When Cubic is Not Isotropic: Phonon–Exciton Decoupling in CuInSnS4 Single Crystals

Linke LK, Tomm Y, Liu X, Gurieva G, Többens DM, Adams P, Calame M, Crisp R, Boland J, Kavanagh S, Schorr S, Dimitrievska M (2026)


Publication Type: Journal article

Publication year: 2026

Journal

DOI: 10.1002/adom.71392

Abstract

Atomic-scale disorder can create hidden optical anisotropy even in crystals that are structurally cubic on average. Here, we show that (Formula presented.) single crystals host locally symmetry-broken environments arising from intrinsic In/Sn cation disorder, which affect vibrational and excitonic properties in markedly different ways. Combining polarization- and temperature-dependent Raman spectroscopy, infrared near-field microscopy, steady-state and time-resolved photoluminescence, and first-principles calculations, we find that phonons remain largely symmetry-averaged and locally homogeneous on the nanoscale. In contrast, photoluminescence reveals a lower-energy band-tail emission with pronounced polarization anisotropy following a well-defined angular symmetry, highlighting the strong sensitivity of excitonic states to local symmetry breaking. This phonon–exciton decoupling reveals that intrinsic disorder can localize excitons while preserving vibrational coherence and dielectric homogeneity, thereby opening new opportunities for polarization-sensitive light sources, anisotropic photodetectors, and exciton-based optical functionalities even in nominally cubic multinary semiconductors.

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APA:

Linke, L.K., Tomm, Y., Liu, X., Gurieva, G., Többens, D.M., Adams, P.,... Dimitrievska, M. (2026). When Cubic is Not Isotropic: Phonon–Exciton Decoupling in CuInSnS4 Single Crystals. Advanced Optical Materials. https://doi.org/10.1002/adom.71392

MLA:

Linke, Lara Kim, et al. "When Cubic is Not Isotropic: Phonon–Exciton Decoupling in CuInSnS4 Single Crystals." Advanced Optical Materials (2026).

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