Low‐Temperature Soft‐Cover Deposition of Uniform Large‐Scale Perovskite Films for High‐Performance Solar Cells

Large-scale high-quality perovskite thin films are crucial to produce high-performance perovskite solar cells. However, for perovskite films fabricated by solvent-rich processes, film uniformity can be prevented by convection during thermal evaporation of the solvent. Here, a scalable low-temperature soft-cover deposition (LT-SCD) method is presented, where the thermal convection-induced defects in perovskite films are eliminated through a strategy of surface tension relaxation. Compact, homogeneous, and convection-induced-defects-free perovskite films are obtained on an area of 12 cm2 , which enables a power conversion efficiency (PCE) of 15.5% on a solar cell with an area of 5 cm2 . This is the highest efficiency at this large cell area. A PCE of 15.3% is also obtained on a flexible perovskite solar cell deposited on the polyethylene terephthalate substrate owing to the advantage of presented low-temperature processing. Hence, the present LT-SCD technology provides a new non-spin-coating route to the deposition of large-area uniform perovskite films for both rigid and flexible perovskite devices.

[1]  T. Ma,et al.  CH3NH3SnxPb(1-x)I3 Perovskite Solar Cells Covering up to 1060 nm. , 2014, The journal of physical chemistry letters.

[2]  Aldo Di Carlo,et al.  Perovskite solar cells and large area modules (100 cm2) based on an air flow-assisted PbI2 blade coating deposition process , 2015 .

[3]  Mercouri G Kanatzidis,et al.  Anomalous band gap behavior in mixed Sn and Pb perovskites enables broadening of absorption spectrum in solar cells. , 2014, Journal of the American Chemical Society.

[4]  Yoshiharu Sato,et al.  Overcoming Short-Circuit in Lead-Free CH3NH3SnI3 Perovskite Solar Cells via Kinetically Controlled Gas-Solid Reaction Film Fabrication Process. , 2016, The journal of physical chemistry letters.

[5]  Teng Zhang,et al.  High-performance hole-extraction layer of sol-gel-processed NiO nanocrystals for inverted planar perovskite solar cells. , 2014, Angewandte Chemie.

[6]  G. Ahlers,et al.  Nusselt number measurements for turbulent Rayleigh-Bénard convection. , 2003, Physical review letters.

[7]  Henry J. Snaith,et al.  Efficient planar heterojunction perovskite solar cells by vapour deposition , 2013, Nature.

[8]  Kam Sing Wong,et al.  Solvent Engineering Boosts the Efficiency of Paintable Carbon‐Based Perovskite Solar Cells to Beyond 14% , 2016 .

[9]  Kiyoyuki Terakura,et al.  Charge-transport in tin-iodide perovskite CH3NH3SnI3: origin of high conductivity. , 2011, Dalton transactions.

[10]  Zhibin Yang,et al.  High‐Performance Fully Printable Perovskite Solar Cells via Blade‐Coating Technique under the Ambient Condition , 2015 .

[11]  M. Grätzel,et al.  Title: Long-Range Balanced Electron and Hole Transport Lengths in Organic-Inorganic CH3NH3PbI3 , 2017 .

[12]  Mohammad Khaja Nazeeruddin,et al.  Improved performance and stability of perovskite solar cells by crystal crosslinking with alkylphosphonic acid ω-ammonium chlorides. , 2015, Nature chemistry.

[13]  Martin Schreyer,et al.  Synthesis and crystal chemistry of the hybrid perovskite (CH3NH3) PbI3 for solid-state sensitised solar cell applications , 2013 .

[14]  Shihe Yang,et al.  Inkjet printing and instant chemical transformation of a CH3NH3PbI3/nanocarbon electrode and interface for planar perovskite solar cells. , 2014, Angewandte Chemie.

[15]  C. Chu,et al.  Using an airbrush pen for layer-by-layer growth of continuous perovskite thin films for hybrid solar cells. , 2015, ACS applied materials & interfaces.

[16]  Robert P. H. Chang,et al.  Lead-free solid-state organic–inorganic halide perovskite solar cells , 2014, Nature Photonics.

[17]  Lifeng Zhang,et al.  Fabrication and characterization of electrospun titania nanofibers , 2009, Journal of Materials Science.

[18]  Namchul Cho,et al.  High‐Performance and Environmentally Stable Planar Heterojunction Perovskite Solar Cells Based on a Solution‐Processed Copper‐Doped Nickel Oxide Hole‐Transporting Layer , 2015, Advanced materials.

[19]  Wei Chen,et al.  Efficient and stable large-area perovskite solar cells with inorganic charge extraction layers , 2015, Science.

[20]  Yaohua Mai,et al.  Controllable Grain Morphology of Perovskite Absorber Film by Molecular Self-Assembly toward Efficient Solar Cell Exceeding 17%. , 2015, Journal of the American Chemical Society.

[21]  Liyong Niu,et al.  Full‐Solution Processed Flexible Organic Solar Cells Using Low‐Cost Printable Copper Electrodes , 2014, Advanced materials.

[22]  Alan D. F. Dunbar,et al.  Efficient planar heterojunction mixed-halide perovskite solar cells deposited via spray-deposition , 2014 .

[23]  Yongli Gao,et al.  Large-area perovskite nanowire arrays fabricated by large-scale roll-to-roll micro-gravure printing and doctor blading. , 2016, Nanoscale.

[24]  Qi Chen,et al.  Improved air stability of perovskite solar cells via solution-processed metal oxide transport layers. , 2016, Nature nanotechnology.

[25]  Blaise J. Thompson,et al.  Solution growth of single crystal methylammonium lead halide perovskite nanostructures for optoelectronic and photovoltaic applications. , 2015, Journal of the American Chemical Society.

[26]  Tsutomu Miyasaka,et al.  Organometal halide perovskites as visible-light sensitizers for photovoltaic cells. , 2009, Journal of the American Chemical Society.

[27]  M. I. Biggerstaff,et al.  Onset of surface-tension-driven Bénard convection , 1986, Journal of Fluid Mechanics.

[28]  P. Lund,et al.  Carbon-double-bond-free printed solar cells from TiO₂/CH₃NH₃PbI₃/CuSCN/Au: structural control and photoaging effects. , 2014, Chemphyschem : a European journal of chemical physics and physical chemistry.

[29]  J. Pearson,et al.  On convection cells induced by surface tension , 1958, Journal of Fluid Mechanics.

[30]  Noel Clark,et al.  3D Printer Based Slot‐Die Coater as a Lab‐to‐Fab Translation Tool for Solution‐Processed Solar Cells , 2015 .

[31]  Qingfeng Dong,et al.  Electron-hole diffusion lengths > 175 μm in solution-grown CH3NH3PbI3 single crystals , 2015, Science.

[32]  Shenghao Wang,et al.  High performance perovskite solar cells by hybrid chemical vapor deposition , 2014 .

[33]  Jegadesan Subbiah,et al.  Toward Large Scale Roll‐to‐Roll Production of Fully Printed Perovskite Solar Cells , 2015, Advanced materials.

[34]  Y. Chai,et al.  Nonstoichiometric acid–base reaction as reliable synthetic route to highly stable CH3NH3PbI3 perovskite film , 2016, Nature Communications.

[35]  Aldo Di Carlo,et al.  Solid state perovskite solar modules by vacuum-vapor assisted sequential deposition on Nd:YVO4 laser patterned rutile TiO2 nanorods , 2015, Nanotechnology.

[36]  Michael Bestehorn,et al.  Square cells in surface-tension-driven Bénard convection: experiment and theory , 1998, Journal of Fluid Mechanics.

[37]  L. Segel,et al.  Finite amplitude cellular convection induced by surface tension , 1967, Journal of Fluid Mechanics.

[38]  M. Green,et al.  The emergence of perovskite solar cells , 2014, Nature Photonics.

[39]  Matthew R. Leyden,et al.  Chemical vapor deposition grown formamidinium perovskite solar modules with high steady state power and thermal stability , 2016 .

[40]  Shuzi Hayase,et al.  Reproducible Fabrication of Efficient Perovskite-based Solar Cells: X-ray Crystallographic Studies on the Formation of CH3NH3PbI3 Layers , 2014 .

[41]  Bernd Rech,et al.  A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells , 2016, Science.

[42]  Jinsong Huang,et al.  Vividly colorful hybrid perovskite solar cells by doctor-blade coating with perovskite photonic nanostructures , 2015 .

[43]  I. B. Palymskii.  Simulation of complex regimes of Rayleigh-Benard convection , 2011 .

[44]  Jinsong Huang,et al.  Scalable fabrication of efficient organolead trihalide perovskite solar cells with doctor-bladed active layers , 2015 .

[45]  Laura M Herz,et al.  High Charge Carrier Mobilities and Lifetimes in Organolead Trihalide Perovskites , 2013, Advanced materials.

[46]  Liyuan Han,et al.  Soft-cover deposition of scaling-up uniform perovskite thin films for high cost-performance solar cells , 2016 .

[47]  Po-Shen Shen,et al.  Low‐Pressure Hybrid Chemical Vapor Growth for Efficient Perovskite Solar Cells and Large‐Area Module , 2016 .