Extreme Ultraviolet Second Harmonic Generation Spectroscopy in a Polar Metal

Emma Berger; Sasawat Jamnuch; Can B Uzundal; Clarisse Woodahl; Hari Padmanabhan; Angelique Amado; Paul Manset; Yasuyuki Hirata; Yuya Kubota; Shigeki Owada; Kensuke Tono; Makina Yabashi; Cuixiang Wang; Youguo Shi; Venkatraman Gopalan; Craig P Schwartz; Walter S Drisdell; Iwao Matsuda; John W Freeland; Tod A Pascal; Michael Zuerch

doi:10.1021/acs.nanolett.1c01502

Extreme Ultraviolet Second Harmonic Generation Spectroscopy in a Polar Metal

Nano Lett. 2021 Jul 28;21(14):6095-6101. doi: 10.1021/acs.nanolett.1c01502. Epub 2021 Jul 15.

Authors

Emma Berger^{1

2}, Sasawat Jamnuch³, Can B Uzundal^{1

2}, Clarisse Woodahl⁴, Hari Padmanabhan⁵, Angelique Amado^{1

2}, Paul Manset⁶, Yasuyuki Hirata⁷, Yuya Kubota^{8

9}, Shigeki Owada^{8

9}, Kensuke Tono^{8

9}, Makina Yabashi^{8

9}, Cuixiang Wang¹⁰, Youguo Shi¹⁰, Venkatraman Gopalan⁵, Craig P Schwartz¹¹, Walter S Drisdell^{11

12}, Iwao Matsuda^{13

14}, John W Freeland¹⁵, Tod A Pascal^{3

16

17}, Michael Zuerch^{1

2

18

19}

Affiliations

¹ Department of Chemistry, University of California, Berkeley, California 94720, United States.
² Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
³ ATLAS Materials Science Laboratory, Department of Nano Engineering and Chemical Engineering, University of California-San Diego, La Jolla, California 92023, United States.
⁴ University of Florida, Gainesville, Florida 32611, United States.
⁵ Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16801, United States.
⁶ Ecole Normale Supérieure - PSL, Paris, France.
⁷ National Defense Academy of Japan, Yokosuka, Kanagawa 239-8686, Japan.
⁸ RIKEN SPring-8 Center, Sayo, Hyogo 679-5148, Japan.
⁹ Japan Synchrotron Radiation Research Institute (JASRI), Sayo, Hyogo 679-5198, Japan.
¹⁰ Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
¹¹ Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
¹² Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
¹³ Institute for Solid State Physics, The University of Tokyo, Kashiwa, Chiba 277-8581, Japan.
¹⁴ Trans-scale Quantum Science Institute, The University of Tokyo, Bunkyo-ku, Tokyo 113-0033, Japan.
¹⁵ X-ray Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States.
¹⁶ Materials Science and Engineering, University of California-San Diego, La Jolla, California 92023, United States.
¹⁷ Sustainable Power and Energy Center, University of California-San Diego, La Jolla, California 92023, United States.
¹⁸ Fritz Haber Institute of the Max Planck Society, 14195 Berlin, Germany.
¹⁹ Friedrich Schiller University, 07743 Jena, Germany.

Abstract

The coexistence of ferroelectricity and metallicity seems paradoxical, since the itinerant electrons in metals should screen the long-range dipole interactions necessary for dipole ordering. The recent discovery of the polar metal LiOsO₃ was therefore surprising [as discussed earlier in Y. Shi et al., Nat. Mater. 2013, 12, 1024]. It is thought that the coordination preferences of the Li play a key role in stabilizing the LiOsO₃ polar metal phase, but an investigation from the combined viewpoints of core-state specificity and symmetry has yet to be done. Here, we apply the novel technique of extreme ultraviolet second harmonic generation (XUV-SHG) and find a sensitivity to the broken inversion symmetry in the polar metal phase of LiOsO₃ with an enhanced feature above the Li K-edge that reflects the degree of Li atom displacement as corroborated by density functional theory calculations. These results pave the way for time-resolved probing of symmetry-breaking structural phase transitions on femtosecond time scales with element specificity.

Keywords: X-ray nonlinear spectroscopy; materials science; polar metal; second harmonic generation.

Publication types

Research Support, Non-U.S. Gov't
Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

Metals
Second Harmonic Generation Microscopy*
Spectrum Analysis

Substances

Metals