☆ 4.8 Article

Ring-Polymer Instanton Tunneling Splittings of Tropolone and Isotopomers using a ?-Machine Learned CCSD(T) Potential: Theory and Experiment Shake Hands

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2023)

相关参考文献

注意：仅列出部分参考文献，下载原文获取全部文献信息。

Article Chemistry, Physical

PESPIP: Software to fit complex molecular and many-body potential energy surfaces with permutationally invariant polynomials

Paul L. L. Houston et al.

Summary: This article describes a method for describing a potential energy surface using a basis of permutationally invariant polynomials. The coefficients of these polynomials are determined through numerical regression to fit a dataset of electronic energies and gradients smoothly. The article addresses questions on how to create an efficient basis, including selecting the appropriate polynomials, determining the number of polynomials needed, ensuring correct reproduction of zero interaction at large distances, maintaining special symmetries, and efficiently calculating gradients. The article also introduces programs to manipulate the polynomials and write efficient Fortran programs for energy and gradient calculations, along with a user-friendly interface for accessing symmetrization approach results. The software for these programs is publicly available.

JOURNAL OF CHEMICAL PHYSICS (2023)

添加到收藏夹

Article Chemistry, Physical

?-Machine Learned Potential Energy Surfaces and Force Fields

Joel M. Bowman et al.

Summary: There has been significant progress in developing machine learned potential energy surfaces (PESs) for molecules and clusters with more than 10 atoms. However, the level of electronic structure theory is generally limited to less than the gold standard CCSD(T) level due to the number of atoms. This Perspective focuses on a Delta-machine learning method that brings DFT-based PESs close to CCSD(T) accuracy. It also explores the extension of Delta-machine learning to force fields with many-body corrections.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2023)

添加到收藏夹

Article Chemistry, Multidisciplinary

Tunnelling assisted hydrogen elimination mechanisms of FeCl3/TEMPO

Shi-Jun Li et al.

Summary: Studies show that the low spin state of FeCl3/TEMPO is more favorable for hydrogen abstraction, with the N atom being the preferred hydrogen acceptor. It is discovered that dispersion interactions and nuclear tunneling can accelerate the reaction process.

CHEMICAL COMMUNICATIONS (2022)

添加到收藏夹

Article Chemistry, Physical

Heavy Atom Tunneling in Organic Reactions at Coupled Cluster Potential Accuracy with a Parallel Implementation of Anharmonic Constant Calculations and Semiclassical Transition State Theory

Giacomo Mandelli et al.

Summary: We describe and test a parallel implementation strategy for computing anharmonic constants and semiclassical transition state theory reaction rates. Our approach is more accurate and efficient compared to other software, and it allows for high-level evaluations of SCTST rates and heavy atom tunneling.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2022)

添加到收藏夹

Article Chemistry, Physical

Enabling Rapid and Accurate Construction of CCSD(T)-Level Potential Energy Surface of Large Molecules Using Molecular Tailoring Approach

Subodh S. Khire et al.

Summary: This study demonstrates the efficient construction of potential energy surfaces (PES) for molecules using the fragment-based molecular tailoring approach (MTA) and off-the-shelf hardware. The MTA method accurately captures energy barriers and shows excellent agreement with full calculation counterparts, with a time advantage factor of 3-5.

JOURNAL OF PHYSICAL CHEMISTRY A (2022)

添加到收藏夹

Article Chemistry, Physical

Vibrational Tunneling Spectra of Molecules with Asymmetric Wells: A Combined Vibrational Configuration Interaction and Instanton Approach

Mihael Erakovic et al.

Summary: A combined approach using VCI and semiclassical instanton theory was developed to study vibrational tunneling spectra of molecules with multiple wells in full dimensionality. The method accurately calculates low-lying vibrational states in systems with arbitrary number of minima, especially suited for systems with large potential barriers between wells and small tunneling splittings.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2022)

添加到收藏夹

Article Chemistry, Physical

Permutation-Invariant-Polynomial Neural-Network-Based Δ-Machine Learning Approach: A Case for the HO2 Self-Reaction and Its Dynamics Study

Yang Liu et al.

Summary: D-machine learning is a highly efficient method that improves the fit of potential energy surfaces using a small number of high-level energies. This study proposes a neural-network based approach to efficiently construct accurate potential energy surfaces for complex reactions.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2022)

添加到收藏夹

Article Chemistry, Multidisciplinary

Heavy-Atom Quantum Tunnelling in Spin Crossovers of Nitrenes

Eric R. Heller et al.

Summary: This study simulates two recent matrix-isolation experiments at cryogenic temperatures, revealing the failure of the commonly used weak-coupling method in describing deep-tunneling reactions. However, the more rigorous approach of semiclassical golden-rule instanton theory combined with double-hybrid density-functional theory and multireference perturbation theory successfully reproduces rate constants and kinetic isotope effects in good agreement with experiment. Additionally, these calculations identify the optimal tunnelling pathways, providing a molecular picture of the reaction mechanism.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2022)

添加到收藏夹

Article Chemistry, Physical

Quantum Calculations on a New CCSD(T) Machine-Learned Potential Energy Surface Reveal the Leaky Nature of Gas-Phase Trans and Gauche Ethanol Conformers

Apurba Nandi et al.

Summary: This study investigates the structure of ethanol using quantum calculations and a new ab initio potential energy surface. The results show that the ground state of ethanol resembles the trans conformer but also exhibits substantial delocalization to the gauche conformer. Deuterating the OH group partially quenches this effect. The findings have important implications for identifying and isolating the conformers of ethanol.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2022)

添加到收藏夹

Article Chemistry, Physical

Transfer Learning for Affordable and High-Quality Tunneling Splittings from Instanton Calculations

Silvan Kaser et al.

Summary: This study explores the combination of transfer learning with a low-level potential energy surface and high-level electronic structure theory, and applies it to malonaldehyde. The results demonstrate that high-level accuracy for tunneling splitting can be achieved by selecting 25-50 judiciously chosen structures, and the resulting high-level PES exhibits good overall quality.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2022)

添加到收藏夹

Article Chemistry, Physical

Permutation-Invariant-Polynomial Neural-Network-Based Delta-Machine Learning Approach: A Case for the HO2 Self-Reaction and Its Dynamics Study

Yang Liu et al.

Summary: The study introduces a neural network-based Delta-machine learning approach for efficiently constructing full-dimensional accurate potential energy surfaces of complex reactions. The flexibility of the neural network is utilized to efficiently sample points from the low-level data set and successfully elevate the newly fitted potential energy surface to a high-quality level.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2022)

添加到收藏夹

Article Chemistry, Multidisciplinary

Instanton calculations of tunneling splittings in chiral molecules

Nityananda Sahu et al.

Summary: The study reports ground state tunneling splittings of various axially chiral molecules using the ring-polymer instanton method. Different electronic structure calculation methods and basis sets were employed, showing results consistent with literature values and providing predictions for previously uncalculated molecules. The RPI method offers an effective way to estimate tunneling dynamics of complex chiral molecules.

JOURNAL OF COMPUTATIONAL CHEMISTRY (2021)

添加到收藏夹

Article Chemistry, Multidisciplinary

Spin Crossover of Thiophosgene via Multidimensional Heavy-Atom Quantum Tunneling

Eric R. Heller et al.

Summary: The study investigates the spin-crossover reaction of thiophosgene and proposes the semiclassical golden-rule instanton theory. It is found that the increase in the speed of the spin-crossover reaction is mainly attributed to multidimensional quantum tunneling effects.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

添加到收藏夹

Article Chemistry, Physical

Δ-machine learning for potential energy surfaces: A PIP approach to bring a DFT-based PES to CCSD(T) level of theory

Apurba Nandi et al.

Summary: The study presents a machine learning approach to improve the accuracy of potential energy surfaces based on low-level density functional theory energies and gradients. By using a simple equation and fitting high-dimensional PESs with the permutationally invariant polynomial method, the approach is demonstrated to be effective for multiple molecules. Results show excellent agreement with benchmark results, even with a relatively small number of CCSD(T) energies used for training.

JOURNAL OF CHEMICAL PHYSICS (2021)

添加到收藏夹

Article Chemistry, Physical

Breaking the Coupled Cluster Barrier for Machine-Learned Potentials of Large Molecules: The Case of 15-Atom Acetylacetone

Chen Qu et al.

Summary: The study represents a significant advancement in applying Delta machine learning method to the challenging case of acetylacetone, successfully deriving a new potential energy surface which shows a barrier height close to the benchmark value.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2021)

添加到收藏夹

Article Chemistry, Physical

Full-dimensional potential energy surface for acetylacetone and tunneling splittings

Chen Qu et al.

Summary: A full-dimensional potential energy surface for acetylacetone was presented using full and fragmented permutationally invariant polynomial approaches, showing tunneling splitting at different barrier heights. Calculations of electronic barrier height for H-atom transfer and splitting values were conducted using various methods, with results indicating fast evaluation of the fragmented surface.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2021)

添加到收藏夹

Review Chemistry, Multidisciplinary

Heavy-Atom Tunneling in Organic Reactions

Claire Castro et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

添加到收藏夹

Article Chemistry, Physical

Efficient Generation of Permutationally Invariant Potential Energy Surfaces for Large Molecules

Riccardo Conte et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2020)

添加到收藏夹

Article Chemistry, Physical

Analytic Route to Tunneling Splittings Using Semiclassical Perturbation Theory

Timothy A. H. Burd et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2020)

添加到收藏夹

Article Physics, Multidisciplinary

Reactive dynamics and spectroscopy of hydrogen transfer from neural network-based reactive potential energy surfaces

Silvan Kaser et al.

NEW JOURNAL OF PHYSICS (2020)

添加到收藏夹

Article Chemistry, Physical

Permutationally invariant polynomial potential energy surfaces for tropolone and H and D atom tunneling dynamics

Paul Houston et al.

JOURNAL OF CHEMICAL PHYSICS (2020)

添加到收藏夹

Article Chemistry, Organic

Heavy-Atom Tunneling Processes during Denitrogenation of 2,3-Diazabicyclo[2.2.1]hept-2-ene and Ring Closure of Cyclopentane-1,3-diyl Diradical. Stereoselectivity in Tunneling and Matrix Effect

Sujan K. Sarkar et al.

JOURNAL OF ORGANIC CHEMISTRY (2020)

添加到收藏夹

Article Chemistry, Physical

Instanton theory of tunneling in molecules with asymmetric isotopic substitutions

Elena Jahr et al.

JOURNAL OF CHEMICAL PHYSICS (2020)

添加到收藏夹

Article Chemistry, Physical

Using Gradients in Permutationally Invariant Polynomial Potential Fitting: A Demonstration for CH4 Using as Few as 100 Configurations

Apurba Nandi et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2019)

添加到收藏夹

Article Multidisciplinary Sciences

Approaching coupled cluster accuracy with a general-purpose neural network potential through transfer learning

Justin S. Smith et al.

NATURE COMMUNICATIONS (2019)

添加到收藏夹

Article Chemistry, Multidisciplinary

The Barrier to Proton Transfer in the Dimer of Formic Acid: A Pure Rotational Study

Weixing Li et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2019)

添加到收藏夹

Review Chemistry, Physical

Permutationally Invariant Potential Energy Surfaces

Chen Qu et al.

ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 69 (2018)

添加到收藏夹

Review Chemistry, Physical

Ring-polymer instanton theory

Jeremy O. Richardson

INTERNATIONAL REVIEWS IN PHYSICAL CHEMISTRY (2018)

添加到收藏夹

Article Chemistry, Physical

Perspective: Ring-polymer instanton theory

Jeremy O. Richardson

JOURNAL OF CHEMICAL PHYSICS (2018)

添加到收藏夹

Article Chemistry, Physical

Dual-Level Approach to Instanton Theory

Jan Meisner et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2018)

添加到收藏夹

Article Chemistry, Physical

Locating Instantons in Calculations of Tunneling Splittings: The Test Case of Malonaldehyde

Marko T. Cvitas et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2016)

添加到收藏夹

Article Multidisciplinary Sciences

Concerted hydrogen-bond breaking by quantum tunneling in the water hexamer prism

Jeremy O. Richardson et al.

SCIENCE (2016)

添加到收藏夹

Article Chemistry, Physical

Communication: An accurate full 15 dimensional permutationally invariant potential energy surface for the OH + CH4 → H2O + CH3 reaction

Jun Li et al.

JOURNAL OF CHEMICAL PHYSICS (2015)

添加到收藏夹

Review Chemistry, Multidisciplinary

Molecular Tailoring Approach: A Route for ab Initio Treatment of Large Clusters

Nityananda Sahu et al.

ACCOUNTS OF CHEMICAL RESEARCH (2014)

添加到收藏夹

Article Chemistry, Physical

A compact and accurate semi-global potential energy surface for malonaldehyde from constrained least squares regression

Wataru Mizukami et al.

JOURNAL OF CHEMICAL PHYSICS (2014)

添加到收藏夹

Article Chemistry, Physical

Theoretical studies of the tunneling splitting of malonaldehyde using the multiconfiguration time-dependent Hartree approach

Markus Schroeder et al.

JOURNAL OF CHEMICAL PHYSICS (2011)

添加到收藏夹

Article Chemistry, Physical

Instanton calculations of tunneling splittings for water dimer and trimer

Jeremy O. Richardson et al.

JOURNAL OF CHEMICAL PHYSICS (2011)

添加到收藏夹

Article Chemistry, Physical

Intramolecular proton transfer in malonaldehyde: Accurate multilayer multi-configurational time-dependent Hartree calculations

Thorsten Hammer et al.

JOURNAL OF CHEMICAL PHYSICS (2011)

添加到收藏夹

Article Chemistry, Physical

Ring-polymer instanton method for calculating tunneling splittings

Jeremy O. Richardson et al.

JOURNAL OF CHEMICAL PHYSICS (2011)

添加到收藏夹

Article Chemistry, Physical

Vibrational specificity of proton-transfer dynamics in ground-state tropolone

Daniel Murdock et al.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2010)

添加到收藏夹

Review Chemistry, Physical

Permutationally invariant potential energy surfaces in high dimensionality

Bastiaan J. Braams et al.

INTERNATIONAL REVIEWS IN PHYSICAL CHEMISTRY (2009)

添加到收藏夹

Article Chemistry, Physical

One-dimensional tunneling calculations in the imaginary-frequency, rectilinear saddle-point normal mode

Yimin Wang et al.

JOURNAL OF CHEMICAL PHYSICS (2008)

添加到收藏夹

Article Chemistry, Physical

Full-dimensional quantum calculations of ground-state tunneling splitting of malonaldehyde using an accurate ab initio potential energy surface

Yimin Wang et al.

JOURNAL OF CHEMICAL PHYSICS (2008)

添加到收藏夹

Article Chemistry, Physical

Tunneling splittings for O•••O Stretching and other vibrations of tropolone isotopomers observed in the infrared spectrum below 800 cm-1

Richard L. Redington et al.

JOURNAL OF PHYSICAL CHEMISTRY A (2008)

添加到收藏夹

Article Chemistry, Physical

Infrared Absorption Spectra in the Hydroxyl Stretching Regions of Gaseous Tropolone OHO Isotopomers

Richard L. Redington et al.

ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS (2008)

添加到收藏夹

Article Chemistry, Physical

A simple and efficient CCSD(T)-F12 approximation

Thomas B. Adler et al.

JOURNAL OF CHEMICAL PHYSICS (2007)

添加到收藏夹

Article Chemistry, Physical

Quantum tunneling in the midrange vibrational fundamentals of tropolone

Richard L. Redington et al.

JOURNAL OF PHYSICAL CHEMISTRY A (2006)

添加到收藏夹

Review Physics, Multidisciplinary

Multidimensional quantum dynamics and infrared spectroscopy of hydrogen bonds

K. Giese et al.

PHYSICS REPORTS-REVIEW SECTION OF PHYSICS LETTERS (2006)

添加到收藏夹

Article Chemistry, Physical

High-resolution studies of tropolone in the S0 and S1 electronic states:: Isotope driven dynamics in the zero-point energy levels -: art. no. 074309

JC Keske et al.

JOURNAL OF CHEMICAL PHYSICS (2006)

添加到收藏夹

Article Chemistry, Physical

The all-Cartesian reaction plane Hamiltonian:: Formulation and application to the H-atom transfer in tropolone -: art. no. 054315

K Giese et al.

JOURNAL OF CHEMICAL PHYSICS (2005)

添加到收藏夹

Article Chemistry, Physical

18O effects on the infrared spectrum and skeletal tunneling of tropolone -: art. no. 224311

RL Redington et al.

JOURNAL OF CHEMICAL PHYSICS (2005)

添加到收藏夹

Article Chemistry, Physical

Tunneling splitting in polyatomic molecules: Application to malonaldehyde

GV Mil'nikov et al.

JOURNAL OF CHEMICAL PHYSICS (2003)

添加到收藏夹

Article Chemistry, Physical

N2 pressure broadened Q branch spikes and vibration-contortion-rotation effects in the high resolution FTIR spectrum of tropolone

RL Redington et al.

CHEMICAL PHYSICS (2002)

添加到收藏夹

Article Chemistry, Physical

State-specific spectral doublets in the FTIR spectrum of gaseous tropolone

RL Redington et al.

JOURNAL OF PHYSICAL CHEMISTRY A (2002)

添加到收藏夹

Article Chemistry, Physical

IR spectra of tropolone(OH) and tropolone(OD)

RL Redington et al.

JOURNAL OF CHEMICAL PHYSICS (2000)

添加到收藏夹

Article Chemistry, Physical

H atom and heavy atom tunneling processes in tropolone

RL Redington

JOURNAL OF CHEMICAL PHYSICS (2000)

添加到收藏夹

© Peeref 2019-2024. All rights reserved.