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Computational Photophysics in the Presence of an Environment
Annual Review of Physical Chemistry ( IF 14.7 ) Pub Date : 2018-04-20 00:00:00 , DOI: 10.1146/annurev-physchem-050317-021013
Juan J. Nogueira 1 , Leticia González 1
Affiliation  

Most processes triggered by ultraviolet (UV) or visible (vis) light in nature take place in complex biological environments. The first step in these photophysical events is the excitation of the absorbing system or chromophore to an electronically excited state. Such an excitation can be monitored by the UV-vis absorption spectrum. A precise calculation of the UV-vis spectrum of a chromophore embedded in an environment is a challenging task that requires the consideration of several ingredients, besides an accurate electronic-structure method for the excited states. Two of the most important are an appropriate description of the interactions between the chromophore and the environment and accounting for the vibrational motion of the whole system. In this contribution, we review the most common theoretical methodologies to describe the environment (including quantum mechanics/continuum and quantum mechanics/molecular mechanics models) and to account for vibrational sampling (including Wigner sampling and molecular dynamics). Further, we illustrate in a series of examples how the lack of these ingredients can lead to a wrong interpretation of the electronic features behind the UV-vis absorption spectrum.

中文翻译:


环境中的计算光物理

自然界中,大多数由紫外线(UV)或可见光(vis)触发的过程都发生在复杂的生物环境中。这些光物理事件的第一步是将吸收系统或生色团激发到电子激发态。可以通过紫外可见吸收光谱监测这种激发。精确计算嵌入环境中的发色团的UV-vis光谱是一项艰巨的任务,除了要考虑激发态的精确电子结构方法外,还需要考虑几种成分。最重要的两个是对发色团与环境之间相互作用的恰当描述,并考虑了整个系统的振动运动。在这笔捐款中,我们回顾了最常见的理论方法来描述环境(包括量子力学/连续谱和量子力学/分子力学模型)并解释振动采样(包括维格纳采样和分子动力学)。此外,我们在一系列示例中说明了这些成分的缺乏如何导致对UV-vis吸收光谱背后的电子特征的错误解释。

更新日期:2018-04-20
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