Resonance Raman Optical Activity Shows Unusual Structural Sensitivity for Systems in Resonance with Multiple Excited States: Vitamin B12 Case.,The Journal of Physical Chemistry Letters

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Resonance Raman Optical Activity Shows Unusual Structural Sensitivity for Systems in Resonance with Multiple Excited States: Vitamin B12 Case.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-06-05 , DOI: 10.1021/acs.jpclett.0c01218
Ewa Machalska _{1,

2} , Grzegorz Zajac ₂ , Anna Gruca _{1,

2} , Fabio Zobi ₃ , Malgorzata Baranska _{1,

2} , Agnieszka Kaczor _{1,

2}

Affiliation

In this work, cobalamins with different upper axial substituents and a cobalamin derivative with a ring modification were studied using chiroptical spectroscopies, in particular resonance Raman optical activity (RROA), to shed light on the influence of structural modifications on RROA spectra in these strongly chiral systems in resonance with multiple excited states at 532 nm excitation. We have demonstrated that for these unique systems RROA possesses augmented structural specificity, surpassing resonance Raman spectroscopy and enabling at the same time measurement of cobalamins at fairy low concentrations of ∼10^–5 mol dm^–3. The enhanced structural specificity of RROA is a result of bisignate spectra due to resonance via more than one electronic state. The observation of increased structural capability of RROA for cobalamins opens a new perspective for studying chiral properties of other biological systems incorporating d-metal ions.

中文翻译：

共振拉曼光学活性显示与多个激发态共振的系统具有异常的结构敏感性：维生素B12案例。

在这项工作中，使用手性光谱学，特别是共振拉曼光学活性（RROA），研究了具有不同上轴向取代基的钴胺素和具有环修饰的钴胺素衍生物，以揭示这些强手性化合物中结构修饰对RROA光谱的影响。系统在532 nm激发下具有多个激发态的共振。我们已经证明，对于这些独特的系统，ROROA具有增强的结构特异性，超越了共振拉曼光谱，并能够同时测量低至约10 ^–5 mol dm ^–3的钴胺素。。RROA增强的结构特异性是由于通过一个以上电子状态的共振而产生的双符号光谱的结果。RROA对钴胺素结构能力增强的观察为研究其他掺入d-金属离子的生物系统的手性提供了新的视角。

更新日期：2020-07-02

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