Electron Transfer Enhanced by a Minimal Energetic Driving Force at the Organic-Semiconductor Interface.

The energetic driving force for electron transfer must be minimized to realize efficient optoelectronic devices including organic light-emitting diodes (OLEDs) and organic photovoltaics (OPVs). Exploring the dynamics of a charge-transfer (CT) state at an interface leads to a comprehension of the relationship between energetics, electron-transfer efficiency, and device performance. Here, we investigate the electron transfer from the CT state to the triplet excited state (T ₁ ) in upconversion OLEDs with 45 material combinations. By analyzing the CT emission and the singlet excited-state emission from triplet-triplet annihilation via the dark T ₁ , their energetics and electron-transfer efficiencies are extracted. We demonstrate that the CT→T ₁ electron transfer is enhanced by the stronger CT interaction and a minimal energetic driving force (<0.1 eV), which is explained using the Marcus theory with a small reorganization energy of <0.1 eV. Through our analysis, a novel donor-acceptor combination for the OLED is developed and shows an efficient blue emission with an extremely low turn-on voltage of 1.57 V. This work provides a solution to control interfacial CT states for efficient optoelectronic devices without energy loss.
(© 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)