Rigsby Emily M, Miyashita Tsumugi, Fishman Dmitry A, Roberts Sean T, Tang Ming L
Department of Chemistry, University of California Riverside Riverside CA 92521 USA
Department of Bioengineering, University of California Riverside Riverside CA 92521 USA.
RSC Adv. 2021 Sep 20;11(49):31042-31046. doi: 10.1039/d1ra06562a. eCollection 2021 Sep 14.
Here, films using CdSe nanocrystal (NC) triplet photosensitizers in conjunction with diphenylanthracene (DPA) emitters were assembled to address several challenges to practical applications for solution-based photon upconversion. By using poly(9-vinylcarbazole) as a phosphorescent host in this film, volatile organic solvents are eliminated, the spontaneous crystallization of the emitter is significantly retarded, and ∼1.5% photon upconversion quantum yield (out of a maximum of 50%) is obtained. Transient absorption spectroscopy on nanosecond-to-microsecond time scales reveals this efficiency is enabled by an exceptionally long triplet lifetime of 3.4 ± 0.3 ms. Ultimately, we find the upconversion efficiency is limited by incomplete triplet-triplet annihilation, which occurs with a rate 3-4 orders of magnitude slower than in solution-phase upconversion systems.
在此,我们组装了使用硒化镉纳米晶体(NC)三重态光敏剂与二苯基蒽(DPA)发光体的薄膜,以应对基于溶液的光子上转换实际应用中的若干挑战。通过在该薄膜中使用聚(9-乙烯基咔唑)作为磷光主体,消除了挥发性有机溶剂,显著延缓了发光体的自发结晶,并获得了约1.5%的光子上转换量子产率(最高可达50%)。在纳秒到微秒时间尺度上的瞬态吸收光谱表明,这种效率是由3.4±0.3毫秒的超长三重态寿命实现的。最终,我们发现上转换效率受到三重态-三重态湮灭不完全的限制,其发生速率比溶液相上转换系统慢3-4个数量级。