量子振动微扰方法及应用
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- 英文论文题名：Quantum Vibrational Perturbation Approach for Computing Infrared Probe Spectra
- 论文作者：薛瑞杰 ; 从阳 ; 侯丹 ; 曲泽星 ; 李辉 ; 高加力
- 英文论文作者：Rui-Jie Xue ; Yang Cong ; Ze-Xing Qu ; Hui Li ; Jiali Gao ; Institute of Theoretical Chemistry ; Jilin University
- 年：2016
- 作者机构：吉林大学理论化学研究所;
- 论文关键词：振动光谱 ; 振动频率位移 ; 气溶胶 ; 量子力学和分子力学 ; 蛋白质动力学
- 英文论文关键词：Infrared spectra ; vibrational frequency shifts ; aerosol ; QM/MM ; protein dynamics
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第十九分会：化学中的量子与经典动力学
- 语种：中文
- 分类号：O657.3
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第十九分会 ; 化学中的量子与经典动力学
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：133k
- 原文格式：D
- 会议级别：全国
摘要
红外探针光谱,不仅在解析复杂生物蛋白质结构和动力学,揭示构象结构、动力学过程与生物蛋白功能的内在联系,理解蛋白质内部的氢键网络、静电势、蛋白质折叠与聚集、酶催化反应机理等方面被广泛应用[1,2],而且在量子溶剂微观超流研究中也扮演重要的角色[3,4]。然而,定量解释实验光谱观测依然是理论物理化学家们长期面临的一项重要挑战,主要归咎于凝聚相体系的大尺度、超快过程、核振动的量子效应。最近,基于微扰理论和离散变分法,结合分子动力学取样和QM/MM势能计算,我们发展了新的一维、二维红外探针光谱计算新方法,并成功的应用于气溶胶、弱酸强酸水溶液等红外探针光谱的模拟。理论光谱的位置和形状与实验结果都很好的吻合。局部振动模间的偶合、非谐性及有效的约化维数的处理方法将进行深入的讨论。
Site-specific infrared(IR) probe spectra provide a unique way to reveal the local electrostatic field, microscopic conformation, interaction and dynamics of the chemical and biological processes in condense phase. However, up to date, quantitative interpretation of experimental spectra is still a major challenge due to the fast time scale, nuclear quantum effects and large-scale systems with complicated surrounding solvent. In this work, we propose a quick and accurate new approach to simulate 1D or 2D-IR spectra, which is a semi-classical method through a combination of the classical sampling the intermolecular structures, and quantum treatment of the time-depended transition frequencies of a specific vibrational mode based on the first-order perturbation approximation. The IR spectra obtained in this way can replicate not only the peak position but also the line shape of the experimental spectra accurately. This method was successfully applied in studies of the infrared spectra of aerosol, weak or strong water solution, and complicated biological systems.
Site-specific infrared(IR) probe spectra provide a unique way to reveal the local electrostatic field, microscopic conformation, interaction and dynamics of the chemical and biological processes in condense phase. However, up to date, quantitative interpretation of experimental spectra is still a major challenge due to the fast time scale, nuclear quantum effects and large-scale systems with complicated surrounding solvent. In this work, we propose a quick and accurate new approach to simulate 1D or 2D-IR spectra, which is a semi-classical method through a combination of the classical sampling the intermolecular structures, and quantum treatment of the time-depended transition frequencies of a specific vibrational mode based on the first-order perturbation approximation. The IR spectra obtained in this way can replicate not only the peak position but also the line shape of the experimental spectra accurately. This method was successfully applied in studies of the infrared spectra of aerosol, weak or strong water solution, and complicated biological systems.
引文
[1]Fried S.D;Bagchi S.;Boxer S.G.,Science.2014,346:1510.
[2]Jeon J.;Yang S.;Choi J.H.and Cho M.,Acc.Chem.Rev.2013,113:5817.
[3]Grebenev S.;Sartakov B.;Toennies J.P.;Vilesov A.F.,Science.2000,289:1532.
[4]Li H.;Le Roy R.J.;Roy P.-N.;Mc Kellar A.R.W,Phys.Rev.Lett.2010,105:133401.
[5]Hou D.,Ma Y.-T.;Zhang X.-L.;Li H.,J.Chem.Phys.2016,144:014301.
[6]Xue R.-J.;Qu Z.-X.;Li H.;Gao J.,2016,submitted.
[2]Jeon J.;Yang S.;Choi J.H.and Cho M.,Acc.Chem.Rev.2013,113:5817.
[3]Grebenev S.;Sartakov B.;Toennies J.P.;Vilesov A.F.,Science.2000,289:1532.
[4]Li H.;Le Roy R.J.;Roy P.-N.;Mc Kellar A.R.W,Phys.Rev.Lett.2010,105:133401.
[5]Hou D.,Ma Y.-T.;Zhang X.-L.;Li H.,J.Chem.Phys.2016,144:014301.
[6]Xue R.-J.;Qu Z.-X.;Li H.;Gao J.,2016,submitted.
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