Michenfelder Rita T, Pashley-Johnson Fred, Guschin Viktor, Delafresnaye Laura, Truong Vinh X, Wagenknecht Hans-Achim, Barner-Kowollik Christopher
School of Chemistry and Physics, Centre for Materials Science, Queensland University of Technology (QUT), 2 George St, Brisbane, QLD, 4000, Australia.
Institute of Organic Chemistry, Karlsruhe Institute of Technology (KIT), Fritz-Haber-Weg 6, 76131, Karlsruhe, Germany.
Adv Sci (Weinh). 2024 Aug;11(29):e2402011. doi: 10.1002/advs.202402011. Epub 2024 Jun 9.
The wavelength-by-wavelength resolved photoreactivity of two photo-caged carboxylic acids, i. e. 7-(diethylamino)-coumarin- and 3-perylene-modified substrates, is investigated via photochemical action plots. The observed wavelength-dependent reactivity of the chromophores is contrasted with their absorption profile. The photochemical action plots reveal a remarkable mismatch between the maximum reactivity and the absorbance. Through the action plot data, the study is able to uncover photochemical reactivity maxima at longer and shorter wavelengths, where the molar absorptivity of the chromophores is strongly reduced. Finally, the laser experiments are translated to light emitting diode (LED) irradiation and show efficient visible-light-induced release in a near fully wavelength-orthogonal, sequence-independent fashion (λ = 405 nm, λ = 505 nm) with both chromophores in the same reaction solution. The herein pioneered wavelength orthogonal release systems open an avenue for releasing two different molecular cargos with visible light in a fully orthogonal fashion.
通过光化学作用曲线研究了两种光笼蔽羧酸（即7-（二乙氨基）-香豆素和3-苝修饰的底物）逐波长分辨的光反应活性。将观察到的发色团波长依赖性反应活性与其吸收光谱进行对比。光化学作用曲线揭示了最大反应活性与吸光度之间存在显著不匹配。通过作用曲线数据，该研究能够发现在较长和较短波长处的光化学反应活性最大值，而在这些波长处发色团的摩尔吸光系数大幅降低。最后，将激光实验转换为发光二极管（LED）照射，并表明在相同反应溶液中使用两种发色团时，能够以几乎完全波长正交、序列无关的方式（λ = 405 nm，λ = 505 nm）实现高效的可见光诱导释放。本文开创性的波长正交释放系统为以完全正交的方式用可见光释放两种不同的分子货物开辟了一条途径。
