JOYCE3.0: A General Protocol for the Specific Parametrization of Accurate Intramolecular Quantum Mechanically Derived Force Fields DOI
Samuele Giannini,

P. M. Martinez,

Abderrahmane Semmeq

et al.

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

Published: March 11, 2025

While the intrinsically multiscale nature of most advanced materials necessitates use cost-effective computational models based on classical physics, a reliable description structure and dynamics their components often requires quantum-mechanical treatment. In this work, we present JOYCE3.0, software package for parametrization accurate, quantum-mechanically derived force fields (QMD-FFs). Since its original release, code has been extensively automated expanded, with all novel implementations thoroughly discussed. To illustrate general applicability, QMD-FFs are parametrized seven benchmark cases, encompassing molecules diverse structures properties. These range from exotic stiff scaffolds, flexible polymeric chains, polyenes biological interest to transition-metal complexes. On one hand, JOYCE3.0 FFs consistently outperform available general-purpose descriptions, achieving excellent agreement higher-level theoretical methods or experimental validation data. other remarkable accuracy found in molecular extends electronic excited states, enabling integration into multilevel protocols aimed at reliably predicting selected properties spectral line shapes optoelectronic materials. The high quality results─spanning structures, condensed-phase properties, spectroscopic features─in combination enhanced interface popular codes engines, as well applicability chemically species, strongly suggests that could play pivotal role rational design functionalized heterogeneous systems.

Language: Английский

Deciphering the Luminescence Spectral Shape of an Oxyluciferin Analogue through a Mixed Quantum-Classical Approach DOI

Houda Moumene,

Giacomo Prampolini, Cristina García‐Iriepa

et al.

The Journal of Physical Chemistry B, Journal Year: 2025, Volume and Issue: unknown

Published: March 10, 2025

In this contribution, we present a computational study on the absorption and emission spectra of cproxy– anion in water, an analogue firefly oxyluciferin phenolate keto form. This compound displays broad spectrum large Stokes shift, two features that remain elusive to approaches, preventing complete understanding photophysics behind molecule. Here attempt fully first-principles computation both spectral shapes positions, explicitly including effect soft molecular flexible modes stiff vibrational motions as well those solvent. Namely, adopt recently developed mixed-quantum classical approach, so-called Adiabatic Molecular Dynamics–generalized vertical Hessian (Ad-MD|gVH) method, which has been revealed be suited reproduce band condensed phases. We also explore performance DFT functionals build potential energy surfaces investigate possible role interstate couplings. By means, are able obtain simulation shape close experimental one, correctly two-peak spectrum, terms their spacing relative intensity. However, low-energy computed is too narrow, shift remarkably underestimated. Through careful analysis different settings, identify some key aspects partly explain these discrepancies, limitations TD-DFT properly describe electronic along torsional degree freedom lowest-excited state mutual polarization solvent dye.

Language: Английский

Citations

0
JOYCE3.0: A General Protocol for the Specific Parametrization of Accurate Intramolecular Quantum Mechanically Derived Force Fields DOI
Samuele Giannini,

P. M. Martinez,

Abderrahmane Semmeq

et al.

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

Published: March 11, 2025

While the intrinsically multiscale nature of most advanced materials necessitates use cost-effective computational models based on classical physics, a reliable description structure and dynamics their components often requires quantum-mechanical treatment. In this work, we present JOYCE3.0, software package for parametrization accurate, quantum-mechanically derived force fields (QMD-FFs). Since its original release, code has been extensively automated expanded, with all novel implementations thoroughly discussed. To illustrate general applicability, QMD-FFs are parametrized seven benchmark cases, encompassing molecules diverse structures properties. These range from exotic stiff scaffolds, flexible polymeric chains, polyenes biological interest to transition-metal complexes. On one hand, JOYCE3.0 FFs consistently outperform available general-purpose descriptions, achieving excellent agreement higher-level theoretical methods or experimental validation data. other remarkable accuracy found in molecular extends electronic excited states, enabling integration into multilevel protocols aimed at reliably predicting selected properties spectral line shapes optoelectronic materials. The high quality results─spanning structures, condensed-phase properties, spectroscopic features─in combination enhanced interface popular codes engines, as well applicability chemically species, strongly suggests that could play pivotal role rational design functionalized heterogeneous systems.

Language: Английский

Citations

0