2The observation of chirality is ubiquitous in nature. Contrary to intuition, the population of opposite chiralities is surprisingly asymmetric at fundamental levels [1,2]. Examples range from parity violation in the subatomic weak force [1] to the homochirality in essential biomolecules [2]. The ability to achieve chiralityselective synthesis (chiral induction) is of great importance in stereochemistry, molecular biology and pharmacology [2]. In condensed matter physics, a crystalline electronic system is geometrically chiral when it lacks any mirror plane, space inversion center or roto-inversion axis [3]. Typically, the geometrical chirality is predefined by a material's chiral lattice structure, which is fixed upon the formation of the crystal. By contrast, a particularly unconventional scenario is the gyrotropic order [4][5][6][7][8], where chirality spontaneously emerges across a phase transition as the electron system breaks the relevant symmetries of an originally achiral lattice. Such a gyrotropic order, proposed as the quantum analogue of the cholesteric liquid crystals, has attracted significant interest [4][5][6][7][8][9][10][11][12][13][14][15][16][17]. However, to date, a clear observation and manipulation of the gyrotropic order remain challenging. We report the realization of optical chiral induction and the observation of a gyrotropically ordered phase in the transition-metal dichalcogenide semimetal 1T -TiSe 2 . We show that shining mid-infrared circularly polarized light near the critical temperature leads to the preferential formation of one chiral domain. As a result, we are able to observe an out-of-plane circular photogalvanic current, whose direction depends on the optical induction. Our study provides compelling evidence for the spontaneous emergence of chirality in the correlated semimetal TiSe 2 [18]. Such chiral induction provides a new way of optical control over novel orders in quantum materials.In the presence of strong correlations, the behavior of electrons in a metal can signficantly deviate from a weakly-interacting Fermi gas, forming a wide range of complex, broken symmetry phases [19]. Recent theoretical works have highlighted their analogy with classical liquids [19], where a rich set of liquid crystalline phases that exhibit varying degrees of symmetry breaking and transport properties have been observed. A well-studied case is the nematic order [19][20][21], i.e., the spontaneous emergence of rotational anisotropy. In classical liquids, this is known as the nematic liquid crystal, whereas in quantum materials, it has recently been observed in quantum Hall systems, ruthenates, high temperature supercon-3 ductors [19], heavy-fermion superconductors [20], and correlated metallic pyrochlores [21].Another fascinating case is the gyrotropic order, i.e., the spontaneous emergence of geometrical chirality. In classical liquids, this is known as the cholesteric liquid crystal. In quantum materials, despite fundamental interest [4][5][6][7][8][9][10][11][12][13][14][15][16], a clear ...