skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Abstract

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.

Authors:
 [1];  [2];  [1];  [3];  [3];  [3]
  1. Kumamoto Univ., Kumamoto (Japan)
  2. Kumamoto Univ., Kumamoto (Japan); Univ. of Southern California, Los Angeles, CA (United States); Kobe Univ., Kobe (Japan)
  3. Univ. of Southern California, Los Angeles, CA (United States)
Publication Date:
Research Org.:
Univ. of California, Los Angeles, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1238777
Report Number(s):
DOE-UCLA-46130
srep19599
DOE Contract Number:  
FG02-04ER46130
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
atomistic models; electronic structure

Citation Formats

Hakamata, Tomoya, Shimamura, Kohei, Shimojo, Fuyuki, Kalia, Rajiv K., Nakano, Aiichiro, and Vashishta, Priya. SELF-HEALING NANOMATERIALS: MULTIMILLION-ATOM REACTIVE MOLECULAR DYNAMICS SIMULATIONS. United States: N. p., 2017. Web. doi:10.1038/srep19599.
Hakamata, Tomoya, Shimamura, Kohei, Shimojo, Fuyuki, Kalia, Rajiv K., Nakano, Aiichiro, & Vashishta, Priya. SELF-HEALING NANOMATERIALS: MULTIMILLION-ATOM REACTIVE MOLECULAR DYNAMICS SIMULATIONS. United States. https://doi.org/10.1038/srep19599
Hakamata, Tomoya, Shimamura, Kohei, Shimojo, Fuyuki, Kalia, Rajiv K., Nakano, Aiichiro, and Vashishta, Priya. 2017. "SELF-HEALING NANOMATERIALS: MULTIMILLION-ATOM REACTIVE MOLECULAR DYNAMICS SIMULATIONS". United States. https://doi.org/10.1038/srep19599. https://www.osti.gov/servlets/purl/1238777.
@article{osti_1238777,
title = {SELF-HEALING NANOMATERIALS: MULTIMILLION-ATOM REACTIVE MOLECULAR DYNAMICS SIMULATIONS},
author = {Hakamata, Tomoya and Shimamura, Kohei and Shimojo, Fuyuki and Kalia, Rajiv K. and Nakano, Aiichiro and Vashishta, Priya},
abstractNote = {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.},
doi = {10.1038/srep19599},
url = {https://www.osti.gov/biblio/1238777}, journal = {},
number = ,
volume = ,
place = {United States},
year = {Fri Oct 20 00:00:00 EDT 2017},
month = {Fri Oct 20 00:00:00 EDT 2017}
}

Works referenced in this record:

Metal-halide perovskites for photovoltaic and light-emitting devices
journal, May 2015


Photocarrier Recombination Dynamics in Perovskite CH 3 NH 3 PbI 3 for Solar Cell Applications
journal, August 2014


Band filling with free charge carriers in organometal halide perovskites
journal, August 2014


Hybrid perovskites for photovoltaics: Insights from first principles
journal, March 2014


Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells
journal, May 2009


Large nonadiabatic quantum molecular dynamics simulations on parallel computers
journal, January 2013


Comparative study on the excitons in lead-halide-based perovskite-type crystals CH3NH3PbBr3 CH3NH3PbI3
journal, September 2003


Impact of microstructure on local carrier lifetime in perovskite solar cells
journal, April 2015


Interface engineering of highly efficient perovskite solar cells
journal, July 2014


Excitons versus free charges in organo-lead tri-halide perovskites
journal, April 2014


Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber
journal, October 2013


Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH3NH3PbI3
journal, October 2013


Structural and electronic properties of organo-halide lead perovskites: a combined IR-spectroscopy and ab initio molecular dynamics investigation
journal, January 2014


Electro-optics of perovskite solar cells
journal, December 2014


Radiative Recombination and Photoconversion of Methylammonium Lead Iodide Perovskite by First Principles: Properties of an Inorganic Semiconductor within a Hybrid Body
journal, October 2014


Efficient planar heterojunction perovskite solar cells by vapour deposition
journal, September 2013


Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites
journal, October 2012


Hydrogen-on-Demand Using Metallic Alloy Nanoparticles in Water
journal, June 2014


Long-range charge-transfer excited states in time-dependent density functional theory require non-local exchange
journal, August 2003


Compositional engineering of perovskite materials for high-performance solar cells
journal, January 2015


Electron-hole diffusion lengths > 175 μm in solution-grown CH 3 NH 3 PbI 3 single crystals
journal, January 2015


Nanoscopic mechanisms of singlet fission in amorphous molecular solid
journal, April 2013


A divide-conquer-recombine algorithmic paradigm for large spatiotemporal quantum molecular dynamics simulations
journal, May 2014


First-Principles Modeling of Mixed Halide Organometal Perovskites for Photovoltaic Applications
journal, July 2013


Electronic processes in fast thermite chemical reactions: A first-principles molecular dynamics study
journal, June 2008