Institute of Physical and Theoretical Chemistry, Goethe University Frankfurt , Max-von-Laue Str. 7, 60438 Frankfurt/Main, Germany.
J Am Chem Soc. 2014 Mar 5;136(9):3430-8. doi: 10.1021/ja410594y. Epub 2014 Feb 25.
The cleavage of a photolabile nitroveratryloxycarbonyl protecting group, which is widely used as caging group, was studied by femtosecond transient absorption spectroscopy in the visible and infrared spectral range and by flash-photolysis experiments on the longer time scale. On the basis of quantum-chemical calculations it is shown that directly after excitation, triplet absorption that is not part of the reactive pathway dominates the transient spectrum and that the molecules following the triplet pathway are trapped in a nonreactive triplet state. By contrast, photolysis proceeds from the singlet manifold. Therefore, trapping in the triplet state lowers the quantum yield of the process for this compound compared with other o-nitrobenzyl protecting groups. With our integrated approach of time-resolved UV and IR measurements and calculations, we can characterize the entire uncaging mechanism and identify the most relevant intermediate states along the reaction pathway. The final uncaging is accomplished within 32 μs.
光解不稳定的硝基香草酰氧基羰基保护基团(被广泛用作笼蔽基团)的裂解,通过飞秒瞬态吸收光谱在可见和红外光谱范围内以及通过更长时间尺度的闪光光解实验进行了研究。基于量子化学计算,结果表明,在直接激发后,不属于反应途径的三重态吸收主导瞬态光谱,并且沿三重态途径的分子被捕获在非反应性三重态中。相比之下,光解是从单重态进行的。因此,与其他邻硝基苄基保护基团相比,该化合物的三重态捕获降低了该过程的量子产率。通过我们的时间分辨 UV 和 IR 测量和计算的综合方法,我们可以表征整个解笼机制,并确定反应途径中最相关的中间状态。最终的解笼在 32 μs 内完成。