In this presentation, I will describe recent advances in using ultrafast coherent multi-dimensional nonlinear optical microscopy to identify resonant electronic excitations in 2D metals. I will demonstrate that resonance matching at harmonic wavelengths results in a population inversion, which in turn saturates SHG transduction. Numerical modeling shows that internal energy transfer on sub-cycle timescales (< 2fs) mediates the population inversion. These effects are determined by atomic-level structure of the 2D metal.
High-order harmonic generation spectroscopy and imaging and were used to study energy transfer in 2D polar metal-graphene heterostructures. Using Fourier transform SHG microscopy, sub-cycle energy transfer between electronic states of crystalline 2D Ag monolayers was resolved. This rapid carrier transfer created a population inversion, which was reflected in depletion of perturbative time-domain SHG signals. In a second example, non-perturbative high harmonic generation was used to measure interfacial carrier transfer from a series of 2D metals (Ag, Ga, In, Pb) to graphene.
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