Beyond Forster Resonance Energy Transfer in Biological and Nanoscale Systems

被引:377
作者
Beljonne, David [4 ]
Curutchet, Carles [1 ,2 ]
Scholes, Gregory D. [1 ,2 ]
Silbey, Robert J. [3 ]
机构
[1] Univ Toronto, Lash Miller Chem Labs, Inst Opt Sci, Toronto, ON M5S 3H6, Canada
[2] Univ Toronto, Ctr Quantum Informat & Quantum Control, Toronto, ON M5S 3H6, Canada
[3] MIT, Dept Chem, Cambridge, MA 02139 USA
[4] Univ Mons, Lab Chem Novel Mat, Ctr Res Mol Elect & Photon, B-7000 Mons, Belgium
基金
美国国家科学基金会;
关键词
LIGHT-HARVESTING COMPLEXES; PHOTOSYNTHETIC ANTENNA COMPLEXES; EXCITON DELOCALIZATION LENGTH; SINGLE-MOLECULE SPECTROSCOPY; PUMP-PROBE SPECTROSCOPY; EXCITATION TRANSFER; PURPLE BACTERIA; AB-INITIO; THROUGH-BOND; TEMPERATURE-DEPENDENCE;
D O I
10.1021/jp900708f
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
After photoexcitation, energy absorbed by a molecule can be transferred efficiently over a distance of up to several tens of angstroms to another molecule by the process of resonance energy transfer, RET (also commonly known as electronic energy transfer, EET). Examples of where RET is observed include natural and artificial antennae for the capture and energy conversion of light, amplification of fluorescence-based sensors, optimization of organic light-emitting diodes, and the measurement of structure in biological systems (FRET). Forster theory has proven to be very successful at estimating the rate of RET in many donor-acceptor systems, but it has also been of interest to discover when this theory does not work. By identifying these cases, researchers have been able to obtain, sometimes surprising, insights into excited-state dynamics in complex systems. In this article, we consider various ways that electronic energy transfer is promoted by mechanisms beyond those explicitly considered in Forster RET theory. First, we recount the important situations when the electronic coupling is not accurately calculated by the dipole-dipole approximation. Second, we examine the related problem of how to describe solvent screening when the dipole approximation fails. Third, there are situations where we need to be careful about the separability of electronic coupling and spectral overlap factors. For example, when the donors and/or acceptors are molecular aggregates rather than individual molecules, then RET occurs between molecular exciton states and we must invoke generalized Forster theory (GFT). In even more complicated cases, involving the intermediate regime of electronic energy transfer, we should consider carefully nonequilibrium processes and coherences and how bath modes can be shared. Lastly, we discuss how information is obscured by various forms of energetic disorder in ensemble measurements and we outline how single molecule experiments continue to be important in these instances.
引用
收藏
页码:6583 / 6599
页数:17
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