VR-SCOSMO: A smooth conductor-like screening model with charge-dependent radii for modeling chemical reactions

Kuechler, Erich R.; Giese, Timothy J.; York, Darrin M.

doi:10.1063/1.4946779

Cited by 3 publications

(3 citation statements)

References 79 publications

(94 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…DFTB methods have similarly been developed to improve polarizabilities [55][56][57] and hydrogen bond strengths [58]. Exploratory DFTB methods have improved nonbond interactions by incorporating multipolar electrostatics [59][60][61][62][63], and DFTB pairwise potentials continue to be parametrized to widen the scope of applications [64][65][66][67][68][69].…”

Section: Intra-fragment Qm Hamiltoniansmentioning

confidence: 99%

Quantum mechanical force fields for condensed phase molecular simulations

Giese

York

2017

J. Phys.: Condens. Matter

View full text Add to dashboard Cite

Molecular simulations are powerful tools for providing atomic-level details into complex chemical and physical processes that occur in the condensed phase. For strongly interacting systems where quantum many-body effects are known to play an important role, density-functional methods are often used to provide the model for the potential energy used to drive dynamics. These methods, however, suffer from two major drawbacks. First, they are often too computationally intensive to practically apply to large systems over long time scales, limiting their scope of application. Second, there remain challenges for these models to obtain the necessary level of accuracy for weak non-bonded interactions to obtain quantitative accuracy for a wide range of condensed phase properties. Quantum mechanical force fields (QMFFs) provide a potential solution to both of these limitations. In this review, we address recent advances in the development of QMFFs for condensed phase simulations. In particular, we examine the development of QMFF models using both approximate and ab initio density-functional models, the treatment of short-ranged non-bonded and long-ranged electrostatic interactions, and stability issues in molecular dynamics calculations. Example calculations are provided for crystalline systems, liquid water, and ionic liquids. We conclude with a perspective for emerging challenges and future research directions.

show abstract

Section: Intra-fragment Qm Hamiltoniansmentioning

confidence: 99%

Quantum mechanical force fields for condensed phase molecular simulations

Giese

York

2017

J. Phys.: Condens. Matter

View full text Add to dashboard Cite

show abstract

“…Previous attempts to include information about the system for the determination of the solute cavity are mostly focusing on water as the solvent and are either limited to certain atoms or functional groups or are developed for specific applications with a narrow range of training data. , Other, more sophisticated approaches based on an isocontour of the electron density introduce a significant additional computational effort and typically lack analytical energy gradients. , …”

mentioning

confidence: 99%

“…21 Previous attempts to include information about the system for the determination of the solute cavity are mostly focusing on water as the solvent and are either limited to certain atoms or functional groups 23 or are developed for specific applications with a narrow range of training data. 24,25 Other, more sophisticated approaches based on an isocontour of the electron density introduce a significant additional computational effort and typically lack analytical energy gradients. 26,27 Here, we present a generally applicable and efficient approach for determining system-specific atom radii for solute cavity construction based on the molecular environment, termed Dynamic Radii Adjustment for COntinuum solvation (DRACO) .…”

mentioning

confidence: 99%

Improving Quantum Chemical Solvation Models by Dynamic Radii Adjustment for Continuum Solvation (DRACO)

Plett,

Stahn,

Bursch

et al. 2024

J. Phys. Chem. Lett.

View full text Add to dashboard Cite

We present the Dynamic Radii Adjustment for COntinuum solvation (DRACO) approach, which employs precomputed atomic partial charges and coordination numbers of the solute atoms to improve the solute cavity. As such, DRACO is compatible with major solvation models, improving their performance significantly and robustly at virtually no extra cost, especially for charged solutes. Combined with the purely electrostatic CPCM and COSMO models, DRACO reduces the mean absolute deviation (MAD) of the solvation free energy by up to 4.5 kcal mol −1 (67%) for a large data set of polar and ionic solutes. Even in combination with the highly empirical universal solvation model (SMD), DRACO substantially reduces the MAD for charged solutes by up to 1.5 kcal mol −1 (39%), while neutral solutes are slightly improved (0.2 kcal mol −1 or 16%). We present an interface of DRACO with two computationally efficient atomic charge models that enables fully automated, out-of-the-box calculations with the widely used program packages ORCA and TURBOMOLE.

show abstract

Excited state gradients for a state-specific continuum solvation approach: The vertical excitation model within a Lagrangian TDDFT formulation

Guido

Scalmani²,

Mennucci

et al. 2017

The Journal of Chemical Physics

View full text Add to dashboard Cite

The accurate modeling of the environment response is a fundamental challenge for accurately describing the photophysics and photochemistry of molecules both in solution and in more complex embeddings. When large rearrangements of the electron density occur after an electronic transition, state-specific formulations, such as the vertical excitation model, are necessary to achieve a proper modeling of the processes. Such a state-specific model is fundamental not only to obtain accurate energies, but also to follow the geometrical relaxation accompanying the evolution of the excited-states. This study presents the analytical expression of the gradients of the vertical excitation model approach by a Lagrangian formulation in the time dependent density functional theory framework. Representative organic chromophores in solution are used to test the reliability of the implementation and provide comparisons with the linear response description.

show abstract

VR-SCOSMO: A smooth conductor-like screening model with charge-dependent radii for modeling chemical reactions

Cited by 3 publications

References 79 publications

Quantum mechanical force fields for condensed phase molecular simulations

Quantum mechanical force fields for condensed phase molecular simulations

Improving Quantum Chemical Solvation Models by Dynamic Radii Adjustment for Continuum Solvation (DRACO)

Excited state gradients for a state-specific continuum solvation approach: The vertical excitation model within a Lagrangian TDDFT formulation

Contact Info

Product

Resources

About