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Nonadiabaticity, i.e., the effect of mixing electronic states by nuclearmotion, is a central phenomenon in molecular science. The strongestnonadiabatic effects arise due to the presence of conical intersections ofelectronic energy surfaces. These intersections are abundant in polyatomicmolecules. Laser light can induce in a controlled manner new conicalintersections, called light-induced conical intersections, which lead to strongnonadiabatic effects similar to those of the natural conical intersections.These effects are, however, controllable and may even compete with those of thenatural intersections. In this work we show that the standard low-energyvibrational spectrum of the electronic ground state can change dramatically byinducing nonadiabaticity via a light-induced conical intersection. This genericeffect is demonstrated for an explicit example by full-dimensional high-levelquantum calculations using a pump-probe scheme with a moderate-intensity pumplaser and a weak probe laser.

Striking light-induced nonadiabatic fingerprint in the low-energy vibronic spectra of polyatomic molecules