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| Open AccessPredicting orientation-dependent plastic susceptibility from static structure in amorphous solids via deep learning
Predicting a priori local defects in amorphous materials remains a grand challenge. Here authors combine a rotationally non-invariant structure representation with deep-learning to predict the propensity for shear transformations of amorphous solids for different loading orientations, only given the static structure.
- Zhao Fan
- & Evan Ma
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Article
| Open AccessPressure-induced ferroelectric-like transition creates a polar metal in defect antiperovskites Hg3Te2X2 (X = Cl, Br)
Generally, ferroelectricity in ABO3 perovskites is suppressed by hydrostatic compression, but the evidence for pressure-induced ferroelectricity remains elusive. Here, the authors find a direct ferroelectric-like structural transition induced by pressure in defect antiperovskites.
- Weizhao Cai
- , Jiangang He
- & Shanti Deemyad
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Article
| Open AccessA family of ionic supersalts with covalent-like directionality and unconventional multiferroicity
Binary ionic crystals, such as NaCl, are non-polar due to directionless ionic bonding interactions. Here, the authors show that polarity can be developed by using superalkali/superhalogen ions as building blocks, leading to ionic supersalts with ferroelectricity, ferroelasticity or even triferroicity.
- Yaxin Gao
- , Menghao Wu
- & Puru Jena
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Article
| Open AccessA tris-spiro metalla-aromatic system featuring Craig-Möbius aromaticity
Spiroaromatic compounds are advantageous platforms for designing expanded aromatic systems. Herein, the authors present a tris‐spiro metalla‐aromatic Vanadium compound which forms a 40π Craig‐Möbius aromatic system.
- Zhe Huang
- , Yongliang Zhang
- & Zhenfeng Xi
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Article
| Open AccessCavity frequency-dependent theory for vibrational polariton chemistry
Vibrational strong coupling controls the ground-state reactivity of molecules in optical cavities, but the underlying theory is still elusive. The authors analyze a molecular system coupled to a cavity mode and find that the reaction rate is suppressed for a particular cavity frequency, related to the topology of the reaction barrier region, analogously to a solvent caging effect.
- Xinyang Li
- , Arkajit Mandal
- & Pengfei Huo
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Article
| Open AccessThe atomistic details of the ice recrystallisation inhibition activity of PVA
Understanding ice re-crystallization is key to improve the current cryopreservation technologies. Here, the authors bring together experiments and simulations to unravel the atomistic details of the ice re-crystallization inhibition (IRI) activity of poly(vinyl)alcohol—the most potent biomimetic IRI agent.
- Fabienne Bachtiger
- , Thomas R. Congdon
- & Gabriele C. Sosso
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Article
| Open AccessAutomated discovery of a robust interatomic potential for aluminum
The accuracy of a machine-learned potential is limited by the quality and diversity of the training dataset. Here the authors propose an active learning approach to automatically construct general purpose machine-learning potentials here demonstrated for the aluminum case.
- Justin S. Smith
- , Benjamin Nebgen
- & Kipton Barros
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Matters Arising
| Open AccessA thermodynamic assessment of the reported room-temperature chemical synthesis of C2
- Henry S. Rzepa
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Matters Arising
| Open AccessReply to “A Thermodynamic assessment of the reported room-temperature chemical synthesis of C2”
- Kazunori Miyamoto
- , Shodai Narita
- & Masanobu Uchiyama
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Article
| Open AccessStability and folding pathways of tetra-nucleosome from six-dimensional free energy surface
The three-dimensional organization of chromatin plays critical roles in regulating genome function. Here the authors apply a near atomistic model to study the structure and dynamics of the chromatin folding unit - the tetra-nucleosome - to provide insight into how chromatin folds.
- Xinqiang Ding
- , Xingcheng Lin
- & Bin Zhang
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Article
| Open AccessBridging scales in disordered porous media by mapping molecular dynamics onto intermittent Brownian motion
The diffusion of fluids in complex nanoporous geometries represents a challenge for modelling approaches. Here, the authors describe the macroscopic diffusivity of a simple fluid in disordered nanoporous materials by bridging microscopic and mesoscopic dynamics with parameters obtained from simple physical laws.
- Colin Bousige
- , Pierre Levitz
- & Benoit Coasne
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Article
| Open AccessColloidal CdSe nanocrystals are inherently defective
Colloidal CdSe nanocrystals hold great promise in applications due to their tunable optical spectrum. Using hybrid time-dependent density functional theory, the authors show that colloidal CdSe nanocrystals are inherently defective with a low energy spectrum dominated by dark, surface-associated excitations.
- Tamar Goldzak
- , Alexandra R. McIsaac
- & Troy Van Voorhis
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Article
| Open AccessDigital navigation of energy–structure–function maps for hydrogen-bonded porous molecular crystals
Energy–structure–function (ESF) maps can facilitate functional materials discovery. Here the authors provide a protocol for the digital navigation of ESF maps, as demonstrated for hydrogen-bonded organic frameworks constructed from triptycene- and spiro-biphenyl-based molecular building block.
- Chengxi Zhao
- , Linjiang Chen
- & Andrew I. Cooper
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Article
| Open AccessSimulating the ghost: quantum dynamics of the solvated electron
The nature of the bulk hydrated electron has been a challenge for both experiment and theory. Here the authors use a machine-learning model trained on MP2 data to achieve an accurate determination of the structure, diffusion mechanisms, and vibrational spectroscopy of the solvated electron.
- Jinggang Lan
- , Venkat Kapil
- & Vladimir V. Rybkin
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Article
| Open AccessElectronic spin separation induced by nuclear motion near conical intersections
Spin polarization is at the basis of quantum information and underlies some natural processes, but many aspects still need to be explored. Here, the authors, by quantum mechanical computations, show that even a weak spin-orbit coupling near a conical intersection can induce large spin selection, with consequences for spin manipulation in photochemical or electrochemical reactions.
- Yanze Wu
- & Joseph E. Subotnik
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Article
| Open AccessQuantum-mechanical exploration of the phase diagram of water
Complex interatomic interactions and diverse structures make computing the phase diagram of water very challenging. Here, a combination of machine learning and advanced free-energy methods at three levels of hybrid DFT enables the prediction of the phase diagram in close agreement with experiment.
- Aleks Reinhardt
- & Bingqing Cheng
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Article
| Open AccessSelective hydrogenation of 5-(hydroxymethyl)furfural to 5-methylfurfural over single atomic metals anchored on Nb2O5
Selective hydrogenation of 5-(hydroxymethyl)furfural (HMF) to 5-Methylfurfural using H2 as reductant is very attractive, but remains challenging. Here, the authors report that isolated single atomic catalysts can catalyze the reaction efficiently with selectivity >99% at complete conversion of HMF.
- Shaopeng Li
- , Minghua Dong
- & Buxing Han
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Article
| Open AccessDynamical strengthening of covalent and non-covalent molecular interactions by nuclear quantum effects at finite temperature
The inclusion of nuclear quantum effects (NQE) in atomistic simulations of chemical systems is of key importance. Here the authors use machine learned force fields trained on coupled cluster reference data to show the dynamical strengthening of covalent and non-covalent molecular interactions induced by NQE.
- Huziel E. Sauceda
- , Valentin Vassilev-Galindo
- & Alexandre Tkatchenko
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| Open AccessA fourth-generation high-dimensional neural network potential with accurate electrostatics including non-local charge transfer
Machine learning potentials do not account for long-range charge transfer. Here the authors introduce a fourth-generation high-dimensional neural network potential including non-local information of charge populations that is able to provide forces, charges and energies in excellent agreement with DFT data.
- Tsz Wai Ko
- , Jonas A. Finkler
- & Jörg Behler
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Article
| Open AccessPure non-local machine-learned density functional theory for electron correlation
Semilocal density functionals, while computationally efficient, do not account for non-local correlation. Here, the authors propose a machine-learning approach to DFT that leads to non-local and transferable functionals applicable to non-covalent, ionic and covalent interactions across system of different sizes.
- Johannes T. Margraf
- & Karsten Reuter
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| Open AccessCoulomb interactions between dipolar quantum fluctuations in van der Waals bound molecules and materials
High-level methods to describe van der Waals interactions are limited due to their computational cost. This work introduces a new theoretical approach, that extends the dipolar many-body dispersion formalism to higher-order contributions, demonstrated to be applicable to practically-relevant systems and nano-environments.
- Martin Stöhr
- , Mainak Sadhukhan
- & Alexandre Tkatchenko
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| Open AccessFunction-oriented design of robust metal cocatalyst for photocatalytic hydrogen evolution on metal/titania composites
Photocatalytic performances require both active catalytic surfaces and efficient electron transfer steps. Here the authors introduce a function-oriented catalyst design strategy optimizing both aspects and generalize an effective electron transfer descriptor on metal/oxide catalysts.
- Dong Wang
- & Xue-Qing Gong
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Article
| Open AccessA cooperative biphasic MoOx–MoPx promoter enables a fast-charging lithium-ion battery
Fast-charging of lithium-ion batteries is hindered by the uncontrollable plating of metallic Li on the graphite anode during cycling. Here, the authors demonstrate the fast chargeability and long cycle lifetimes via surface engineering of graphite with a cooperative biphasic MoOx–MoPx promoter.
- Sang-Min Lee
- , Junyoung Kim
- & Min-Sik Park
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Article
| Open AccessMachine learned features from density of states for accurate adsorption energy prediction
Computational catalysis would strongly benefit from general descriptors applicable for predicting adsorption energetics. Here the authors propose a machine-learning approach for adsorption energy predictions based on learning the relevant descriptors in a surface atom's density of states as part of the training.
- Victor Fung
- , Guoxiang Hu
- & Bobby G. Sumpter
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Article
| Open AccessPredicting materials properties without crystal structure: deep representation learning from stoichiometry
Predicting the structure of unknown materials’ compositions represents a challenge for high-throughput computational approaches. Here the authors introduce a new stoichiometry-based machine learning approach for predicting the properties of inorganic materials from their elemental compositions.
- Rhys E. A. Goodall
- & Alpha A. Lee
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Article
| Open AccessKey activity descriptors of nickel-iron oxygen evolution electrocatalysts in the presence of alkali metal cations
It is commonly accepted that electrolyte alkali metal cations modify the catalytic activity for oxygen evolution reaction. Here the authors challenge this assumption, showing that the activity is actually affected by a change in the electrolyte pH rather than a specific alkali cation.
- Mikaela Görlin
- , Joakim Halldin Stenlid
- & Oscar Diaz-Morales
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Article
| Open AccessBayesian learning of chemisorption for bridging the complexity of electronic descriptors
Developing a generalizable model to describe adsorption processes at metal surfaces can be extremely challenging due to complex phenomena involved. Here the authors introduce a Bayesian learning approach based on ab initio data and the d-band model to capture the essential physics of adsorbate–substrate interactions.
- Siwen Wang
- , Hemanth Somarajan Pillai
- & Hongliang Xin
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Article
| Open AccessDifferential guest location by host dynamics enhances propylene/propane separation in a metal-organic framework
Porous materials acting as molecular sieves for propylene/propane separation are important for the petrochemical industry. Here the authors show an example of how specific guest-host interactions can result in structural changes in the porous host and shut down diffusion of one of the two similar guest molecules.
- Dmytro Antypov
- , Aleksander Shkurenko
- & Matthew S. Dyer
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Article
| Open AccessHow to speed up ion transport in nanopores
Narrowing pores filled with an electrolyte usually slows down their charge-discharge dynamics. Here the authors demonstrate through molecular dynamics simulations and experiments with novolac-derived carbon electrodes how non-linear voltage sweeps can accelerate charging and discharging of subnanometer pores.
- Konrad Breitsprecher
- , Mathijs Janssen
- & Svyatoslav Kondrat
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Article
| Open AccessLiquid water contains the building blocks of diverse ice phases
Molecular understanding of water is challenging due to the structural complexity of liquid water and the large number of ice phases. Here the authors use a machine-learning potential trained on liquid water to demonstrate the structural similarity of liquid water and that of 54 real and hypothetical ice phases.
- Bartomeu Monserrat
- , Jan Gerit Brandenburg
- & Bingqing Cheng
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| Open AccessMachine learning with physicochemical relationships: solubility prediction in organic solvents and water
Accurate prediction of solubility represents a challenge for traditional computational approaches due to the complex nature of phenomena involved. Here the authors report a successful approach to solubility prediction in organic solvents and water using combination of machine learning and computational chemistry.
- Samuel Boobier
- , David R. J. Hose
- & Bao N. Nguyen
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Article
| Open AccessComplex reaction processes in combustion unraveled by neural network-based molecular dynamics simulation
Gaining insights into combustion processes is challenging due to the complex reactions involved. The present work proposes a neural network potential model trained to ab initio data that enables to simulate the combustion of methane by predicting reactants, products and reaction intermediates.
- Jinzhe Zeng
- , Liqun Cao
- & John Z. H. Zhang
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Article
| Open AccessState-of-the-art augmented NLP transformer models for direct and single-step retrosynthesis
Development of algorithms to predict reactant and reagents given a target molecule is key to accelerate retrosynthesis approaches. Here the authors demonstrate that applying augmentation techniques to the SMILE representation of target data significantly improves the quality of the reaction predictions.
- Igor V. Tetko
- , Pavel Karpov
- & Guillaume Godin
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| Open AccessMachine learning in chemical reaction space
Application of machine-learning approaches to exploring chemical reaction networks is challenging due to need of including open-shell reaction intermediates. Here the authors introduce a density functional theory database of closed and open-shell molecules for machine-learning predictions of reaction energies.
- Sina Stocker
- , Gábor Csányi
- & Johannes T. Margraf
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Article
| Open AccessAtomically dispersed Lewis acid sites boost 2-electron oxygen reduction activity of carbon-based catalysts
H2O2 production via oxygen reduction offers a renewable approach to obtain an often-used oxidant. Here, authors show the incorporation of Lewis acid sites into carbon-based materials to improve H2O2 electrosynthesis.
- Qihao Yang
- , Wenwen Xu
- & Liang Chen
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| Open AccessInfrared spectroscopic study of hydrogen bonding topologies in the smallest ice cube
Spectroscopic studies of water clusters provide insight into the hydrogen bond structure of water and ice. The authors measure infrared spectra of neutral water octamers using a threshold photoionization technique based on a tunable vacuum-UV free electron laser, identifying two cubic isomers in addition to those previously observed.
- Gang Li
- , Yang-Yang Zhang
- & Ling Jiang
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| Open AccessFast site-to-site electron transfer of high-entropy alloy nanocatalyst driving redox electrocatalysis
The design of nanostructured catalysts plays a key role in the electrocatalytic redox reaction performances. Here, authors prepared uniform and small-sized high-entropy alloy PtNiFeCoCu nanoparticles that showed improved activities for H2 evolution methanol oxidation reactions.
- Hongdong Li
- , Yi Han
- & Lei Wang
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Article
| Open AccessDispersion state phase diagram of citrate-coated metallic nanoparticles in saline solutions
Citrate-stabilized metallic colloids are key materials towards chemosensing and catalysis applications. Here the authors introduce a new theoretical model to estimate how the stoichiometry of citrate molecules absorbed onto spherical metallic nanoparticles influences their aggregation phenomena.
- Sebastian Franco-Ulloa
- , Giuseppina Tatulli
- & Marco De Vivo
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Article
| Open AccessXenon iron oxides predicted as potential Xe hosts in Earth’s lower mantle
The abnormally low concentration of xenon compared to other noble gases in Earth’s atmosphere remains debated, as the identification of mantle minerals that can capture and stabilize xenon is challenging. Here, the authors propose that xenon iron oxides could be potential Xe hosts in Earth’s lower mantle.
- Feng Peng
- , Xianqi Song
- & Yanming Ma
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Article
| Open AccessQuantum chemical accuracy from density functional approximations via machine learning
High-level ab initio quantum chemical methods carry a high computational burden, thus limiting their applicability. Here, the authors employ machine learning to generate coupled-cluster energies and forces at chemical accuracy for geometry optimization and molecular dynamics from DFT densities.
- Mihail Bogojeski
- , Leslie Vogt-Maranto
- & Kieron Burke
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| Open AccessUnderstanding high pressure molecular hydrogen with a hierarchical machine-learned potential
Hydrogen has multiple molecular phases which are challenging to explore computationally. The authors develop a machine-learning approach, learning from reference ab initio molecular dynamics simulations, to derive a transferable hierarchical force model that provides insight into high pressure phases and the melting line of H2.
- Hongxiang Zong
- , Heather Wiebe
- & Graeme J. Ackland
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Comment
| Open AccessRetrospective on a decade of machine learning for chemical discovery
Over the last decade, we have witnessed the emergence of ever more machine learning applications in all aspects of the chemical sciences. Here, we highlight specific achievements of machine learning models in the field of computational chemistry by considering selected studies of electronic structure, interatomic potentials, and chemical compound space in chronological order.
- O. Anatole von Lilienfeld
- & Kieron Burke
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Article
| Open AccessClarifying the quantum mechanical origin of the covalent chemical bond
The origin of the covalent H–H bond is understood to be driven by kinetic energy lowering. Here the authors show this is not the case for bonds between heavier elements likely due to the presence of core electrons, and that constructive quantum interference instead drives bond formation.
- Daniel S. Levine
- & Martin Head-Gordon
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Article
| Open AccessOptical gap and fundamental gap of oligoynes and carbyne
Carbyne, a linear sp-hybridized carbon allotrope, is synthetically inaccessible and its properties are extrapolated from those of defined oligomers. Here the authors analyze weak optical bands in two series of oligoynes and reassess the optical and fundamental gap of carbyne to lower values than previously suggested.
- Johannes Zirzlmeier
- , Stephen Schrettl
- & Holger Frauenrath
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Article
| Open AccessPredicting heterogeneous ice nucleation with a data-driven approach
Heterogenous ice nucleation is a ubiquitous phenomenon, but predicting the ice nucleation ability of a substrate is challenging. Here the authors develop a machine-learning data-driven approach to predict the ice nucleation ability of substrates, which is based on four descriptors related to physical properties of the interface.
- Martin Fitzner
- , Philipp Pedevilla
- & Angelos Michaelides
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Article
| Open AccessComputational screen-out strategy for electrically pumped organic laser materials
Though the goal of current organic solid-state laser research remains the realization of electrically pumped lasing, identifying organic semiconductors with ideal properties remains a challenge. Here, the authors report a computational strategy for screening electrical pumping lasing molecules.
- Qi Ou
- , Qian Peng
- & Zhigang Shuai
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Article
| Open AccessEnhanced carbon dioxide conversion at ambient conditions via a pore enrichment effect
Currently the cost of CO2 chemical fixation remains high because of harsh reaction conditions. Here, the authors report a covalent organic framework screened from 10994 candidates as the efficient CO2 fixation catalyst under ambient conditions based on the finding of a “pore enrichment effect”.
- Wei Zhou
- , Qi-Wen Deng
- & Wei-Qiao Deng
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Article
| Open AccessIdentifying domains of applicability of machine learning models for materials science
Machine learning models insufficient for certain screening tasks can still provide valuable predictions in specific sub-domains of the considered materials. Here, the authors introduce a diagnostic tool to detect regions of low expected model error as demonstrated for the case of transparent conducting oxides.
- Christopher Sutton
- , Mario Boley
- & Matthias Scheffler
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Article
| Open AccessAnharmonic quantum nuclear densities from full dimensional vibrational eigenfunctions with application to protonated glycine
Accurate interpretation of molecular vibrational spectroscopic signals is key to understand chemical processes. Here the authors introduce a new computational approach to represent vibrational modes in terms of nuclear densities that captures anharmonic effects in protonated glycine.
- Chiara Aieta
- , Marco Micciarelli
- & Michele Ceotto