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Spin-orbit-enhanced magnetic surface second-harmonic generation in Sr₂IrO₄

Seyler, K. L. and de la Torre, A. and Porter, Z. and Zoghlin, E. and Polski, R. and Nguyen, M. and Nadj-Perge, S. and Wilson, S. D. and Hsieh, D. (2020) Spin-orbit-enhanced magnetic surface second-harmonic generation in Sr₂IrO₄. Physical Review B, 102 (20). Art. No. 201113(R). ISSN 2469-9950. doi:10.1103/physrevb.102.201113.

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An anomalous optical second-harmonic generation (SHG) signal was previously reported in Sr₂IrO₄ and attributed to a hidden odd-parity bulk magnetic state. Here we investigate the origin of this SHG signal using a combination of bulk magnetic susceptibility, magnetic-field-dependent SHG rotational anisotropy, and overlapping wide-field SHG imaging and atomic force microscopy measurements. We find that the anomalous SHG signal exhibits a twofold rotational symmetry as a function of in-plane magnetic field orientation that is associated with a crystallographic distortion. We also show a change in SHG signal across step edges that tracks the bulk antiferromagnetic stacking pattern. While we do not rule out the existence of hidden order in Sr₂IrO₄, our results altogether show that the anomalous SHG signal in parent Sr₂IrO₄ originates instead from a surface-magnetization-induced electric-dipole process that is enhanced by strong spin-orbit coupling.

Item Type:Article
Related URLs:
URLURL TypeDescription Information Paper
Seyler, K. L.0000-0003-1553-4518
Zoghlin, E.0000-0002-8160-584X
Polski, R.0000-0003-0887-8099
Nadj-Perge, S.0000-0002-2916-360X
Hsieh, D.0000-0002-0812-955X
Alternate Title:Spin-orbit-enhanced magnetic surface second-harmonic generation in Sr2IrO4
Additional Information:© 2020 American Physical Society. (Received 26 July 2020; revised 30 October 2020; accepted 2 November 2020; published 13 November 2020) We acknowledge helpful conversations with Gang Cao, Nicholas Laurita, Sergio Di Matteo, Mike Norman, Alon Ron, Chandra Varma, and Liuyan Zhao. This work is supported by an ARO PECASE award W911NF-17-1-0204. D.H. also acknowledges support for instrumentation from the David and Lucile Packard Foundation and from the Institute for Quantum Information and Matter (IQIM), an NSF Physics Frontiers Center (PHY-1733907). K.L.S. acknowledges a Caltech Prize Postdoctoral Fellowship. A.d.l.T. acknowledges support from the Swiss National Science Foundation through an Early Postdoc Mobility Fellowship (P2GEP2_165044). S.D.W., E.Z., and Z.P. acknowledge support from ARO Award No. W911NF-16-1-0361. R.P. acknowledges support from IQIM.
Group:Institute for Quantum Information and Matter
Funding AgencyGrant Number
Army Research Office (ARO)W911NF-17-1-0204
David and Lucile Packard FoundationUNSPECIFIED
Institute for Quantum Information and Matter (IQIM)UNSPECIFIED
Robert A. Millikan FellowshipUNSPECIFIED
Swiss National Science Foundation (SNSF)P2GEP2_165044
Army Research Office (ARO)W911NF-16-1-0361
Issue or Number:20
Record Number:CaltechAUTHORS:20201113-100152383
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:106666
Deposited By: George Porter
Deposited On:16 Nov 2020 15:13
Last Modified:03 Jan 2022 22:44

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