300% Enhancement of Carrier Mobility in Uniaxial‐Oriented Perovskite Films Formed by Topotactic‐Oriented Attachment

Organic-inorganic perovskites with intriguing optical and electrical properties have attracted significant research interests due to their excellent performance in optoelectronic devices. Recent efforts on preparing uniform and large-grain polycrystalline perovskite films have led to enhanced carrier lifetime up to several microseconds. However, the mobility and trap densities of polycrystalline perovskite films are still significantly behind their single-crystal counterparts. Here, a facile topotactic-oriented attachment (TOA) process to grow highly oriented perovskite films, featuring strong uniaxial-crystallographic texture, micrometer-grain morphology, high crystallinity, low trap density (≈4 × 1014 cm-3 ), and unprecedented 9 GHz charge-carrier mobility (71 cm2 V-1 s-1 ), is demonstrated. TOA-perovskite-based n-i-p planar solar cells show minimal discrepancies between stabilized efficiency (19.0%) and reverse-scan efficiency (19.7%). The TOA process is also applicable for growing other state-of-the-art perovskite alloys, including triple-cation and mixed-halide perovskites.

[1]  T. Aida,et al.  Comprehensive approach to intrinsic charge carrier mobility in conjugated organic molecules, macromolecules, and supramolecular architectures. , 2012, Accounts of chemical research.

[2]  Jean-Pierre Wolf,et al.  Organometal halide perovskite solar cell materials rationalized: ultrafast charge generation, high and microsecond-long balanced mobilities, and slow recombination. , 2014, Journal of the American Chemical Society.

[3]  Nripan Mathews,et al.  Low-temperature solution-processed wavelength-tunable perovskites for lasing. , 2014, Nature materials.

[4]  Young Chan Kim,et al.  Compositional engineering of perovskite materials for high-performance solar cells , 2015, Nature.

[5]  Jinsong Huang,et al.  Solvent Annealing of Perovskite‐Induced Crystal Growth for Photovoltaic‐Device Efficiency Enhancement , 2014, Advanced materials.

[6]  Felix Deschler,et al.  Bright light-emitting diodes based on organometal halide perovskite. , 2014, Nature nanotechnology.

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

[8]  Sang Il Seok,et al.  High-performance photovoltaic perovskite layers fabricated through intramolecular exchange , 2015, Science.

[9]  A. Jen,et al.  Role of chloride in the morphological evolution of organo-lead halide perovskite thin films. , 2014, ACS nano.

[10]  J. Blackburn,et al.  Photoinduced spontaneous free-carrier generation in semiconducting single-walled carbon nanotubes , 2015, Nature Communications.

[11]  Tonu Pullerits,et al.  Thermally Activated Exciton Dissociation and Recombination Control the Carrier Dynamics in Organometal Halide Perovskite. , 2014, The journal of physical chemistry letters.

[12]  Yang Yang,et al.  Solution-processed hybrid perovskite photodetectors with high detectivity , 2014, Nature Communications.

[13]  Sergei Tretiak,et al.  High-efficiency solution-processed perovskite solar cells with millimeter-scale grains , 2015, Science.

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

[15]  Gang Li,et al.  Single Crystal Formamidinium Lead Iodide (FAPbI3): Insight into the Structural, Optical, and Electrical Properties , 2016, Advanced materials.

[16]  N. Kopidakis,et al.  Grain-Size-Limited Mobility in Methylammonium Lead Iodide Perovskite Thin Films , 2016 .

[17]  Shuzi Hayase,et al.  Improved understanding of the electronic and energetic landscapes of perovskite solar cells: high local charge carrier mobility, reduced recombination, and extremely shallow traps. , 2014, Journal of the American Chemical Society.

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

[19]  Cherie R. Kagan,et al.  Limits of Carrier Diffusion in n-Type and p-Type CH3NH3PbI3 Perovskite Single Crystals. , 2016, The journal of physical chemistry letters.

[20]  E. Sargent,et al.  Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals , 2015, Science.

[21]  Mercouri G Kanatzidis,et al.  Semiconducting tin and lead iodide perovskites with organic cations: phase transitions, high mobilities, and near-infrared photoluminescent properties. , 2013, Inorganic chemistry.

[22]  N. Kopidakis,et al.  Revealing the Dynamics of Charge Carriers in Polymer:Fullerene Blends Using Photoinduced Time-Resolved Microwave Conductivity , 2013 .

[23]  Yanfa Yan,et al.  Unusual defect physics in CH3NH3PbI3 perovskite solar cell absorber , 2014 .

[24]  M. Johnston,et al.  Hybrid Perovskites for Photovoltaics: Charge-Carrier Recombination, Diffusion, and Radiative Efficiencies. , 2016, Accounts of chemical research.

[25]  J. Teuscher,et al.  Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites , 2012, Science.

[26]  L. Kazmerski,et al.  Investigation of polycrystalline CdTe thin films deposited by physical vapor deposition, close‐spaced sublimation, and sputtering , 1995 .

[27]  Jaehong Park,et al.  Photoinduced Carrier Generation and Recombination Dynamics of a Trilayer Cascade Heterojunction Composed of Poly(3-hexylthiophene), Titanyl Phthalocyanine, and C60. , 2015, The journal of physical chemistry. B.

[28]  N. Park,et al.  Lead Iodide Perovskite Sensitized All-Solid-State Submicron Thin Film Mesoscopic Solar Cell with Efficiency Exceeding 9% , 2012, Scientific Reports.

[29]  M. Toney,et al.  Drastic Control of Texture in a High Performance n-Type Polymeric Semiconductor and Implications for Charge Transport , 2011 .

[30]  Dong Wang,et al.  Reproducible One-Step Fabrication of Compact MAPbl(3-x)Cl(x) Thin Films Derived from Mixed-Lead-Halide Precursors , 2014 .

[31]  G. Eperon,et al.  Charge Carriers in Planar and Meso-Structured Organic-Inorganic Perovskites: Mobilities, Lifetimes, and Concentrations of Trap States. , 2015, The journal of physical chemistry letters.

[32]  Kai Zhu,et al.  Towards stable and commercially available perovskite solar cells , 2016, Nature Energy.

[33]  Laura M. Herz,et al.  Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber , 2013, Science.

[34]  J. Berry,et al.  Efficient charge extraction and slow recombination in organic–inorganic perovskites capped with semiconducting single-walled carbon nanotubes , 2016 .

[35]  Shenqiang Ren,et al.  Symmetry-Defying Iron Pyrite (FeS2) Nanocrystals through Oriented Attachment , 2013, Scientific Reports.

[36]  Banfield,et al.  Imperfect oriented attachment: dislocation generation in defect-free nanocrystals , 1998, Science.