Photoswitching an Isolated Donor–Acceptor Stenhouse Adduct,The Journal of Physical Chemistry Letters

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Photoswitching an Isolated Donor–Acceptor Stenhouse Adduct
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-01-24 00:00:00 , DOI: 10.1021/acs.jpclett.7b03402
James N. Bull ₁ , Eduardo Carrascosa ₁ , Neil Mallo ₂ , Michael S. Scholz ₁ , Gabriel da Silva ₃ , Jonathon E. Beves ₂ , Evan J. Bieske ₁

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Donor–acceptor Stenhouse adducts (DASAs) are a new class of photoswitching molecules with excellent fatigue resistance and synthetic tunability. Here, tandem ion mobility mass spectrometry coupled with laser excitation is used to characterize the photocyclization reaction of isolated, charge-tagged DASA molecules over the 450–580 nm range. The experimental maximum response at 530 nm agrees with multireference perturbation theory calculations for the S₁ ← S₀ transition maximum at 533 nm. Photocyclization in the gas phase involves absorption of at least two photons; the first photon induces Z–E isomerization from the linear isomer to metastable intermediate isomers, while the second photon drives another E–Z isomerization and 4π-electrocyclization reaction. Cyclization is thermally reversible in the gas phase with collisional excitation.

中文翻译：

光电开关隔离的供体-受体Stenhouse加合物

供体-受体Stenhouse加合物（DASAs）是一类新型的光开关分子，具有出色的抗疲劳性和合成可调性。在这里，串联离子迁移质谱与激光激发被用来表征在450-580 nm范围内分离的带电荷标签的DASA分子的光环化反应。在530 nm处的实验最大响应与在533 nm处的S ₁ ←S ₀跃迁最大值的多参考扰动理论计算相符。气相中的光环化涉及至少两个光子的吸收。第一个光子诱导Z – E异构化，从线性异构体转变为亚稳的中间异构体，而第二个光子驱动另一个E –Z异构化和4π-电环化反应。在碰撞激发下，环化反应在气相中是可热逆的。

更新日期：2018-01-24

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