Probing weak dipole-dipole interaction using phase-modulated non-linear spectroscopy

Abstract

Phase-modulated non-linear spectroscopy with higher harmonic demodulation has recently been suggested to provide information on many-body excitations. In the present work we theoretically investigate the application of this method to infer the interaction strength between two particles that interact via weak dipole-dipole interaction. To this end we use full numerical solution of the Schrödinger equation with time-dependent pulses. For interpretation purpose we also derive analytical expressions in perturbation theory. We find one can detect dipole-dipole interaction via peak intensities (in contrast to line-shifts which typically are used in conventional spectroscopy). We provide a detailed study on the dependence of these intensities on the parameters of the laser pulse and the dipole-dipole interaction strength. Interestingly, we find that there is a phase between the first and second harmonic demodulated signal, whose value depends on the sign of the dipole-dipole interaction.

12 pages, 8 figures, Supporting information provided with the source files

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• Efficient isolation of multiphoton processes and detection of collective states in dilute samples
• Vibronic Lineshapes of PTCDA Oligomers in Helium Nanodroplets
• Phase-modulated electronic wave-packet interferometry reveals high resolution vibronic spectra of free Rb atoms and Rb*He molecules
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