Facet {100} Fosters Resonance Energy Transfer in Ni/Co-doped CsPbBr3 Nanocrystals

10 July 2024, Version 2
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

The design of an effective light harvester with metal-doped perovskite nanocrystals (M:PNCs) aims at achieving directional energy flow. The potential of crystal facets needs to be assessed for dictating energy transfer dynamics of M:PNCs. Herein we have engineered facets of amine-capped CsPbBr3 perovskite nanocrystals by doping with a trace amount of Ni and Co ions. Ni-doped CsPbBr3 (Ni:PNC) showcases structural heterogeneity with regular cubic and rod shapes whereas bimetallic-doped CsPbBr3 (Ni:Co:PNC) evolves to an elongated dodecahedron structure. Structural analysis using Rietveld Refinement strongly corroborates the construction of dodecahedron structure for Ni:Co:PNC through systematic displacement of Cs ions. Energy transfer from doped nanocrystals to Rhodamine B (RhB) occurs through dipole-dipole interaction, known as Fluorescence Resonance Energy Transfer (FRET). The emergence of isoemissive point, and rise-time of RhB conclusively establish Resonance Energy Transfer mechanism. Energy transfer in thin films occurs at much faster rate than in toluene medium. {100} facet-dominated Ni:PNC registers a FRET efficiency of 94% whereas {111}, {002} facet-dominated Ni:Co:PNC restricts at 21% FRET efficiency. The distance between donor and acceptor, RDA dictates the dynamics of energy transfer, rather than spectral overlap, and photoluminescence quantum yield of these doped-nanocrystals. Surface composition of facets, typically Cs ions perhaps plays a decisive role in regulating the binding constant of donor and acceptor. Our study demonstrates the importance of facets of nanocrystals in tuning the desired energy transfer processes for photocatalytic applications.

Keywords

CsPbBr3 Nanocrystals
Metal Doping
Facet (100)
Resonance Energy Transfer
Photocatalysis

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