Excited-state solvation structure of transition metal complexes from molecular dynamics simulations and assessment of partial atomic charge methods

Mostafa Abedi, Gianluca Levi, Diana B. Zederkof, Niels E. Henriksen, Mátyás Pápai, Klaus B. Møller*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

In this work, we investigate the excited-state solute and solvation structure of [Ru(bpy)3]2+, [Fe(bpy)3]2+, [Fe(bmip)2]2+ and [Cu(phen)2]+ (bpy = 2,2'-bipyridine; bmip = 2,6-bis(3-methyl-imidazole-1-ylidine)-pyridine; phen = 1,10-phenanthroline) transition metal complexes (TMCs) in terms of solute-solvent radial distribution functions (RDFs) and evaluate the performance of some of the most popular partial atomic charge (PAC) methods for obtaining these RDFs by molecular dynamics (MD) simulations. To this end, we compare classical MD of a frozen solute in water and acetonitrile (ACN) with quantum mechanics/molecular mechanics Born-Oppenheimer molecular dynamics (QM/MM BOMD) simulations. The calculated RDFs show that the choice of a suitable PAC method is dependent on the coordination number of the metal, denticity of the ligands, and type of solvent. It is found that this selection is less sensitive for water than ACN. Furthermore, a careful choice of the PAC method should be considered for TMCs that exhibit a free direct coordination site, such as [Cu(phen)2]+. The results of this work show that fast classical MD simulations with ChelpG/RESP or CM5 PACs can produce RDFs close to those obtained by QM/MM MD and thus, provide reliable solvation structures of TMCs to be used, e.g. in the analysis of scattering data.
Original languageEnglish
JournalPhysical Chemistry Chemical Physics
Volume21
Issue number7
Pages (from-to)4082-4095
Number of pages14
ISSN1463-9076
DOIs
Publication statusPublished - 2019

Cite this

@article{5d5eef3d1e9e4c8684cdf7562591fccd,
title = "Excited-state solvation structure of transition metal complexes from molecular dynamics simulations and assessment of partial atomic charge methods",
abstract = "In this work, we investigate the excited-state solute and solvation structure of [Ru(bpy)3]2+, [Fe(bpy)3]2+, [Fe(bmip)2]2+ and [Cu(phen)2]+ (bpy = 2,2'-bipyridine; bmip = 2,6-bis(3-methyl-imidazole-1-ylidine)-pyridine; phen = 1,10-phenanthroline) transition metal complexes (TMCs) in terms of solute-solvent radial distribution functions (RDFs) and evaluate the performance of some of the most popular partial atomic charge (PAC) methods for obtaining these RDFs by molecular dynamics (MD) simulations. To this end, we compare classical MD of a frozen solute in water and acetonitrile (ACN) with quantum mechanics/molecular mechanics Born-Oppenheimer molecular dynamics (QM/MM BOMD) simulations. The calculated RDFs show that the choice of a suitable PAC method is dependent on the coordination number of the metal, denticity of the ligands, and type of solvent. It is found that this selection is less sensitive for water than ACN. Furthermore, a careful choice of the PAC method should be considered for TMCs that exhibit a free direct coordination site, such as [Cu(phen)2]+. The results of this work show that fast classical MD simulations with ChelpG/RESP or CM5 PACs can produce RDFs close to those obtained by QM/MM MD and thus, provide reliable solvation structures of TMCs to be used, e.g. in the analysis of scattering data.",
author = "Mostafa Abedi and Gianluca Levi and Zederkof, {Diana B.} and Henriksen, {Niels E.} and M{\'a}ty{\'a}s P{\'a}pai and M{\o}ller, {Klaus B.}",
year = "2019",
doi = "10.1039/c8cp06567e",
language = "English",
volume = "21",
pages = "4082--4095",
journal = "Physical Chemistry Chemical Physics",
issn = "1463-9076",
publisher = "Royal Society of Chemistry",
number = "7",

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TY - JOUR

T1 - Excited-state solvation structure of transition metal complexes from molecular dynamics simulations and assessment of partial atomic charge methods

AU - Abedi, Mostafa

AU - Levi, Gianluca

AU - Zederkof, Diana B.

AU - Henriksen, Niels E.

AU - Pápai, Mátyás

AU - Møller, Klaus B.

PY - 2019

Y1 - 2019

N2 - In this work, we investigate the excited-state solute and solvation structure of [Ru(bpy)3]2+, [Fe(bpy)3]2+, [Fe(bmip)2]2+ and [Cu(phen)2]+ (bpy = 2,2'-bipyridine; bmip = 2,6-bis(3-methyl-imidazole-1-ylidine)-pyridine; phen = 1,10-phenanthroline) transition metal complexes (TMCs) in terms of solute-solvent radial distribution functions (RDFs) and evaluate the performance of some of the most popular partial atomic charge (PAC) methods for obtaining these RDFs by molecular dynamics (MD) simulations. To this end, we compare classical MD of a frozen solute in water and acetonitrile (ACN) with quantum mechanics/molecular mechanics Born-Oppenheimer molecular dynamics (QM/MM BOMD) simulations. The calculated RDFs show that the choice of a suitable PAC method is dependent on the coordination number of the metal, denticity of the ligands, and type of solvent. It is found that this selection is less sensitive for water than ACN. Furthermore, a careful choice of the PAC method should be considered for TMCs that exhibit a free direct coordination site, such as [Cu(phen)2]+. The results of this work show that fast classical MD simulations with ChelpG/RESP or CM5 PACs can produce RDFs close to those obtained by QM/MM MD and thus, provide reliable solvation structures of TMCs to be used, e.g. in the analysis of scattering data.

AB - In this work, we investigate the excited-state solute and solvation structure of [Ru(bpy)3]2+, [Fe(bpy)3]2+, [Fe(bmip)2]2+ and [Cu(phen)2]+ (bpy = 2,2'-bipyridine; bmip = 2,6-bis(3-methyl-imidazole-1-ylidine)-pyridine; phen = 1,10-phenanthroline) transition metal complexes (TMCs) in terms of solute-solvent radial distribution functions (RDFs) and evaluate the performance of some of the most popular partial atomic charge (PAC) methods for obtaining these RDFs by molecular dynamics (MD) simulations. To this end, we compare classical MD of a frozen solute in water and acetonitrile (ACN) with quantum mechanics/molecular mechanics Born-Oppenheimer molecular dynamics (QM/MM BOMD) simulations. The calculated RDFs show that the choice of a suitable PAC method is dependent on the coordination number of the metal, denticity of the ligands, and type of solvent. It is found that this selection is less sensitive for water than ACN. Furthermore, a careful choice of the PAC method should be considered for TMCs that exhibit a free direct coordination site, such as [Cu(phen)2]+. The results of this work show that fast classical MD simulations with ChelpG/RESP or CM5 PACs can produce RDFs close to those obtained by QM/MM MD and thus, provide reliable solvation structures of TMCs to be used, e.g. in the analysis of scattering data.

U2 - 10.1039/c8cp06567e

DO - 10.1039/c8cp06567e

M3 - Journal article

VL - 21

SP - 4082

EP - 4095

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

SN - 1463-9076

IS - 7

ER -