Polarizable Embedding Combined with the Algebraic Diagrammatic Construction: Tackling Excited States in Biomolecular Systems.
Polarizable Embedding Combined with the Algebraic Diagrammatic Construction: Tackling Excited States in Biomolecular Systems.
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极化嵌入与代数示意图构建相结合：解决生物分子系统中的激发态
DOI：
10.1021/acs.jctc.8b00576
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发表时间：
2018
影响因子：
5.5
通讯作者：
J. Kongsted
中科院分区：
文献类型：
--
作者：
M. Scheurer;M. F. Herbst;P. Reinholdt;J. M. H. Olsen;A. Dreuw;J. Kongsted
通过将代数图构造(ADC)与可极化嵌入(PE)模型相结合，提出了一种改进的ADC方案。提出的PE-ADC方法通过二阶和三阶实现，旨在对大分子体系中的激发态进行精确计算。通过三个算例验证了该方法的准确性和大规模适用性，并进一步分析了在可极化环境存在的情况下，状态特定和线性响应型修正对激发能量的重要性。我们展示了我们的组合方法如何容易地应用于研究光诱导的生化过程，因为我们模拟了电荷转移(CT)激发，这是使用PE-ADC(2)的十二素蛋白光保护机制的关键。通过直接获取最新的激发态分析，我们发现极化环境起着决定性的作用，它显著增加了十二烷基酚的电子激发的CT特征。因此，PE-ADC适合于以高精度和合理的计算成本破译复杂的生物分子系统中的光诱导过程。
We present a variant of the algebraic diagrammatic construction (ADC) scheme by combining ADC with the polarizable embedding (PE) model. The presented PE-ADC method is implemented through second and third order and is designed with the aim of performing accurate calculations of excited states in large molecular systems. Accuracy and large-scale applicability are demonstrated with three case studies, and we further analyze the importance of both state-specific and linear-response-type corrections to the excitation energies in the presence of the polarizable environment. We demonstrate how our combined method can be readily applied to study photoinduced biochemical processes as we model the charge-transfer (CT) excitation which is key to the photoprotection mechanism in the dodecin protein with PE-ADC(2). Through direct access to state-of-the-art excited state analysis, we find that the polarizable environment plays a decisive role by significantly increasing the CT character of the electronic excitation in dodecin. PE-ADC is thus suited to decipher photoinduced processes in complex, biomolecular systems at high precision and at reasonable computational cost.
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影响因子：
3.3
作者：
Beerepoot, Maarten T. P.;Steindal, Arnfinn Hykkerud;Olsen, Jogvan Magnus Haugaard
通讯作者：
Olsen, Jogvan Magnus Haugaard
阻尼响应理论与可极化环境相结合：可极化嵌入复极化传播器方法。
影响因子：
5.5
作者：
Morten N. Pedersen;E. Hedegård;Jógvan Magnus Haugaard Olsen;J. Kauczor;P. Norman;J. Kongsted
通讯作者：
J. Kongsted
仔细研究 QM/MM 激发态计算中偏振的影响。
DOI：
10.1039/c1cp22067e
发表时间：
2011
期刊：
Physical chemistry chemical physics : PCCP
影响因子：
--
作者：
Kristian Sneskov;Tobias Schwabe;O. Christiansen;J. Kongsted
通讯作者：
J. Kongsted
评估偏振传播器代数图解构造方案中的受限虚拟空间近似以加速激发态计算
影响因子：
3
作者：
Chong Yang;A. Dreuw
通讯作者：
A. Dreuw
影响因子：
5.5
作者：
Mewes, Stefanie A.;Plasser, Felix;Dreuw, Andreas
通讯作者：
Dreuw, Andreas