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Title: Effect of wavefunction delocalization on shift current generation

Abstract

We derive upper bounds on the magnitude of shift photocurrent generation of materials in two limiting cases: the flat-band limit of almost-isolated systems such as molecular crystals, and the wide-band limit of one-dimensional or quasi-one-dimensional materials such as ferroelectric polymers or other materials with chain-like motifs. These bounds relate the magnitudes of the shift current bulk photovoltaic effect to materials parameters. In both cases, we find that ratio of electron hopping amplitudes to the band gap plays a vital role in maximizing the amount of nonlinear response. Furthermore, by using the Wannier function formalism, we quantify the effect of long-range hopping amplitudes, showing how delocalization of electronic states gives rise to larger photocurrents. These results inform the design and selection of new materials for large shift current generation.

Authors:
ORCiD logo [1]; ORCiD logo [2]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  2. Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1542288
DOE Contract Number:  
AC02-05CH11231; FG02-07ER46431
Resource Type:
Journal Article
Journal Name:
Journal of Physics. Condensed Matter
Additional Journal Information:
Journal Volume: 31; Journal Issue: 8; Journal ID: ISSN 0953-8984
Country of Publication:
United States
Language:
English

Citation Formats

Tan, Liang Z., and Rappe, Andrew M. Effect of wavefunction delocalization on shift current generation. United States: N. p., 2019. Web. doi:10.1088/1361-648X/aaf74b.
Tan, Liang Z., & Rappe, Andrew M. Effect of wavefunction delocalization on shift current generation. United States. doi:10.1088/1361-648X/aaf74b.
Tan, Liang Z., and Rappe, Andrew M. Tue . "Effect of wavefunction delocalization on shift current generation". United States. doi:10.1088/1361-648X/aaf74b.
@article{osti_1542288,
title = {Effect of wavefunction delocalization on shift current generation},
author = {Tan, Liang Z. and Rappe, Andrew M.},
abstractNote = {We derive upper bounds on the magnitude of shift photocurrent generation of materials in two limiting cases: the flat-band limit of almost-isolated systems such as molecular crystals, and the wide-band limit of one-dimensional or quasi-one-dimensional materials such as ferroelectric polymers or other materials with chain-like motifs. These bounds relate the magnitudes of the shift current bulk photovoltaic effect to materials parameters. In both cases, we find that ratio of electron hopping amplitudes to the band gap plays a vital role in maximizing the amount of nonlinear response. Furthermore, by using the Wannier function formalism, we quantify the effect of long-range hopping amplitudes, showing how delocalization of electronic states gives rise to larger photocurrents. These results inform the design and selection of new materials for large shift current generation.},
doi = {10.1088/1361-648X/aaf74b},
journal = {Journal of Physics. Condensed Matter},
issn = {0953-8984},
number = 8,
volume = 31,
place = {United States},
year = {2019},
month = {1}
}