In 1T-TiSe2, left- and right-circularly polarized pump pulses suppress the CDW diffraction peak asymmetrically, with the asymmetry varying across momentum and reversing sign at a mosaic domain.
Breaking symmetry with light: photo-induced chirality in a non-chiral crystal
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abstract
Chirality is a pervasive form of symmetry that is intimately connected to the physical properties of solids, as well as the chemical and biological activity of molecular systems. However, its control with light is challenging, because inducing chirality in a non-chiral material requires that all mirrors and all roto-inversions be simultaneously broken. Electromagnetic fields exert only oscillatory forces that vanish on average, mostly leading to entropy increase that does not break symmetries, per se. Here, we show that chirality of either handedness can be generated in the non-chiral piezoelectric material BPO$_4$, in which two compensated sub-structures of opposite handedness coexist within the same unit cell. By resonantly driving either one of two orthogonal, doubly degenerate vibrational modes at Terahertz frequency, we rectify the lattice distortion and exert a displacive force onto the crystal. The staggered chirality is in this way uncompensated in either direction, inducing chiral structure with either handedness. The rotary power of the photo-induced phases is comparable to the static value of prototypical chiral alpha-quartz, limited by the strength of the pump laser pulse.
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Photo-induced Dynamics and Momentum Distribution of Chiral Charge Density Waves in 1T-TiSe$_{2}$
In 1T-TiSe2, left- and right-circularly polarized pump pulses suppress the CDW diffraction peak asymmetrically, with the asymmetry varying across momentum and reversing sign at a mosaic domain.