Abstract
Recent years have seen swift increase in the power conversion efficiency of perovskite solar cells (PSCs). Interface engineering is a promising route for further improving the performance of PSCs. Here we perform first-principles calculations to explore the effect of four candidate buffer materials (MACl, MAI, PbCl2 and PbI2) on the electronic structures of the interface between MAPbI3 absorber and TiO2. We find that MAX (X = Cl, I) as buffer layers will introduce a high electron barrier and enhance the electron-hole recombination. Additionally, MAX does not passivate the surface states well. The conduction band minimum of PbI2 is much lower than that of MAPbI3 absorber, which significantly limits the band bending of the absorber and open-circuit voltage of solar cells. On the other side, suitable bandedge energy level positions, small lattice mismatch with TiO2 surfaces, and excellent surface passivation make PbCl2 a promising buffer material for absorber/electron-transport-layer interface engineering in PSCs. Our results in this work thus provide deep understanding on the effects of interface engineering with a buffer layer, which shall be useful for improving the performance of PSCs and related optoelectronics.
摘要
近年来钙钛矿太阳能电池的能量转换效率迅速提高. 界面工程是进一步改善钙钛矿太阳能电池性能的有前途的途径. 本文中, 我们进行第一性原理计算, 以探索四种候选缓冲材料(MACl, MAI, PbCl2与PbI2)对MAPbI3吸收层与TiO2之间界面电子结构的影响. 我们发现MAX (X = Cl, I)作为缓冲层将引入高电子势垒并增强电子-空穴复合. 此外, MAX不能很好地钝化表面状态. PbI2的导带最小值远低于MAPbI3吸收层的导带最小值, 这极大地限制了吸收层的能带弯曲和太阳能电池的开路电压. 另一方面, 合适的带边能级位置, 与TiO2表面的小的晶格失配以及出色的表面钝化性能使得PbCl2成为钙钛矿太阳能电池吸收层/电子传输层界面工程的有希望的缓冲材料. 因此, 我们在这项工作中获得的结果可以使人们对具有缓冲层的界面工程的效果有更深入的理解, 这有利于改善钙钛矿太阳能电池和相关光电器件的性能.
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References
Kojima A, Teshima K, Shirai Y, et al. Organometal halide perovskites as visible-light sensitizers for photovoltaic cells. J Am Chem Soc, 2009, 131: 6050–6051
Kim HS, Lee CR, Im JH, et al. Lead iodide perovskite sensitized all-solid-state submicron thin film mesoscopic solar cell with efficiency exceeding 9%. Sci Rep, 2012, 2: 591
Lee MM, Teuscher J, Miyasaka T, et al. Efficient hybrid solar cells based on meso-superstructured organometal halide perovskites. Science, 2012, 338: 643–647
Zhou H, Chen Q, Li G, et al. Interface engineering of highly efficient perovskite solar cells. Science, 2014, 345: 542–546
Jeon NJ, Noh JH, Yang WS, et al. Compositional engineering of perovskite materials for high-performance solar cells. Nature, 2015, 517: 476–480
Nie W, Tsai H, Asadpour R, et al. High-efficiency solution-processed perovskite solar cells with millimeter-scale grains. Science, 2015, 347: 522–525
Bi D, Yi C, Luo J, et al. Polymer-templated nucleation and crystal growth of perovskite films for solar cells with efficiency greater than 21%. Nat Energy, 2016, 1: 16142
Jiang Q, Zhang L, Wang H, et al. Enhanced electron extraction using SnO2 for high-efficiency planar-structure HC(NH2)2PbI3-based perovskite solar cells. Nat Energy, 2016, 2: 16177
Tan H, Jain A, Voznyy O, et al. Efficient and stable solution-processed planar perovskite solar cells via contact passivation. Science, 2017, 355: 722–726
Anaraki EH, Kermanpur A, Steier L, et al. Highly efficient and stable planar perovskite solar cells by solution-processed tin oxide. Energy Environ Sci, 2016, 9: 3128–3134
Zheng X, Chen B, Dai J, et al. Defect passivation in hybrid perovskite solar cells using quaternary ammonium halide anions and cations. Nat Energy, 2017, 2: 17102
Yang WS, Park BW, Jung EH, et al. Iodide management in formamidinium-lead-halide-based perovskite layers for efficient solar cells. Science, 2017, 356: 1376–1379
Green MA, Hishikawa Y, Dunlop ED, et al. Solar cell efficiency tables (version 51). Prog Photovolt Res Appl, 2018, 26: 3–12
Jiang Q, Zhao Y, Zhang X, et al. Surface passivation of perovskite film for efficient solar cells. Nat Photonics, 2019, 13: 460–466
Wang Q, Dong Q, Li T, et al. Thin insulating tunneling contacts for efficient and water-resistant perovskite solar cells. Adv Mater, 2016, 28: 6734–6739
Buin A, Pietsch P, Xu J, et al. Materials processing routes to trap-free halide perovskites. Nano Lett, 2014, 14: 6281–6286
Yuan ZK, Chen S, Xiang H, et al. Engineering solar cell absorbers by exploring the band alignment and defect disparity: The case of Cu- and Ag-based kesterite compounds. Adv Funct Mater, 2015, 25: 6733–6743
Würfel P. Physics of Solar Cells. Weinheim: Wiley-VCH, 2007, Ch. 6
Chirilă A, Buecheler S, Pianezzi F, et al. Highly efficient Cu(In,Ga)Se2 solar cells grown on flexible polymer films. Nat Mater, 2011, 10: 857–861
Liu Z, Hu J, Jiao H, et al. Chemical reduction of intrinsic defects in thicker heterojunction planar perovskite solar cells. Adv Mater, 2017, 29: 1606774
Yin WJ, Shi T, Yan Y. Unusual defect physics in CH3NH3PbI3 perovskite solar cell absorber. Appl Phys Lett, 2014, 104: 063903
Yin WJ, Yang JH, Kang J, et al. Halide perovskite materials for solar cells: a theoretical review. J Mater Chem A, 2015, 3: 8926–8942
Zhang Q, Su R, Liu X, et al. High-quality whispering-gallery-mode lasing from cesium lead halide perovskite nanoplatelets. Adv Funct Mater, 2016, 26: 6238–6245
Wojciechowski K, Stranks SD, Abate A, et al. Heterojunction modification for highly efficient organic-inorganic perovskite solar cells. ACS Nano, 2014, 8: 12701–12709
Li Y, Zhao Y, Chen Q, et al. Multifunctional fullerene derivative for interface engineering in perovskite solar cells. J Am Chem Soc, 2015, 137: 15540–15547
Yang D, Zhou X, Yang R, et al. Surface optimization to eliminate hysteresis for record efficiency planar perovskite solar cells. Energy Environ Sci, 2016, 9: 3071–3078
Christians JA, Schulz P, Tinkham JS, et al. Tailored interfaces of unencapsulated perovskite solar cells for >1,000 hour operational stability. Nat Energy, 2018, 3: 68–74
Correa Baena JP, Steier L, Tress W, et al. Highly efficient planar perovskite solar cells through band alignment engineering. Energy Environ Sci, 2015, 8: 2928–2934
Zu FS, Amsalem P, Salzmann I, et al. Impact of white light illumination on the electronic and chemical structures of mixed halide and single crystal perovskites. Adv Opt Mater, 2017, 5: 1700139
Schulz P, Cahen D, Kahn A. Halide perovskites: Is it all about the interfaces? Chem Rev, 2019, 119: 3349–3417
Chen Q, Zhou H, Song TB, et al. Controllable self-induced passivation of hybrid lead iodide perovskites toward high performance solar cells. Nano Lett, 2014, 14: 4158–4163
Wang L, McCleese C, Kovalsky A, et al. Femtosecond time-resolved transient absorption spectroscopy of CH3NH3PbI3 perovskite films: Evidence for passivation effect of PbI2. J Am Chem Soc, 2014, 136: 12205–12208
Cho KT, Paek S, Grancini G, et al. Highly efficient perovskite solar cells with a compositionally engineered perovskite/hole transporting material interface. Energy Environ Sci, 2017, 10: 621–627
Shang Q, Wang Y, Zhong Y, et al. Unveiling structurally engineered carrier dynamics in hybrid quasi-two-dimensional perovskite thin films toward controllable emission. J Phys Chem Lett, 2017, 8: 4431–4438
Chen P, Bai Y, Wang S, et al. In situ growth of 2D perovskite capping layer for stable and efficient perovskite solar cells. Adv Funct Mater, 2018, 28: 1706923
Cho Y, Soufiani AM, Yun JS, et al. Mixed 3D-2D passivation treatment for mixed-cation lead mixed-halide perovskite solar cells for higher efficiency and better stability. Adv Energy Mater, 2018, 8: 1703392
Cho KT, Grancini G, Lee Y, et al. Selective growth of layered perovskites for stable and efficient photovoltaics. Energy Environ Sci, 2018, 11: 952–959
Yoo HS, Park NG. Post-treatment of perovskite film with phenylalkylammonium iodide for hysteresis-less perovskite solar cells. Sol Energy Mater Sol Cells, 2018, 179: 57–65
Li N, Zhu Z, Dong Q, et al. Enhanced moisture stability of cesium-containing compositional perovskites by a feasible interfacial engineering. Adv Mater Interfaces, 2017, 4: 1700598
Li C, Liu Z, Shang Q, et al. Surface-plasmon-assisted metal halide perovskite small lasers. Adv Opt Mater, 2019, 7: 1900279
Matteocci F, Busby Y, Pireaux JJ, et al. Interface and composition analysis on perovskite solar cells. ACS Appl Mater Interfaces, 2015, 7: 26176–26183
Ralaiarisoa M, Busby Y, Frisch J, et al. Correlation of annealing time with crystal structure, composition, and electronic properties of CH3NH3PbI3−xClx mixed-halide perovskite films. Phys Chem Chem Phys, 2017, 19: 828–836
Busby Y, Agresti A, Pescetelli S, et al. Aging effects in interface-engineered perovskite solar cells with 2D nanomaterials: A depth profile analysis. Mater Today Energy, 2018, 9: 1–10
Blöchl PE. Projector augmented-wave method. Phys Rev B, 1994, 50: 17953–17979
Kresse G, Joubert D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys Rev B, 1999, 59: 1758–1775
Kresse G, Furthmüller J. Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set. Comput Mater Sci, 1996, 6: 15–50
Perdew JP, Yue W. Accurate and simple density functional for the electronic exchange energy: Generalized gradient approximation. Phys Rev B, 1986, 33: 8800–8802
Perdew JP, Burke K, Ernzerhof M. Generalized gradient approximation made simple. Phys Rev Lett, 1996, 77: 3865–3868
Grimme S, Antony J, Ehrlich S, et al. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. J Chem Phys, 2010, 132: 154104
Yang Y, Gao F, Gao S, et al. Origin of the stability of two-dimensional perovskites: a first-principles study. J Mater Chem A, 2018, 6: 14949–14955
Wei S, Zunger A. Band offsets and optical bowings of chalcopyrites and Zn-based II-VI alloys. J Appl Phys, 1995, 78: 3846–3856
Butler KT, Frost JM, Walsh A. Band alignment of the hybrid halide perovskites CH3NH3PbCl3, CH3NH3PbBr3 and CH3NH3PbI3. Mater Horiz, 2015, 2: 228–231
Lindblad R, Bi D, Park BW, et al. Electronic structure of TiO2/CH3NH3PbI3 perovskite solar cell interfaces. J Phys Chem Lett, 2014, 5: 648–653
Mosconi E, Ronca E, De Angelis F. First-principles investigation of the TiO2/organohalide perovskites interface: The role of interfacial chlorine. J Phys Chem Lett, 2014, 5: 2619–2625
Li W, Niu S, Zhao B, et al. Band gap evolution in Ruddlesden-Popper phases. Phys Rev Mater, 2019, 3: 101601
Shang Q, Li C, Zhang S, et al. Enhanced optical absorption and slowed light of reduced-dimensional CsPbBr3 nanowire crystal by exciton-polariton. Nano Lett, 2020, 20: 1023–1032
Acknowledgements
This work was financially supported by the National Natural Science Foundation of China (11804058, 61571415, 11674310 and 61622406). Cheng Y thanks the financial support from RIE2020 AME Programmatic Grant A18A1b0045 funded by A*STAR-SERC, Singapore. Cheng Y and Zhang G are grateful for the supports from the Agency for Science, Technology and Research (A*STAR) and the use of A*STAR Computational Resource Centre, Singapore (ACRC) and National Supercomputing Centre, Singapore (NSCC).
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Author contributions Huang L conceived and conducted the calculations, analyzed the results and wrote the paper; Cheng Y and Li J supervised the project, analyzed the results and revised the paper. Dong H and Huo N performed some calculations and analyzed the results. Zheng Z analyzed the results of band alignment. Deng H and Zhang G analyzed the results and revised the paper. All authors contributed to the general discussion.
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Le Huang received his Bachelor degree from Lanzhou University, China in July 2012, and PhD degree from the Institute of Semiconductors, Chinese Academy of Sciences in January 2017. He joined Guangdong University of Technology in 2017 and has been working there till present. His research interests include electronic and optical properties of perovskite materials and low-dimensional semiconductors.
Yuan Cheng is currently a Senior Scientist in the Institute of High Performance Computing (IHPC) in Singapore. She received her Bachelor degree from Fudan University, China in July 2003, and PhD degree from National University of Singapore in April 2008. She joined IHPC in 2007. Dr. Yuan Cheng’s research interest involves mechanical and physical properties of bio- and nano-materials, and machine-learning-assisted material design.
Jingbo Li received his PhD degree from the Institute of Semiconductors, Chinese Academy of Sciences, in 2001. Then, he spent six years at the Lawrence Berkeley National Laboratory and National Renewable Energy Laboratory in USA. From 2007 to 2019, he worked as a professor at the Institute of Semiconductors, Chinese Academy of Sciences. Since 2019, he has been a full-time professor and the dean of the Institute of Semiconductors, South China Normal University. His research interests include the design, fabrication, and application of novel nanostructured semiconductors.
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Huang, L., Dong, H., Huo, N. et al. Deep insights into interface engineering by buffer layer for efficient perovskite solar cells: a first-principles study. Sci. China Mater. 63, 1588–1596 (2020). https://doi.org/10.1007/s40843-020-1322-2
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DOI: https://doi.org/10.1007/s40843-020-1322-2