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 1$T$-TaS${}_2$, 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 1$T$-TaS${}_2$. Our results pave the way for RA-SHG to probe candidate materials where broken mirror symmetry may play a pivotal role.

arXiv comment13 pages, 10 figures. Edited (v2) to include Bilal Gökce in the authors list who was mistakenly excluded. Edited again (v3) to incorporate modifications recommended by referees. Replaced (v4) with version published in Physical Review B

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Cited by in corpus (11)

• Visualization of Chiral Electronic Structure and Anomalous Optical Response in a Material with Chiral Charge Density Waves
• Electrical switching of ferro-rotational order in nano-thick 1T-TaS${}_2$ crystals
• Observation of giant surface second harmonic generation coupled to nematic orders in the van der Waals antiferromagnet FePS${}_3$
• Polarization-Resolved Extreme Ultraviolet Second Harmonic Generation from LiNbO${}_3$
• Electric quadrupole second harmonic generation revealing dual magnetic orders in a magnetic Weyl semimetal
• Phase shifts, band geometry and responses in triple-Q charge and spin density waves
• A compact and stable incidence-plane-rotating second harmonics detector
• Dynamic phase transition into a mixed-CDW state in 1$T$-TaS${}_2$ via a thermal quench
• Light-induced reorientation transition in an antiferromagnetic semiconductor
• Automated Polarization Rotation for Multi-Axis Rotational-Anisotropy Second Harmonic Generation Experiments
• A versatile setup for symmetry-resolved ultrafast dynamics of quantum materials