Coupling of electronic transition to ferroelectric order in a 2D semiconductor

Huang, Chun-Ying; Chica, Daniel G.; Cui, Zhi-Hao; Handa, Taketo; Thinel, Morgan; Olsen, Nicholas; Liu, Yufeng; Ziebel, Michael E.; He, Guiying; Shao, Yinming; Occhialini, Connor A.; Pelliciari, Jonathan; Basov, Dmitri N.; Sfeir, Matthew; Pasupathy, Abhay; Bisogni, Valentina; Reichman, David R.; Roy, Xavier; Zhu, Xiaoyang

doi:10.1038/s41467-025-57061-9

Title: Coupling of electronic transition to ferroelectric order in a 2D semiconductor

Journal Article · Sun Feb 23 00:00:00 UTC 2025 · Nature Communications

DOI: https://doi.org/10.1038/s41467-025-57061-9 · OSTI ID:2529404

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Columbia Univ., New York, NY (United States)
City Univ. of New York (CUNY), NY (United States)
Columbia Univ., New York, NY (United States); Pennsylvania State Univ., University Park, PA (United States)
Columbia Univ., New York, NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

A ferroelectric material often exhibits a soft transverse optical (TO) phonon mode which governs its phase transition. Charge coupling to this ferroelectric soft mode may further mediate emergent physical properties, including superconductivity and defect tolerance in semiconductors. However, direct experimental evidence for such coupling is scarce. Here we show that a photogenerated coherent phonon couples strongly to the electronic transition above the bandgap in the van der Waals (vdW) two-dimensional (2D) ferroelectric semiconductor NbOI₂. Using terahertz time-domain spectroscopy and first-principles calculations, we identify this mode as the TO phonon responsible for ferroelectric order. This exclusive coupling occurs only with the above-gap electronic transition and is absent in the valence band as revealed by resonant inelastic X-ray scattering. Our findings suggest a new role of the soft TO phonon mode in electronic and optical properties of ferroelectric semiconductors.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704; SC0019443

OSTI ID:: 2529404

Report Number(s):: BNL--227671-2025-JAAM

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 16; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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