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Triple sum-frequency (TSF) spectroscopy is a recently-developed methodologythat enables collection of multidimensional spectra by resonantly excitingmultiple quantum coherences of vibrational and electronic states. This workreports the first application of TSF to the electronic states ofsemiconductors. Two independently tunable ultrafast pulses excite the A, B, andC features of a MoS2 thin film. The measured TSF spectrum differs markedly fromabsorption and second harmonic generation spectra. The differences arisebecause of the relative importance of transition moments and the joint densityof states. We develop a simple model and globally fit the absorption andharmonic generation spectra to extract the joint density of states and thetransition moments from these spectra. Our results validate previousassignments of the C feature to a large joint density of states created by bandnesting.

Multidimensional Triple Sum-Frequency Spectroscopy of MoS2 and Comparisons with Absorption and Second Harmonic Generation Spectroscopies