Revealing subterahertz atomic vibrations in quantum paraelectrics by surface-sensitive spintronic terahertz spectroscopy

Chu, Zhaodong; Yang, Junyi; Li, Yan; Hwangbo, Kyle; Wen, Jianguo; Bielinski, Ashley R.; Zhang, Qi; Martinson, Alex B. F.; Hruszkewycz, Stephan O.; Fong, Dillon D.; Xu, Xiaodong; Norman, Michael R.; Bhattacharya, Anand; Wen, Haidan

doi:10.1126/sciadv.ads8601

Revealing subterahertz atomic vibrations in quantum paraelectrics by surface-sensitive spintronic terahertz spectroscopy

Journal Article · Fri Nov 29 00:00:00 EST 2024 · Science Advances

DOI:https://doi.org/10.1126/sciadv.ads8601· OSTI ID:2997154

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Argonne National Laboratory (ANL), Argonne, IL (United States)
Univ. of Washington, Seattle, WA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Understanding surface collective dynamics in quantum materials is crucial for advancing quantum technologies. For example, surface phonon modes in quantum paraelectrics are thought to be essential in facilitating interfacial superconductivity. However, detecting these modes, especially below 1 terahertz, is challenging because of limited sampling volumes and the need for high spectroscopic resolution. Here, we report surface soft transverse optical (TO1) phonon dynamics in KTaO₃ and SrTiO₃ by surface-sensitive spintronic terahertz spectroscopy that can sense the collective modes only a few nanometers deep from the surface. In KTaO₃, the TO1 mode softens and sharpens with decreasing temperature, leveling off at 0.7 terahertz. In contrast, this mode in SrTiO₃ broadens substantially below the quantum paraelectric crossover and coincides with the hardening of a sub–milli–electron volt phonon mode related to the antiferrodistortive transition. These observations that deviate from their bulk properties may have implications for interfacial superconductivity and ferroelectricity. The developed technique opens opportunities for sensing low-energy surface collective excitations.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; SC0012509

OSTI ID:: 2997154

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 48 Vol. 10; ISSN 2375-2548

Publisher:: American Association for the Advancement of Science (AAAS)Copyright Statement

Country of Publication:: United States

Language:: English

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