Article
Multidisciplinary Sciences
Enrico Ridente, Diptarka Hait, Eric A. Haugen, Andrew D. Ross, Daniel M. Neumark, Martin Head-Gordon, Stephen R. Leone
Summary: Understanding the relaxation pathways of photoexcited molecules is crucial for gaining atomistic-level insight into photochemistry. In this study, the geometric relaxation (Jahn-Teller distortion) of the methane cation was investigated using time-resolved attosecond transient absorption spectroscopy. The results revealed that the distortion occurred within a few femtoseconds after strong-field ionization of methane. Coherent oscillations in the vibrational mode of the symmetry-broken cation were activated and detected in the x-ray signal, but damped within a few tens of femtoseconds. This study provides a comprehensive understanding of the molecular relaxation dynamics and has implications for studying complex systems.
Article
Chemistry, Multidisciplinary
Shutaro Karashima, Alexander Humeniuk, Ryuta Uenishi, Takuya Horio, Manabu Kanno, Tetsuro Ohta, Junichi Nishitani, Roland Mitric, Toshinori Suzuki
Summary: The photoinduced ring-opening reaction of 1,3-cyclohexadiene to produce 1,3,5-hexatriene plays a crucial role in the photobiological synthesis of vitamin D-3, following the Woodward-Hoffmann rule and proceeding via nonadiabatic transitions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Benjamin A. Laws, Zachariah D. Levey, Timothy W. Schmidt, Stephen T. Gibson
Summary: In this study, a multifaceted approach was used to investigate the CH2CN- dipole-bound state, leading to precise numerical values and a complete model for further astronomical implications, showing good agreement with the diffuse interstellar band at wavelength 8040.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Pauf Neupane, David M. Bartels, Ward H. Thompson
Summary: Using the Kirkwood-Buff approach, the partial molar volume is found to provide valuable insights into the structure of the hydrated electron. It not only indicates the size of the cavity, but also provides information about the solvation structure. This information is important for developing and evaluating models of the hydrated electron.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Physical
Kenneth A. Jung, Joseph Kelly, Thomas E. Markland
Summary: Electron transfer at electrode interfaces to molecules in solution or at the electrode surface is essential for technological processes, and it necessitates a comprehensive and accurate understanding of the fermionic states of the electrode and their coupling to the molecule being oxidized or reduced in electrochemical processes. A physically transparent quasiclassical scheme is proposed to treat these electron transfer processes in the presence of molecular vibrations, effectively mapping the fermionic variables. This approach accurately captures the electron transfer dynamics even in weak coupling regimes, providing a scalable strategy for treating electron transfer from electrode interfaces in condensed-phase molecular systems.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Axel Gomez, Zeke A. Piskulich, Ward H. Thompson, Damien Laage
Summary: This study uses molecular dynamics simulations and analytical modeling to determine the molecular mechanism of water diffusion, establishing a quantitative relationship between the water diffusion coefficient and hydrogen-bond jump exchanges. It explains the different temperature dependences of dynamics and discusses the implications for water diffusion in supercooled conditions and water transport in complex aqueous systems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Axel Gomez, Zeke A. Piskulich, Ward H. Thompson, Damien Laage
Summary: This study investigates the molecular mechanism of water diffusion through molecular dynamics simulations and analytic modeling. The researchers establish a quantitative connection between the water diffusion coefficient and hydrogen-bond jump exchanges, and provide an explanation for the coupling between translational, rotational, and hydrogen-bond dynamics in liquid water.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Tao E. Li, Abraham Nitzan, Sharon Hammes-Schiffer, Joseph E. Subotnik
Summary: This study presents a quantum simulation of vibrational strong coupling in the collective regime using thermostated ring-polymer molecular dynamics. The simulation shows that including nuclear and photonic quantum effects does not change the Rabi splitting but broadens polaritonic line widths. Additionally, both quantum and classical simulations predict that the static dielectric constant of liquid water remains largely unchanged inside vs outside the cavity under thermal equilibrium. However, this disagrees with a recent experiment, suggesting potential limitations of the approach or unexplored experimental factors.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Graziano Amati, Maximilian A. C. Saller, Aaron Kelly, Jeremy O. Richardson
Summary: The formalism of the generalized quantum master equation (GQME) is an effective tool for improving the accuracy and efficiency of quasiclassical trajectory methods in nonadiabatic quantum dynamics. This paper investigates the approximate solution of GQME using two methods and tests them on spin-boson models. The accuracy of the predictions of GQME depends strongly on the specific technique used to calculate the memory kernels.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Biochemistry & Molecular Biology
Jose Angel Martinez-Gonzalez, Prithwish K. K. Nandi, Niall J. J. English, Aoife Gowen
Summary: Classical molecular-dynamics simulations were used to investigate the interaction between ubiquitin and its hydration-water sub-layers. The results showed that the first solvation sub-shell exhibited confined characteristics, while layers further from the surface demonstrated bulk-like spectral behavior within a range of 6-7 angstrom.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Chemistry, Multidisciplinary
Arup Kumar Pathak, Alok Kumar Samanta
Summary: The ab initio electronic structure method using second-order Moller-Plesset (MP2) perturbation theory with correlated consistent basis functions was employed to study the structures, energetics, and photoelectron spectral properties of F(CO2)(n)(-) species. Strong F-CO2 bonding is observed in systems with up to four solvated CO2 molecules, with a sudden decrease in interaction energy when n surpasses 4 due to the lack of such bonding. The nucleophilicity of the F- ion is expected to decrease in the presence of CO2 in H2O. Additionally, excellent agreement between theory and experiment is observed for vertical detachment energy and solvation energy values in the studied species.
NEW JOURNAL OF CHEMISTRY
(2021)
Article
Chemistry, Physical
Xiang Huang, Weiwei Xie, Nada Doslic, Maxim F. Gelin, Wolfgang Domcke
Summary: The passage discusses the technique of 2D electronic spectroscopy and its application in simulating molecular photodynamics. By using ab initio theoretical framework and classical trajectory simulations, researchers can gain detailed insights into the ultrafast photodynamics of molecules.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Materials Science, Multidisciplinary
Laurent Van Brutzel, Paul Fossati, Alain Chartier
Summary: This article presents molecular dynamics simulations of the microstructural evolution of (U,Pu)O-2 solid solutions under irradiation, and discusses the description of X-ray diffraction patterns for well characterized damage microstructure snapshots. The attempt to correlate the X-ray diffraction peak features with the microstructural evolution at different irradiation doses is emphasized, with particular attention to the swelling effect.
JOURNAL OF NUCLEAR MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Euihyun Lee, Carlos R. Baiz
Summary: This study characterizes the interactions between DMSO and water, showing that DMSO disrupts the hydrogen bond networks and this disruption increases with decreasing temperature.
Article
Engineering, Chemical
Guoqiang Song, Wenjun Zhou, Claudia Li, Zhigang Wang, Feiyang Hu, Tianchang Wang, Ziwei Li, Anjiang Tang, Michael P. Harold, Shaomin Liu, Sibudjing Kawi
Summary: In this study, a water-conducting LTA membrane with well-distributed non-penetrative macroholes was prepared, resulting in a cheese-like structure that combines the advantages of micro-nanochannels for high water selective permeability and macroholes for quick water diffusion. The optimized SH-LTA membranes showed high water permeability and good stability, with permeances of methanol, H2, and CO2. The dissolution-recrystallization route of the SH morphology was confirmed, and molecular dynamics simulations were used to elucidate the superior water separation behavior in the SH-LTA membrane compared to the pristine LTA membrane.
JOURNAL OF MEMBRANE SCIENCE
(2023)