Papers nuevos sobre Química molecular y computacional
56 papers nuevos sobre química molecular y computacional en los últimos 7 días, dentro de Química y materiales. Acá están los 50 que Pipette considera más valiosos, con el resultado principal en palabras de sus autores.
Lo mejor de la semana
Direct Visualization of a Hydroperoxy Intermediate in Fluorescent Protein Chromophore Maturation in PAmCherry1
Collectively, these results support a hydroperoxy intermediate as a key species in oxidative chromophore maturation, which is stabilized in non-photoactivated PAmCherry1.
Revista con revisión por paresDice ser un gran avanceUnlocking 17O Natural-Abundance Nuclear Magnetic Resonance Detection in Solids
This method enables us to obtain 17O NMR spectra with excellent signal-to-noise ratios and natural abundance within minutes using samples at room temperature and straight from the shelf.
Revista con revisión por paresAfirmaciones fuertes, leer con cuidadoDouble Boron-Deleting Annulation: Modular Access to Chiral Nonalternant B,N-Helicenes with Enhanced Chiroptical Properties
Herein, we report an unprecedented modular synthesis of nonalternant B,N-embedded helical molecular carbons (HMCs) (BN-HMCs, 12 examples) featuring diaza-pentagon-heptagon pairs via double boron-deleting annulation (dBDA).
Revista con revisión por paresDice ser un gran avanceRedox-Switchable Tristable 1,3,2,4,5-Triboradiazoles
Here we report a 1,3,2,4,5-triboradiazole (2), an all-inorganic BN-heterocycle isoelectronic with Cp–, that undergoes clean and fully reversible 0/+1/+2 redox interconversion, enabling the isolation and structural characterization of three discrete redox states based on a single B3N2 ring.
Revista con revisión por parescboamd: A Machine Learning Molecular Dynamics Framework for Vibrational Strong Coupling
In this work, we develop a machine-learning interatomic potential (MLIP) based framework to study VSC inside optical cavities.
PreprintHolistic Assessment of Actinide-Borohydride Covalency Using NMR and X-ray Absorption Spectroscopies
Herein, we report the first comparative assessment of actinide-ligand covalency using B K-edge XAS and multinuclear NMR spectroscopy.
Revista con revisión por paresComposition-Dependent Self-Diffusion Coefficients in Liquid Mixtures from Hybrid Machine Learning
Here, we extend this approach to concentration-dependent self-diffusion coefficients and multicomponent solvents with HADES.
PreprintA Coordination Cage That Shrinks via Single-Site Labilization to Reshape Encapsulated Guests
This design enables the cage to switch between expanded and contracted states without releasing its guest, thereby mechanically controlling the guest’s shape.
Revista con revisión por paresCoherent Vibrational Wave Packet Motion in Er Cry4a Proteins Monitors the Redox State of the Flavin Chromophore
Our results provide insight into the role of nonadiabatic couplings for the initial steps of cryptochrome photoactivation and suggest a general strategy for redox-state-specific monitoring of charge transfer dynamics by probing coherent vibrational motion.
Revista con revisión por paresA System-Independent Metadynamics Strategy for Reactive Training Data: Application to Gas-Phase Organic Reactions
Within a concurrent-learning workflow, this produces OpenRxn26, a dataset of 1.8~M DFT-labeled configurations covering neutral singlet unimolecular reactions in the H/C/N/O chemical space (), containing reactive atomic environments underrepresented in community datasets.
PreprintBeyond the Virial Expansion: Microscopic Origins of Partial Molar Volumes in LiCl Solutions
The resulting data enable the development of highly accurate force fields for Li+ and Cl–, revealing a clear progression from isolated ions to ion pairs and ultimately to higher-order chain and ring structures.
Revista con revisión por paresPhonon chirality as an additive control of CISS: a symmetry-protected law
The phonon contribution can therefore enhance, cancel, or reverse the molecular CISS signal.
PreprintECENet: An Edge Cluster Expansion Line-Graph Neural Network
Here we introduce the edge cluster expansion (ECE), an analogue of the atomic cluster expansion in which the environment is expanded around edges between atom pairs rather than single atoms, and build upon it to develop the line-graph neural network ECENet.
PreprintSynthesis, Evaluation, and Context for Applications of SF5-Containing [1.1.1]Bicyclopentane and [ 2 ]Staffane “Hybrid Bioisosteres”
Together, the results of this extensive study position SF5-BCPs and SF5-[2]staffanes as practical hybrid bioisosteres for tuning molecular properties in drug discovery.
Revista con revisión por paresFrom Heuristics to Machine Learning: The Performance Ceiling for Single-Ion Magnets and Its Electronic Origin
The electronic-structure and connectivity information needed to identify SIMs is therefore not accessible to geometric methods alone.
PreprintOrbital-Free Surrogate Functionals Yield Transferable Interatomic Potentials and Electron Densities
Here, we extend the recently introduced (weak) surrogate functional framework - designed to predict ground-state electron densities only - to also yield their energy, resulting in "strong" surrogate functionals.
PreprintAfirmaciones fuertes, leer con cuidadoDisentangling Electronic and Lattice Contributions to Transient Absorption in Metal Halide Perovskites: A First-Principles Study of CH3NH3PbBr3
This approach can quantitatively disentangle electronic and thermal lattice contributions across femtosecond-to-picosecond time scales.
Revista con revisión por paresEvaluation of Binding and Cell Penetration of Imidazolium Amino Acids as Novel Bioisosteres for Trimethyllysine, Dimethylarginine, and Arginine
We find that these biomimetics can replace Kme3, Rme2, and Arg, with similar or even improved binding in some cases, while also providing unique selectivity patterns relative to the parent amino acid.
Revista con revisión por paresUso en el mundo realFirst-Principles Nonadiabatic Dynamics via the Multi-Orbital Anderson-Newns Model
We develop a first-principles theory for nonadiabatic surface dynamics, providing a fit-free connection between density functional theory (DFT) calculations and the effective multi-orbital Anderson-Newns (AN) theory.
PreprintA Task-Based Framework for Evaluating Raman Spectral Quality Measures
We present a controlled-perturbation framework for testing this relationship.
PreprintCódigo disponibleThe role of shape and interaction directionality in the crystalline phase behaviour of octahedral metal-organic cages
Here, we present a computationally inexpensive methodology that combines semi-empirical dimer calculations with coarse-grained modelling to predict the packing behaviour of MOCs.
Revista con revisión por paresFull-frequency GW from Cayley-transformed self-energy moments
We reformulate this approximation, representing the particle and hole parts of the GW self-energy through a highly compact set of Cayley-transformed moment constraints.
PreprintHelicity Synchronization-Induced Kinetic Stabilization against Helix Inversion in Stapled Peptides: Effects of 310/α Block Sequence and Double-Stapling Topology
These results demonstrate how communication between distinct peptide helices gives rise to emergent dynamic behavior and provide a general strategy for programming helical dynamics in abiotic peptide systems.
Revista con revisión por paresThe phosphorus analogues of diazomethane and isomeric diazirine
Here, the authors report the preparation and characterization of methyleneaminophosphinidene and 3H-azaphosphirine.
Revista con revisión por paresDecongested 2D IR Spectra Reveal N-Terminal Helices in Amyloid Oligomers Associated with Type 2 Diabetes
Spectra acquired at a waiting time of 1.2 ps are decongested of disordered structures, revealing features originating from the oligomeric N-terminal α-helix and the adjacent kink and disulfide-loop regions.
Revista con revisión por paresFrom sparse quantum-computing data to atomistic simulation with universal machine-learning interatomic potentials
These results demonstrate that the proposed framework provides a practical route for incorporating quantum-computing calculations into realistic atomistic simulations and that quantum-computing reference data can improve pretrained uMLIPs.
PreprintAttosecond charge migration timescales are dominated by transition dipoles, not correlations
Employing a semi-analytical theory that reconstructs the hole moments in the cationic reference frame, we show that the attosecond timescale of CM is determined by molecular dipoles that filter out specific frequency responses with an analogy to optical selection rules.
PreprintAfirmaciones fuertes, leer con cuidadoAsymmetric Hydration and Protonation Switching of Dual Aspartates Drive Flagellar Rotation
Our findings reveal that MotA rotation requires two essential prerequisites: plug removal and alternating D22 protonation switching, coupled with dynamic gauche-trans conformational changes in the side chain of D22.
Revista con revisión por paresMolExplain: An Interactive Tool for Explainable Molecular Property Prediction
MolExplain addresses this gap by combining property prediction with sub-structure level visual explainability in an interactive web interface.
PreprintUso en el mundo realNear Chemical Accuracy From Size-Consistent Pad\'e Resummed M{\o}ller-Plesset Perturbation Theory
We find that damping the third-order same-spin contribution leads to substantially increased accuracy, with the resulting same-spin damped orbital Pad\'e resummed (SSD-OPMP3) approach attaining near-chemical accuracy (mean absolute error 1 kcal/mol) for total atomization energies of non-multireference molecules in the W4-17 dataset against the gold standard CCSD(T) method.
PreprintEnriching molecular Raman spectroscopy with vibrational strong coupling
We theoretically show that vibrational strong coupling (VSC) can reshape Raman spectra by reorganizing vibrational energies and intensities.
PreprintSeparating multi-particle dynamics by intensity cycling
The key result is a general formula expressing the extracted nonlinear signal terms by multi-excitation propagators.
PreprintOn the Electronic Path-Integral Normal Modes of the Spin-Mapping Representation of Nonadiabatic Dynamics
We find, perhaps surprisingly, that the higher normal modes of the spin-vector -component, the difference in state populations, are constrained by the QBD, that the time-evolved state population observable is a function of only the spin-mapping centroid, and that the full -bead computational results are replicated using only the spin-mapping centroid, leading to accurate, QBD conserving dynamics.
PreprintSolvent Inertia Changes Product Probability by Relocating the Phase-Space Reactivity Boundary
The calculation connects solvent inertia to product probability through the geometry of the full Hamiltonian flow, rather than through a change in the PES.
PreprintDisentangling Direct Coupling from Charge-Transfer-Mediated Coupling in Singlet Fission of Weakly Interacting Dimers
Our findings support a primarily direct i-SF mechanism, facilitated by weak, yet direct excitonic coupling between singlet- and triplet-pair states, that decreases with increasing dihedral angle, while superexchange coupling via the dark CT states increases.
Revista con revisión por paresTotal Synthesis and Structure Determination of Mutanolins Detected in a Human Oral Microbiome Symbiont
Herein, we present streamlined total syntheses to elucidate the structures of mutanolins A–F.
Revista con revisión por paresAdsorption of Phosgene Gas on Pristine and Noble Metal-Doped B12N12 Nanocages: Insights from Density Functional Theory
Platinum doping is therefore the most effective strategy for reversible phosgene detection using B12N12 nanocages.
PreprintUso en el mundo realReaxKit: A Modular Python Toolkit for Preparing, Parsing, and Analyzing ReaxFF Molecular Dynamics Simulations
Here, we present ReaxKit, a modular Python toolkit for preparing, parsing, analyzing, and managing ReaxFF molecular dynamics simulations.
PreprintHow the Energy Gaps between Partners Rule ns-Scale Sensitization and Back-Energy Transfer in Lanthanide(III) Complexes?
These results elucidate the complex kinetic picture of lanthanide(III) sensitization, highlighting the energy gap as the fundamental parameter that governs both photosensitization kinetics and the subsequent photophysical pathways.
Revista con revisión por paresHydration States of Transplutonium (Am, Cm, Bk, and Cf) Ions Alter Electronic Structure
By combining crystallographic and spectroscopic data with ab initio multiconfigurational wave function calculations, we demonstrate that differences between the two hydration motifs give rise to distinct trends in bond lengths, spectral features, and crystal-field strengths.
Revista con revisión por paresPauli exclusion as a necessary condition for the existence of the H + H atom transfer barrier
This approach reveals that Pauli exclusion is necessary for the existence of the energy barrier to H+H atom transfer, which is consistent with a complementary analysis using absolutely-localized molecular orbitals.
PreprintStrong-Field-Driven Non-Linear Electron Dynamics in Thiophene Oligomers
We demonstrate that extended -conjugation in 4T lowers nonlinear excitation thresholds by orders of magnitude compared to 1T.
PreprintUncertainty prediction in composite quantum chemistry approaches
To remedy this, we propose a method of estimating the total uncertainty of the composite scheme which does not rely on the assumption that the components are independent.
PreprintContinuous perception and adaptive metrics for scalable structure refinement
We present a geometry-refinement workflow that adapts to the cost of an energy--gradient evaluation and the reliability of molecular topology.
PreprintMass-Scaling of Quantum Tunnelling in Hydrogen Bonds: Analytical Model and Comparison with Multidimensional Potentials
Comparison with multidimensional reaction-space calculations for the formic acid dimer shows that this scaling persists in fully coupled 3D and 5D quantum models, yielding an empirical relation .
Preprint con versión publicadaCan Chemically Inspired Parameter Initialization Mitigate Barren Plateaus in Variational Quantum Eigensolvers?
In the benchmarks considered here, chemically initialized starting points and variational trajectories show polynomial decay of local gradient variance with system size instead of the exponential BP-like decay observed for random controls, indicating that chemical initialization mitigates barren plateaus in the local optimization regions and highlights the trainability advantage of chemically motivated VQE strategies.
Preprintfix uvt and fix pimd/uvt: A Unified LAMMPS Framework for Constant-Potential Constant-Temperature Molecular Dynamics
In this work, we implement fix uvt and fix pimd/uvt in LAMMPS for constant-potential classical MD and path integral molecular dynamics (PIMD), respectively.
PreprintSelectivity in Tip-Induced Skeletal Editing via Heteroatom Substitution
Here we show that tip-induced reactions of an analogous sulfur-containing seven-membered ring mainly result in sulfur deletion.
Revista con revisión por paresDisentangling Surface Charge and Electrolyte Effects on Interfacial Water at Electrified Pt(111)
These results suggest that surface charge controls the average structural response, whereas electrolyte ions and their solvation shells become visible only when locally refined descriptors are investigated or probed, e.g. the H-bond network topology and vibrational fingerprints of the interfacial bilayer.
PreprintOn the importance of multi-configurational and exchange effects in molecular aggregates
We present an extension of the Frenkel exciton model to incorporate exchange interactions between monomers in molecular aggregates in conjunction with {a multi-reference electronic structure approach}.
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