Multidimensional phase-sensitive single-molecule spectroscopy with time-and-frequency-gated fluorescence detection

Abstract

($n$ $+$ 1)-dimensional gated fluorescence signals induced by $n$ impulsive pulses are calculated using a superoperator formalism. The signals are given by a time-and-frequency convolution of a bare signal, expressed in terms of multipoint dipole correlation functions, with a gating spectrogram. Different groups of quantum pathways can be separated by their variation with the phases of the pulses (phase cycling), as is commonly done in nuclear magnetic resonance. Comparison is made with heterodyne-detected coherent signals.