Probing topological phase transitions using high-harmonic generation

Heide, Christian; Kobayashi, Yuki; Baykusheva, Denitsa R.; Jain, Deepti; Sobota, Jonathan A.; Hashimoto, Makoto; Kirchmann, Patrick S.; Oh, Seongshik; Heinz, Tony F.; Reis, David A.; Ghimire, Shambhu

doi:10.1038/s41566-022-01050-7

Title: Probing topological phase transitions using high-harmonic generation

Journal Article · 18 August 2022 · Nature Photonics

DOI: https://doi.org/10.1038/s41566-022-01050-7 · OSTI ID:1886923

^[1];

^[2];

^[3]; Jain, Deepti ^[4];

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^[6]; Kirchmann, Patrick S. ^[5];

^[4]; Heinz, Tony F. ^[2]; Reis, David A. ^[2];

^[7]

SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stanford University, CA (United States); SLAC
SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stanford University, CA (United States)
Harvard University, Cambridge, MA (United States)
Rutgers University, Piscataway, NJ (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)

We report the prediction and realization of topological insulators have sparked great interest in experimental approaches to the classification of materials. The phase transition between non-trivial and trivial topological states is important, not only for basic materials science but also for next-generation technology, such as dissipation-free electronics. It is therefore crucial to develop advanced probes that are suitable for a wide range of samples and environments. Here we demonstrate that circularly polarized laser-field-driven high-harmonic generation is distinctly sensitive to the non-trivial and trivial topological phases in the prototypical three-dimensional topological insulator bismuth selenide. The phase transition is chemically initiated by reducing the spin–orbit interaction strength through the substitution of bismuth with indium atoms. We find strikingly different high-harmonic responses of trivial and non-trivial topological surface states that manifest themselves as a conversion efficiency and elliptical dichroism that depend both on the driving laser ellipticity and the crystal orientation. The origins of the anomalous high-harmonic response are corroborated by calculations using the semiconductor optical Bloch equations with pairs of surface and bulk bands. As a purely optical approach, this method offers sensitivity to the electronic structure of the material, including its nonlinear response, and is compatible with a wide range of samples and sample environments.

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Research Organization:: SLAC

Sponsoring Organization:: Humboldt Fellowship; Multidisciplinary University Research Initiative (MURI); National Science Foundation; Stanford University; Swiss National Science Foundation (SNSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; W. M. Keck Foundation

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1886923

Journal Information:: Nature Photonics, Journal Name: Nature Photonics Journal Issue: 9 Vol. 16; ISSN 1749-4885

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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