Ultrafast Nanoscopy of High-Density Exciton Phases in WSe2

T. Siday, F. Sandner, S. Brem, M. Zizlsperger, R. Perea-Causin, F. Schiegl, S. Nerreter, M. Plankl, P. Merkl, F. Mooshammer, M.A. Huber, E. Malic and R. Huber

Nano Letters 22, 2561 (2022)
The density-driven transition of an exciton gas into an electron–hole plasma remains a compelling question in condensed matter physics. In two-dimensional transition metal dichalcogenides, strongly bound excitons can undergo this phase change after transient injection of electron–hole pairs. Unfortunately, unavoidable nanoscale inhomogeneity in these materials has impeded quantitative investigation into this elusive transition. Here, we demonstrate how ultrafast polarization nanoscopy can capture the Mott transition through the density-dependent recombination dynamics of electron–hole pairs within a WSe2 homobilayer. For increasing carrier density, an initial monomolecular recombination of optically dark excitons transitions continuously into a bimolecular recombination of an unbound electron–hole plasma above 7 × 1012 cm–2. We resolve how the Mott transition modulates over nanometer length scales, directly evidencing the strong inhomogeneity in stacked monolayers. Our results demonstrate how ultrafast polarization nanoscopy could unveil the interplay of strong electronic correlations and interlayer coupling within a diverse range of stacked and twisted two-dimensional materials.