Spectroscopic signatures of biexcitons: A case study in Ruddlesden-Popper lead-halides

Fuente: arXiv
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Main Authors: Koch, Katherine A., Rojas-Gatjens, Esteban, Gomez-Dominguez, Martin, Correa-Baena, Juan-Pablo, Silva-Acuna, Carlos, Kandada, Ajay Ram Srimath
Format: Preprint
Published: 2025
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author Koch, Katherine A.
Rojas-Gatjens, Esteban
Gomez-Dominguez, Martin
Correa-Baena, Juan-Pablo
Silva-Acuna, Carlos
Kandada, Ajay Ram Srimath
author_facet Koch, Katherine A.
Rojas-Gatjens, Esteban
Gomez-Dominguez, Martin
Correa-Baena, Juan-Pablo
Silva-Acuna, Carlos
Kandada, Ajay Ram Srimath
contents Exciton-exciton interactions are fundamental to the light-emitting properties of semiconductors, influencing applications from lasers to quantum light sources. In this study, we investigate the spectroscopic signatures and binding energy of biexcitons in a metal halide two-dimensional Ruddlesden-Popper structure, which is known for hosting distinct excitonic resonances with unique lattice coupling. Using three spectroscopic techniques - photoluminescence (PL) and two variations of two-dimensional electronic spectroscopy (2DES) - we map coherent one-quantum and two-quantum correlations to gain deeper insight into the biexciton characteristics. While PL spectroscopy is hindered by spectral broadening and reabsorption, 2DES provides a more accurate characterization, revealing multiple biexciton states and uncovering a mixed biexciton species arising from exciton cross-coupling. These findings highlight the importance of advanced spectroscopic approaches in accurately determining biexciton binding energies and offer new perspectives on many-body interactions in exciton-polarons within layered perovskites.
format Preprint
id arxiv_https___arxiv_org_abs_2503_11890
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Spectroscopic signatures of biexcitons: A case study in Ruddlesden-Popper lead-halides
Koch, Katherine A.
Rojas-Gatjens, Esteban
Gomez-Dominguez, Martin
Correa-Baena, Juan-Pablo
Silva-Acuna, Carlos
Kandada, Ajay Ram Srimath
Materials Science
Exciton-exciton interactions are fundamental to the light-emitting properties of semiconductors, influencing applications from lasers to quantum light sources. In this study, we investigate the spectroscopic signatures and binding energy of biexcitons in a metal halide two-dimensional Ruddlesden-Popper structure, which is known for hosting distinct excitonic resonances with unique lattice coupling. Using three spectroscopic techniques - photoluminescence (PL) and two variations of two-dimensional electronic spectroscopy (2DES) - we map coherent one-quantum and two-quantum correlations to gain deeper insight into the biexciton characteristics. While PL spectroscopy is hindered by spectral broadening and reabsorption, 2DES provides a more accurate characterization, revealing multiple biexciton states and uncovering a mixed biexciton species arising from exciton cross-coupling. These findings highlight the importance of advanced spectroscopic approaches in accurately determining biexciton binding energies and offer new perspectives on many-body interactions in exciton-polarons within layered perovskites.
title Spectroscopic signatures of biexcitons: A case study in Ruddlesden-Popper lead-halides
topic Materials Science
url https://arxiv.org/abs/2503.11890