Hidden order revealed by light-driven Kerr rotation in centrosymmetric bulk WSe2

Single-layer semiconducting transition-metal dichalcogenides, lacking point inversion symmetry, provide an efficient platform for valleytronics, where the electronic, orbital, magnetic, valley, and lattice degrees of freedom can be selectively manipulated by using polarized light. This task is, however, thought to be impeded in parent bulk compounds where the point inversion symmetry is restored. Exploiting the underlying quantum physics in bulk materials is thus one of the biggest paradigmatic challenges. Here we show that a sizable optical Kerr rotation can be efficiently generated without breaking point-inversion symmetry in a wide energy range on ultrafast timescales in bulk WSe₂, by means of circularly-polarized light. We rationalize this finding as a result of the hidden spin/layer/orbital/valley order. The spectral analysis reveals distinct A-, B-, and C-exciton features, which we show to stem from a selective Pauli blocking effect on top of the hidden-order pseudospin order and of the spin Berry curvature. The Kerr response lifetime (<i>τ</i> ~ 500 fs), common to all the peaks, suggests that excitonic dynamics dominate over single-particle decay. The present report demonstrates that the hidden order at play in bulk centrosymmetric layered materials can stem out in macroscopical bulk features, opening the way for an effective exploitation of bulk WSe₂ in novel optoelectronic and orbitronics applications.