Emergence and Relaxation of an e–h Quantum Liquid Phase in Photoexcited MoS2 Nanoparticles at Room Temperature

Abstract

AbstractLow‐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.