Work

Quantitative benchmarking of spectroscopic homogeneous and inhomogeneous linewidth separation

Year: 2026

Type: article

Abstract: Separating homogeneous and inhomogeneous contributions to a spectral linewidth is essential for connecting optical spectra to microscopic dephasing and disorder. We quantitatively compare linewidth separation by one-dimensional Voigt analysis and two-dimensional coherent spectroscopy (2DCS). Using photoluminescence and 2DCS measurements of the same hBN-encapsulated monolayer MoSe 2 sample, we construct uncertainty-weighted χ 2 landscapes for the Gaussian inhomogeneous width and Lorentzian homogeneous half-width. Although a Voigt profile accurately reproduces the photoluminescence spectrum, the two widths are strongly anticorrelated and therefore poorly determined independently. By contrast, joint fitting of diagonal and cross-diagonal 2DCS slices produces more compact confidence regions with reduced parameter correlation and elongation. These results quantitatively demonstrate the improved linewidth separation provided by 2DCS and illustrate the limitations of assigning homogeneous and inhomogeneous contributions from one-dimensional Voigt fits alone.

Source: Optics Letters

DOI: 10.1364/ol.618833

Authors: Adam Alfrey, Cole Tait, Joshua R. Hendrickson, Steven T. Cundiff

Institution: United States Air Force Research Laboratory

Language: English

Topic: 2D Materials and Applications

Subfield: Materials Chemistry

Field: Materials Science

Domain: Physical Sciences

Open Access status: green

Funders: National Science Foundation, Air Force Office of Scientific Research

Awards: Quantum Interference Control of Photoexcited Carriers for K-Space Microscopy, G1523888516, G1778466097