Spatiotemporal intensity-cycling microscopy unveils many-body interactions and correlated transport in van der Waals semiconductors.

Abstract

Spatiotemporal optical microscopies are powerful tools to image the propagation of energy carriers in materials, including electrons, excitons, magnons and polaritons, providing key functional metrics inaccessible to contact-based transport measurements. Nevertheless, these approaches do not distinguish single-particle from multi-particle quantum states, hindering the study of many-body correlations that underlie the complex phase diagrams at the heart of contemporary materials research. Here we extend a concept derived from multidimensional spectroscopy, called intensity cycling, to the spatiotemporal domain using transient scattering microscopy. We leverage this approach to selectively image single-particle and multi-particle transport in van der Waals semiconductors. We demonstrate a series of sought-after capabilities, including clean isolation of single-particle charge transport with high signal-to-noise ratio, spatiotemporal tracking of exciton-exciton annihilation, high-throughput mapping of dielectric disorder, and imaging the emergence of a polaronic Mott transition and correlated transport in a superatomic solid. This work delivers a precision tool capable of visualizing how many-body interactions shape material function.

Abstract as supplied by the indexing source. © the authors / publisher.