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Terahertz emission spectroscopy of ultrafast exciton shift current in the noncentrosymmetric semiconductor CdS

Journal Article · · Physical Review. B
 [1];  [2];  [3];  [4];  [5];  [6];  [6];  [7];  [8]
  1. RIKEN Center for Emergent Matter Science (CEMS), Wako (Japan); 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)
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  5. RIKEN Center for Emergent Matter Science (CEMS), Wako (Japan); National Taiwan Univ., Taipei (Taiwan); National Center for Theoretical Sciences, Taipei (Taiwan)
  6. RIKEN Center for Emergent Matter Science (CEMS), Wako (Japan); Univ. of Tokyo (Japan)
  7. RIKEN Center for Emergent Matter Science (CEMS), Wako (Japan); Univ. of Tokyo (Japan); Univ. of Tokyo (Japan)
  8. RIKEN Center for Emergent Matter Science (CEMS), Wako (Japan); Japan Science and Technology Agency (JST), Kawaguchi (Japan). PRESTO; Univ. of Tokyo (Japan)
The charge-neutral exciton has been predicted to carry genuine photocurrent due to the geometric Berry phase of the electronic bands, if the inversion symmetry in a crystal is broken. Here we detect such exciton shift current in a prototypical polar semiconductor CdS by using terahertz emission spectroscopy. A distinct peak emerges in the photocurrent spectra at the energy of the exciton resonance, which is demonstrated to result from the distinct displacements of electrons and holes in real space within the excitons to produce a finite transient charge current at subpicosecond time scale. Our findings elucidate the Berry phase physics of the charge-neutral photoexcitations and also shed light on the novel energy harvesting mechanism by exciton generation.
Research Organization:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Organization:
Japan Science and Technology Agency (JST); Japan Society for the Promotion of Science (JSPS); USDOE Office of Science (SC)
Grant/Contract Number:
SC0018945
OSTI ID:
1852722
Journal Information:
Physical Review. B, Journal Name: Physical Review. B Journal Issue: 24 Vol. 103; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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