The Topography Trap: Sifting Interlayer Excitons from Strain-Related Artifacts in Real-World 2D Hetrostructures

TL;DR

This paper introduces a decision-tree protocol for accurately identifying interlayer excitons in 2D heterostructures, clarifying previous ambiguities caused by strain artifacts and providing a reliable spectroscopic framework.

Contribution

The authors develop and validate a novel, spatially resolved protocol to distinguish true interlayer excitons from strain-related artifacts in TMDC heterostructures.

Findings

Identified momentum-direct KK-IX in MoS2-MoSe2 and MoS2-WSe2 heterostructures at room temperature.

Contested the existence of previously reported $ ext{Γ}$K-IX in MoS2-WSe2, attributing signals to strain artifacts.

Demonstrated that strain-induced features can mimic interlayer excitons, emphasizing the need for spatially resolved analysis.

Abstract

Novel excitonic phenomena emerging in transition metal dichalcogenide (TMDC) heterostructures belong to the most exciting topics in contemporary physics of van der Waals materials. Interlayer excitons (IXs) stand out among those due to their long radiative lifetimes and tunability by electric fields, strain, and twist angle. However, many ambiguities persist in the optical identification and manipulation of IXs, highlighting the need for reliable spectroscopic criteria that distinguish interlayer species from spurious signals. Here, we present a decision-tree protocol that evaluates interlayer coupling via intralayer exciton quenching and correlates photoluminescence (PL) with atomic force microscopy (AFM) to correctly assign room-temperature PL features in TMDC-based heterostructures. Applying this protocol, we identify momentum-direct IX between the K valleys of the two layers (KK-IX) in MoS2-MoSe2 and MoS2-WSe2 heterostructures at room temperature. In contrast, our protocol contests the reported bright, momentum-indirect, twist-angle-independent $\Gamma$K-IX in MoS2-WSe2. Comprehensive experimental data, including infrared and tip-enhanced photoluminescence (TEPL) with sub-diffraction-limited resolution, show no compelling evidence for this excitonic species, despite numerous reports. Instead, the spectroscopic features previously assigned to this $\Gamma$K-IX originate from locally strained WSe2 at topographical inhomogeneities of the heterostructure interface, underscoring the need for robust, spatially resolved characterization of real-world samples in this highly accessible field and providing a generally applicable framework for identifying interlayer excitons in 2D semiconductor heterostructures.