Article
Chemistry, Physical
Lucien Dupuy, Francesco Talotta, Federica Agostini, David Lauvergnat, Bill Poirier, Yohann Scribano
Summary: In this study, a quantum dynamics method based on the propagation of interacting quantum trajectories is presented to describe both adiabatic and nonadiabatic processes. The method determines the quantum force using only information about quantum trajectories, resulting in stable dynamics. Its performance is discussed by applying the method to analytical potentials in the adiabatic regime, and by combining it with the exact factorization method in the nonadiabatic regime.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Huajing Song, Yeonsig Nam, Daniel Keefer, Marco Garavelli, Shaul Mukamel, Sergei Tretiak
Summary: In this study, nonadiabatic and adiabatic molecular dynamics simulations were used to investigate the transition-state dynamics of photoexcited cyclooctatetraene (COT). The simulations revealed an active excited to ground state relaxation pathway and a double-bond shifting mechanism, with results in good agreement with experimental data. These findings provide valuable insights into the photochemistry of COT and lay a foundation for further research on bond-order inversion and photoswitching processes.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Multidisciplinary
Pedro Recio, Silvia Alessandrini, Gianmarco Vanuzzo, Giacomo Pannacci, Alberto Baggioli, Demian Marchione, Adriana Caracciolo, Vanessa J. Murray, Piergiorgio Casavecchia, Nadia Balucani, Carlo Cavallotti, Cristina Puzzarini, Vincenzo Barone
Summary: This study reveals that intersystem crossing between the pre-reactive complex and the reaction barrier can control the rate of bimolecular reactions for weakly coupled potential energy surfaces, even in the absence of heavy atoms. By conducting crossed-beam experiments and computational simulations, it is found that for the O(P-3) plus pyridine reaction, the main products are pyrrole and CO, obtained through a spin-forbidden ring-contraction mechanism. The reaction rates at low to moderate temperatures are mainly dominated by intersystem crossing.
Article
Multidisciplinary Sciences
Guang Yuan Zhu, Yi Qin, Miao Meng, Suman Mallick, Hang Gao, Xiaoli Chen, Tao Cheng, Ying Ning Tan, Xuan Xiao, Mei Juan Han, Mei Fang Sun, Chun Y. Liu
Summary: The Landau-Zener formula, a semiclassical model for nonadiabatic transitions, is shown to be valid in a broader range of conditions approaching the adiabatic regime than previously expected, as demonstrated by investigating electron transfer reactions in a series of mixed-valence complexes.
NATURE COMMUNICATIONS
(2021)
Article
Materials Science, Multidisciplinary
Junji Fujimoto
Summary: The study constructs a microscopic theory of spin-transfer torques on slowly varying staggered magnetization in antiferromagnets with weak canting, revealing the relationship between nonadiabatic and adiabatic spin-transfer torques. The findings suggest that the conventional explanation for spin-transfer torques in antiferromagnets may need to be revised.
Article
Biochemistry & Molecular Biology
Shuwen Zhang, Qixin Chen, Junxiang Zuo, Xixi Hu, Daiqian Xie
Summary: The O(P-3) + C2H2 reaction plays a vital role in hydrocarbon combustion, with two competing channels: H + HCCO and CO + CH2. A quasi-classical trajectory study was conducted on a full-dimensional potential energy surface to understand the microscopic dynamic mechanism of this reaction. The study revealed that the entrance barrier TS1 is rate-limiting, and translational motion of the reactants significantly enhances reactivity. Additionally, the reaction proceeds through a complex-forming mechanism, where the intermediate HCCHO exhibits high vibrational and rotational excitation for an extended period.
Article
Thermodynamics
N. Hansen, B. Yang, M. Braun-Unkhoff, A. Ramirez, G. Kukkadapu
Summary: In this study, the molecular-growth pathways in propyne-doped low-pressure premixed flames of benzene and toluene were investigated through a combined experimental and modeling approach. The chemical structures of the flames were determined using flame-sampling molecular-beam mass spectrometry. Reaction path analyses revealed the important pathways for the formation of indene, naphthalene, and phenanthrene. The molecular growth was found to be driven by radical-radical recombination reactions, as well as ring-closure and ring-enlargement reactions, with little contribution from the classical HACA (hydrogen abstraction-acetylene addition) mechanism.
COMBUSTION AND FLAME
(2022)
Article
Chemistry, Physical
Moritz Heindl, Leticia Gonzalez
Summary: Laser control of chemical reactions is a challenging field of research, especially when it comes to the theoretical description of coupled electronic and nuclear motion in the presence of laser fields. This study demonstrates how the excited state dynamics of [Ru((S-S)bpy)(bpy)(2)](2+) can be controlled using explicit laser fields. Simple laser fields that can slow down or completely stop S-S bond dissociation are defined based on the transient properties along the excited state dynamics leading to the population of the T-1 minimum energy structure.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Krupa Ramasesha, John D. Savee, Judit Zador, David L. Osborn
Summary: The study investigated the reaction of O(P-3) with cyclo-pentene using time-resolved multiplexed photoionization mass spectrometry, revealing that at least 60% of the products are formed by triplet reactivity. The results suggest that the reactivity of cyclic alkenes with O(P-3) is influenced by their greater degree of unsaturation, and that searches for minimum-energy crossing points connecting triplet surfaces to singlet surfaces should extend beyond initial adducts.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Physics, Fluids & Plasmas
Qizhen Hong, Massimiliano Bartolomei, Fernando Pirani, Fabrizio Esposito, Quanhua Sun, Cecilia Coletti
Summary: The accurate modelling of vibrational quenching events in air plasmas is crucial for the design of aircrafts and simulation of atmospheric conditions. The study also highlights the significance of new computational approaches in understanding non-adiabatic vibro-electronic deactivation processes.
PLASMA SOURCES SCIENCE & TECHNOLOGY
(2022)
Article
Biochemistry & Molecular Biology
Yunju Zhang, Yongguo Liu, Meilian Zhao, Huaming Du, Yuxi Sun, Huirong Li, Zhiguo Wang
Summary: The study investigated the O(P-3)-initiated conversion mechanism of CH3CHCO in the atmosphere using DFT computations, revealing that O(P-3) association is more energetically favorable than H abstraction. The rate coefficients were predicted using RRKM theory, showing that the rate coefficient of ketene derivatives increases with methylation degree.
JOURNAL OF MOLECULAR MODELING
(2021)
Article
Chemistry, Multidisciplinary
Ran Liu, Wenfeng Shen
Summary: The kinetic characteristics of the oxidation of SO2 to SO3 were studied using the non-adiabatic transition state theory coupled with the master equation method. The results were compared with experimental data, showing good consistency. This study demonstrates the potential application of the NA-TST/ME method in investigating similar spin-forbidden reactions.
Review
Physics, Multidisciplinary
Oleh V. Ivakhnenko, Sergey N. Shevchenko, Franco Nori
Summary: This article systematically studies various aspects of LZSM physics and reviews the relevant literature, significantly expanding on the previous review article. The interfernce between transitions in LZSM has recently become accessible, controllable, and useful for manipulating a growing number of quantum systems.
PHYSICS REPORTS-REVIEW SECTION OF PHYSICS LETTERS
(2023)
Article
Chemistry, Physical
C. Cavallotti, A. Della Libera, C-W Zhou, P. Recio, A. Caracciolo, N. Balucani, P. Casavecchia
Summary: This study reveals the product channels and branching fractions of the reaction between atomic oxygen and 1,3-butadiene through experiments and theoretical simulations, providing important data for the kinetic modeling of 1,3-butadiene oxidation.
FARADAY DISCUSSIONS
(2022)
Article
Chemistry, Physical
Alexander N. Morozov, Iakov A. Medvedkov, Valeriy N. Azyazov, Alexander M. Mebel
Summary: Quantum chemical calculations were used to study the mechanisms of phenoxy + O(P-3) and phenyl + O-2 reactions. Multi-reference calculations were utilized to map out the minimum energy path for the entrance channels, exploring stationary points on the PES, and assessing temperature and pressure-dependent phenomenological rate constants and product branching ratios. Collisional stabilization of peroxybenzene at low temperatures and high pressures competes with the bimolecular product channels in both reactions.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Multidisciplinary
Haihui Peng, Jialong Jie, Ifor P. Mortimer, Zehan Ma, Hongmei Su, Marc M. Greenberg
Summary: Oxidative stress generates various radicals in DNA, including the 2'-deoxycytidin-N4-yl radical (dC center dot), which oxidizes the opposing dG in DNA damage. In appropriate sequences, dC center dot leads to deleterious tandem lesions and hole transfer.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Yu Tian, Aiji Wang, Yaqing Wei, Minghui Pei, Rongrong Cao, Zhenao Gu, Qi Yuan, Yiwen Hu, Jing Wang, Kunhui Liu, Dashan Shang, Jiebin Niu, Xiaoqiang An, Run Long, Jinxing Zhang
Summary: This study demonstrates a controllable water splitting reaction by constructing a hydroxyls-bonded surface on a ferroelectric material. The up-shift of band edge positions at this surface enhances the transfer of holes and electrons, leading to enhanced oxygen or hydrogen evolutions, respectively. Additionally, the introduction of ferroelectric super-domains with electric fields improves the separation of photogenerated carriers, resulting in a significant increase in photocurrent.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Cetao Hu, Sixuan Zhang, Mingliang Wu, Xingyu Chen, Jingwen Xu, Hao Shen, Huan Wang, Di Wu, Jianlong Xia
Summary: This study presents the design and synthesis of a propeller-shaped PDI hexamer T-DPDI, which exhibits superior photovoltaic performance in organic solar cells due to its stronger absorption and more favorable morphology, achieved by hybridizing the direct and indirect linkage manners of PDI units.
CHEMISTRY-AN ASIAN JOURNAL
(2021)
Article
Chemistry, Physical
Junjie Dong, Chunhua Huang, Shaoshi Guo, Ye Xia, Yue Hou, Chunfan Yang, Xianwang Zhang, Jialong Jie, Ben-Zhan Zhu, Hongmei Su
Summary: By real-time observation of radical intermediates and product analysis, it is revealed that UVA excitation of 6-TG triggers direct covalent cross-linking with tryptophan, establishing a mechanistic framework for understanding mutagenic DPCs formation.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Kangwei Wang, Guangwei Shao, Shaoqian Peng, Xiaoxiao You, Xingyu Chen, Jingwen Xu, Huaxi Huang, Huan Wang, Di Wu, Jianlong Xia
Summary: By mediating interchromophore coupling, symmetry-breaking charge separation can be achieved in a nonpolar solvent through the combination of bridge resonance and N-functionalization. Observation of the CT band confirms the enhanced electronic coupling. Transient absorption spectroscopy demonstrates the feasibility of photoinduced SB-CS in a nonpolar solvent.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Min Tao, Yang Li, Quan Huang, Hongmei Zhao, Jingbo Lan, Yan Wan, Zhuoran Kuang, Andong Xia
Summary: This study demonstrates the feasibility of continuously modulating ESIPT dynamics in HPO derivatives by investigating electron population variations on proton donor and acceptor. An index Δpdif was proposed to evaluate the overall promotion effect on proton transfer, showing high reliability in interpreting the ESIPT tendency. This method has great potential in ESIPT molecular design with chemical substitution of electron-donating/withdrawing moieties.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Organic
Jie Wen, Lei Feng, Hongmei Zhao, Li Zheng, Pericles Stavropoulos, Lin Ai, Jiaxin Zhang
Summary: This study successfully established an unconventional enantiomeric discrimination method for hydantoin derivatives, representatives of five-membered N,N-heterocycles, and observed non-equivalent chemical shifts through H-1 NMR spectroscopy. Additionally, theoretical calculations were performed to understand the intermolecular interactions between chiral solvating agents and enantiomers.
JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Zheng Hu, Qian Zhou, Zeqing Jiao, Peixuan Qin, Fei Wang, Ye Xia, Tianfeng Zhang, Jialong Jie, Hongmei Su
Summary: This study demonstrates that phosphorothioate modified oligonucleotides undergo photoionization upon UV excitation, leading to the formation of hemi-bonded radicals. The presence of phosphorothioate moiety protects the remaining bases from ionization damage.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Zeqing Jiao, Chunfan Yang, Qian Zhou, Zheng Hu, Jialong Jie, Xianwang Zhang, Hongmei Su
Summary: Triplex DNA structure has potential therapeutic application in inhibiting the expression of genes involved in cancer and other diseases. Coralyne, a DNA-targeting antitumor and antibiotic drug, shows remarkable binding propensity to triplex over canonical duplex, providing a prospective gene targeting strategy. By combining multiple spectroscopy techniques, the binding behaviors of coralyne with typical triplexes have been investigated, revealing the preferences and contributions of different binding modes. The strong pi-pi stacking of intercalated coralyne monomer with base-triplets plays an important role in stabilizing the triplex structure, offering mechanistic insights for the selective binding of coralyne to triplex DNA.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Qian Zhou, Tianfeng Zhang, Jialong Jie, Yue Hou, Zheng Hu, Zeqing Jiao, Hongmei Su
Summary: TiO2 has been found to exhibit photocatalytic properties similar to natural enzymes, showing its potential as a nanozyme to mimic photolyase in repairing DNA damage.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Shaoqian Peng, Guangwei Shao, Kangwei Wang, Xingyu Chen, Jingwen Xu, Huan Wang, Di Wu, Jianlong Xia
Summary: Investigated two antenna molecules with simplified structures to avoid complex exciton dynamics caused by conformational mobility. TP and TBP heterodimers with a PDI donor and TDI acting as an energy sink were studied. TP showed strong chromophore coupling, while TBP exhibited weak chromophore coupling. TP underwent ultrafast vibrational relaxation and electron transfer, while TBP demonstrated ultrafast excitation energy transfer with quenched charge transfer. This finding provides insight for designing novel small molecules capable of efficient energy transfer.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Biochemistry & Molecular Biology
Qian Zhou, Wenwen Guo, Zheng Hu, Shuyi Yan, Jialong Jie, Hongmei Su
Summary: Methylation significantly enhances the photoionization of DNA bases, with methylated purines exhibiting higher ionization yields and potentially acting as hotspots for DNA photoionization damage in living organisms.
PHOTOCHEMISTRY AND PHOTOBIOLOGY
(2023)
Article
Chemistry, Physical
Chunfan Yang, Fang Wang, Qian Zhou, Jialong Jie, Hongmei Su
Summary: This study investigates the fluorescence quenching dynamics of AMND in AP-containing DNA single/double strands and reveals that AMND only targets cytosine to form a pseudo-base pair. Subtle conformational variations induced by different flanking nucleobases are found to modulate efficiencies of electron transfer and fluorescence quenching, providing critical mechanistic insights for the design of fluorescent ligands for single-base recognition.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Wenshan Xiao, Mingwei Wu, Huan Wang, Qiu He, Yan Zhao
Summary: This article proposes a method for obtaining ideal artificial solid-electrolyte interface (SEI) materials for lithium metal anodes (LMAs) through chemical stability assessments, electronic conductivity measurements, and accurate predictions of key parameters. The method was demonstrated by finding optimal SEI materials from 76 binary selenides for LMAs.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Wei Yang, Chen Wang, Kunhui Liu, Chao Liu, Jianzhuang Jiang
Summary: A pair of chiral metallic porphyrin cages have been synthesized and their structure and photophysical properties have been studied. These cages exhibit superior photosensitive performance compared to the monomeric compound in solution.
NEW JOURNAL OF CHEMISTRY
(2022)