Accelerating Molecular Dynamics Simulations Using Socket-Based Interprocess Communication DOI
Matheus de Oliveira Bispo, Mario Barbatti

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: unknown, P. 11891 - 11895

Published: Nov. 21, 2024

Molecular dynamics (MD) simulations are essential for studying the time evolution of molecular systems. Still, their efficiency is often bottlenecked by file-based interprocess communication (IPC) between MD and electronic structure programs. We present a socket-based IPC implementation that dramatically accelerates simulations, reducing computational >10-fold compared to those traditional methods. Our approach, applied nonadiabatic with Newton-X program, eliminates disk read/write overhead, allowing faster over longer scales. This method opens door more efficient high-throughput providing new opportunities exploring complex processes in real time.

Language: Английский

Photoexcited dynamics of the valence states of norbornadiene DOI Creative Commons
Joseph C. Cooper, Crum Brown, Janaka Kara

et al.

The Journal of Chemical Physics, Journal Year: 2025, Volume and Issue: 162(9)

Published: March 3, 2025

The non-radiative decay of photoexcited norbornadiene, which together with its isomer quadricyclane forms a molecular photoswitch, is investigated using surface-hopping non-adiabatic dynamics. simulations are performed four levels electronic structure theory: CASSCF(2,2), CASSCF(4,4), XMS-CASPT2(2,2), and XMS-CASPT2(4,4). These models yield two distinct classes excited-state reaction pathways, different quantum yields for the isomerization. This illustrates significance potential energy surfaces when simulating nature pathways related to topographical features on surfaces, suggesting “design rules” chemical modification via substituent groups. How molecule approaches conical intersection also shown play decisive role in outcome.

Language: Английский

Citations

1
ULaMDyn: Enhancing Excited-State Dynamics Analysis Through Streamlined Unsupervised Learning DOI Creative Commons
Max Pinheiro, Matheus de Oliveira Bispo, Rafael S. Mattos

et al.

Digital Discovery, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

The analysis of nonadiabatic molecular dynamics (NAMD) data presents significant challenges due to its high dimensionality and complexity. To address these issues, we introduce ULaMDyn, a Python-based, open-source package designed automate the unsupervised large datasets generated by NAMD simulations. ULaMDyn integrates seamlessly with Newton-X platform employs advanced reduction clustering techniques uncover hidden patterns in trajectories, enabling more intuitive understanding excited-state processes. Using photochemical fulvene as test case, demonstrate how efficiently identifies critical geometries transitions. offers streamlined, scalable solution for interpreting datasets. It is poised facilitate advances study across wide range systems.

Language: Английский

Citations

0
Solvent Effects on Nonadiabatic Dynamics: Ab Initio Multiple Spawning Propagated on CASPT2/xTB Potentials DOI
Davide Avagliano

Journal of Chemical Theory and Computation, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 11, 2025

An approach to simulate nonadiabatic dynamics in solution is introduced, which relies on the propagation of nuclear wavepacket with Ab Initio Multiple Spawning (AIMS) method under effect potential energy calculated a hybrid but fully quantum mechanical scheme (QM/QM′). The electronic energies excited states chromophore are multireference perturbation theory (CASPT2), and embedding molecules described tight binding Hamiltonian (GFN2-xTB). This implementation open source combination PySpawn, OpenMolcas, xTB. Additionally, ORCA used properly generate initial conditions solution, showing how cutting-edge implementations several commonly software can push state art toward new high standard accuracy. ethylene vacuum, acetone, chloroform reported as test case, detailed analysis AIMS runs that shows important geometrical effects solvents decay mechanism chromophore.

Language: Английский

Citations

0
Legion: A Platform for Gaussian Wavepacket Nonadiabatic Dynamics DOI
Rafael S. Mattos, Saikat Mukherjee, Mario Barbatti

et al.

Journal of Chemical Theory and Computation, Journal Year: 2025, Volume and Issue: unknown

Published: March 2, 2025

Nonadiabatic molecular dynamics is crucial in investigating the time evolution of excited states systems. Among various methods for performing such dynamics, those employing frozen Gaussian wavepacket propagation, particularly multiple spawning approach, offer a favorable balance between computational cost and reliability. It propagates on-the-fly trajectories used to build propagate nuclear wavepacket. Despite its potential, efficient, flexible, easily accessible software propagation less common compared other methods, as surface hopping. To address this, we present Legion, that facilitates development application classical-trajectory-guided quantum methods. The version presented here already contains highly flexible fully functional ab initio implementation, with different strategies improve efficiency. Legion written Python data management NumPy/Fortran numerical operations. created under umbrella Newton-X platform inherits all electronic structure interfaces beyond direct interfaces. also new approximations allow it circumvent computation nonadiabatic coupling, extending can be dynamics. We test, validate, demonstrate Legion's functionalities through fulvene (CASSCF CASPT2) DMABN (TDDFT).

Language: Английский

Citations

0
Assessing the performance of coupled-trajectory schemes on full-dimensional two-state linear vibronic coupling models DOI
Peter Schürger, Lea M. Ibele, David Lauvergnat

et al.

The Journal of Chemical Physics, Journal Year: 2025, Volume and Issue: 162(10)

Published: March 14, 2025

We investigate the performance of coupled-trajectory methods for nonadiabatic molecular dynamics in simulating photodynamics 4-(dimethylamino)benzonitrile (DMABN) and fulvene, with electronic structure provided by linear vibrational coupling models. focus on mixed quantum-classical (CTMQC) algorithm (combined) Tully surface hopping [(C)CTTSH] comparison to independent-trajectory approaches, such as multi-trajectory Ehrenfest hopping. Our analysis includes not only populations but also additional nuclear properties position momentum space. For both DMABN recently developed CCTTSH successfully resolves internal inconsistencies Instead, we find that highlights a significant weakness CTMQC, which arises when trajectories remain long time vicinity region strong nonadiabaticity.

Language: Английский

Citations

0
Accelerating Molecular Dynamics Simulations Using Socket-Based Interprocess Communication DOI
Matheus de Oliveira Bispo, Mario Barbatti

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: unknown, P. 11891 - 11895

Published: Nov. 21, 2024

Molecular dynamics (MD) simulations are essential for studying the time evolution of molecular systems. Still, their efficiency is often bottlenecked by file-based interprocess communication (IPC) between MD and electronic structure programs. We present a socket-based IPC implementation that dramatically accelerates simulations, reducing computational >10-fold compared to those traditional methods. Our approach, applied nonadiabatic with Newton-X program, eliminates disk read/write overhead, allowing faster over longer scales. This method opens door more efficient high-throughput providing new opportunities exploring complex processes in real time.

Language: Английский

Citations

0