From $\langle n \rangle$ to $n$: Separating multi-particle dynamics by intensity cycling

Abstract

We address the interpretation of transient spectroscopy signals proportional to average excitation number in terms of discrete number of excitations. Building on our recent intensity cycling approach, we derive a general scheme to isolate multi-particle dynamics from any transient signal under minimal assumptions. The key result is a general formula expressing the extracted nonlinear signal terms by multi-excitation propagators. We demonstrate the approach on exciton transport and annihilation in organic nanoparticles, and carrier recombination in silicon nanocrystals.