Surface hopping modeling of two-dimensional spectra.
Surface hopping modeling of two-dimensional spectra.
复制标题
二维光谱的表面跳跃建模。
DOI：
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发表时间：
2013
影响因子：
4.4
通讯作者：
T. I. Jansen
中科院分区：
文献类型：
--
作者：
Roel Tempelaar;C. P. van der Vegte;J. Knoester;T. I. Jansen
最近，二维（2D）电子光谱已成为揭示复杂分子组装体（例如生物光捕获系统）激发态特性的重要工具。在这项工作中，我们提出了一种基于表面跳跃方法模拟二维电子光谱的方法。这种方法自洽地描述了光敏发色团与环境之间的相互作用，这使我们能够重现光谱可观察的动态斯托克斯位移。通过对二聚体的应用，该方法还可以解释量子布居的正确热平衡，这对于电子领域的过程非常重要。结果发现，所得到的二维光谱与运动方程计算的层次结构非常吻合。与后者相反，我们的方法在描述发色团与环境之间的相互作用方面不受限制，我们期望它适用于各种分子系统。
Recently, two-dimensional (2D) electronic spectroscopy has become an important tool to unravel the excited state properties of complex molecular assemblies, such as biological light harvesting systems. In this work, we propose a method for simulating 2D electronic spectra based on a surface hopping approach. This approach self-consistently describes the interaction between photoactive chromophores and the environment, which allows us to reproduce a spectrally observable dynamic Stokes shift. Through an application to a dimer, the method is shown to also account for correct thermal equilibration of quantum populations, something that is of great importance for processes in the electronic domain. The resulting 2D spectra are found to nicely agree with hierarchy of equations of motion calculations. Contrary to the latter, our method is unrestricted in describing the interaction between the chromophores and the environment, and we expect it to be applicable to a wide variety of molecular systems.
影响因子：
3.3
作者：
Olbrich, Carsten;Jansen, Thomas L. C.;Liebers, Joerg;Aghtar, Mortaza;Struempfer, Johan;Schulten, Klaus;Knoester, Jasper;Kleinekathoefer, Ulrich
通讯作者：
Kleinekathoefer, Ulrich
影响因子：
56.9
作者：
Aeschlimann, Martin;Brixner, Tobias;Voronine, Dmitri V.
通讯作者：
Voronine, Dmitri V.