Thermodynamic Equilibrium between Excitons and Excitonic Molecules Dictates Optical Gain in Colloidal CdSe Quantum Wells

Pieter Geiregat, Renu Tomar, Kai Chen, Shalini Singh, Justin M. Hodgkiss, Zeger Hens

Research output: Contribution to journalArticlepeer-review

Abstract

We show that optical gain in 2D CdSe colloidal quantum wells (CQWs) shows little saturation and coexists with exciton absorption over a broad range of excitation densities, in stark contrast with 0D CdSe colloidal quantum dots (CQDs). In addition, we demonstrate that photoexcited CQWs can absorb or emit light through the thermodynamically driven formation or radiative recombination of singlet excitonic molecules. Invoking stimulated emission through the molecule-exciton transition, we can quantify all of the remarkable gain characteristics of CQWs using only experimentally determined parameters, an advance that highlights a fundamental difference between multiexcitons in CQWs and CQDs. While strong confinement prohibits the dissociation of multiexcitons into separate excitons in 0D CQDs, excitons and excitonic molecules coexist in a 2D CQW at room temperature, with densities governed by an association/dissociation equilibrium, not by state-filling. Our finding points out future directions to optimize stimulated emission by excitonic 2D materials in general.

Original languageEnglish
Pages (from-to)3637-3644
Number of pages8
JournalJournal of Physical Chemistry Letters
Volume10
Issue number13
DOIs
Publication statusPublished - 5 Jul 2019
Externally publishedYes

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