Application of reference-modified density functional theory: Temperature and pressure dependences of solvation free energy

Tomonari Sumi, Yutaka Maruyama, Ayori Mitsutake, Kenji Mochizuki, Kenichiro Koga

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

Recently, we proposed a reference-modified density functional theory (RMDFT) to calculate solvation free energy (SFE), in which a hard-sphere fluid was introduced as the reference system instead of an ideal molecular gas. Through the RMDFT, using an optimal diameter for the hard-sphere reference system, the values of the SFE calculated at room temperature and normal pressure were in good agreement with those for more than 500 small organic molecules in water as determined by experiments. In this study, we present an application of the RMDFT for calculating the temperature and pressure dependences of the SFE for solute molecules in water. We demonstrate that the RMDFT has high predictive ability for the temperature and pressure dependences of the SFE for small solute molecules in water when the optimal reference hard-sphere diameter determined for each thermodynamic condition is used. We also apply the RMDFT to investigate the temperature and pressure dependences of the thermodynamic stability of an artificial small protein, chignolin, and discuss the mechanism of high-temperature and high-pressure unfolding of the protein.

Original languageEnglish
JournalJournal of Computational Chemistry
DOIs
Publication statusAccepted/In press - 2017

Fingerprint

Solvation
Density Functional
Free energy
Density functional theory
Free Energy
Molecules
Hard Spheres
Water
Thermodynamics
Temperature
Hard-sphere Fluid
Proteins
Protein
Unfolding
Thermodynamic stability
Gases
Calculate
Fluids
Demonstrate
Experiment

Keywords

  • 3D-RISM theory
  • Chignolin
  • Classical density functional theory
  • High-pressure unfolding
  • Hydrophobic solute
  • Protein
  • Temperature and pressure dependences of solvation free energy
  • Thermal denaturation

ASJC Scopus subject areas

  • Chemistry(all)
  • Computational Mathematics

Cite this

@article{c4b6321c0e2e4154a513f0a04053f393,
title = "Application of reference-modified density functional theory: Temperature and pressure dependences of solvation free energy",
abstract = "Recently, we proposed a reference-modified density functional theory (RMDFT) to calculate solvation free energy (SFE), in which a hard-sphere fluid was introduced as the reference system instead of an ideal molecular gas. Through the RMDFT, using an optimal diameter for the hard-sphere reference system, the values of the SFE calculated at room temperature and normal pressure were in good agreement with those for more than 500 small organic molecules in water as determined by experiments. In this study, we present an application of the RMDFT for calculating the temperature and pressure dependences of the SFE for solute molecules in water. We demonstrate that the RMDFT has high predictive ability for the temperature and pressure dependences of the SFE for small solute molecules in water when the optimal reference hard-sphere diameter determined for each thermodynamic condition is used. We also apply the RMDFT to investigate the temperature and pressure dependences of the thermodynamic stability of an artificial small protein, chignolin, and discuss the mechanism of high-temperature and high-pressure unfolding of the protein.",
keywords = "3D-RISM theory, Chignolin, Classical density functional theory, High-pressure unfolding, Hydrophobic solute, Protein, Temperature and pressure dependences of solvation free energy, Thermal denaturation",
author = "Tomonari Sumi and Yutaka Maruyama and Ayori Mitsutake and Kenji Mochizuki and Kenichiro Koga",
year = "2017",
doi = "10.1002/jcc.25101",
language = "English",
journal = "Journal of Computational Chemistry",
issn = "0192-8651",
publisher = "John Wiley and Sons Inc.",

}

TY - JOUR

T1 - Application of reference-modified density functional theory

T2 - Temperature and pressure dependences of solvation free energy

AU - Sumi, Tomonari

AU - Maruyama, Yutaka

AU - Mitsutake, Ayori

AU - Mochizuki, Kenji

AU - Koga, Kenichiro

PY - 2017

Y1 - 2017

N2 - Recently, we proposed a reference-modified density functional theory (RMDFT) to calculate solvation free energy (SFE), in which a hard-sphere fluid was introduced as the reference system instead of an ideal molecular gas. Through the RMDFT, using an optimal diameter for the hard-sphere reference system, the values of the SFE calculated at room temperature and normal pressure were in good agreement with those for more than 500 small organic molecules in water as determined by experiments. In this study, we present an application of the RMDFT for calculating the temperature and pressure dependences of the SFE for solute molecules in water. We demonstrate that the RMDFT has high predictive ability for the temperature and pressure dependences of the SFE for small solute molecules in water when the optimal reference hard-sphere diameter determined for each thermodynamic condition is used. We also apply the RMDFT to investigate the temperature and pressure dependences of the thermodynamic stability of an artificial small protein, chignolin, and discuss the mechanism of high-temperature and high-pressure unfolding of the protein.

AB - Recently, we proposed a reference-modified density functional theory (RMDFT) to calculate solvation free energy (SFE), in which a hard-sphere fluid was introduced as the reference system instead of an ideal molecular gas. Through the RMDFT, using an optimal diameter for the hard-sphere reference system, the values of the SFE calculated at room temperature and normal pressure were in good agreement with those for more than 500 small organic molecules in water as determined by experiments. In this study, we present an application of the RMDFT for calculating the temperature and pressure dependences of the SFE for solute molecules in water. We demonstrate that the RMDFT has high predictive ability for the temperature and pressure dependences of the SFE for small solute molecules in water when the optimal reference hard-sphere diameter determined for each thermodynamic condition is used. We also apply the RMDFT to investigate the temperature and pressure dependences of the thermodynamic stability of an artificial small protein, chignolin, and discuss the mechanism of high-temperature and high-pressure unfolding of the protein.

KW - 3D-RISM theory

KW - Chignolin

KW - Classical density functional theory

KW - High-pressure unfolding

KW - Hydrophobic solute

KW - Protein

KW - Temperature and pressure dependences of solvation free energy

KW - Thermal denaturation

UR - http://www.scopus.com/inward/record.url?scp=85033565824&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85033565824&partnerID=8YFLogxK

U2 - 10.1002/jcc.25101

DO - 10.1002/jcc.25101

M3 - Article

C2 - 29116647

AN - SCOPUS:85033565824

JO - Journal of Computational Chemistry

JF - Journal of Computational Chemistry

SN - 0192-8651

ER -