TY - JOUR
T1 - Emergence and Relaxation of an e–h Quantum Liquid Phase in Photoexcited MoS2 Nanoparticles at Room Temperature
AU - Dey, Pritha
AU - Dixit, Tejendra
AU - Mishra, Vikash
AU - Sahoo, Anubhab
AU - Vijayan, Cheriyanath
AU - Krishnan, Sivarama
N1 - Publisher Copyright:
© 2023 Wiley-VCH GmbH.
PY - 2023/8/7
Y1 - 2023/8/7
N2 - Low-dimensional transition metal dichalcogenide (TMDC) materials are heralding a new era in optoelectronics and valleytronics owing to their unique properties. Photo-induced dynamics in these systems is mostly studied from the perspective of individual quasi-particles—excitons, bi-excitons, or, even, trions—their formation, evolution, and decay. The role of multi-body and exciton dynamics, the associated collective behavior, condensation, and inter-excitonic interactions remain intriguing and seek attention, especially in room-temperature scenarios that are relevant for device applications. In this work, the formation and decay of an unexpected electron–hole quantum liquid phase at room-temperature on ultrafast timescales in multi-layer MoS2 nanoparticles is evidenced through femtosecond broadband transient absorption spectroscopy. The studies presented here reveal the complete dynamical picture: the initial electron–hole plasma (EHP) condenses into a quantum electron–hole liquid (EHL) phase that typically lasts as long as 10 ps, revealing its robustness, whereafter the system decays through phonons. The authors employ a successful physical model using a set of coupled nonlinear rate equations governing the individual populations of these constituent phases to extract their contributions to bandgap renormalization (BGR). Beyond the observation of the electron–hole liquid-like state at room temperature, this work reveals the ultrafast dynamics of photo-excited low-dimensional systems arising out of collective many-particle behavior and correlations.
AB - Low-dimensional transition metal dichalcogenide (TMDC) materials are heralding a new era in optoelectronics and valleytronics owing to their unique properties. Photo-induced dynamics in these systems is mostly studied from the perspective of individual quasi-particles—excitons, bi-excitons, or, even, trions—their formation, evolution, and decay. The role of multi-body and exciton dynamics, the associated collective behavior, condensation, and inter-excitonic interactions remain intriguing and seek attention, especially in room-temperature scenarios that are relevant for device applications. In this work, the formation and decay of an unexpected electron–hole quantum liquid phase at room-temperature on ultrafast timescales in multi-layer MoS2 nanoparticles is evidenced through femtosecond broadband transient absorption spectroscopy. The studies presented here reveal the complete dynamical picture: the initial electron–hole plasma (EHP) condenses into a quantum electron–hole liquid (EHL) phase that typically lasts as long as 10 ps, revealing its robustness, whereafter the system decays through phonons. The authors employ a successful physical model using a set of coupled nonlinear rate equations governing the individual populations of these constituent phases to extract their contributions to bandgap renormalization (BGR). Beyond the observation of the electron–hole liquid-like state at room temperature, this work reveals the ultrafast dynamics of photo-excited low-dimensional systems arising out of collective many-particle behavior and correlations.
UR - https://www.scopus.com/pages/publications/85156134143
UR - https://www.scopus.com/pages/publications/85156134143#tab=citedBy
U2 - 10.1002/adom.202202567
DO - 10.1002/adom.202202567
M3 - Article
AN - SCOPUS:85156134143
SN - 2195-1071
VL - 11
JO - Advanced Optical Materials
JF - Advanced Optical Materials
IS - 15
M1 - 2202567
ER -