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Suppression of cracking in drying colloidal suspensions with chain-like particles J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-24 Zhaoxia Niu, Yiping Zhao, Qiuting Zhang, Zhiyuan Zhao, Dengteng Ge, Jiajia Zhou, Ye Xu
The prevention of drying-induced cracking is crucial in maintaining the mechanical integrity and functionality of colloidal deposits and coatings. Despite exploring various approaches, controlling drying-induced cracking remains a subject of great scientific interest and practical importance. By introducing chain-like particles composed of the same material and with comparable size into commonly used
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A variance-based optimization for determining ground and excited N-electron wave functions within the doubly occupied configuration interaction scheme J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-24 Diego R. Alcoba, Ofelia B. Oña, Alicia Torre, Luis Lain, Guadalupe Sierra, Gustavo E. Massaccesi
This work describes optimizations of N-electron system wave functions by means of the simulated annealing technique within the doubly occupied configuration interaction framework. Using that technique, we minimize the energy variance of a Hamiltonian, providing determinations of wave functions corresponding to ground or excited states in an identical manner. The procedure that allows us to determine
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AB-G0W0: A practical G0W0 method without frequency integration based on an auxiliary boson expansion J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-24 Johannes Tölle, Garnet Kin-Lic Chan
Common G0W0 implementations rely on numerical or analytical frequency integration to determine the G0W0 self-energy, which results in a variety of practical complications. Recently, we have demonstrated an exact connection between the G0W0 approximation and equation-of-motion quantum chemistry approaches [J. Tölle and G. Kin-Lic Chan, J. Chem. Phys. 158, 124123 (2023)]. Based on this connection, we
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Interfacial water on collagen nanoribbons by 3D AFM J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-24 Diana M. Arvelo, Clara Garcia-Sacristan, Enrique Chacón, Pedro Tarazona, Ricardo Garcia
Collagen is the most abundant structural protein in mammals. Type I collagen in its fibril form has a characteristic pattern structure that alternates two regions called gap and overlap. The structure and properties of collagens are highly dependent on the water and mineral content of the environment. Here, we apply 3D AFM to characterize at angstrom-scale resolution the interfacial water structure
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Observation of liquid glass in molecular dynamics simulations J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-24 Mohammed Alhissi, Andreas Zumbusch, Matthias Fuchs
Molecular anisotropy plays an important role in the glass transition of a liquid. Recently, a novel bulk glass state has been discovered by optical microscopy experiments on suspensions of ellipsoidal colloids. “Liquid glass” is a disordered analog of a nematic liquid crystal, in which rotation motion is hindered but particles diffuse freely. Global nematic order is suppressed as clusters of aligned
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Understanding the effect of density functional choice and van der Waals treatment on predicting the binding configuration, loading, and stability of amine-grafted metal organic frameworks J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-24 Jonathan R. Owens, Bojun Feng, Jie Liu, David Moore
Metal organic frameworks (MOFs) are crystalline, three-dimensional structures with high surface areas and tunable porosities. Made from metal nodes connected by organic linkers, the exact properties of a given MOF are determined by node and linker choice. MOFs hold promise for numerous applications, including gas capture and storage. M2(4,4′-dioxidobiphenyl-3,3′-dicarboxylate)—henceforth simply M2(dobpdc)
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Collapse and expansion kinetics of a single polyelectrolyte chain with hydrodynamic interactions J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-24 Jiaxing Yuan, Tine Curk
We investigate the collapse and expansion dynamics of a linear polyelectrolyte (PE) with hydrodynamic interactions. Using dissipative particle dynamics with a bead–spring PE model, long-range electrostatics, and explicit ions, we examine how the timescales of collapse tcol and expansion texp depend on the chain length N and obtain scaling relationships tcol ∼ Nα and texp ∼ Nβ. For neutral polymers
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Dynamical properties of solid and hydrated collagen: Insight from nuclear magnetic resonance relaxometry J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-24 Elzbieta Masiewicz, Farman Ullah, Adrianna Mieloch, Janusz Godlewski, Danuta Kruk
1H spin-lattice Nuclear Magnetic Resonance relaxometry experiments have been performed for collagen and collagen-based artificial tissues in the frequency range of 10 kHz–20 MHz. The studies were performed for non-hydrated and hydrated materials. The relaxation data have been interpreted as including relaxation contributions originating from 1H–1H and 1H–14N dipole–dipole interactions, the latter leading
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Photogenerated carrier dynamics of Mn2+ doped CsPbBr3 assembled with TiO2 systems: Effect of Mn doping content J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-24 Luchao Du, Jie An, Tetsuro Katayama, Menghan Duan, XiaoPing Shi, Yunpeng Wang, Akihiro Furube
In recent years, all-inorganic perovskite materials have become an ideal choice for new thin film solar cells due to their excellent photophysical properties and have become a research hotspot. Studying the ultrafast dynamics of photo-generated carriers is of great significance for further improving the performance of such devices. In this work, we focus on the transient dynamic process of CsPbBr3/TiO2
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Finite temperature dynamics in a polarized sub-Ohmic heat bath: A hierarchical equations of motion-tensor train study J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-24 Hideaki Takahashi, Raffaele Borrelli, Maxim F. Gelin, Lipeng Chen
The dynamics of the sub-Ohmic spin-boson model under polarized initial conditions at finite temperatures is investigated by employing both analytical tools and the numerically accurate hierarchical equations of motion-tensor train method. By analyzing the features of nonequilibrium dynamics, we discovered a bifurcation phenomenon, which separates two regimes of the dynamics. It is found that before
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Promoting effect of lanthanum doping on photovoltaic performance of CZTSSe solar cells J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-24 Zhengjun Luo, Lei Yu, Tingting Zheng, Xiaofei Dong, Fengxia Yang, Jiangtao Chen, Xuqiang Zhang, Yun Zhao, Yan Li
A large open-circuit voltage (VOC) deficit is the major challenge hindering the efficiency improvement of Cu2ZnSn(S,Se)4 (CZTSSe) solar cells. Cation substitution, or doping, is usually an effective strategy to achieve carrier regulation and improve efficiency. In this work, we developed a rare-earth element lanthanum (La) doped CZTSSe thin-film solar cell by directly introducing La3+ ions into the
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Light-induced photoluminescence enhancement in chiral CdSe quantum dot films J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 Yang Wang, Pan Liang, Yumeng Men, Meizhen Jiang, Lin Cheng, Jinlei Li, Tianqing Jia, Zhenrong Sun, Donghai Feng
Chiral quantum dots (QDs) are promising materials applied in many areas, such as chiral molecular recognition and spin selective filter for charge transport, and can be prepared by facile ligand exchange approaches. However, ligand exchange leads to an increase in surface defects and reduces the efficiencies of radiative recombination and charge transport, which restricts further applications. Here
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Molecular chirality quantification: Tools and benchmarks J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 Ethan Abraham, Abraham Nitzan
Molecular chirality has traditionally been viewed as a binary property where a molecule is classified as either chiral or achiral, yet in recent decades, mathematical methods for quantifying chirality have been explored. Here, we use toy molecular systems to systematically compare the performance of two state-of-the-art chirality measures: (1) the Continuous Chirality Measure (CCM) and (2) the Chirality
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Generalized Helmholtz model describes capacitance profiles of ionic liquids and concentrated aqueous electrolytes J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 Suehyun Park, Jesse G. McDaniel
In this work, we propose and validate a generalization of the Helmholtz model that can account for both “bell-shaped” and “camel-shaped” differential capacitance profiles of concentrated electrolytes, the latter being characteristic of ionic liquids. The generalization is based on introducing voltage dependence of both the dielectric constant “ϵr(V)” and thickness “L(V)” of the inner Helmholtz layer
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Floquet non-equilibrium Green’s function and Floquet quantum master equation for electronic transport: The role of electron–electron interactions and spin current with circular light J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 Vahid Mosallanejad, Yu Wang, Wenjie Dou
The non-equilibrium Green’s function (NEGF) and quantum master equation (QME) are two main classes of approaches for electronic transport. We discuss various Floquet variances of these formalisms for transport properties of a quantum dot driven via interaction with an external periodic field. We first derived two versions of the Floquet NEGF. We also explore an ansatz of the Floquet NEGF formalism
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Laboratory study of rotationally inelastic collisions of CO2 at low temperatures J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 C. Álvarez, G. Tejeda, J. M. Fernández
The rotational relaxation of CO2 by inelastic collisions has been studied in three supersonic jets. The jets were probed by means of Raman spectroscopy with high spectral and spatial resolutions, measuring the rotational populations and the total number density. The time evolution of the rotational populations was analyzed by means of a kinetic master equation, with the help of the energy-corrected
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The tale of HORTON: Lessons learned in a decade of scientific software development J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 Matthew Chan, Toon Verstraelen, Alireza Tehrani, Michelle Richer, Xiaotian Derrick Yang, Taewon David Kim, Esteban Vöhringer-Martinez, Farnaz Heidar-Zadeh, Paul W. Ayers
HORTON is a free and open-source electronic-structure package written primarily in Python 3 with some underlying C++ components. While HORTON’s development has been mainly directed by the research interests of its leading contributing groups, it is designed to be easily modified, extended, and used by other developers of quantum chemistry methods or post-processing techniques. Most importantly, HORTON
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The propagation behavior of reaction wave for Ni/Al clad particle composites under shock loading J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 Yifan Xie, Jian-Li Shao, Pengwan Chen
Prior studies indicate that the reaction wave can propagate from the impact surface, but the possibility and the influencing factors of the reaction wave formation are still unclear. This work investigates the propagation behavior of the shock-induced reaction wave for Ni/Al clad particle composites with varying stoichiometry (from 0.5 to 0.75 of the Ni mole fraction) through molecular dynamics simulations
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What is the best simulation approach for measuring local density fluctuations near solvo-/hydrophobes? J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 Nigel B. Wilding, Robert Evans, Francesco Turci
Measurements of local density fluctuations are crucial to characterizing the interfacial properties of equilibrium fluids. A specific case that has been well-explored involves the heightened compressibility of water near hydrophobic entities. Commonly, a spatial profile of local fluctuation strength is constructed from the measurements of the mean and variance of solvent particle number fluctuations
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A novel non-adiabatic spin relaxation mechanism in molecular qubits J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 Philip Shushkov
The interaction of electronic spin and molecular vibrations mediated by spin–orbit coupling governs spin relaxation in molecular qubits. We derive an extended molecular spin Hamiltonian that includes both adiabatic and non-adiabatic spin-dependent interactions, and we implement the computation of its matrix elements using state-of-the-art density functional theory. The new molecular spin Hamiltonian
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Cation effects in hydrogen evolution and CO2-to-CO conversion: A critical perspective J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 Yu-Shen Hsu, Sachinthya T. Rathnayake, Matthias M. Waegele
The rates of many electrocatalytic reactions can be strongly affected by the structure and dynamics of the electrochemical double layer, which in turn can be tuned by the concentration and identity of the supporting electrolyte’s cation. The effect of cations on an electrocatalytic process depends on a complex interplay between electrolyte components, electrode material and surface structure, applied
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High spatial resolution surface plasmon resonance imaging using a plasmonic chip J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 Yasunori Nawa, Keiko Tawa
The surface plasmon resonance (SPR) technique has been widely applied to biosensing technologies for the rapid quantification of biomolecules without enzyme and fluorescent labeling. However, the conventional prism-coupling SPR method generally has a detection area of a few mm2, and the large contribution of the background signal forms a barrier to highly sensitive detection. Based on a highly spatially
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Time-resolved solvation of alkali ions in superfluid helium nanodroplets J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-23 Ernesto García-Alfonso, Manuel Barranco, Nadine Halberstadt, Martí Pi
The sinking of alkali cations in superfluid 4He nanodroplets is investigated theoretically using liquid 4He time-dependent density functional theory at zero temperature. The simulations illustrate the dynamics of the buildup of the first solvation shell around the ions. The number of helium atoms in this shell is found to linearly increase with time during the first stages of the dynamics. This points
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The bond energy of UN+: Guided ion beam studies of the reactions of U+ with N2 and NO J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Amanda R. Bubas, Arjun Kafle, Brandon C. Stevenson, P. B. Armentrout
A guided ion beam tandem mass spectrometer was used to study the reactions of U+ with N2 and NO. Reaction cross sections were measured over a wide range of energy for both systems. In each reaction, UN+ is formed by an endothermic process, thereby enabling the direct measurement of the threshold energy and determination of the UN+ bond dissociation energy. For the reaction of U+ + N2, a threshold energy
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Deposition of Ca on the 2H–NbSe2 surface: Competing processes J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 H. I. Starnberg
The interaction of Ca evaporated in vacuum onto a 2H–NbSe2 surface held at room temperature was studied by photoelectron spectroscopy. Indications of an intercalation reaction were observed initially, but larger Ca depositions resulted in a layer-breaking reaction producing a disordered overlayer of varying compositions. The layer-breaking reaction is likely due to the intercalation compound becoming
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Hot carrier relaxation dynamics of an aza-covalent organic framework during photoexcitation: An insight from ab initio quantum dynamics J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Atish Ghosh, Priya Das, Subhash Kumar, Pranab Sarkar
In order to develop an efficient metal-free solar energy harvester, we herein performed the electronic structure calculation, followed by the hot carrier relaxation dynamics of two dimensional (2D) aza-covalent organic framework by time domain density functional calculations in conjunction with non-adiabatic molecular dynamics (NAMD) simulation. The electronic structure calculation shows that the aza-covalent
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Confinement effects of mandrel degradation in ICF target fabrication J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Yue Xin, Xinrui Yang, Chenxi Wan, Rui Wang, Yu Zhu, Yong Yi, Zhanwen Zhang, Yongjian Tang, Qiang Chen, Zhigang Wang
Understanding and further regulating the degradation of mandrel materials is a key aspect of target fabrication in inertial confinement fusion (ICF). Here, a quasi-one-dimensional confinement model is developed using a series of single-walled carbon nanotubes with varying diameters (Dm), and the degradation of poly-α-methylstyrene (PAMS) as a typical mandrel material is investigated under such confined
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Ternary recombination of excited Ar+(P1/22) ions, established experimental results reinterpreted with a new extended model J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 F. T. Nongni, R. Kalus, M. Benhenni, F. X. Gadéa, M. Yousfi
For many years, the recombination of excited ions of argon, Ar+(P1/22), has been assumed negligible under ambient conditions as compared to the recombination of ground-state ions, Ar+(P3/22). This opinion was confronted with detailed experimental results that seem to clearly support it. Here, we propose a new interpretation in light of our recent calculations, which shows that the recombination efficiency
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Bond dissociation energy of O2 measured by fully state-to-state resolved threshold fragment yield spectra J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Peng Wang, Shiyan Gong, Yuxiang Mo
We have determined the bond dissociation energy of O2 by measuring fully state-to-state resolved threshold fragment yield spectra in the XUV energy region, O2X3Σg−,N″,J″→O(PJ3)+O(S1o3)/O(S2o5). Our results have yielded a bond dissociation energy value of 41 269.19 ± 0.10 cm−1, which is consistent with previous measurements but exhibits a significantly lower uncertainty, approximately five times smaller
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HCl trimer: HCl-stretch excited intramolecular and intermolecular vibrational states from 12D fully coupled quantum calculations employing contracted intra- and inter-molecular bases J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Irén Simkó, Peter M. Felker, Zlatko Bačić
We present fully coupled, full-dimensional quantum calculations of the inter- and intra-molecular vibrational states of HCl trimer, a paradigmatic hydrogen-bonded molecular trimer. They are performed utilizing the recently developed methodology for the rigorous 12D quantum treatment of the vibrations of the noncovalently bound trimers of flexible diatomic molecules [Felker and Bačić, J. Chem. Phys
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The effect of ligands on the size distribution of copper nanoclusters: Insights from molecular dynamics simulations J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Oren Elishav, Ofir Blumer, T. Kyle Vanderlick, Barak Hirshberg
Controlling the size distribution in the nucleation of copper particles is crucial for achieving nanocrystals with desired physical and chemical properties. However, their synthesis involves a complex system of solvents, ligands, and copper precursors with intertwining effects on the size of the nanoclusters. We combine molecular dynamics simulations and density functional theory calculations to provide
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Cocatalyst activity mapping for photocatalytic materials revealed by the pattern-illumination time-resolved phase microscopy J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Yuta Egawa, Kei Kawaguchi, Zhenhua Pan, Kenji Katayama
Photocatalytic water-splitting represents a promising avenue for clean hydrogen production, necessitating an in-depth understanding of the photocatalytic reaction mechanism. The majority of the photocatalytic materials need cocatalysts to enhance the photo-oxidation or reduction reactions. However, the working mechanism, such as collecting charge carriers or reducing the reaction barrier, is not clear
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Theoretical model of femtosecond coherence spectroscopy of vibronic excitons in molecular aggregates J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Alexander J. Rode, Paul C. Arpin, Daniel B. Turner
When used as pump pulses in transient absorption spectroscopy measurements, femtosecond laser pulses can produce oscillatory signals known as quantum beats. The quantum beats arise from coherent superpositions of the states of the sample and are best studied in the Fourier domain using Femtosecond Coherence Spectroscopy (FCS), which consists of one-dimensional amplitude and phase plots of a specified
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Solar energy broadband capturing by metamaterial absorber based on titanium metal J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Xiaoqing Zhu, Bo Wang
In recent years, the exploration of solar absorbers has grown in favor due to the scarcity of energy. Here, we propose an absorber with an array of a circular ring surrounding disk (RSD) for solar energy capture. The novel structure keeps above 93.5% absorption with an average absorption of 96.95% in wavelengths from 300 to 4000 nm. Meanwhile, the proposed absorber is advantageous in that the structure
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Large-cage occupation and quantum dynamics of hydrogen molecules in sII clathrate hydrates J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Umbertoluca Ranieri, Leonardo del Rosso, Livia Eleonora Bove, Milva Celli, Daniele Colognesi, Richard Gaal, Thomas C. Hansen, Michael Marek Koza, Lorenzo Ulivi
Hydrogen clathrate hydrates are ice-like crystalline substances in which hydrogen molecules are trapped inside polyhedral cages formed by the water molecules. Small cages can host only a single H2 molecule, while each large cage can be occupied by up to four H2 molecules. Here, we present a neutron scattering study on the structure of the sII hydrogen clathrate hydrate and on the low-temperature dynamics
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Surface tension of aqueous electrolyte solutions. A thermomechanical approach J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Yury A. Budkov, Nikolai N. Kalikin, Petr E. Brandyshev
We determine the surface tension of aqueous electrolyte solutions in contact with non-polar dielectric media using a thermomechanical approach, which involves deriving the stress tensor from the thermodynamic potential of an inhomogeneous fluid. To obtain the surface tension, we calculate both the normal and tangential pressures using the components of the stress tensor, recently derived by us [Y.
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Effect of the presence of pinned particles on the structural parameters of a liquid and correlation between structure and dynamics at the local level J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Palak Patel, Sarika Maitra Bhattacharyya
Pinning particles at the equilibrium configuration of the liquid is expected not to affect the structure and any property that depends on the structure while slowing down the dynamics. This leads to a breakdown of the structure dynamics correlation. Here, we calculate two structural quantities: the pair excess entropy, S2, and the mean field caging potential, the inverse of which is our structural
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Theoretical investigation of distal charge separation in a perylenediimide trimer J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Ke Wang, Yihe Xu, Xiaoyu Xie, Haibo Ma
An exciton–phonon (ex–ph) model based on our recently developed block interaction product basis framework is introduced to simulate the distal charge separation (CS) process in aggregated perylenediimide (PDI) trimer incorporating the quantum dynamic method, i.e., the time-dependent density matrix renormalization group. The electronic Hamiltonian in the ex–ph model is represented by nine constructed
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Structural evolution and bonding properties of Nb1–2Gen−/0 (n = 3–7) clusters: Anion photoelectron spectroscopy and theoretical calculations J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-22 Sheng-Jie Lu, Zhao-Ou Gao
This study presents a collaborative experimental and theoretical investigation into the structures and electronic properties of niobium-doped germanium clusters. Anion photoelectron spectra for Nb1–2Gen− (n = 3–7) clusters were acquired using 266 nm photon energies, enabling the determination of adiabatic detachment energies and vertical detachment energies. In conjunction with these experimental measurements
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Enhancing torsional sampling using fully adaptive simulated tempering J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-19 Miroslav Suruzhon, Khaled Abdel-Maksoud, Michael S. Bodnarchuk, Antonella Ciancetta, Ian D. Wall, Jonathan W. Essex
Enhanced sampling algorithms are indispensable when working with highly disconnected multimodal distributions. An important application of these is the conformational exploration of particular internal degrees of freedom of molecular systems. However, despite the existence of many commonly used enhanced sampling algorithms to explore these internal motions, they often rely on system-dependent parameters
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Tunneling splittings using modified WKB method in Cartesian coordinates: The test case of vinyl radical J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-19 Mihael Eraković, Marko T. Cvitaš
Modified WKB theory for calculating tunneling splittings in symmetric multi-well systems in full dimensionality is re-derived using Cartesian coordinates. It is explicitly shown that the theory rests on the wavefunction that is exact for harmonic potentials. The theory was applied to calculate tunneling splittings in vinyl radical and some of its deuterated isotopologues in their vibrational ground
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JEDI: A versatile code for strain analysis of molecular and periodic systems under deformation J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-19 Henry Wang, Sanna Benter, Wilke Dononelli, Tim Neudecker
Stretching or compression can induce significant energetic, geometric, and spectroscopic changes in materials. To fully exploit these effects in the design of mechano- or piezo-chromic materials, self-healing polymers, and other mechanoresponsive devices, a detailed knowledge about the distribution of mechanical strain in the material is essential. Within the past decade, Judgement of Energy DIstribution
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PigmentHunter: A point-and-click application for automated chlorophyll-protein simulations J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-19 S. Ahad, C. Lin, M. Reppert
Chlorophyll proteins (CPs) are the workhorses of biological photosynthesis, working together to absorb solar energy, transfer it to chemically active reaction centers, and control the charge-separation process that drives its storage as chemical energy. Yet predicting CP optical and electronic properties remains a serious challenge, driven by the computational difficulty of treating large, electronically
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Ultrasound enhanced diffusion in hydrogels: An experimental and non-equilibrium molecular dynamics study J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-19 Sebastian E. N. Price, Caroline Einen, Othonas A. Moultos, Thijs J. H. Vlugt, Catharina de Lange Davies, Erika Eiser, Anders Lervik
Focused ultrasound has experimentally been found to enhance the diffusion of nanoparticles; our aim with this work is to study this effect closer using both experiments and non-equilibrium molecular dynamics. Measurements from single particle tracking of 40 nm polystyrene nanoparticles in an agarose hydrogel with and without focused ultrasound are presented and compared with a previous experimental
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Potential energy landscape of a flexible water model: Equation of state, configurational entropy, and Adam–Gibbs relationship J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-19 Ali Eltareb, Gustavo E. Lopez, Nicolas Giovambattista
The potential energy landscape (PEL) formalism is a tool within statistical mechanics that has been used in the past to calculate the equation of states (EOS) of classical rigid model liquids at low temperatures, where computer simulations may be challenging. In this work, we use classical molecular dynamics (MD) simulations and the PEL formalism to calculate the EOS of the flexible q-TIP4P/F water
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A personal perspective of the present status and future challenges facing thermal reaction rate theory J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-19 Eli Pollak
Reaction rate theory has been at the center of physical chemistry for well over one hundred years. The evolution of the theory is not only of historical interest. Reliable and accurate computation of reaction rates remains a challenge to this very day, especially in view of the development of quantum chemistry methods, which predict the relevant force fields. It is still not possible to compute the
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Theoretical and practical investigation of ion–ion association in electrolyte solutions J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-19 Saman Naseri Boroujeni, B. Maribo-Mogensen, X. Liang, G. M. Kontogeorgis
In this study, we present a new equation of state for electrolyte solutions, integrating the statistical associating fluid theory for variable range interactions utilizing the generic Mie form and binding Debye–Hückel theories. This equation of state underscores the pivotal role of ion–ion association in determining the properties of electrolyte solutions. We propose a unified framework that simultaneously
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Vibrational ADAPT-VQE: Critical points lead to problematic convergence J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-18 Marco Majland, Patrick Ettenhuber, Nikolaj Thomas Zinner, Ove Christiansen
Quantum chemistry is one of the most promising applications for which quantum computing is expected to have a significant impact. Despite considerable research in the field of electronic structure, calculating the vibrational properties of molecules on quantum computers remains a relatively unexplored field. In this work, we develop a vibrational Adaptive Derivative-Assembled Pseudo-Trotter Variational
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Cation doping and oxygen vacancies in the orthorhombic FeNbO4 material for solid oxide fuel cell applications: A density functional theory study J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-18 Xingyu Wang, David Santos-Carballal, Nora H. de Leeuw
The orthorhombic phase of FeNbO4, a promising anode material for solid oxide fuel cells (SOFCs), exhibits good catalytic activity toward hydrogen oxidation. However, the low electronic conductivity of the material specifically in the pure structure without defects or dopants limits its practical applications as an SOFC anode. In this study, we have employed density functional theory (DFT + U) calculations
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Revisiting fulgide photochromism: Mechanistic decoding and electron transport from computational exploration J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-18 Biman Medhi, Upasana Nath, Manabendra Sarma
The photochromic behavior of the fulgide molecule relies on ring-closure and ring-opening processes involving conical intersections during excited state transformation between isomers. The precise location and topography of these conical intersections significantly shape the decay process and fluorescence phenomena inherent to the molecule. This work combines electronic structure theory calculations
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Thermophysical properties of H2O and D2O ice Ih with contributions from proton disorder, quenching, relaxation, and extended defects: A model case for solids with quenching and relaxation J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-18 W. B. Holzapfel, S. Klotz
Application of the coherent thermodynamic model [W. Holzapfel and S. Klotz, J. Chem. Phys. 155, 024506 (2021)] for H2O ice Ih to the more detailed data for D2O ice Ih provides better insight into the contributions from quenched proton disorder and offers a new basis for understanding the apparent differences between the data for thermal expansion measured with neutron diffraction on polycrystalline
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Pattern dynamics of density and velocity fields in segregation of fluid mixtures J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-18 Prasenjit Das, Awadhesh Kumar Dubey, Sanjay Puri
We present comprehensive numerical results from a study of model H, which describes phase separation kinetics in binary fluid mixtures. We study the pattern dynamics of both density and velocity fields in d = 2, 3. The density length scales show three distinct regimes, in accordance with analytical arguments. The velocity length scale shows a diffusive behavior. We also study the scaling behavior of
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Silver-doped CdSe magic-sized nanocrystals J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-18 Andrew B. Pun, Alexandra J. Lyons, David J. Norris
Magic-sized nanocrystals (MSNCs) grow via jumps between very specific sizes. This discrete growth is a possible avenue toward monodisperse nanomaterials that are completely identical in size and shape. In spite of this potential, MSNCs have seen limited study and application due to their poor optical properties. Specifically, MSNCs are limited in their range of emission wavelengths and commonly exhibit
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Insights into hydrogen and methane storage capacities: Grand canonical Monte Carlo simulations of SIGSUA J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-18 A. Granja-DelRío, I. Cabria
In the pursuit of sustainable energy solutions, the development of materials with efficient hydrogen and methane storage capacities is imperative, particularly for advancing hydrogen-powered vehicles. Metal–organic frameworks (MOFs) have emerged as promising candidates to meet the stringent targets set by the Department of Energy for both hydrogen and methane storage. This study employs Grand Canonical
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h-BN in the making: The surface chemistry of borazine on Rh(111) J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-17 Eva Marie Freiberger, Fabian Düll, Phiona Bachmann, Johann Steinhauer, Federico J. Williams, Hans-Peter Steinrück, Christian Papp
Borazine is a well-established precursor molecule for the growth of hexagonal boron nitride (h-BN) via chemical vapor deposition on metal substrates. To understand the formation of the h-BN/Rh(111) moiré from borazine on a molecular level, we investigated the low-temperature adsorption and thermally induced on-surface reaction of borazine on Rh(111) in situ using synchrotron radiation-based high-resolution
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Self-assembly of chemical shakers J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-17 Liyan Qiao, Raymond Kapral
Chemical shakers are active particles with zero propulsion velocity whose activity derives from chemical reactions on portions of their surfaces. Although they do not move, except through Brownian motion, the nonequilibrium concentration and velocity fields that they generate endow them with properties that differ from their equilibrium counterparts. In particular, collections of such shakers can actively
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Thermodynamics of reversible hydrogen storage: Does alkoxy-substitution of naphthalene yield functional advantages for LOHC systems? J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-17 Sergey P. Verevkin, Artemiy A. Samarov, Sergey V. Vostrikov
The reversible hydrogenation/dehydrogenation of aromatic molecules, known as liquid organic hydrogen carriers (LOHCs), is considered an attractive option for the safe storage and release of elemental hydrogen. The LOHC systems based on the alkoxy-naphthalene/alkoxy-decalin studied in this work can become potentially attractive from the point of view of the thermodynamic conditions of the reversible
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Tin-oxo nanoclusters for extreme ultraviolet photoresists: Effects of ligands, counterions, and doping J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-17 Tingli Du, Xiaowei Yang, Yanyan Zhao, Pingping Han, Jijun Zhao, Si Zhou
The extreme ultraviolet (EUV) nanolithography technology is the keystone for developing the next-generation chips. As conventional chemically amplified resists are approaching the resolution limit, metal-containing photoresists, especially tin-oxo clusters, seize the opportunity to embrace this challenge owing to their small sizes, precise atomic structures, and strong EUV absorption. However, atomistic
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Kinetics of dissociative congruent evaporation based on the transition state theory J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-17 Shiori Inada, Tetsuya Hama, Shogo Tachibana
Non-transition metal oxides, including major minerals of the early Solar System, are known to evaporate decomposing into multiple gas molecules, while maintaining their stoichiometric compositions (dissociative congruent evaporation). Here, we derived the absolute rate of this type of evaporation using the transition state theory. In our modified transition state theory, the activation energy closely
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Microscopic dynamics of gas molecules confined in porous channel-like ice structure J. Chem. Phys. (IF 4.4) Pub Date : 2024-04-17 L. del Rosso, D. Colognesi, A. Donati, S. Rudić, M. Celli
In the rich ice polymorphism landscape, ice XVII, metastable at ambient pressure and at temperatures below 130 K, is surely one of the most interesting from both fundamental and technological perspectives due to its porosity, i.e., its capability to repeatedly absorb and desorb molecular hydrogen by dosing the gas at pressures even below the ambient one. Here, owing to this exceptional key feature