Journal
NATURE PHOTONICS
Volume 16, Issue 9, Pages 620-+Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41566-022-01050-7
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Funding
- US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division through the AMOS program
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- Humboldt Fellowship
- W. M. Keck Foundation
- Stanford University
- Swiss National Science Foundation (SNSF) [P2EZP2_184255, P400P2_194343]
- National Science Foundation [DMR2004125]
- Department of Energy, Office of Basic Energy Sciences, Division of Materials Science and Engineering
- MURI [W911NF2020166]
- Swiss National Science Foundation (SNF) [P2EZP2_184255, P400P2_194343] Funding Source: Swiss National Science Foundation (SNF)
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Researchers have found that circularly polarized laser-field-driven high-harmonic generation is highly sensitive to the non-trivial and trivial topological phases in topological insulators. By chemically reducing the spin-orbit interaction strength, the phase transition between non-trivial and trivial topological states can be achieved. This purely optical method offers sensitivity to the electronic structure of the material and is compatible with a wide range of samples and sample environments.
The prediction and realization of topological insulators have sparked great interest in experimental approaches to the classification of materials(1-3). 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(4). 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(5). The phase transition is chemically initiated by reducing the spin-orbit interaction strength through the substitution of bismuth with indium atoms(6,7). 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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