5 years ago

Optically Activated Delayed Fluorescence

Optically Activated Delayed Fluorescence
Jung-Cheng Hsiang, Jeffrey T. Petty, Blake C. Fleischer, Robert M. Dickson
We harness the photophysics of few-atom silver nanoclusters to create the first fluorophores capable of optically activated delayed fluorescence (OADF). In analogy with thermally activated delayed fluorescence, often resulting from oxygen- or collision-activated reverse intersystem crossing from triplet levels, this optically controllable/reactivated visible emission occurs with the same 2.2 ns fluorescence lifetime as that produced with primary excitation alone but is excited with near-infrared light from either of two distinct, long-lived photopopulated dark states. In addition to faster ground-state recovery under long-wavelength co-illumination, this “repumped” visible fluorescence occurs many microsceconds after visible excitation and only when gated by secondary near-IR excitation of ∼1–100 μs-lived dark excited states. By deciphering the Ag nanocluster photophysics, we demonstrate that OADF improves upon previous optical modulation schemes for near-complete background rejection in fluorescence detection. Likely extensible to other fluorophores with photopopulatable excited dark states, OADF holds potential for drastically improving fluorescence signal recovery from high backgrounds.

Publisher URL: http://dx.doi.org/10.1021/acs.jpclett.7b01215

DOI: 10.1021/acs.jpclett.7b01215

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