Coherent multi-dimensional widefield microscopy

Abstract

Understanding how electronic excitations evolve across space and time is essential for revealing the microscopic processes underlying quantum and optoelectronic materials. However, existing approaches cannot simultaneously resolve ultrafast coherent dynamics with microscopic spatial information: pump-probe microscopy lacks access to quantum coherence, while two-dimensional electronic spectroscopy (2DES) requires slow point-by-point scanning for spatial resolution. Here we introduce a widefield two-dimensional electronic spectroscopy microscope (2DESM) combining multidimensional coherent spectroscopy with widefield imaging, enabling simultaneous femtosecond temporal and micrometer spatial resolution across a broadband spectral range. Applying 2DESM to hBN-encapsulated WSe2, we directly visualize spatial variations in exciton coherence and relaxation associated with the local environment, establishing 2DESM as a powerful platform for probing many-body interactions, energy transport, and structure-function relationships in low-dimensional materials and devices.