Featured
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Article
| Open AccessThermal dependence of the hydrated proton and optimal proton transfer in the protonated water hexamer
Water’s pivotal role is tied to the quantum nature of its hydrogen bond dynamics. Here, the authors investigate the thermal behavior of the protonated water hexamer through accurate path integral molecular dynamics, revealing that near-room temperature conditions are optimal for proton transfer.
- Félix Mouhat
- , Matteo Peria
- & Michele Casula
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Article
| Open AccessKnowledge-driven design of solid-electrolyte interphases on lithium metal via multiscale modelling
The application of Li metal electrodes in rechargeable batteries is limited by inherent high reactivity. Here, the authors provide model-based insights into the composition and formation mechanisms of the solid-electrolyte interphase on the µs-scale and suggest design strategies for the interphase.
- Janika Wagner-Henke
- , Dacheng Kuai
- & Ulrike Krewer
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Article
| Open AccessHighly active, ultra-low loading single-atom iron catalysts for catalytic transfer hydrogenation
Highly effective and selective noble metal-free catalysts continue to attract significant attention but require reaction specific tuning. Here, the authors fabricate a single-atom iron catalyst at low loading, which shows excellent transfer hydrogenation performance even at low reaction temperatures.
- Zhidong An
- , Piaoping Yang
- & Dionisios G. Vlachos
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Article
| Open AccessMulti-scale molecular dynamics simulations of enhanced energy transfer in organic molecules under strong coupling
Placing an organic material in an optical cavity can enhance exciton transport, but the mechanism is poorly understood. Here, using molecular dynamics simulations, the authors obtained atomistic insights into that mechanism.
- Ilia Sokolovskii
- , Ruth H. Tichauer
- & Gerrit Groenhof
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Article
| Open AccessStructural basis of dimerization of chemokine receptors CCR5 and CXCR4
Here, authors report chemokine receptors structures obtained using coarse-grained metadynamics. CCR5 and CXCR4 homo- and heterodimers differ in the conformations of ligand binding sites and of the G protein interaction interface, suggesting structural basis for the rational design of biased ligands.
- Daniele Di Marino
- , Paolo Conflitti
- & Vittorio Limongelli
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Article
| Open AccessChallenging an old paradigm by demonstrating transition metal-like chemistry at a neutral nonmetal center
The scope of and knowledge about the chemistry of nonmetal-adducts remains very limited. Here, the authors describe nonmetal adducts of the phosphorus center of terminal phosphinidene complexes using classical C- and N-ligands from metal coordination chemistry.
- David Biskup
- , Gregor Schnakenburg
- & Rainer K. Streubel
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Article
| Open AccessUniversal machine learning for the response of atomistic systems to external fields
External fields, despite their significant influence on chemical processes, have been largely ignored in current machine learning potentials. Here, the authors introduce a field-induced model that captures system-field interactions rigorously.
- Yaolong Zhang
- & Bin Jiang
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Article
| Open AccessMachine learning electronic structure methods based on the one-electron reduced density matrix
Electronic structure methods are vital, yet they are often too computationally expensive. Here, the authors develop machine learned density matrices to fully represent electronic structures in a computationally cheap and accurate way.
- Xuecheng Shao
- , Lukas Paetow
- & Michele Pavanello
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Article
| Open AccessControlling piezoresistance in single molecules through the isomerisation of bullvalenes
The quest for miniaturisation of electromechanical nanosystems requires the use of single molecules as active components. Here, the authors develop a piezoresistor based on a single bullvalene molecule that changes its shape by a Cope rearrangement.
- Jeffrey R. Reimers
- , Tiexin Li
- & Nadim Darwish
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Article
| Open AccessMachine learning coarse-grained potentials of protein thermodynamics
Understanding protein dynamics is a complex scientific challenge. Here, authors construct coarse-grained molecular potentials using artificial neural networks, significantly accelerating protein dynamics simulations while preserving their thermodynamics.
- Maciej Majewski
- , Adrià Pérez
- & Gianni De Fabritiis
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Article
| Open AccessResonating holes vs molecular spin-orbit coupled states in group-5 lacunar spinels
Dressing is a concept used to describe moderately interacting electrons. Here authors present the notion of dressed spin-orbit 3/2 moments and how this picture breaks down with increasing electronic interactions across group-5 lacunar spinel magnets.
- Thorben Petersen
- , Pritam Bhattacharyya
- & Liviu Hozoi
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Article
| Open AccessMinimizing non-radiative decay in molecular aggregates through control of excitonic coupling
Exciton delocalization in molecular aggregates is suggested to counteract the Energy Gap Law. Here, authors reveal the underlying physical picture and find the optimal excitonic coupling that minimizes nonradiative decay by nearly exact simulations.
- Yuanheng Wang
- , Jiajun Ren
- & Zhigang Shuai
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Article
| Open AccessTheory predicts UV/vis-to-IR photonic down conversion mediated by excited state vibrational polaritons
Vibrational polaritons steer chemical reactions and control quantum states for information processing. Here the authors predict their formation during electronic photo-excitation, enabling a down-conversion of visible to infrared photons.
- Connor K. Terry Weatherly
- , Justin Provazza
- & Roel Tempelaar
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Article
| Open AccessSynergy of dual-atom catalysts deviated from the scaling relationship for oxygen evolution reaction
The utilization of dual-atom catalysts holds the potential in surpassing single-atom catalysts for oxygen evolution reactions. Here, the authors examine the mechanism of dual-atom catalysts for oxygen evolution reaction and identify catalyst optimization recipes via large-scale computations.
- Cong Fang
- , Jian Zhou
- & Xiaoyan Sun
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Article
| Open AccessActinide inverse trans influence versus cooperative pushing from below and multi-center bonding
Actinide-ligand bonds with high multiplicities remain poorly understood. Here, the authors investigate covalency in actinide complexes and identify terminal O and N ligands that are triply to quadruply bonded to the actinide, facilitated by electrostatic, steric, and covalent interactions.
- Laura C. Motta
- & Jochen Autschbach
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Article
| Open AccessPotential-dependent transition of reaction mechanisms for oxygen evolution on layered double hydroxides
The mechanisms for oxygen evolution reaction on layered double hydroxides remain controversial. Here, the authors use a computational methodology by combining grand-canonical methods and microkinetic modeling to unravel the potential-dependent transitions mechanisms for electrochemical reactions.
- Zeyu Wang
- , William A. Goddard III
- & Hai Xiao
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Article
| Open AccessTemperature-pressure phase diagram of confined monolayer water/ice at first-principles accuracy with a machine-learning force field
Understanding the phase behaviour of nanoconfined water is of importance in science & engineering. Here the authors use machine-learning force field molecular dynamics to report two new quasi-bilayer ice phases in the phase diagram of monolayer ices.
- Bo Lin
- , Jian Jiang
- & Lei Li
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Article
| Open AccessQuantum simulation of exact electron dynamics can be more efficient than classical mean-field methods
It is often assumed that systems that can be analyzed accurately via mean-field theory would not be worth looking at using quantum algorithms, given entanglement plays no key role. Here, the authors show instead that a quantum advantage can be expected for simulating the exact time evolution of such electronic systems.
- Ryan Babbush
- , William J. Huggins
- & Joonho Lee
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Article
| Open AccessTunably strained metallacycles enable modular differentiation of aza-arene C–H bonds
The ability to selectively functionalize different sites on simple starting materials is a constant pursuit in organic chemistry. Here, the authors report a catalytic system to regioselectively differentiate and alkynylate different positions on azaarenes via rhodium catalysis.
- Longlong Xi
- , Minyan Wang
- & Zhuangzhi Shi
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Matters Arising
| Open AccessOn the existence of collective interactions reinforcing the metal-ligand bond in organometallic compounds
- Jordi Poater
- , Pascal Vermeeren
- & Miquel Solà
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Matters Arising
| Open AccessReply to: On the existence of collective interactions reinforcing the metal-ligand bond in organometallic compounds
- Vojtech Šadek
- , Shahin Sowlati-Hashjin
- & Cina Foroutan-Nejad
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Article
| Open AccessDesigning main-group catalysts for low-temperature methane combustion by ozone
Automated reaction route mapping is used to design catalysts for low-temperature CH4 combustion with ozone. A suitable proton-type zeolite catalyst with Brønsted acid sites was predicted and shown to have superior performance in CH4 combustion.
- Shunsaku Yasumura
- , Kenichiro Saita
- & Ken-ichi Shimizu
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Article
| Open AccessBayesian-optimization-assisted discovery of stereoselective aluminum complexes for ring-opening polymerization of racemic lactide
Stereoselective catalysts impact polymer’s properties, but discovering such catalysts is expensive and based on trial-and-error. Here, the authors develop a machine-learning tool to guide catalyst discovery and reveal mechanistic features affecting stereoselectivity.
- Xiaoqian Wang
- , Yang Huang
- & Rong Tong
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Article
| Open AccessStochastic representation of many-body quantum states
Variational approaches combined with machine learning are promising for solving quantum many-body problems, but they often suffer from scaling and optimization issues. Here the authors demonstrate that a stochastic representation of wavefunctions enables reducing the ground state search to standard regression.
- Hristiana Atanasova
- , Liam Bernheimer
- & Guy Cohen
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Article
| Open AccessEfficient interatomic descriptors for accurate machine learning force fields of extended molecules
Accurate description of non-local interactions represents a challenge for machine learning force fields. Here, authors develop linearly scaling global descriptors and analyse the non-local interatomic features that contribute to accurate predictions.
- Adil Kabylda
- , Valentin Vassilev-Galindo
- & Alexandre Tkatchenko
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Article
| Open AccessReaction performance prediction with an extrapolative and interpretable graph model based on chemical knowledge
Predictive modelling remains a key challenge for designing synthetic transformations. Here, the authors develop a knowledge-based graph model to predict reaction yield and stereoselectivity, offering an extrapolative and interpretable approach for evaluating reaction performance.
- Shu-Wen Li
- , Li-Cheng Xu
- & Xin Hong
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Article
| Open AccessManipulating hydrogen bond dissociation rates and mechanisms in water dimer through vibrational strong coupling
Mechanistic understanding of how light-matter interaction alters chemical reactivities remains a challenge. Here, the authors show both hydrogen bond dissociation rate and pathways can be modified through cavity-modified molecular coupling patterns.
- Qi Yu
- & Joel M. Bowman
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Article
| Open AccessRealistic phase diagram of water from “first principles” data-driven quantum simulations
The molecular modelling of water has been a long sought-after goal in computational sciences for more than 50 years. Here, the authors show that the data-driven many-body MB-pol potential can provide a realistic representation of the phase diagram of water.
- Sigbjørn Løland Bore
- & Francesco Paesani
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Article
| Open AccessAssessment of the technological viability of photoelectrochemical devices for oxygen and fuel production on Moon and Mars
Long-term space missions to the Moon and Mars rely on sunlight as an energy source. Here, authors assess the performance of monolithic photoelectrochemical devices for light-assisted O2 and fuel production on the Moon and Mars as potential complementary technologies to existing life support systems.
- Byron Ross
- , Sophia Haussener
- & Katharina Brinkert
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Article
| Open AccessLanthanide-doped MoS2 with enhanced oxygen reduction activity and biperiodic chemical trends
Oxygen reduction reaction plays a key role in many applications of MoS2-based materials. Here, using first-principles simulations, the authors find the enhanced oxygen-reduction activity with a biperiodic chemical trend on the lanthanide-doped MoS2.
- Yu Hao
- , Liping Wang
- & Liang-Feng Huang
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Article
| Open AccessIncoherent nonadiabatic to coherent adiabatic transition of electron transfer in colloidal quantum dot molecules
The transition between nonadiabatic and adiabatic electron transfer regimes has been observed in molecular donor-bridge-acceptor complexes. Here, the authors computationally show how to control this transition in colloidal quantum dot molecules and achieve coherent electron transfer at room temperature.
- Bokang Hou
- , Michael Thoss
- & Eran Rabani
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Article
| Open AccessRetrosynthesis prediction using an end-to-end graph generative architecture for molecular graph editing
Retrosynthesis prediction is a fundamental problem in organic synthesis. Here, inspired by simplified arrow-pushing reaction mechanisms, the authors develop a graph-to-edits framework, Graph2Edits, based on graph neural network for retrosynthesis prediction.
- Weihe Zhong
- , Ziduo Yang
- & Calvin Yu-Chian Chen
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Article
| Open AccessMachine learning-enabled exploration of the electrochemical stability of real-scale metallic nanoparticles
Surface Pourbaix diagrams are critical to understanding the stability of nanomaterials. Here, the authors develop a bond-type embedded crystal graph convolutional neural network model and construct reliable Pourbaix diagrams for real-scale nanoparticles.
- Kihoon Bang
- , Doosun Hong
- & Hyuck Mo Lee
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Article
| Open AccessArchitector for high-throughput cross-periodic table 3D complex building
Rare-earth and actinide complexes are critical for a wealth of clean-energy applications but Three dimensional (3D) structural generation and prediction for these organometallic systems remains challenging. Here, the authors propose a high-throughput in-silico synthesis code for s-, p-, d-, and f-block mononuclear organometallic complexes.
- Michael G. Taylor
- , Daniel J. Burrill
- & Ping Yang
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Article
| Open AccessComputational study on the catalytic control of endo/exo Diels-Alder reactions by cavity quantum vacuum fluctuations
Strong light-matter interactions are a pathway to chemical control at the molecular level. Here, authors theoretically show that an optical cavity allows to control catalysis, inhibition, and endo/exo stereoselectivity in Diels-Alder reactions.
- Fabijan Pavošević
- , Robert L. Smith
- & Angel Rubio
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Article
| Open AccessQuantum dynamical effects of vibrational strong coupling in chemical reactivity
Experiments suggest that placing molecules in an infrared cavity alters their reactivity, an effect lacking a clear theoretical explanation. Here, the authors show that the key to understanding this process may lie in quantum light-matter interactions.
- Lachlan P. Lindoy
- , Arkajit Mandal
- & David R. Reichman
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Article
| Open AccessProbing excitations and cooperatively rearranging regions in deeply supercooled liquids
Experimental data of the transition of a supercooled liquid into glass is compatible with both dynamic and thermodynamic theories. Here the authors use experiments and MD simulations at very low temperatures to show that both theories are connected.
- Levke Ortlieb
- , Trond S. Ingebrigtsen
- & C. Patrick Royall
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Article
| Open AccessThe importance of a charge transfer descriptor for screening potential CO2 reduction electrocatalysts
The electric double layer controls the product selectivity and conversion rate of electrochemical processes. Here the author presents a double layer-corrected computational electrocatalyst screening approach using CO2 reduction as an example that highlights the importance of the potential of zero charge descriptor.
- Stefan Ringe
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Article
| Open AccessSingle-step retrosynthesis prediction by leveraging commonly preserved substructures
Retrosynthesis is a critical task for organic chemistry with numerous industrial applications. Here, the authors build a machine learning model to learn the concept of substructures from a large reaction dataset to achieve chemist-like intuitions.
- Lei Fang
- , Junren Li
- & Jian-Guang Lou
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Article
| Open AccessInsights into solvent and surface charge effects on Volmer step kinetics on Pt (111)
Excess free charges on electrode surfaces drive changes in hydrogen electrocatalysis kinetics. Here, the authors show how redox solvent reorganization energy is insensitive to interfacial electric field strength; instead, the charged surface directly modulates proton electrochemical potential.
- Jon C. Wilson
- , Stavros Caratzoulas
- & Yushan Yan
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Article
| Open AccessTuning the reactivity of carbon surfaces with oxygen-containing functional groups
Distinguishing the influence of oxygen functional groups in carbon materials is important but elusive. Here, the authors combine experimental and machine learning techniques and reveal that phenolic groups are more acidic than carboxylic groups.
- Jiahua Zhou
- , Piaoping Yang
- & Dionisios G. Vlachos
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Article
| Open AccessCentral cavity dehydration as a gating mechanism of potassium channels
The hydrophobic gating is believed to function in various ion channels. Here, the authors use MD simulations to assess how dewetting of the channel pore modulates the function and conformational transition of the potassium channels.
- Ruo-Xu Gu
- & Bert L. de Groot
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Article
| Open AccessPerformance efficient macromolecular mechanics via sub-nanometer shape based coarse graining
Here the authors report SBCG2 an update to the neural network based, Shape-Based Coarse Graining (SBCG) approach for creating coarse grained molecular topologies with atomistic detail. They show how SBCG2 can reduce the computational costs of simulating very large assemblies like the HIV-1 capsid allowing simulation on commodity hardware.
- Alexander J. Bryer
- , Juan S. Rey
- & Juan R. Perilla
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Article
| Open AccessDeducing subnanometer cluster size and shape distributions of heterogeneous supported catalysts
IR spectra are great for characterizing single-crystals and large nanoparticles, but not for highly dispersed heterogeneous catalysts made up of single-atoms and ultra-small clusters. To solve this, the authors developed a method to generate synthetic IR spectra using data-based approaches and physics-driven surrogate models.
- Vinson Liao
- , Maximilian Cohen
- & Dionisios G. Vlachos
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Article
| Open AccessTwo-dimensional infrared-Raman spectroscopy as a probe of water’s tetrahedrality
Direct spectroscopic probes of the impact of structure on dynamical processes in liquids remain scarce. Here, the authors use molecular dynamics simulations to show that the correlation between vibrational coupling and the local tetrahedral structure of liquid water can be studied via hybrid terahertz- and infrared-Raman spectroscopy.
- Tomislav Begušić
- & Geoffrey A. Blake
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Article
| Open AccessEvaluating the evidence for exponential quantum advantage in ground-state quantum chemistry
The extent of problems in quantum chemistry for which quantum algorithms could provide a speedup is still unclear, as well as the kind of speedup one should expect. Here, the authors look at the problem of ground state energy estimation, and gather theoretical and numerical evidence for the fact that an exponential quantum advantage is unlikely for generic problems of interest.
- Seunghoon Lee
- , Joonho Lee
- & Garnet Kin-Lic Chan
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Article
| Open AccessTowards the ground state of molecules via diffusion Monte Carlo on neural networks
An accurate ab initio calculation of molecules is fundamental to chemical and physical sciences. Here, the authors integrate a neural-network wavefunction into the fixed-node diffusion Monte Carlo, resulting in accurate calculations of a diverse range of systems, offering insights into complex many-body electronic wave functions.
- Weiluo Ren
- , Weizhong Fu
- & Ji Chen
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Article
| Open AccessTheory of sigma bond resonance in flat boron materials
Here, the authors present a resonance theory to describe the bonding configuration of flat boron materials without quantum calculation. Like aromaticity theory in carbon, it allows to intuitively understand the stability and properties of boron-related materials
- Lu Qiu
- , Xiuyun Zhang
- & Feng Ding
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Article
| Open AccessGas phase synthesis of the C40 nano bowl C40H10
Nanobowls represent building blocks of fullerenes and nanotubes as detected in combustion systems and deep space, but their formation mechanisms in these environments have remained elusive. Here, the authors explore the gas-phase formation of benzocorannulene and beyond to the C40 nanobowl.
- Lotefa B. Tuli
- , Shane J. Goettl
- & Ralf I. Kaiser