TY - JOUR
T1 - In-situ observation of trapped carriers in organic metal halide perovskite films with ultra-fast temporal and ultra-high energetic resolutions
AU - Kobbekaduwa, Kanishka
AU - Shrestha, Shreetu
AU - Adhikari, Pan
AU - Liu, Exian
AU - Coleman, Lawrence
AU - Zhang, Jianbing
AU - Shi, Ying
AU - ZHOU, Yuanyuan
AU - Bekenstein, Yehonadav
AU - Yan, Feng
AU - Rao, Apparao M.
AU - Tsai, Hsinhan
AU - Beard, Matthew C.
AU - Nie, Wanyi
AU - Gao, Jianbo
N1 - Funding Information:
K.K., P.A., and J.G. acknowledge the support from the South Carolina Research Authority (SCRA) and start-up fund from Clemson University. S.S., H.T., and W.N. acknowledge 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 by Los Alamos National Laboratory (Contract 89233218CNA000001) and Sandia National Laboratories (Contract DE-NA-0003525). W.N. acknowledges Los Alamos National Laboratory’s LDRD program for support. We also wish to thank Russell Reynolds, Barrett Barker, and Michael Denz at Clemson University for their instrumental support.
PY - 2021/3/12
Y1 - 2021/3/12
N2 - We in-situ observe the ultrafast dynamics of trapped carriers in organic methyl ammonium lead halide perovskite thin films by ultrafast photocurrent spectroscopy with a sub-25 picosecond time resolution. Upon ultrafast laser excitation, trapped carriers follow a phonon assisted tunneling mechanism and a hopping transport mechanism along ultra-shallow to shallow trap states ranging from 1.72–11.51 millielectronvolts and is demonstrated by time-dependent and independent activation energies. Using temperature as an energetic ruler, we map trap states with ultra-high energy resolution down to < 0.01 millielectronvolt. In addition to carrier mobility of ~4 cm2V−1s−1 and lifetime of ~1 nanosecond, we validate the above transport mechanisms by highlighting trap state dynamics, including trapping rates, de-trapping rates and trap properties, such as trap density, trap levels, and capture-cross sections. In this work we establish a foundation for trap dynamics in high defect-tolerant perovskites with ultra-fast temporal and ultra-high energetic resolution.
AB - We in-situ observe the ultrafast dynamics of trapped carriers in organic methyl ammonium lead halide perovskite thin films by ultrafast photocurrent spectroscopy with a sub-25 picosecond time resolution. Upon ultrafast laser excitation, trapped carriers follow a phonon assisted tunneling mechanism and a hopping transport mechanism along ultra-shallow to shallow trap states ranging from 1.72–11.51 millielectronvolts and is demonstrated by time-dependent and independent activation energies. Using temperature as an energetic ruler, we map trap states with ultra-high energy resolution down to < 0.01 millielectronvolt. In addition to carrier mobility of ~4 cm2V−1s−1 and lifetime of ~1 nanosecond, we validate the above transport mechanisms by highlighting trap state dynamics, including trapping rates, de-trapping rates and trap properties, such as trap density, trap levels, and capture-cross sections. In this work we establish a foundation for trap dynamics in high defect-tolerant perovskites with ultra-fast temporal and ultra-high energetic resolution.
UR - http://www.scopus.com/inward/record.url?scp=85102385971&partnerID=8YFLogxK
U2 - 10.1038/s41467-021-21946-2
DO - 10.1038/s41467-021-21946-2
M3 - Journal article
C2 - 33712623
AN - SCOPUS:85102385971
SN - 2041-1723
VL - 12
JO - Nature Communications
JF - Nature Communications
M1 - 1636
ER -