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Updated: Sep 30, 2025

High Resolution Phonon-assisted Quasi-resonance Fluorescence Spectroscopy
Published on: June 28, 2016
Measuring Exciton Fine-Structure in Randomly Oriented Perovskite Nanocrystal Ensembles Using Nonlinear Optical
1Condensed Matter Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, 22761 Hamburg, Germany.
Abstract:
Lead halide perovskite nanocrystals (PNCs) exhibit unique optoelectronic properties, many of which originate from a purported bright-triplet exciton fine-structure. A major impediment to measuring this fine-structure is inhomogeneous spectral broadening, which has limited most experimental studies to single-nanocrystal spectroscopies. It is shown here that the linearly polarized single-particle selection rules in PNCs are preserved in nonlinear spectroscopies of randomly oriented ensembles. Simulations incorporating rotational averaging demonstrate that techniques such as transient absorption and two-dimensional coherent spectroscopy are capable of resolving exciton fine-structure in PNCs, even in the presence of inhomogeneous broadening and orientation disorder.
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