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A composite electrodynamic mechanism to reconcile spatiotemporally resolved exciton transport in quantum dot superlattices.
Yuan, Rongfeng; Roberts, Trevor D; Brinn, Rafaela M; Choi, Alexander A; Park, Ha H; Yan, Chang; Ondry, Justin C; Khorasani, Siamak; Masiello, David J; Xu, Ke; Alivisatos, A Paul; Ginsberg, Naomi S.
Afiliação
  • Yuan R; Department of Chemistry, University of California Berkeley, Berkeley, CA 94720, USA.
  • Roberts TD; Department of Chemistry, University of California Berkeley, Berkeley, CA 94720, USA.
  • Brinn RM; Department of Chemistry, University of California Berkeley, Berkeley, CA 94720, USA.
  • Choi AA; Department of Chemistry, University of California Berkeley, Berkeley, CA 94720, USA.
  • Park HH; Department of Chemistry, University of California Berkeley, Berkeley, CA 94720, USA.
  • Yan C; Department of Chemistry, University of California Berkeley, Berkeley, CA 94720, USA.
  • Ondry JC; Department of Chemistry, University of California Berkeley, Berkeley, CA 94720, USA.
  • Khorasani S; Department of Materials Science and Engineering, University of Washington, Seattle, WA 98195, USA.
  • Masiello DJ; Department of Materials Science and Engineering, University of Washington, Seattle, WA 98195, USA.
  • Xu K; Department of Chemistry, University of Washington, Seattle, WA 98195, USA.
  • Alivisatos AP; Department of Chemistry, University of California Berkeley, Berkeley, CA 94720, USA.
  • Ginsberg NS; STROBE, National Science Foundation Science and Technology Center, University of California Berkeley, Berkeley, CA 94720, USA.
Sci Adv ; 9(42): eadh2410, 2023 Oct 20.
Article em En | MEDLINE | ID: mdl-37862422
ABSTRACT
Quantum dot (QD) solids are promising optoelectronic materials; further advancing their device functionality requires understanding their energy transport mechanisms. The commonly invoked near-field Förster resonance energy transfer (FRET) theory often underestimates the exciton hopping rate in QD solids, yet no consensus exists on the underlying cause. In response, we use time-resolved ultrafast stimulated emission depletion (STED) microscopy, an ultrafast transformation of STED to spatiotemporally resolve exciton diffusion in tellurium-doped cadmium selenide-core/cadmium sulfide-shell QD superlattices. We measure the concomitant time-resolved exciton energy decay due to excitons sampling a heterogeneous energetic landscape within the superlattice. The heterogeneity is quantified by single-particle emission spectroscopy. This powerful multimodal set of observables provides sufficient constraints on a kinetic Monte Carlo simulation of exciton transport to elucidate a composite transport mechanism that includes both near-field FRET and previously neglected far-field emission/reabsorption contributions. Uncovering this mechanism offers a much-needed unified framework in which to characterize transport in QD solids and additional principles for device design.
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Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Sci Adv Ano de publicação: 2023 Tipo de documento: Article País de afiliação: Estados Unidos
Texto completo
Imprimir
XML
PubMed Links
Buscar no Google

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Sci Adv Ano de publicação: 2023 Tipo de documento: Article País de afiliação: Estados Unidos