Disentanglement of excited-state dynamics with implications for FRET measurements: two-dimensional electronic spectroscopy of a BODIPY-functionalized cavitand

Chemical Science
John P OttoMelanie Chiu

Abstract

Förster Resonance Energy Transfer (FRET) is the incoherent transfer of an electronic excitation from a donor fluorophore to a nearby acceptor. FRET has been applied as a probe of local chromophore environments and distances on the nanoscale by extrapolating transfer efficiencies from standard experimental parameters, such as fluorescence intensities or lifetimes. Competition from nonradiative relaxation processes is often assumed to be constant in these extrapolations, but in actuality, this competition depends on the donor and acceptor environments and can, therefore, be affected by conformational changes. To study the effects of nonradiative relaxation on FRET dynamics, we perform two-dimensional electronic spectroscopy (2DES) on a pair of azaboraindacene (BODIPY) dyes, attached to opposite arms of a resorcin[4]arene cavitand. Temperature-induced switching between two equilibrium conformations, vase at 294 K to kite at 193 K, increases the donor-acceptor distance from 0.5 nm to 3 nm, affecting both FRET efficiency and nonradiative relaxation. By disentangling different dynamics based on lifetimes extracted from a series of 2D spectra, we independently observe nonradiative relaxation, FRET, and residual fluorescence from the d...Continue Reading

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Citations

Sep 3, 2020·Chemical Science·Zhiyun ZhangHe Tian
Apr 24, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·İpek ÖmeroğluMahmut Durmuş
Jun 17, 2021·Chemical Reviews·Meera MadhuMahesh Hariharan
Jan 15, 2020·The Journal of Physical Chemistry. a·Patrick C TappingTak W Kee

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Methods Mentioned

BETA
FRET

Software Mentioned

Vinci
Gaussian

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