Coherent nonlinear spectroscopy offers us a window into the system-bath interactions in materials. Specifically, the spectral lineshapes can reveal the nature and dynamics of the environmental fluctuations surrounding the system of interest. Here we will discuss how stochastic non-equilibrium exciton dynamics manifest in the peculiar lineshapes and how they provide mechanistic insights into the nature of exciton-phonon and exciton-exciton interactions in nanostructured derivatives of metal halide perovskites. Despite the success of such classical optical probes in unveiling the many-body physics in materials, we will elaborate on the ambiguities still present in the resultant photophysical models that stem primarily due to the high excitation intensities used in the measurements. We will also discuss alternative experimental methodologies based on quantum entangled photons, which may offer superior signal to noise ratio and thus enabling the measurement of many-body interactions at close to single photon excitation densities.
Non-geminate charge recombination is a significant source of carrier loss in organic photovoltaic systems. Recent
experiments by Rao, et al. (Nature, 2013 500, 435-439) suggest that the recombination of triplet charge-transfer
(3CT) states can be suppressed by careful control of the molecular order in the vicinity of the phase boundary
between donor and acceptor materials polymer/fullerene bulk-heterojunction devices. In short, recombination
of 3CT states is effectively suppressed when the fullerene phase exhibits a high degree of local order near the
interface. Here we report upon our theoretical model that connects energetic disorder, dimensionality, and wave
function localization to show that inhomogeneous broadening introduces strong coupling between the interfacial
3CT and nearby fullerene triplet excitons and can enhance the decay of these states in systems with higher
degrees of energetic disorder.
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