A Feynman dispersion correction: a proof of principle for MNDO

Kriebel, Maximilian; Weber, K.; Clark, Timothy

doi:10.1007/s00894-018-3874-6

Cited by 8 publications

(7 citation statements)

References 51 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…This issue has been addressed by including special hydrogen bond corrections in MNDO-type methods. ,− , In contrast, the OM x methods treat hydrogen-bonding interactions even without such corrections reasonably well, ,,, while inclusion of dispersion corrections generally further improves the accuracy. , One should note, however, that the addition of empirical attractive dispersion corrections to any semiempirical Hamiltonian parametrized without such corrections will inevitably deteriorate the accuracy of the computed heats of formation (which will become too small), while the computed relative energies may become more or less accurate. , Hence, it is more consistent to reparametrize the Hamiltonian with inclusion of dispersion corrections. This has so far been done only in PM7, which however suffers from error accumulation in very large noncovalent complexes, , and in the proof-of-principle MNDO-F method, which still has large errors in heats of formation.…”

Section: Introductionmentioning

confidence: 99%

Semiempirical Quantum-Chemical Methods with Orthogonalization and Dispersion Corrections

Dral

Thiel

2019

J. Chem. Theory Comput.

View full text Add to dashboard Cite

We present two new semiempirical quantum-chemical methods with orthogonalization and dispersion corrections: ODM2 and ODM3 (ODMx). They employ the same electronic structure model as the OM2 and OM3 (OMx) methods, respectively. In addition, they include Grimme’s dispersion correction D3 with Becke–Johnson damping and three-body corrections EABC for Axilrod–Teller–Muto dispersion interactions as integral parts. Heats of formation are determined by adding explicitly computed zero-point vibrational energy and thermal corrections, in contrast to standard MNDO-type and OMx methods. We report ODMx parameters for hydrogen, carbon, nitrogen, oxygen, and fluorine that are optimized with regard to a wide range of carefully chosen state-of-the-art reference data. Extensive benchmarks show that the ODMx methods generally perform better than the available MNDO-type and OMx methods for ground-state and excited-state properties, while they describe noncovalent interactions with similar accuracy as OMx methods with a posteriori dispersion corrections.

show abstract

Section: Introductionmentioning

confidence: 99%

Semiempirical Quantum-Chemical Methods with Orthogonalization and Dispersion Corrections

Dral

Thiel

2019

J. Chem. Theory Comput.

View full text Add to dashboard Cite

show abstract

“…Van der Waals interactions are divided into an attractive (dispersion) and a repulsive (Pauli repulsion) component. Several correction schemes have been discussed − for electronic-structure methods, which suffer from an insufficient description of dispersion interactions due to their incomplete description of electron correlation; a common point of view considers the classical case of an attractive interaction resulting from oscillating dipoles originally introduced by London, which then lends itself to add attractive potential energy contributions defined in terms of internuclear distances to the total electronic energy, analogous to the attractive part in Lennard-Jones potentials of classical force fields.…”

Section: Automated Parametrization Of Sfammentioning

confidence: 99%

Self-Parametrizing System-Focused Atomistic Models

Brunken

Reiher

2020

J. Chem. Theory Comput.

View full text Add to dashboard Cite

Computational studies of chemical reactions in complex environments such as proteins, nanostructures, or on surfaces require accurate and efficient atomistic models applicable to the nanometer scale. In general, an accurate parametrization of the atomistic entities will not be available for arbitrary system classes, but demands a fast automated system-focused parametrization procedure to be quickly applicable, reliable, flexible, and reproducible. Here, we develop and combine an automatically parametrizable quantum chemically derived molecular mechanics model with machine-learned corrections under autonomous uncertainty quantification and refinement. Our approach first generates an accurate, physically motivated model from a minimum energy structure and its corresponding Hessian matrix by a partial Hessian fitting procedure of the force constants. This model is then the starting point to generate a large number of configurations for which additional off-minimum reference data can be evaluated on the fly. A ∆-machine learning model is trained on these data to provide a correction to energies and forces including uncertainty estimates. During the procedure, the flexibility of the machine learning model is tailored to the amount of available training data. The parametrization of large systems is enabled by a fragmentation approach. Due to their modular nature, all model construction steps allow for model improvement in a rolling fashion. Our approach may also be employed for the generation of system-focused electrostatic molecular mechanics embedding environments in a quantum mechanical molecular-mechanical hybrid model for arbitrary atomistic structures at the nanoscale.

show abstract

“…Nanosecond dynamics of proton escape from NH 4 + @C 60 MNDO-F [44,45] was used to investigate the escape of a proton through the fullerene wall for the reaction Fig. 3 Time dependence of the dipole moment along the molecular axis and snapshots from an NVE dynamic simulation of the radical cation of compound 1.…”

Section: Applications Reorganization Dynamics Upon Ionizationmentioning

confidence: 99%

EMPIRE: a highly parallel semiempirical molecular orbital program: 3: Born-Oppenheimer molecular dynamics

2020

Self Cite

View full text Add to dashboard Cite

Direct NDDO-based Born-Oppenheimer molecular dynamics (MD) have been implemented in the semiempirical molecular orbital program EMPIRE. Fully quantum mechanical MD simulations on unprecedented time and length scales are possible, since the calculation of self-consistent wavefunctions and gradients is performed in a massively parallel manner. MD simulations can be performed in the NVE and NVT ensembles, using either deterministic (Berendsen) or stochastic (Langevin) thermostats. Furthermore, dynamics for condensed-phase systems can be performed under periodic boundary conditions. We show three exemplary applications: the dynamics of molecular reorganization upon ionization, long timescale dynamics of an endohedral fullerene, and calculation of the vibrational spectrum of a nanoparticle consisting of more than eight hundred atoms.

show abstract

A Feynman dispersion correction: a proof of principle for MNDO

Cited by 8 publications

References 51 publications

Semiempirical Quantum-Chemical Methods with Orthogonalization and Dispersion Corrections

Semiempirical Quantum-Chemical Methods with Orthogonalization and Dispersion Corrections

Self-Parametrizing System-Focused Atomistic Models

EMPIRE: a highly parallel semiempirical molecular orbital program: 3: Born-Oppenheimer molecular dynamics

Contact Info

Product

Resources

About