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High-pressure control of optical nonlinearity in the polar Weyl semimetal TaAs

Li, Chen and Li, Xiang and Deshpande, T. and Li, Xinwei and Nair, N. and Analytis, J. G. and Silevitch, D. M. and Rosenbaum, T. F. and Hsieh, D. (2022) High-pressure control of optical nonlinearity in the polar Weyl semimetal TaAs. Physical Review B, 106 (1). Art. No. 014101. ISSN 2469-9950. doi:10.1103/physrevb.106.014101.

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The transition metal monopnictide family of Weyl semimetals recently has been shown to exhibit anomalously strong second-order optical nonlinearity, which is theoretically attributed to a highly asymmetric polarization distribution induced by their polar structure. We experimentally test this hypothesis by measuring optical second harmonic generation (SHG) from TaAs across a pressure-tuned polar-to-nonpolar structural phase transition. Despite the high-pressure structure remaining noncentrosymmetric, the SHG yield is reduced by more than 60% by 20 GPa as compared to the ambient pressure value. By examining the pressure dependence of distinct groups of SHG susceptibility tensor elements, we find that the yield is primarily controlled by a single element that governs the response along the polar axis. Our results confirm a connection between the polar axis and the giant optical nonlinearity of Weyl semimetals and demonstrate pressure as a means to tune this effect in situ.

Item Type:Article
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URLURL TypeDescription Information Paper
Li, Chen0000-0001-6750-5925
Deshpande, T.0000-0003-0326-1372
Li, Xinwei0000-0003-0555-2624
Analytis, J. G.0000-0002-7657-7688
Silevitch, D. M.0000-0002-6347-3513
Hsieh, D.0000-0002-0812-955X
Additional Information:© 2022 American Physical Society. (Received 8 April 2022; revised 18 June 2022; accepted 22 June 2022; published 5 July 2022) We thank D. Torchinsky, G. Rossman, J. Jackson, and L. Wu for helpful discussions. High-pressure optical second harmonic generation measurements, as well as construction of the instrument, were supported by the U.S. Department of Energy under Grant No. DE SC0010533. T.F.R. acknowledges support from AFOSR Grant No. FA9550-20-1-0263. X.L. acknowledges support from an IQIM postdoctoral fellowship. Work by N.N. and J.G.A. was supported by the National Science Foundation under Grant No. 1905397.
Group:Institute for Quantum Information and Matter
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0010533
Air Force Office of Scientific Research (AFOSR)FA9550-20-1-0263
Institute for Quantum Information and Matter (IQIM)UNSPECIFIED
Issue or Number:1
Record Number:CaltechAUTHORS:20220705-671865000
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:115309
Deposited By: George Porter
Deposited On:08 Jul 2022 22:49
Last Modified:23 Dec 2022 20:50

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