SELF-HEALING NANOMATERIALS: MULTIMILLION-ATOM REACTIVE MOLECULAR DYNAMICS SIMULATIONS

Hakamata, Tomoya; Shimamura, Kohei; Shimojo, Fuyuki; Kalia, Rajiv K.; Nakano, Aiichiro; Vashishta, Priya

doi:10.1038/srep19599

Title: SELF-HEALING NANOMATERIALS: MULTIMILLION-ATOM REACTIVE MOLECULAR DYNAMICS SIMULATIONS

Technical Report · Fri Oct 20 00:00:00 EDT 2017

DOI:https://doi.org/10.1038/srep19599· OSTI ID:1238777

Hakamata, Tomoya ^[1]; Shimamura, Kohei ^[2]; Shimojo, Fuyuki ^[1]; Kalia, Rajiv K. ^[3]; Nakano, Aiichiro ^[3]; Vashishta, Priya ^[3]

Kumamoto Univ., Kumamoto (Japan)
Kumamoto Univ., Kumamoto (Japan); Univ. of Southern California, Los Angeles, CA (United States); Kobe Univ., Kobe (Japan)
Univ. of Southern California, Los Angeles, CA (United States)

Organometal halide perovskites are attracting great attention as promising material for solar cells because of their high power conversion efficiency. The high performance has been attributed to the existence of free charge carriers and their large diffusion lengths, but the nature of carrier transport at the atomistic level remains elusive. Here, nonadiabatic quantum molecular dynamics simulations elucidate the mechanisms underlying the excellent free-carrier transport in CH₃NH₃PbI₃. Pb and I sublattices act as disjunct pathways for rapid and balanced transport of photoexcited electrons and holes, respectively, while minimizing efficiency-degrading charge recombination. On the other hand, CH₃NH₃ sublattice quickly screens out electrostatic electron-hole attraction to generate free carriers within 1 ps. Together this nano-architecture lets photoexcited electrons and holes dissociate instantaneously and travel far away to be harvested before dissipated as heat. As a result, this work provides much needed structure-property relationships and time-resolved information that potentially lead to rational design of efficient solar cells.

View Technical Report

Cite

Export

Save

Research Organization:: Univ. of California, Los Angeles, CA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: FG02-04ER46130

OSTI ID:: 1238777

Report Number(s):: DOE-UCLA-46130; srep19599

Country of Publication:: United States

Language:: English

References (25)

Metal-halide perovskites for photovoltaic and light-emitting devices Stranks, Samuel D.; Snaith, Henry J. Nature Nanotechnology, Vol. 10, Issue 5 https://doi.org/10.1038/nnano.2015.90	journal	May 2015
Photocarrier Recombination Dynamics in Perovskite CH ₃ NH ₃ PbI ₃ for Solar Cell Applications Yamada, Yasuhiro; Nakamura, Toru; Endo, Masaru Journal of the American Chemical Society, Vol. 136, Issue 33 https://doi.org/10.1021/ja506624n	journal	August 2014
Band filling with free charge carriers in organometal halide perovskites Manser, Joseph S.; Kamat, Prashant V. Nature Photonics, Vol. 8, Issue 9 https://doi.org/10.1038/nphoton.2014.171	journal	August 2014
Hybrid perovskites for photovoltaics: Insights from first principles Filippetti, A.; Mattoni, A. Physical Review B, Vol. 89, Issue 12 https://doi.org/10.1103/PhysRevB.89.125203	journal	March 2014
Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells Kojima, Akihiro; Teshima, Kenjiro; Shirai, Yasuo Journal of the American Chemical Society, Vol. 131, Issue 17, p. 6050-6051 https://doi.org/10.1021/ja809598r	journal	May 2009
Large nonadiabatic quantum molecular dynamics simulations on parallel computers Shimojo, Fuyuki; Ohmura, Satoshi; Mou, Weiwei Computer Physics Communications, Vol. 184, Issue 1 https://doi.org/10.1016/j.cpc.2012.08.001	journal	January 2013
Comparative study on the excitons in lead-halide-based perovskite-type crystals CH₃NH₃PbBr₃ CH₃NH₃PbI₃ Tanaka, Kenichiro; Takahashi, Takayuki; Ban, Takuma Solid State Communications, Vol. 127, Issue 9-10, p. 619-623 https://doi.org/10.1016/S0038-1098(03)00566-0	journal	September 2003
Impact of microstructure on local carrier lifetime in perovskite solar cells de Quilettes, D. W.; Vorpahl, S. M.; Stranks, S. D. Science, Vol. 348, Issue 6235 https://doi.org/10.1126/science.aaa5333	journal	April 2015
Interface engineering of highly efficient perovskite solar cells Zhou, H.; Chen, Q.; Li, G. Science, Vol. 345, Issue 6196 https://doi.org/10.1126/science.1254050	journal	July 2014
Excitons versus free charges in organo-lead tri-halide perovskites D’Innocenzo, Valerio; Grancini, Giulia; Alcocer, Marcelo J. P. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4586	journal	April 2014
Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber Stranks, S. D.; Eperon, G. E.; Grancini, G. Science, Vol. 342, Issue 6156, p. 341-344 https://doi.org/10.1126/science.1243982	journal	October 2013
Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH₃NH₃PbI₃ Xing, G.; Mathews, N.; Sun, S. Science, Vol. 342, Issue 6156, p. 344-347 https://doi.org/10.1126/science.1243167	journal	October 2013
Structural and electronic properties of organo-halide lead perovskites: a combined IR-spectroscopy and ab initio molecular dynamics investigation Mosconi, Edoardo; Quarti, Claudio; Ivanovska, Tanja Phys. Chem. Chem. Phys., Vol. 16, Issue 30 https://doi.org/10.1039/C4CP00569D	journal	January 2014
Electro-optics of perovskite solar cells Lin, Qianqian; Armin, Ardalan; Nagiri, Ravi Chandra Raju Nature Photonics, Vol. 9, Issue 2 https://doi.org/10.1038/nphoton.2014.284	journal	December 2014
Radiative Recombination and Photoconversion of Methylammonium Lead Iodide Perovskite by First Principles: Properties of an Inorganic Semiconductor within a Hybrid Body Filippetti, Alessio; Delugas, Pietro; Mattoni, Alessandro The Journal of Physical Chemistry C, Vol. 118, Issue 43 https://doi.org/10.1021/jp507430x	journal	October 2014
Efficient planar heterojunction perovskite solar cells by vapour deposition Liu, Mingzhen; Johnston, Michael B.; Snaith, Henry J. Nature, Vol. 501, Issue 7467, p. 395-398 https://doi.org/10.1038/nature12509	journal	September 2013
Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites Lee, M. M.; Teuscher, J.; Miyasaka, T. Science, Vol. 338, Issue 6107, p. 643-647 https://doi.org/10.1126/science.1228604	journal	October 2012
Hydrogen-on-Demand Using Metallic Alloy Nanoparticles in Water Shimamura, Kohei; Shimojo, Fuyuki; Kalia, Rajiv K. Nano Letters, Vol. 14, Issue 7 https://doi.org/10.1021/nl501612v	journal	June 2014
Long-range charge-transfer excited states in time-dependent density functional theory require non-local exchange Dreuw, Andreas; Weisman, Jennifer L.; Head-Gordon, Martin The Journal of Chemical Physics, Vol. 119, Issue 6 https://doi.org/10.1063/1.1590951	journal	August 2003
Compositional engineering of perovskite materials for high-performance solar cells Jeon, Nam Joong; Noh, Jun Hong; Yang, Woon Seok Nature, Vol. 517, Issue 7535 https://doi.org/10.1038/nature14133	journal	January 2015
Electron-hole diffusion lengths > 175 μm in solution-grown CH ₃ NH ₃ PbI ₃ single crystals Dong, Qingfeng; Fang, Yanjun; Shao, Yuchuan Science, Vol. 347, Issue 6225 https://doi.org/10.1126/science.aaa5760	journal	January 2015
Nanoscopic mechanisms of singlet fission in amorphous molecular solid Mou, Weiwei; Hattori, Shinnosuke; Rajak, Pankaj Applied Physics Letters, Vol. 102, Issue 17 https://doi.org/10.1063/1.4795138	journal	April 2013
A divide-conquer-recombine algorithmic paradigm for large spatiotemporal quantum molecular dynamics simulations Shimojo, Fuyuki; Hattori, Shinnosuke; Kalia, Rajiv K. The Journal of Chemical Physics, Vol. 140, Issue 18 https://doi.org/10.1063/1.4869342	journal	May 2014
First-Principles Modeling of Mixed Halide Organometal Perovskites for Photovoltaic Applications Mosconi, Edoardo; Amat, Anna; Nazeeruddin, Md. K. The Journal of Physical Chemistry C, Vol. 117, Issue 27 https://doi.org/10.1021/jp4048659	journal	July 2013
Electronic processes in fast thermite chemical reactions: A first-principles molecular dynamics study Shimojo, Fuyuki; Nakano, Aiichiro; Kalia, Rajiv K. Physical Review E, Vol. 77, Issue 6 https://doi.org/10.1103/PhysRevE.77.066103	journal	June 2008

Similar Records

Large dielectric constant, high acceptor density, and deep electron traps in perovskite solar cell material CsGeI₃

Journal Article · Fri Jan 01 00:00:00 EST 2016 · Journal of Materials Chemistry. A · OSTI ID:1238777

Ming, Wenmei; Shi, Hongliang; Du, Mao-Hua

Thin-film semiconductor perspective of organometal trihalide perovskite materials for high-efficiency solar cells

Journal Article · Fri Feb 19 00:00:00 EST 2016 · Materials Science and Engineering. R, Reports · OSTI ID:1238777

Xiao, Zhengguo; Yuan, Yongbo; Wang, Qi; +7 more

Rashba Spin–Orbit Coupling Enhanced Carrier Lifetime in CH₃NH₃PbI₃

Journal Article · Fri Nov 06 00:00:00 EST 2015 · Nano Letters · OSTI ID:1238777

Zheng, Fan; Tan, Liang Z.; Liu, Shi; +1 more

Related Subjects

atomistic models
electronic structure

Title: SELF-HEALING NANOMATERIALS: MULTIMILLION-ATOM REACTIVE MOLECULAR DYNAMICS SIMULATIONS

Citation Formats

References (25)

Similar Records

Related Subjects