The OpenMolcas Web: A Community-Driven Approach to Advancing Computational Chemistry

Journal of Chemical Theory and Computation, Journal Year: 2023, Volume and Issue: 19(20), P. 6933 - 6991

Published: May 22, 2023

The developments of the open-source OpenMolcas chemistry software environment since spring 2020 are described, with a focus on novel functionalities accessible in stable branch package or via interfaces other packages. These span wide range topics computational and presented thematic sections: electronic structure theory, spectroscopy simulations, analytic gradients molecular optimizations, ab initio dynamics, new features. This report offers an overview chemical phenomena processes can address, while showing that is attractive platform for state-of-the-art atomistic computer simulations.

Language: Английский

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Corresponding Active Orbital Spaces along Chemical Reaction Paths

The Journal of Physical Chemistry Letters, Journal Year: 2023, Volume and Issue: 14(8), P. 2112 - 2118

Published: Feb. 20, 2023

The accuracy of reaction energy profiles calculated with multiconfigurational electronic structure methods and corrected by multireference perturbation theory depends crucially on consistent active orbital spaces selected along the path. However, it has been challenging to choose molecular orbitals that can be considered corresponding in different structures. Here, we demonstrate how consistently coordinates a fully automatized way. approach requires no interpolation between reactants products. Instead, emerges from synergy Direct Orbital Selection mapping ansatz combined our automated space selection algorithm autoCAS. We for potential profile homolytic carbon-carbon bond dissociation rotation around double 1-pentene ground state. also applies electronically excited Born-Oppenheimer surfaces.

Language: Английский

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A human-machine interface for automatic exploration of chemical reaction networks

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: May 1, 2024

Abstract Autonomous reaction network exploration algorithms offer a systematic approach to explore mechanisms of complex chemical processes. However, the resulting networks are so vast that an all potentially accessible intermediates is computationally too demanding. This renders brute-force explorations unfeasible, while with completely pre-defined or hard-wired constraints, such as element-specific coordination numbers, not flexible enough for systems. Here, we introduce STEERING WHEEL guide otherwise unbiased automated exploration. The algorithm intuitive, generally applicable, and enables one focus on specific regions emerging network. It also allows guiding data generation in context mechanism exploration, catalyst design, other optimization challenges. demonstrated elucidation transition metal catalysts. We highlight how catalytic cycles reproducible way. objectives fully adjustable, allowing harness both structure-specific (accurate) calculations well broad high-throughput screening possible intermediates.

Language: Английский

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SCINE—Software for chemical interaction networks

The Journal of Chemical Physics, Journal Year: 2024, Volume and Issue: 160(22)

Published: June 10, 2024

The software for chemical interaction networks (SCINE) project aims at pushing the frontier of quantum calculations on molecular structures to a new level. While individual as well simple relations between them have become routine in chemistry, developments pushed field high-throughput calculations. Chemical may be created by search specific properties design attempt, or they can defined set elementary reaction steps that form network. modules SCINE been designed facilitate such studies. features are (i) general applicability applied methodologies ranging from electronic structure (no restriction elements periodic table) microkinetic modeling (with little restrictions molecularity), full modularity so also stand-alone programs exchanged external packages fulfill similar purpose (to increase options computational campaigns and provide alternatives case tasks hard impossible accomplish with certain programs), (ii) high stability autonomous operations control steering an operator easy possible, (iii) embedding into complex heterogeneous environments taken individually context A graphical user interface unites all ensures interoperability. All components made available open source free charge.

Language: Английский

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Deep reaction network exploration of glucose pyrolysis

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(34)

Published: Aug. 14, 2023

Resolving the reaction networks associated with biomass pyrolysis is central to understanding product selectivity and aiding catalyst design produce more valuable products. However, even network of relatively simple [Formula: see text]-D-glucose remains unresolved due its significant complexity in terms depth number major Here, a transition-state-guided exploration has been performed that provides complete pathways most experimental products text]-D-glucose. The resulting involves over 31,000 reactions transition states computed at semiempirical quantum chemistry level approximately 7,000 kinetically relevant characterized density function theory, comprising largest reported for pyrolysis. was conducted using graph-based rules explore reactivities intermediates an adaption Dijkstra algorithm identify intermediates. This policy surprisingly (re)identified products, many proposed by previous computational studies, also identified new low-barrier mechanisms resolve outstanding discrepancies between yields isotope labeling experiments. explanatory high yield hydroxymethylfurfural pathway contributes formation hydroxyacetaldehyde during glucose Due limited domain knowledge required generate this network, approach should be transferable other complex prediction problems

Language: Английский

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Nanoscale chemical reaction exploration with a quantum magnifying glass

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 22, 2024

Abstract Nanoscopic systems exhibit diverse molecular substructures by which they facilitate specific functions. Theoretical models of them, aim at describing, understanding, and predicting these capabilities, are difficult to build. Viable quantum-classical hybrid come with challenges regarding atomistic structure construction quantum region selection. Moreover, if their dynamics mapped onto a state-to-state mechanism such as chemical reaction network, its exhaustive exploration will be impossible due the combinatorial explosion space. Here, we introduce “quantum magnifying glass” that allows one interactively manipulate nanoscale structures level. The glass seamlessly combines autonomous model parametrization, ultra-fast mechanical calculations, automated exploration. It represents an approach investigate complex sequences in physically consistent manner unprecedented effortlessness real time. We demonstrate features for reactions bio-macromolecules metal-organic frameworks, highlight general applicability.

Language: Английский

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Chemical Reaction Networks from Scratch with Reaction Prediction and Kinetics-Guided Exploration

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

Published: Jan. 30, 2025

Algorithmic reaction explorations based on transition state searches can now routinely predict relatively short sequences involving small molecules. However, applying these algorithms to deeper chemical network (CRN) exploration still requires the development of more efficient and accurate policies. Here, an algorithm, which we name yet another kinetic strategy (YAKS), is demonstrated that uses microkinetic simulations nascent achieve cost-effective, deep exploration. Key features algorithm are automatic incorporation bimolecular reactions between intermediates, compatibility with short-lived but kinetically important species, rate uncertainty into policy. In validation case studies glucose pyrolysis, rediscovers pathways previously discovered by heuristic policies elucidates new for experimentally obtained products. The resulting CRN first connect all major experimental pyrolysis products glucose. Additional presented investigate role rules, uncertainty, reactions. These show naïve exponential growth estimates vastly overestimate actual number relevant in physical networks. light this, further improvements prediction make it feasible CRNs might soon be predictable some contexts.

Language: Английский

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Ten Problems in Polymer Reactivity Prediction

Macromolecules, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 17, 2025

Language: Английский

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Optimal transport for generating transition states in chemical reactions

Nature Machine Intelligence, Journal Year: 2025, Volume and Issue: 7(4), P. 615 - 626

Published: April 23, 2025

Language: Английский

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Exploring Chemical Space Using Ab Initio Hyperreactor Dynamics

ACS Central Science, Journal Year: 2024, Volume and Issue: 10(2), P. 302 - 314

Published: Jan. 31, 2024

In recent years, first-principles exploration of chemical reaction space has provided valuable insights into intricate networks. Here, we introduce ab initio hyperreactor dynamics, which enables rapid screening the accessible from a given set initial molecular species, predicting new synthetic routes that can potentially guide subsequent experimental studies. For this purpose, different hyperdynamics derived bias potentials are applied along with pressure-inducing spherical confinement system in dynamics simulations to efficiently enhance reactivity under mild conditions. To showcase advantages and flexibility approach, present systematic study method's parameters on HCN toy model apply it recently introduced for prebiotic formation glycinal acetamide interstellar ices, yields results line findings. addition, show how developed framework complicated transitions like first step nonenzymatic DNA nucleoside synthesis an aqueous environment, where fragmentation problem earlier nanoreactor approaches is avoided.

Language: Английский

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