Robust valley-polarized excitonic Mott states and doublons enabled by stacking-controlled moir\'e geometry

TL;DR

This paper demonstrates that stacking-controlled moiré geometry in atomically-thin heterostructures enhances intersite exciton interactions, stabilizing long-lived, valley-polarized Mott states and doublons against dissipation at elevated temperatures.

Contribution

It introduces a method to stabilize excitonic Mott states by engineering intersite interactions through moiré geometry in 2D heterostructures.

Findings

Enhanced intersite exciton repulsion V_{xx} by a factor of two in H-stacked WSe2/WS2.

Long-lived valley-polarized Mott state persists for ~12 ns up to 50 K.

Valley-polarized doublons have fourfold longer lifetimes than in R-stacks.

Abstract

Atomically-thin moir\'e superlattices offer an optically accessible platform for interacting bosons, where strong onsite repulsion $U_{xx}$ suppresses double occupancy and supports excitonic Mott states at unit filling. However, moir\'e confinement also enhances phonon- and disorder-assisted relaxation, challenging the robustness of these correlated states under dissipation. Here we show that strengthening the intersite exciton repulsion $V_{xx}$ between neighboring moir\'e cells offers a distinct route to stabilizing unit-filling excitonic Mott states. In H-stacked WSe2/WS2, moir\'e confinement endows interlayer excitons with an out-of-plane dipole and a pronounced in-plane quadrupolar charge distribution. Helicity-resolved transient photoluminescence, supported by first-principles-informed modelling, reveals that this quadrupolar geometry increases $V_{xx}$ at unit filling by at least a factor of two relative to the dipolar R-stacked excitons. Despite a slight reduction in $U_{xx}$, the enhanced $V_{xx}$ yields a long-lived, valley-polarized excitonic Mott state at unit filling that persists for ~12 ns - more than twice as long as in R-stacks - and remains robust up to ~50 K. Beyond unit filling, the same geometry supports valley-polarized doublons with fourfold longer lifetimes than in R-stacks. These results establish moir\'e-geometric control of intersite interactions as a route to stabilizing excitonic Mott states and doublons against dissipation in solids.