Second harmonic generation as a probe of broken mirror symmetry
Abstract
The notion of spontaneous symmetry breaking has been used to describe phase transitions in a variety of physical systems. In crystalline solids, the breaking of certain symmetries, such as mirror symmetry, is difficult to detect unambiguously. Using 1T−TaS₂, we demonstrate here that rotational-anisotropy second harmonic generation (RA-SHG) is not only a sensitive technique for the detection of broken mirror symmetry, but also that it can differentiate between mirror symmetry-broken structures of opposite planar chirality. We also show that our analysis is applicable to a wide class of different materials with mirror symmetry-breaking transitions. Lastly, we find evidence for bulk mirror symmetry-breaking in the incommensurate charge density wave phase of 1T−TaS₂. Our results pave the way for RA-SHG to probe candidate materials where broken mirror symmetry may play a pivotal role.
Copyright and License
© 2020 American Physical Society.
Acknowledgement
We would like to thank A. Po and L. Fu for helpful discussions regarding this work.
Funding
This work was supported by the Gordon and Betty Moore Foundation's EPiQS Initiative Grant No. GBMF4540 to N.G. (data analysis and manuscript writing) and Grant No. GBMF3848 to J.G.C. (instrumentation), Shell through the MIT Energy Initiative (experimental setup and material development), and through DARPA DSO under DRINQS program Grant No. D18AC00014 (sample growth and data taking). L.Y. acknowledges support by the STC Center for Integrated Quantum Materials, NSF Grant No. DMR-1231319 and by the Tsinghua Education Foundation. B.G. gratefully acknowledges the German Academic Exchange Service (DAAD) for supporting his research stay with a fellowship.
Attached Files
https://journals.aps.org/prb/supplemental/10.1103/PhysRevB.101.241106/NCtas2sup.pdf First, a formal description of the effect of mirror reflection on the RA-SHG signal from 1T-TaS2.
Then, elaboration on the symmetry arguments used in the main text to argue that the sample bulk breaks mirror symmetry.
Includes a table outlining how to detect broken mirror symmetry in a general material with RA-SHG.
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Additional details
- ISSN
- 2469-9969
- Gordon and Betty Moore Foundation
- GBMF4540
- Gordon and Betty Moore Foundation
- GBMF3848
- Defense Advanced Research Projects Agency
- D18AC00014
- National Science Foundation
- DMR-1231319
- German Academic Exchange Service
- Available
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2020-06-08Published online