Abstract

Quadrupolar excitons in van der Waals heterostructures – quantum superpositions of anti-aligned dipolar excitons – offer a novel platform to explore exotic many-body physics, with applications to quantum sensing and photonic devices. Yet their internal structure, symmetry, and real-space localisation remain largely unknown. Here, we reveal the atomic-scale structure of quadrupolar excitons in twisted WSe₂/WS₂/WSe₂ trilayers by solving the Bethe–Salpeter equation within a large-scale atomistic framework. We discover that large atomic relaxations at small twist angles give rise to two distinct quadrupolar excitons trapped at moiré lattice sites, differing in the in-plane symmetry of the electron density about the hole: one azimuthally symmetric, with the density maximal at the hole, and one threefold symmetric, with a node at the hole. Moiré trapping, neglected in commonly used models of quadrupolar exciton formation, is critical to their many-exciton phases. Without moiré trapping, quadrupolar excitons transition into anti-parallel dipolar excitons on a bipartite square lattice, while with trapping, the same dipoles are confined to a triangular lattice and experience geometric frustration. Our study uncovers the highly non-trivial nature of quadrupolar excitons, with direct implications for simulating frustrated quantum magnetism in a fully tunable excitonic platform.

Abstract

Quadrupolar excitons in van der Waals heterostructures – quantum superpositions of anti-aligned dipolar excitons – offer a novel platform to explore exotic many-body physics, with applications to quantum sensing and photonic devices. Yet their internal structure, symmetry, and real-space localisation remain largely unknown. Here, we reveal the atomic-scale structure of quadrupolar excitons in twisted WSe₂/WS₂/WSe₂ trilayers by solving the Bethe–Salpeter equation within a large-scale atomistic framework. We discover that large atomic relaxations at small twist angles give rise to two distinct quadrupolar excitons trapped at moiré lattice sites, differing in the in-plane symmetry of the electron density about the hole: one azimuthally symmetric, with the density maximal at the hole, and one threefold symmetric, with a node at the hole. Moiré trapping, neglected in commonly used models of quadrupolar exciton formation, is critical to their many-exciton phases. Without moiré trapping, quadrupolar excitons transition into anti-parallel dipolar excitons on a bipartite square lattice, while with trapping, the same dipoles are confined to a triangular lattice and experience geometric frustration. Our study uncovers the highly non-trivial nature of quadrupolar excitons, with direct implications for simulating frustrated quantum magnetism in a fully tunable excitonic platform.

Abstract

Quadrupolar excitons in van der Waals heterostructures – quantum superpositions of anti-aligned dipolar excitons – offer a novel platform to explore exotic many-body physics, with applications to quantum sensing and photonic devices. Yet their internal structure, symmetry, and real-space localisation remain largely unknown. Here, we reveal the atomic-scale structure of quadrupolar excitons in twisted WSe₂/WS₂/WSe₂ trilayers by solving the Bethe–Salpeter equation within a large-scale atomistic framework. We discover that large atomic relaxations at small twist angles give rise to two distinct quadrupolar excitons trapped at moiré lattice sites, differing in the in-plane symmetry of the electron density about the hole: one azimuthally symmetric, with the density maximal at the hole, and one threefold symmetric, with a node at the hole. Moiré trapping, neglected in commonly used models of quadrupolar exciton formation, is critical to their many-exciton phases. Without moiré trapping, quadrupolar excitons transition into anti-parallel dipolar excitons on a bipartite square lattice, while with trapping, the same dipoles are confined to a triangular lattice and experience geometric frustration. Our study uncovers the highly non-trivial nature of quadrupolar excitons, with direct implications for simulating frustrated quantum magnetism in a fully tunable excitonic platform.

Abstract

Quadrupolar excitons in van der Waals heterostructures – quantum superpositions of anti-aligned dipolar excitons – offer a novel platform to explore exotic many-body physics, with applications to quantum sensing and photonic devices. Yet their internal structure, symmetry, and real-space localisation remain largely unknown. Here, we reveal the atomic-scale structure of quadrupolar excitons in twisted WSe₂/WS₂/WSe₂ trilayers by solving the Bethe–Salpeter equation within a large-scale atomistic framework. We discover that large atomic relaxations at small twist angles give rise to two distinct quadrupolar excitons trapped at moiré lattice sites, differing in the in-plane symmetry of the electron density about the hole: one azimuthally symmetric, with the density maximal at the hole, and one threefold symmetric, with a node at the hole. Moiré trapping, neglected in commonly used models of quadrupolar exciton formation, is critical to their many-exciton phases. Without moiré trapping, quadrupolar excitons transition into anti-parallel dipolar excitons on a bipartite square lattice, while with trapping, the same dipoles are confined to a triangular lattice and experience geometric frustration. Our study uncovers the highly non-trivial nature of quadrupolar excitons, with direct implications for simulating frustrated quantum magnetism in a fully tunable excitonic platform.