期刊
CHEMPHYSCHEM
卷 17, 期 19, 页码 2956-2961出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201600662
关键词
light-emitting diodes; reverse intersystem crossing; thermally activated delay fluorescence; vibronic coupling; quantum dynamics
资金
- EPSRC [EP/N028511/1]
- Engineering and Physical Sciences Research Council [EP/N028511/1] Funding Source: researchfish
- EPSRC [EP/N028511/1] Funding Source: UKRI
Factors influencing the rate of reverse intersystem crossing (k(rISC)) in thermally activated delayed fluorescence (TADF) emitters are critical for improving the efficiency and performance of third-generation heavy-metal-free organic light-emitting diodes (OLEDs). However, present understanding of the TADF mechanism does not extend far beyond a thermal equilibrium between the lowest singlet and triplet states and consequently research has focused almost exclusively on the energy gap between these two states. Herein, we use a model spin-vibronic Hamiltonian to reveal the crucial role of non-Born-Oppenheimer effects in determining k(rISC). We demonstrate that vibronic (nonadiabatic) coupling between the lowest local excitation triplet (3LE) and lowest charge transfer triplet (3CT) opens the possibility for significant second-order coupling effects and increases k(rISC) by about four orders of magnitude. Crucially, these simulations reveal the dynamical mechanism for highly efficient TADF and opens design routes that go beyond the BornOppenheimer approximation for the future development of high-performing systems.
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