorber. Through spectroscopic measurements, we find that electron transfer from the perovskite to the TiO2 in the standard planar junction cells is very slow. By modifying the n-type contact with a self-assembled fullerene monolayer, electron transfer is "switched on", and both the n-type and p-type heterojunctions with the perovskite are active in driving the photovoltaic operation. The fullerene-modified devices achieve up to 17.3% power conversion efficiency with significantly reduced hysteresis, and stabilized power output reaching 15.7% in the planar p-i-n heterojunction solar cells measured under simulated AM 1.5 sunlight.

  1. Multicolor fluorescent light-emitting diodes based on cesium lead halide perovskite quantum dots

    NASA Astrophysics Data System (ADS)

    Wang, Peng; Bai, Xue; Sun, Chun; Zhang, Xiaoyu; Zhang, Tieqiang; Zhang, Yu

    2016-08-01

    High quantum yield, narrow full width at half-maximum and tunable emission color of perovskite quantum dots (QDs) make this kind of material good prospects for light-emitting diodes (LEDs). However, the relatively poor stability under high temperature and air condition limits the device performance. To overcome this issue, the liquid-type packaging structure in combination with blue LED chip was employed to fabricate the fluorescent perovskite quantum dot-based LEDs. A variety of monochromatic LEDs with green, yellow, reddish-orange, and red emission were fabricated by utilizing the inorganic cesium lead halide perovskite quantum dots as the color-conversion layer, which exhibited the narrow full width at half-maximum (<35 nm), the relatively high luminous efficiency (reaching 75.5 lm/W), and the relatively high external quantum efficiency (14.6%), making it the best-performing perovskite LEDs so far. Compared to the solid state LED device, the liquid-type LED devices exhibited excellent color stability against the various working currents. Furthermore, we demonstrated the potential prospects of all-inorganic perovskite QDs for the liquid-type warm white LEDs.

  2. Elastodynamic behavior of the three dimensional layer-by-layer metamaterial structure

    NASA Astrophysics Data System (ADS)

    Aravantinos-Zafiris, N.; Sigalas, M. M.; Economou, E. N.

    2014-10-01

    In this work, we numerically investigate for the first time the elastodynamic behavior of a three dimensional layer-by-layer rod structure, which is easy to fabricate and has already proved to be very efficient as a photonic crystal. The Finite Difference Time Domain method was used for the numerical calculations. For the rods, several materials were examined and the effects of all the geometric parameters of the structure were also numerically investigated. Additionally, two modifications of the structure were included in our calculations. The results obtained here (for certain geometric parameters), exhibiting a high ratio of longitudinal over transverse sound velocity and therefore a close approach to ideal pentamode behavior over a frequency range, clearly show that the layer-by-layer rod structure, besides being an efficient photonic crystal, is a very serious contender as an elastodynamic metamaterial.

  3. Elastodynamic behavior of the three dimensional layer-by-layer metamaterial structure

    SciTech Connect

    Aravantinos-Zafiris, N.; Sigalas, M. M.; Economou, E. N.

    2014-10-07

    In this work, we numerically investigate for the first time the elastodynamic behavior of a three dimensional layer-by-layer rod structure, which is easy to fabricate and has already proved to be very efficient as a photonic crystal. The Finite Difference Time Domain method was used for the numerical calculations. For the rods, several materials were examined and the effects of all the geometric parameters of the structure were also numerically investigated. Additionally, two modifications of the structure were included in our calculations. The results obtained here (for certain geometric parameters), exhibiting a high ratio of longitudinal over transverse sound velocity and therefore a close approach to ideal pentamode behavior over a frequency range, clearly show that the layer-by-layer rod structure, besides being an efficient photonic crystal, is a very serious contender as an elastodynamic metamaterial.

  4. Structural characterization of a new vacancy ordered perovskite modification found for Ba{sub 3}Fe{sub 3}O{sub 7}F (BaFeO{sub 2.333}F{sub 0.333}): Towards understanding of vacancy ordering for different perovskite-type ferrites

    SciTech Connect

    Clemens, Oliver

    2015-05-15

    The new vacancy ordered perovskite-type compound Ba{sub 3}Fe{sub 3}O{sub 7}F (BaFeO{sub 2.33}F{sub 0.33}) was prepared by topochemical low-temperature fluorination of Ba{sub 2}Fe{sub 2}O{sub 5} (BaFeO{sub 2.5}) using stoichiometric amounts of polyvinylidene difluoride (PVDF). The vacancy order was found to be unique so far for perovskite compounds, and the connectivity pattern can be explained by the formula Ba{sub 3}(FeX{sub 6/2}) (FeX{sub 5/2}) (FeX{sub 3/2}X{sub 1/1}), with X=O/F. Mössbauer measurements were used to confirm the structural analysis and agree with the presence of Fe{sup 3+} in the above mentioned coordination environments. Group–subgroup relationships were used to build a starting model for the structure solution and to understand the relationship to the cubic perovskite structure. Furthermore, a comparison of a variety of vacancy-ordered iron-containing perovskite-type structures is given, highlighting the factors which favour one structure type over the other depending on the composition. - Graphical abstract: The crystal structure of Ba{sub 3}Fe{sub 3}O{sub 7}F in comparison to other perovskite type ferrites. - Highlights: • The crystal structure of Ba{sub 3}Fe{sub 3}O{sub 7}F in comparison to other perovskite type ferrites. • Ba{sub 3}Fe{sub 3}O{sub 7}F was synthesized by low temperature fluorination of Ba{sub 2}Fe{sub 2}O{sub 5}. • Ba{sub 3}Fe{sub 3}O{sub 7}F shows a unique vacancy order not found for other perovskite type compounds. • The structure of Ba{sub 3}Fe{sub 3}O{sub 7}F was solved using group–subgroup relationships. • A systematic comparison to other ferrite type compounds reveals structural similarities and differences. • The A-site coordination of the cation is shown to play an important role for the type of vacancy order found.

  5. X-ray absorption spectroscopy of Ru-doped relaxor ferroelectrics with a perovskite-type structure

    NASA Astrophysics Data System (ADS)

    Vitova, T.; Mangold, S.; Paulmann, C.; Gospodinov, M.; Marinova, V.; Mihailova, B.

    2014-04-01

    X-ray absorption near-edge structure and extended x-ray absorption fine structure spectroscopy at the Ru K edge of Ru-doped PbSc0.5Ta0.5O3 (PST-Ru), PbSc0.5Nb0.5O3 (PSN-Ru), and 0.9PbZn1/3Nb2/3O3-0.1PbTiO3 (PZN-0.1PT-Ru) as well as at the Ta L3 edge of PST-Ru and the Nb K edge of PSN-Ru was applied to study the short- and intermediate-range atomic arrangements in perovskite-type (ABO3) relaxor ferroelectrics. The compounds were also analyzed by complementary Raman scattering, visible/near-visible absorption spectroscopy, and synchrotron x-ray single-crystal diffraction. The results show that Ru is octahedrally coordinated in all three relaxor host matrices but the average oxidation state of Ru in PST-Ru and PSN-Ru is ˜4.4, whereas it is ˜3.8 in PZN-0.1PT-Ru. In PbSc0.5B''0.5O3 (B'' = Ta, Nb) Ru substitutes for the B'' cations in the form of isolated point defects, while in PZN-0.1PT-Ru Ru replaces adjacent A and B sites, forming a chainlike structural species of face-sharing elongated octahedra. Chemical 1:1 B-site order as well as dynamic BO6 tilting is observed around both the Ru dopant and the major B'' cation in PST-Ru and PSN-Ru regardless of the fact that according to x-ray diffraction at ambient conditions, the average structure is cubic with weak or no long-range chemical order. Pb cations are off-center displaced from the prototypic cubic A site for all three compounds and in Ru-doped PbSc0.5B''0.5O3 the BO6 tilt angle correlates with the degree of coherent B-Pb distances.

  6. Synthesis of anion-deficient layered perovskites, ACa[sub 2]Nb[sub 3-x]M[sub x]O[sub 10-x] (A = Rb, Cs; M = Al, Fe), exhibiting ion-exchange and intercalation. Evidence for the formation of layered brownmillerites, ACa[sub 2]Nb[sub 2]AlO[sub 9] (A = Cs, H)

    SciTech Connect

    Uma, S.; Gopalakrishnan, J. )

    1994-07-01

    Anion-deficient layered perovskite oxides of the formula, ACa[sub 2]Nb[sub 3-x]M[sub x]O[sub 10-x] (A = Rb, Cs; M = Al, Fe) for 0 < x [le] 1.0, possessing tetragonal structures similar to the parent ACa[sub 2]Nb[sub 3]O[sub 10], have been synthesized. The interlayer A cations in these materials are readily exchanged with protons in aqueous HNO[sub 3] to give the protonated derivatives, HCa[sub 2]Nb[sub 3-x]M[sub x]O[sub 10-x]; the latter are solid Bronsted acids intercalating a number of organic amines including aniline (pK[sub a] = 4.63). The distribution of acid sites in the interlaying region of HCa[sub 2]Nb[sub 2]MO[sub 9] inferred from n-alkylamine intercalation suggests that oxygen vacancies and Nb/M atoms are disordered in the ACa[sub 2]Nb[sub 2]MO[sub 9] samples prepared at 1100-1200[degrees]C. Annealing a disordered sample of CsCa[sub 2]Nb[sub 2]AlO[sub 9] for a long time at lower temperatures tends to order the Nb/Al atoms and oxygen vacancies to produce octahedral (NbO[sub 6/2])-tetrahedral (AlO[sub 4/2])-octahedral (NbO[sub 6/2]) layer sequence reminiscent of the brownmillerite structure. 22 refs., 7 figs., 5 tabs.

  7. Synthesis, crystal structure and magnetic properties of a new B-site ordered double perovskite Sr{sub 2}CuIrO{sub 6}

    SciTech Connect

    Vasala, Sami; Yamauchi, Hisao; Karppinen, Maarit

    2014-12-15

    Here we synthesize and characterize a new double-perovskite oxide Sr{sub 2}CuIrO{sub 6}. The synthesis requires the use of high oxygen pressure to stabilize the VI oxidation state of iridium. The compound has a tetragonally-distorted crystal structure due to the Jahn–Teller active Cu{sup II} ion, and a high degree of B-site cation order. Magnetic transition is apparent at 15 K, but the zero-field-cooled and field-cooled susceptibilities diverge below this temperature. The high degree of cation order would exclude the possibility of a typical spin-glass, indicating that the divergence is probably due to a frustration of the magnetic interactions between Cu and Ir, with a high frustration factor of f≈25. - Graphical abstract: A new member of the A{sub 2}B′B″O{sub 6} double-perovskite family with JT-active Cu{sup II} at the B′ site and Ir{sup VI} at the B″ site is synthesized through high pressure synthesis and characterized for the structural and magnetic properties. - Highlights: • New member of the A{sub 2}CuB″O{sub 6} double-perovskite family is synthesized with B″=Ir. • Stabilization of Ir{sup VI} requires the use of high oxygen pressure synthesis. • Crystal structure is tetragonally distorted due to JT-active Cu{sup II}. • Divergence of ZFC and FC curves is seen below the T{sub N} of 15 K. • This is presumably due to a frustration effect.

  8. Low-temperature fabrication of efficient wide-bandgap organolead trihalide perovskite solar cells

    DOE PAGES

    Bi, Cheng; Yuan, Yongbo; Fang, Yanjun; Huang, Jinsong

    2014-11-25

    A mixed halide perovskite solar cell with a 1.72 eV bandgap is developed by incorporating Br into perovskite through a low-temperature solution process. A high efficiency of 13.1% is achieved by carefully tuning the thickness, morphology, and surface passivation of the perovskite layers. Furthermore, the fabrication techniques and conditions are compatible with future perovskite/Si tandem cell studies.

  9. Perovskite LaPbMSbO{sub 6} (M=Co, Ni): Structural distortion, magnetic and dielectric properties

    SciTech Connect

    Bai, Yijia; Han, Lin; Liu, Xiaojuan; Deng, Xiaolong; Wu, Xiaojie; Yao, Chuangang; Liang, Qingshuang; Meng, Junling; Meng, Jian

    2014-09-15

    The B-site ordered double perovskite oxides LaPbMSbO{sub 6} (M=Co, Ni) have been synthesized via the modified Sol–Gel precursor two-step route. Rietveld refinements reveal strong abnormal structural distortion and BO{sub 6} octahedral deformation appearing along the ab plane. Owing to the cooperative Jahn–Teller effect of Co{sup 2+} and Pb{sup 2+} ions, the Co-related compound exhibits almost complete Co{sup 2+}–Sb{sup 5+} order. For magnetic properties, spin-canted antiferromagnetic state with high extent of magnetic frustration is confirmed. The Ni-related compound presents heavier magnetic frustration for introducing tiny disorder on site occupation accompanied with valence state and further enhancing the complexity of magnetic competition. Dielectric measurements present a considerable temperature dependent dielectric relaxation with great dc-like loss feature in the LaPbCoSbO{sub 6}. For LaPbNiSbO{sub 6}, however, the permittivity with low dielectric loss is shown to be insensitive to either temperature or frequency. The corresponding electronic active energy manifests that the weakly bounded 3d-electron is prone to hop in a more distorted Co–Sb sublattice. - Graphical abstract: XRD Rietveld refinement result of LaPbCoSbO{sub 6} presented a large BO{sub 6} octahedral distortion along the ab plane. Based upon the variations from Co–O–Sb bond angles, a fierce competition from many extended magnetic coupling routes (M–O–O–M) would induce a considerably large magnetic frustration and electron hopping restriction. - Highlights: • Highly ordered LaPbMSbO{sub 6} (M=Co, Ni) were synthesized. • Abnormal structural distortion appeared in the ab plane. • Strong magnetic frustration was confirmed via M{sup 2+}–O–O–M{sup 2+} route. • Dielectric measurements presented a large difference between Co and Ni samples. • 3d-electronic structure determines lattice distortion and physical properties.

  10. A perovskite cell with a record-high-Voc of 1.61 V based on solvent annealed CH3NH3PbBr3/ICBA active layer

    NASA Astrophysics Data System (ADS)

    Wu, Chun-Guey; Chiang, Chien-Hung; Chang, Sheng Hsiung

    2016-02-01

    A high open-circuit voltage inverted perovskite solar cell based on a CH3NH3PbBr3 absorber and ICBA acceptor is reported. The CH3NH3PbBr3 film fabricated under ambient atmosphere at a moderate temperature (~100 °C) using a two-step spin-coating method is composed of aggregated nano-grains. Upon solvent annealing of the CH3NH3PbBr3/ICBA film, the efficiency of the resulting cell increases from 1.71% to 7.50% with a remarkably high open circuit voltage (Voc) of ca. 1.60 V. ICBA acts not only as a high LUMO acceptor to realize high Voc but also as a mending agent to increase the efficiency of the cell by penetrating into the defects/voids of the CH3NH3PbBr3 film via solvent annealing as evidenced by TRPL, XPS and SEM data. Solvent annealing of the active layer was proved to be simple and effective device engineering to improve the efficiency of the perovskite cell based on a low quality film and the Voc of the inverted perovskite cell can be tuned by the LUMO level of the acceptor were revealed. The CH3NH3PbBr3/ICBA film is semi-transparent with an average 50% transmittance under visible light. The moderatetemperature processed CH3NH3PbBr3 solar cell with high Voc and a semi-transparent absorber has great potential for application as the top cell in a tandem solar cell.A high open-circuit voltage inverted perovskite solar cell based on a CH3NH3PbBr3 absorber and ICBA acceptor is reported. The CH3NH3PbBr3 film fabricated under ambient atmosphere at a moderate temperature (~100 °C) using a two-step spin-coating method is composed of aggregated nano-grains. Upon solvent annealing of the CH3NH3PbBr3/ICBA film, the efficiency of the resulting cell increases from 1.71% to 7.50% with a remarkably high open circuit voltage (Voc) of ca. 1.60 V. ICBA acts not only as a high LUMO acceptor to realize high Voc but also as a mending agent to increase the efficiency of the cell by penetrating into the defects/voids of the CH3NH3PbBr3 film via solvent annealing as evidenced by TRPL

  11. Effect of hydration on the structure of perovskite-like cuprates

    NASA Astrophysics Data System (ADS)

    Bobylev, I. B.; Naumov, S. V.; Zyuzeva, N. A.

    2016-09-01

    The effect of hydration at T = 150 and 200°C on the structures of YBa2Cu3O y (123) and a number of binary cuprates has been studied. It has been shown that the compounds containing oxygen vacancies in their structures interact with hydrogen significantly more strongly than cuprates without vacancies. Depending on the cuprate structure, hydrogen can be embedded in interstitial sites with the formation of hydrides and be attached to oxygen with the formation of hydroxides. The phase transition of the 123 phase to a defect tetragonal 124-type phase occurs only for the compounds with a high oxygen content. All the cuprates under study are more stable to reduction as compared to CuO.

  12. The defect structure and chemical lattice strain of the double perovskites Sr2BMoO6-δ (B = Mg, Fe).

    PubMed

    Tsvetkov, D S; Ivanov, I L; Malyshkin, D A; Steparuk, A S; Zuev, A Yu

    2016-08-01

    The defect structure of B-site ordered double perovskites Sr2BMoO6-δ was analyzed. The defect structure model was proposed and successfully verified using data on oxygen nonstoichiometry of Sr2MgMoO6-δ and Sr2FeMoO6-δ. As a result, equilibrium constants of the defect reactions involved were estimated. Fe and Mo in Sr2FeMoO6-δ were found to be in the mixed oxidation state close to +2.5 and +5.5, respectively. Chemical strain of the Sr2FeMoO6-δ double perovskite lattice was studied by in situ high temperature XRD at 1100 °C depending on pO2. Parameter a of the Sr2FeMoO6-δ cubic cell was found to increase with decreasing pO2 because of lattice chemical expansion. The tetragonal polymorph of Sr2FeMoO6-δ was shown to exhibit transversal isotropy with respect to chemical expansion. It was also found that its crystal lattice expands in the ab-plane and simultaneously contracts along the c-axis when the oxygen content in the double perovskite decreases. In order to describe the degree of anisotropy of chemical strain a new phenomenological coefficient was introduced. This coefficient was shown to affect both the magnitude and change direction of an oxide cell volume caused by its reduction/oxidation. Excellent agreement between the chemical expansion along the a-axis calculated for both polymorphs of Sr2FeMoO6-δ according to the model recently developed and that measured experimentally was shown. Chemical contraction observed along the c-axis with a decreasing oxygen content in the tetragonal polymorph was also found to coincide completely with that calculated using the approach developed in the present study. PMID:27476830

  13. Crystal structure, phase transitions, and magnetic properties of titanium doped La0.5Sr0.5MnO3 perovskites

    NASA Astrophysics Data System (ADS)

    Hazzez, M.; Ihzaz, N.; Boudard, M.; Oumezzine, M.

    2016-04-01

    The current paper investigates the effect of titanium substitution on the structure as well as the magnetic properties of La0.5Sr0.5Mn1-xTixO3 (0≤x≤0.5) polycrystalline powder. The samples studied crystallize in a distorted perovskite structures of tetragonal (space group I4/mcm) symmetry with octahedral tilting scheme (a0a0c-), leading to the absence of octahedral tilting all along two perovskite main directions and to an out-of-phase along the third direction, or rhombohedral (space group R 3 bar c) symmetry with octahedral tilting scheme (a-a-a-) yielding to out-of-phase along the three perovskite main directions. As the Ti content increases, a better matching of the (Mn/Ti)-O distances and (Mn/Ti)-O-(Mn/Ti) bond angle occurs. This phenomenon is created by an elongation of the (Mn/Ti)-O distance, as Mn4+ is substituted by the larger ion Ti4+. In the whole compositional range, the symmetry-adapted to atomic displacements, responsible for the out-of-phase tilting of the (Mn/Ti)O6 octahedra, stays active, anticipating tetragonal-to-rhombohedral phase transition. Taking in to account what has been explained above, measurements of magnetic properties show a decrease of magnetic ordering temperature when Ti content increases, which in turn leads to the diminution of the exchange interaction caused by reducing the FM coupling and the replacement of neighboring manganese Mn3+-O-Mn4+ by Mn3+-O-Ti4+ bonds. This phenomenon results in broadening of the paramagnetic to ferromagnetic phase transition range. Further changes in magnetic properties with the increase in Ti concentration are studied.

  14. The defect structure and chemical lattice strain of the double perovskites Sr2BMoO6-δ (B = Mg, Fe).

    PubMed

    Tsvetkov, D S; Ivanov, I L; Malyshkin, D A; Steparuk, A S; Zuev, A Yu

    2016-08-01

    The defect structure of B-site ordered double perovskites Sr2BMoO6-δ was analyzed. The defect structure model was proposed and successfully verified using data on oxygen nonstoichiometry of Sr2MgMoO6-δ and Sr2FeMoO6-δ. As a result, equilibrium constants of the defect reactions involved were estimated. Fe and Mo in Sr2FeMoO6-δ were found to be in the mixed oxidation state close to +2.5 and +5.5, respectively. Chemical strain of the Sr2FeMoO6-δ double perovskite lattice was studied by in situ high temperature XRD at 1100 °C depending on pO2. Parameter a of the Sr2FeMoO6-δ cubic cell was found to increase with decreasing pO2 because of lattice chemical expansion. The tetragonal polymorph of Sr2FeMoO6-δ was shown to exhibit transversal isotropy with respect to chemical expansion. It was also found that its crystal lattice expands in the ab-plane and simultaneously contracts along the c-axis when the oxygen content in the double perovskite decreases. In order to describe the degree of anisotropy of chemical strain a new phenomenological coefficient was introduced. This coefficient was shown to affect both the magnitude and change direction of an oxide cell volume caused by its reduction/oxidation. Excellent agreement between the chemical expansion along the a-axis calculated for both polymorphs of Sr2FeMoO6-δ according to the model recently developed and that measured experimentally was shown. Chemical contraction observed along the c-axis with a decreasing oxygen content in the tetragonal polymorph was also found to coincide completely with that calculated using the approach developed in the present study.

  15. A perovskite cell with a record-high-V(oc) of 1.61 V based on solvent annealed CH3NH3PbBr3/ICBA active layer.

    PubMed

    Wu, Chun-Guey; Chiang, Chien-Hung; Chang, Sheng Hsiung

    2016-02-21

    A high open-circuit voltage inverted perovskite solar cell based on a CH3NH3PbBr3 absorber and ICBA acceptor is reported. The CH3NH3PbBr3 film fabricated under ambient atmosphere at a moderate temperature (∼100 °C) using a two-step spin-coating method is composed of aggregated nano-grains. Upon solvent annealing of the CH3NH3PbBr3/ICBA film, the efficiency of the resulting cell increases from 1.71% to 7.50% with a remarkably high open circuit voltage (Voc) of ca. 1.60 V. ICBA acts not only as a high LUMO acceptor to realize high Voc but also as a mending agent to increase the efficiency of the cell by penetrating into the defects/voids of the CH3NH3PbBr3 film via solvent annealing as evidenced by TRPL, XPS and SEM data. Solvent annealing of the active layer was proved to be simple and effective device engineering to improve the efficiency of the perovskite cell based on a low quality film and the Voc of the inverted perovskite cell can be tuned by the LUMO level of the acceptor were revealed. The CH3NH3PbBr3/ICBA film is semi-transparent with an average 50% transmittance under visible light. The moderatetemperature processed CH3NH3PbBr3 solar cell with high Voc and a semi-transparent absorber has great potential for application as the top cell in a tandem solar cell.

  16. Optical analysis of CH3NH3SnxPb1–xI3 absorbers: a roadmap for perovskite-on-perovskite tandem solar cells† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c6ta04840d Click here for additional data file.

    PubMed Central

    Anaya, Miguel; Lozano, Gabriel; Saliba, Michael; Anguita, Pablo; Roose, Bart; Abate, Antonio; Steiner, Ullrich; Grätzel, Michael; Calvo, Mauricio E.; Hagfeldt, Anders

    2016-01-01

    Organic–inorganic perovskite structures in which lead is substituted by tin are exceptional candidates for broadband light absorption. Herein we present a thorough analysis of the optical properties of CH3NH3SnxPb1–xI3 films, providing the field with definitive insights about the possibilities of these materials for perovskite solar cells of superior efficiency. We report a user's guide based on the first set of optical constants obtained for a series of tin/lead perovskite films, which was only possible to measure due to the preparation of optical quality thin layers. According to the Shockley–Queisser theory, CH3NH3SnxPb1–xI3 compounds promise a substantial enhancement of both short circuit photocurrent and power conversion efficiency in single junction solar cells. Moreover, we propose a novel tandem architecture design in which both top and bottom cells are made of perovskite absorbers. Our calculations indicate that such perovskite-on-perovskite tandem devices could reach efficiencies over 35%. Our analysis serves to establish the first roadmap for this type of cells based on actual optical characterization data. We foresee that this study will encourage the research on novel near-infrared perovskite materials for photovoltaic applications, which may have implications in the rapidly emerging field of tandem devices. PMID:27774148

  17. Rational Strategies for Efficient Perovskite Solar Cells.

    PubMed

    Seo, Jangwon; Noh, Jun Hong; Seok, Sang Il

    2016-03-15

    A long-standing dream in the large scale application of solar energy conversion is the fabrication of solar cells with high-efficiency and long-term stability at low cost. The realization of such practical goals depends on the architecture, process and key materials because solar cells are typically constructed from multilayer heterostructures of light harvesters, with electron and hole transporting layers as a major component. Recently, inorganic-organic hybrid lead halide perovskites have attracted significant attention as light absorbers for the fabrication of low-cost and high-efficiency solar cells via a solution process. This mainly stems from long-range ambipolar charge transport properties, low exciton binding energies, and suitable band gap tuning by managing the chemical composition. In our pioneering work, a new photovoltaic platform for efficient perovskite solar cells (PSCs) was proposed, which yielded a high power conversion efficiency (PCE) of 12%. The platform consisted of a pillared architecture of a three-dimensional nanocomposite of perovskites fully infiltrating mesoporous TiO2, resulting in the formation of continuous phases and perovskite domains overlaid with a polymeric hole conductor. Since then, the PCE of our PSCs has been rapidly increased from 3% to over 20% certified efficiency. The unprecedented increase in the PCE can be attributed to the effective integration of the advantageous attributes of the refined bicontinuous architecture, deposition process, and composition of perovskite materials. Specifically, the bicontinuous architectures used in the high efficiency comprise a layer of perovskite sandwiched between mesoporous metal-oxide layer, which is a very thinner than that of used in conventional dye-sensitized solar cells, and hole-conducting contact materials with a metal back contact. The mesoporous scaffold can affect the hysteresis under different scan direction in measurements of PSCs. The hysteresis also greatly depends on

  18. Novel nanoscroll structures from carbon nitride layers.

    PubMed

    Perim, Eric; Galvao, Douglas S

    2014-08-01

    Nanoscrolls (papyrus-like nanostructures) are very attractive structures for a variety of applications, owing to their tunable diameter and large accessible surface area. They have been successfully synthesized from different materials. In this work, we investigate, through fully atomistic molecular dynamics simulations, the dynamics of scroll formation for a series of graphene-like carbon nitride (CN) two-dimensional systems: g-CN, triazine-based g-C3 N4 , and heptazine-based g-C3 N4 . Our results show that stable nanoscrolls can be formed for each of these structures. Possible synthetic routes to produce these nanostructures are also addressed. PMID:24819427

  19. Band gap engineering strategy via polarization rotation in perovskite ferroelectrics

    SciTech Connect

    Wang, Fenggong Grinberg, Ilya; Rappe, Andrew M.

    2014-04-14

    We propose a strategy to engineer the band gaps of perovskite oxide ferroelectrics, supported by first principles calculations. We find that the band gaps of perovskites can be substantially reduced by as much as 1.2 eV through local rhombohedral-to-tetragonal structural transition. Furthermore, the strong polarization of the rhombohedral perovskite is largely preserved by its tetragonal counterpart. The B-cation off-center displacements and the resulting enhancement of the antibonding character in the conduction band give rise to the wider band gaps of the rhombohedral perovskites. The correlation between the structure, polarization orientation, and electronic structure lays a good foundation for understanding the physics of more complex perovskite solid solutions and provides a route for the design of photovoltaic perovskite ferroelectrics.

  20. The anionic superconductor Bi[sub 3]BaO[sub 5. 5]: A bcc structure closely related to the perovskite. Relationships with anti [alpha]-AgI

    SciTech Connect

    Michel, C.; Pelloquin, D.; Hervieu, M.; Raveau, B. ); Abbattista, F.; Vallino, M. )

    1994-03-01

    The average bcc structure of Bi[sub 3]BaO[sub 5.5] (a = 4.3822(2) [angstrom]) has been determined by powder neutron diffraction. The calculations performed in the space group Im3m have shown that the Bi and Ba atoms are statistically distributed over the 2(a) sites (0,0,0), whereas oxygen and anionic vacancies are statistically distributed over the 6(b) sites (1/2,0,0). The cationic positions and the large anisotropic thermal factors of the oxygen atoms resemble the anti [alpha]-AgI structure. However, the anionic positions correspond to those observed in the perovskite. Thus, contrary to Cd[sub 0.79]Cd[sub 0.21]O[sub 1.39], this phase cannot be considered as an anti [alpha]-AgI structure. It can better be described as the coexistence of the two configurations of the perovskite inside the crystals. Ionic conductivity measurements show that this phase is an anionic conductor with an activation energy of 0.90 eV and T[sub 673 K] [approximately] 10[sup [minus]3] [Omega][sup [minus]1] cm[sup [minus]1].