Perturbation facilitated two-color four-wave-mixing spectroscopy of C3

Perturbation-facilitated two-color resonant four-wave-mixing spectroscopy is realized to access the (dark) triplet manifold of the C3 molecule from the singlet X̃(1)Σg (+) ground state. The inherent nonlinear signal dependence and coherence of the technique result in a favorable detection of the excited triplet states of interest. The observation of a newly found (3)Δu electronic state is achieved by a two-step excitation via "gate-way" levels (i.e., singlet-triplet mixed levels). Additionally, by fixing the probe laser on a transition exhibiting mainly triplet-triplet character and scanning the pump laser, we demonstrate an effective spin-filtering in a four-wave mixing measurement where only transitions to the perturber (3)Σu(-) state appear exclusively in an otherwise congested spectral range of the Comet band. Ab initio calculations of excited triplet states complement our analysis with the electronic assignment of the observed resonances.