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Title: Spectral dynamics of shift current in ferroelectric semiconductor SbSI

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
 [1];  [2];  [3];  [4];  [5];  [6];  [7];  [8];  [8];  [8];  [2]
  1. RIKEN Center for Emergent Matter Science (CEMS), Wako (Japan); DOE/OSTI
  2. RIKEN Center for Emergent Matter Science (CEMS), Wako (Japan); Japan Science and Technology Agency (JST), Kawaguchi (Japan). PRESTO
  3. Japan Science and Technology Agency (JST), Kawaguchi (Japan). PRESTO; Univ. of Tokyo (Japan). Quantum Phase Electronics CEnter
  4. Univ. of Tokyo (Japan). Quantum Phase Electronics Center
  5. RIKEN Center for Emergent Matter Science (CEMS), Wako (Japan)
  6. Univ. of California, Berkeley, CA (United States)
  7. Max Planck Inst. for Chemical Physics of Solids, Dresden (Germany); Leibniz Inst. for Solid State and Materials Research, Dresden (Germany). Inst. for Theoretical Solid State Physics
  8. RIKEN Center for Emergent Matter Science (CEMS), Wako (Japan); Univ. of Tokyo (Japan). Quantum Phase Electronics Center

Photoexcitation in solids brings about transitions of electrons/holes between different electronic bands. If the solid lacks an inversion symmetry, these electronic transitions support spontaneous photocurrent due to the geometric phase of the constituting electronic bands: the Berry connection. This photocurrent, termed shift current, is expected to emerge on the timescale of primary photoexcitation process. We observe ultrafast evolution of the shift current in a prototypical ferroelectric semiconductor antimony sulfur iodide (SbSI) by detecting emitted terahertz electromagnetic waves. By sweeping the excitation photon energy across the bandgap, ultrafast electron dynamics as a source of terahertz emission abruptly changes its nature, reflecting a contribution of Berry connection on interband optical transition. The shift excitation carries a net charge flow and is followed by a swing over of the electron cloud on a subpicosecond timescale. Understanding these substantive characters of the shift current with the help of first-principles calculation will pave the way for its application to ultrafast sensors and solar cells.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC); Japan Society for the Promotion of Science (JSPS)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1625016
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 6 Vol. 116; ISSN 0027-8424
Publisher:
National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English

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Switchable magnetic bulk photovoltaic effect in the two-dimensional magnet CrI3 journal August 2019
Chiral terahertz wave emission from the Weyl semimetal TaAs journal February 2020
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Strong bulk photovoltaic effect in chiral crystals in the visible spectrum journal December 2019
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Chiral terahertz wave emission from the Weyl semimetal TaAs text January 2019
Strong bulk photovoltaic effect in chiral crystal in the visible spectrum text January 2019