Biexcitons in Ruddlesden-Popper Metal Halides Probed by Nonlinear Coherent Spectroscopy

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Autori principali: Koch, Katherine A., Silva-Acuña, Carlos, Kandada, Ajay Ram Srimath
Natura: Preprint
Pubblicazione: 2026
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author Koch, Katherine A.
Silva-Acuña, Carlos
Kandada, Ajay Ram Srimath
author_facet Koch, Katherine A.
Silva-Acuña, Carlos
Kandada, Ajay Ram Srimath
contents Excitons and their correlated complexes underpin the rich photophysics of quantum-confined semiconductors. Among these, biexcitons -- bound states of two electrons and two holes -- provide a sensitive probe of Coulomb correlations, exciton-exciton interactions, and the role of the dielectric environment. In Ruddlesden-Popper metal halide materials (RPMHs), strong quantum and dielectric confinement stabilize excitons with binding energies of hundreds of meV, creating an ideal platform for multi-exciton phenomena. Conventional linear spectroscopies, such as photoluminescence and transient absorption, reveal biexciton signatures but suffer from spectral congestion and reabsorption artifacts. Two-dimensional coherent spectroscopies, particularly two-quantum (2Q) multidimensional techniques, uniquely access multi-exciton coherences and provide unambiguous estimates of biexciton binding energies. This minireview surveys the spectroscopic evidence for biexcitons in RPMHs, highlights the advantages of nonlinear multidimensional approaches, and situates biexciton physics within the broader context of excitonic materials, including GaAs quantum wells, quantum dots, and transition-metal dichalcogenides. By emphasizing the interplay of exciton-exciton annihilation, excitation-induced dephasing, and biexciton formation, we argue that multidimensional coherent spectroscopy offers the most reliable pathway to disentangle many-body interactions in quantum-well derivatives of metal-halide perovskites.
format Preprint
id arxiv_https___arxiv_org_abs_2601_16101
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Biexcitons in Ruddlesden-Popper Metal Halides Probed by Nonlinear Coherent Spectroscopy
Koch, Katherine A.
Silva-Acuña, Carlos
Kandada, Ajay Ram Srimath
Materials Science
Excitons and their correlated complexes underpin the rich photophysics of quantum-confined semiconductors. Among these, biexcitons -- bound states of two electrons and two holes -- provide a sensitive probe of Coulomb correlations, exciton-exciton interactions, and the role of the dielectric environment. In Ruddlesden-Popper metal halide materials (RPMHs), strong quantum and dielectric confinement stabilize excitons with binding energies of hundreds of meV, creating an ideal platform for multi-exciton phenomena. Conventional linear spectroscopies, such as photoluminescence and transient absorption, reveal biexciton signatures but suffer from spectral congestion and reabsorption artifacts. Two-dimensional coherent spectroscopies, particularly two-quantum (2Q) multidimensional techniques, uniquely access multi-exciton coherences and provide unambiguous estimates of biexciton binding energies. This minireview surveys the spectroscopic evidence for biexcitons in RPMHs, highlights the advantages of nonlinear multidimensional approaches, and situates biexciton physics within the broader context of excitonic materials, including GaAs quantum wells, quantum dots, and transition-metal dichalcogenides. By emphasizing the interplay of exciton-exciton annihilation, excitation-induced dephasing, and biexciton formation, we argue that multidimensional coherent spectroscopy offers the most reliable pathway to disentangle many-body interactions in quantum-well derivatives of metal-halide perovskites.
title Biexcitons in Ruddlesden-Popper Metal Halides Probed by Nonlinear Coherent Spectroscopy
topic Materials Science
url https://arxiv.org/abs/2601.16101