Hot Carrier Cooling and Recombination Dynamics of Chlorine Doped Hybrid Perovskite Single Crystals

ORAL

Abstract

Controlling the photoexcited properties and behavior of hybrid perovskites by halide doping has the potential to impact a wide range of emerging technologies, including solar cells and radiation detectors. We examined crystalline samples of methyl ammonium lead bromide substituted with chlorine (MAPbBr3-xClx) by transient reflectivity spectroscopy and non-adiabatic molecular dynamics (NAMD) simulations. At picosecond timescales, the addition of chlorine to the perovskite crystal increased the observed rate of hot carrier cooling by approximately 30%. Calculated nonadiabatic electron-phonon coupling constants increased with chlorine doping percentage mimicking the experimental data. At longer times, chlorine doped samples exhibit smaller ambipolar mobility and slower surface recombination velocity which may be a key factor in enhancing perovskite photoelectric devices.

*This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science.

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Presenters

  • La Moyne Mix

    • Los Alamos National Laboratory
    • CINT, Los Alamos National Lab

Authors

  • La Moyne Mix

    • Los Alamos National Laboratory
    • CINT, Los Alamos National Lab

  • Dibyajyoti Ghosh

    • Los Alamos National Laboratory
    • CINT, Los Alamos National Lab

  • Jeremy Tisdale

    • CINT, Los Alamos National Lab

  • Min Cheol Lee

    • Los Alamos National Laboratory
    • CINT, Los Alamos National Lab

  • Ken ONeal

    • Los Alamos National Laboratory
    • Department of Chemistry, University of Tennessee
    • CINT, Los Alamos National Lab

  • Nicholas Sirica

    • Los Alamos National Laboratory
    • CINT, Los Alamos National Lab

  • Amanda Neukirch

    • CINT, Los Alamos National Lab
    • Los Alamos National Laboratory

  • Wanyi Nie wanyi@lanl.gov

    • CINT, Los Alamos National Lab

  • Antoinette Taylor

    • Los Alamos National Laboratory
    • Los Alamos Natl Lab
    • CINT, Los Alamos National Lab

  • Rohit P Prasankumar

    • Los Alamos National Laboratory
    • CINT, Los Alamos National Lab
    • Center for Integrated Nanotechnologies, Los Alamos National Laboratory

  • Sergei Tretiak

    • Los Alamos National Laboratory
    • Theoretical Division and Center for Integrated Nanotechnologies, Los Alamos National Laboratory
    • CINT, Los Alamos National Lab

  • Dmitry Yarotski

    • Los Alamos National Laboratory
    • CINT, Los Alamos National Lab
    • Department of Physics, Massachusetts Institute of Technology
    • Center for Integrated Nanotechnologies, Los Alamos National Laboratory