Nonlinear Photocurrent Spectroscopy and Polarization-Tunable Shift Current in the Layered Semiconductor CuScP2S6
Abstract
The class of layered metal thiophosphates and selenophosphates are emerging as promising candidates for non-linear photonic and optoelectronic applications. Here we report one-photon absorption (1PA) and two-photon absorption (2PA) induced photocurrents in CuScP2S6, establishing it as an optoelectronically-active non-centrosymmetric semiconductor. Spectrally-resolved 1PA and 2PA photoresponsivity paired with photoluminescence and differential reflectance measurements reveal a band gap of 2.35 eV, several higher energy interband transitions, and sub-band gap multiphoton excitonic transitions. Vertical graphite/CuScP2S6/graphite devices exhibit zero-bias photocurrent with a polarity controlled by both photon energy and optical polarization orientation within the ab-plane. This sign-dependence combined with a characteristic power-law transition from linear to square-root scaling are consistent with a shift-current origin to this bulk photovoltaic effect (BPVE). These findings establish CuScP2S6 as a multi-functional platform for polarization-sensitive non-linear optoelectronics.
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BibTeX
@misc{blackston2026nonlinear,
title = {{Nonlinear Photocurrent Spectroscopy and Polarization-Tunable Shift Current in the Layered Semiconductor $\mathrmCuScP_2S_6$}},
author = {Alexander M. Blackston and Md Kazi Rokunuzzaman and Ryan P. Siebenaller and Shashu Tomar and Enam Chowdhury and Michael A. Susner and Roberto C. Myers},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.16577},
eprint = {2609.16577},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.16577},
}
RIS
TY - UNPB
TI - Nonlinear Photocurrent Spectroscopy and Polarization-Tunable Shift Current in the Layered Semiconductor CuScP_2S_6
AU - Alexander M. Blackston
AU - Md Kazi Rokunuzzaman
AU - Ryan P. Siebenaller
AU - Shashu Tomar
AU - Enam Chowdhury
AU - Michael A. Susner
AU - Roberto C. Myers
PY - 2026
DA - 2026/09/15
PB - arXiv
DO - 10.48550/arxiv.2609.16577
UR - https://arxiv.org/abs/2609.16577
AB - The class of layered metal thiophosphates and selenophosphates are emerging as promising candidates for non-linear photonic and optoelectronic applications. Here we report one-photon absorption (1PA) and two-photon absorption (2PA) induced photocurrents in CuScP_2S_6, establishing it as an optoelectronically-active non-centrosymmetric semiconductor. Spectrally-resolved 1PA and 2PA photoresponsivity paired with photoluminescence and differential reflectance measurements reveal a band gap of 2.35 eV, several higher energy interband transitions, and sub-band gap multiphoton excitonic transitions. Vertical graphite/CuScP_2S_6/graphite devices exhibit zero-bias photocurrent with a polarity controlled by both photon energy and optical polarization orientation within the ab-plane. This sign-dependence combined with a characteristic power-law transition from linear to square-root scaling are consistent with a shift-current origin to this bulk photovoltaic effect (BPVE). These findings establish CuScP_2S_6 as a multi-functional platform for polarization-sensitive non-linear optoelectronics.
ER -