Efficient Calculation of Absorption Spectra in Solution: Approaches for Selecting Representative Solvent Configurations and for Reducing the Number of Explicit Solvent Molecules

Citation: XUE Bai, CHEN Tiannan, SIEPMANN J. Ilja. Efficient Calculation of Absorption Spectra in Solution: Approaches for Selecting Representative Solvent Configurations and for Reducing the Number of Explicit Solvent Molecules[J]. Acta Physico-Chimica Sinica, 2018, 34(10): 1106-1115. doi: 10.3866/PKU.WHXB201701083 shu

Efficient Calculation of Absorption Spectra in Solution: Approaches for Selecting Representative Solvent Configurations and for Reducing the Number of Explicit Solvent Molecules

1.
Department of Chemistry and Chemical Theory Center, University of Minnesota, 207 Pleasant Street SE, Minneapolis, MN 55455-0240, USA
2.
Department of Chemical Engineering and Materials Science, University of Minnesota, 421 Washington Avenue SE, Minneapolis, MN 55455-0132, USA
†.
Current address: Department of Computer Science and Engineering, University of Minnesota, 200 Union Street SE, Minneapolis, MN 55455-0154, USA

通讯作者: SIEPMANNJ.Ilja, siepmann@umn.edu

摘要: Dye-sensitized solar cells (DSSCs) are one of the most promising renewable energy technologies. Charge transfer and charge transport are pivotal processes in DSSCs, which govern solar energy capture and conversion. These processes can be probed using modern electronic structure methods. Because of the heterogeneity and complexity of the local environment of a chromophore in DSSCs (such as solvatochromism and chromophore aggregation), a part of the solvation environment should be treated explicitly during the calculation. However, because of the high computational cost and unfavorable scaling with the number of electrons of high-level quantum mechanical methods, approaches to explicitly treat the local environment need careful consideration. Two problems must be tackled to reduce computational cost. First, the number of configurations representing the solvent distribution should be limited as much as possible. Second, the size of the explicit region should be kept relatively small. The purpose of this study is to develop efficient computational approaches to select representative configurations and to limit the explicit solvent region to reduce the computational cost for later (higher-level) quantum mechanical calculations. For this purpose, an ensemble of solvent configurations around a 1-methyl-8-oxyquinolinium betaine (QB) dye molecule was generated using Monte Carlo simulations and molecular mechanics force fields. Then, a fitness function was developed using data from inexpensive electronic structure calculations to reduce the number of configurations. Specific solvent molecules were also selected for explicit treatment based on a distance criterion, and those not selected were treated as background charges. The configurations and solvent molecules selected proved to be good representatives of the entire ensemble; thus, expensive electronic structure calculations need to be performed only on this subset of the system, which significantly reduces the computational cost.

关键词:

English

Efficient Calculation of Absorption Spectra in Solution: Approaches for Selecting Representative Solvent Configurations and for Reducing the Number of Explicit Solvent Molecules

1.
Department of Chemistry and Chemical Theory Center, University of Minnesota, 207 Pleasant Street SE, Minneapolis, MN 55455-0240, USA
2.
Department of Chemical Engineering and Materials Science, University of Minnesota, 421 Washington Avenue SE, Minneapolis, MN 55455-0132, USA
†.
Current address: Department of Computer Science and Engineering, University of Minnesota, 200 Union Street SE, Minneapolis, MN 55455-0154, USA

Corresponding author: SIEPMANN J. Ilja, siepmann@umn.edu

Received Date: 14 December 2017
Accepted Date: 04 January 2018
Revised Date: 03 January 2018
Available Online: 15 October 2018

Abstract: Dye-sensitized solar cells (DSSCs) are one of the most promising renewable energy technologies. Charge transfer and charge transport are pivotal processes in DSSCs, which govern solar energy capture and conversion. These processes can be probed using modern electronic structure methods. Because of the heterogeneity and complexity of the local environment of a chromophore in DSSCs (such as solvatochromism and chromophore aggregation), a part of the solvation environment should be treated explicitly during the calculation. However, because of the high computational cost and unfavorable scaling with the number of electrons of high-level quantum mechanical methods, approaches to explicitly treat the local environment need careful consideration. Two problems must be tackled to reduce computational cost. First, the number of configurations representing the solvent distribution should be limited as much as possible. Second, the size of the explicit region should be kept relatively small. The purpose of this study is to develop efficient computational approaches to select representative configurations and to limit the explicit solvent region to reduce the computational cost for later (higher-level) quantum mechanical calculations. For this purpose, an ensemble of solvent configurations around a 1-methyl-8-oxyquinolinium betaine (QB) dye molecule was generated using Monte Carlo simulations and molecular mechanics force fields. Then, a fitness function was developed using data from inexpensive electronic structure calculations to reduce the number of configurations. Specific solvent molecules were also selected for explicit treatment based on a distance criterion, and those not selected were treated as background charges. The configurations and solvent molecules selected proved to be good representatives of the entire ensemble; thus, expensive electronic structure calculations need to be performed only on this subset of the system, which significantly reduces the computational cost.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

Efficient Calculation of Absorption Spectra in Solution: Approaches for Selecting Representative Solvent Configurations and for Reducing the Number of Explicit Solvent Molecules

通讯作者: SIEPMANNJ.Ilja, siepmann@umn.edu

English

Efficient Calculation of Absorption Spectra in Solution: Approaches for Selecting Representative Solvent Configurations and for Reducing the Number of Explicit Solvent Molecules

Corresponding author: SIEPMANN J. Ilja, siepmann@umn.edu

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Efficient Calculation of Absorption Spectra in Solution: Approaches for Selecting Representative Solvent Configurations and for Reducing the Number of Explicit Solvent Molecules

通讯作者: SIEPMANNJ.Ilja, siepmann@umn.edu

English

Efficient Calculation of Absorption Spectra in Solution: Approaches for Selecting Representative Solvent Configurations and for Reducing the Number of Explicit Solvent Molecules

Corresponding author: SIEPMANN J. Ilja, siepmann@umn.edu

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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