Quantitative Benchmarking of Spectroscopic Homogeneous and Inhomogeneous Linewidth Separation
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 MoSe2 sample, we construct uncertainty-weighted \c{hi}^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.
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BibTeX
@misc{alfrey2026quantitative,
title = {{Quantitative Benchmarking of Spectroscopic Homogeneous and Inhomogeneous Linewidth Separation}},
author = {Adam Alfrey and Cole Tait and Joshua R. Hendrickson and Steven T. Cundiff},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2607.05564},
eprint = {2607.05564},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2607.05564},
note = {CC BY-NC-ND 4.0},
}
RIS
TY - UNPB
TI - Quantitative Benchmarking of Spectroscopic Homogeneous and Inhomogeneous Linewidth Separation
AU - Adam Alfrey
AU - Cole Tait
AU - Joshua R. Hendrickson
AU - Steven T. Cundiff
PY - 2026
DA - 2026/10/07
PB - arXiv
DO - 10.48550/arxiv.2607.05564
UR - https://arxiv.org/abs/2607.05564
AB - 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 MoSe2 sample, we construct uncertainty-weighted \c{hi}^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.
ER -