Article
Chemistry, Analytical
Pei-Ling Luo, I-Yun Chen
Summary: In this study, a spectrometer based on synchronized two-color time-resolved dual-comb spectroscopy was developed for simultaneous spectral acquisitions in two molecular fingerprint regions. By using high-resolution rovibrational absorption spectroscopy, the concentration of target molecules can be quantitatively detected and simulated, enabling exploration of reaction mechanisms and pathways related to the formation of HOx radicals.
ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Physical
Ernest Antwi, Rachel E. Bush, Barbara Marchetti, Tolga N. V. Karsili
Summary: Criegee intermediates, highly reactive molecules with vital roles in various fields, were studied using state-of-the-art techniques. The study revealed the impact of long-range internal conversion on the products of photoinduced fragmentation.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Lauri Franzon, Jari Peltola, Rashid Valiev, Niko Vuorio, Theo Kurten, Arkke Eskola
Summary: Direct kinetic measurements were performed on the reactions of CH2OO + RCN (R = H, CH3, C2H5) in the temperature and pressure ranges of 233-360 K and 10-250 Torr, respectively, using time-resolved UV-absorption spectroscopy. Chloroiodomethane (CH2ICl) was used as a photolytic precursor to produce CH2OO through its photolysis in the presence of O2 at 193 nm. The observed bimolecular rate coefficients for the reactions of CH2OO with HCN, CH3CN, and C2H5CN at 296 K were determined to be (2.22 +/- 0.65) x 10-14 cm3 molecule-1 s-1, (1.02 +/- 0.10) x 10-14 cm3 molecule-1 s-1, and (2.55 +/- 0.13) x 10-14 cm3 molecule-1 s-1, respectively, indicating that the reaction with CH2OO can be a significant degradation pathway for nitriles in the atmosphere. Both the temperature and pressure dependencies of all the reactions were found to be negligible in the studied conditions. Quantum chemical calculations and master equation modeling results suggested that the lowest-energy reaction path of CH2OO + RCN led to the formation of a 1,2,4-dioxazole compound through ring closure. Subsequent decomposition of 1,2,4-dioxazole could generate important atmospheric end products such as CH2O + RNCO and CO + RC(NH)OH.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Xiaohu Zhou, Yang Chen, Yiqiang Liu, Xinyong Li, Wenrui Dong, Xueming Yang
Summary: The kinetics of reactions between CH2OO and syn-CH3CHOO with acrolein in the atmosphere were studied, showing negative temperature-dependence with activation energies derived from the Arrhenius equation. The rate coefficients for these reactions were measured at different temperatures and pressures, with no significant pressure dependence observed.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Biochemistry & Molecular Biology
Ernest Antwi, Niamh A. A. Packer, Jordyn M. M. Ratliff, Barbara Marchetti, Tolga N. V. Karsili
Summary: This passage discusses the formation of Criegee intermediates (CIs) from isoprene ozonolysis and how the increasing molecular complexity affects their photodynamics. The excited state chemistry of CH2OO, MVK-oxide, and MACR-oxide is compared to understand the different product channels and quantum yields, providing insights into the atmospheric implications.
PHOTOCHEMISTRY AND PHOTOBIOLOGY
(2022)
Article
Chemistry, Physical
Vincent J. Esposito, Tianlin Liu, Guanghan Wang, Adriana Caracciolo, Michael F. Vansco, Barbara Marchetti, Tolga N. Karsili, Marsha Lester
Summary: UV excitation of the CH2OO Criegee intermediate leads to prompt dissociation into two energetically accessible asymptotes: O (D-1) + H2CO (X(-1)A(1)) and O (P-3) + H2CO (a(-3)A ''). Velocity map imaging studies show a bimodal total kinetic energy release (TKER) distribution for the O (D-1) + H2CO (X(-1)A(1)) products, with two different dynamical pathways contributing to the observed distribution. The study provides insight into the photodissociation of CH2OO via multiple dissociation pathways through two regions of conical intersection (CoIn).
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Multidisciplinary
Pei-Ling Luo, I-Yun Chen, M. Anwar H. Khan, Dudley E. Shallcross
Summary: The authors investigated the reaction mechanisms between the primary products of isoprene ozonolysis, formaldehyde oxide and formaldehyde, and evaluated their atmospheric implications using a global chemistry-transport model. The reaction kinetics and product yields were studied using time-resolved infrared laser spectrometry. The results showed temperature dependence of the reaction rate and provided insights into the formation of formic acid (HCOOH).
COMMUNICATIONS CHEMISTRY
(2023)
Article
Chemistry, Physical
Torsha Moitra, Sonia Coriani, Bruno Nunes Cabral Tenorio
Summary: The study adapted the asymmetric-Lanczos-based equation-of-motion coupled cluster formalism to calculate photoabsorption and photoionisation spectral signatures from inner-shell electrons of valence excited states. Two different methodologies were used to generate total cross-section profiles for the first two electronically excited states of water, ammonia, ethylene, and uracil, showing remarkable differences in core-ionisation cross-section results between the two quadrature approaches.
Article
Physics, Multidisciplinary
N. Jourdain, L. Lecherbourg, V Recoules, P. Renaudin, F. Dorchies
Summary: The ultrafast dynamics of the loss of crystalline periodicity in femtosecond laser heated warm dense copper was studied using x-ray absorption near-edge structures above the L3 edge. A characteristic time of approximately 1 ps was observed for energy densities ranging from 1 to 5 MJ/kg, with the experimental data well reproduced by two-temperature hydrodynamic simulations, indicating a thermal phase transition.
PHYSICAL REVIEW LETTERS
(2021)
Article
Mechanics
M. A. S. Al-Malki, S. J. Garrett, S. Camarri, Z. Hussain
Summary: This study investigates the effects of surface roughness on the convective stability behavior of boundary-layer flow over a rotating disk. Both anisotropic and isotropic surface roughness have different impacts on the instability properties of the flow. It was found that radial grooves have a destabilizing effect on type II mode, while concentric grooves and isotropic surface roughness stabilize the type I mode.
Article
Optics
Peter Bernath, Anton M. Fernando
Summary: Spectra of pure isobutane were recorded at high temperature, and the absorption cross sections were determined for six temperatures. These data may be useful for simulations of hot Jupiter exoplanets and brown dwarfs, and were compared with adjusted cross section data from the PNNL database.
JOURNAL OF QUANTITATIVE SPECTROSCOPY & RADIATIVE TRANSFER
(2021)
Article
Mechanics
M. A. S. Al-Malki, M. Fildes, Z. Hussain
Summary: This study investigates the effects of different types of surface roughness on stationary and non-stationary disturbances in boundary-layer flow. The results show that increasing concentric grooves and isotropic roughness stabilize the flow, while streamwise grooves have a destabilizing effect. Decreasing the cone half-angle enhances the stabilizing effect of isotropic roughness. For non-stationary modes, concentric grooves and isotropic roughness have a stronger stabilization effect on the flow, while streamwise grooves have a weaker effect. Increasing concentric grooves and isotropic roughness increases the frequency of the most dangerous modes, while streamwise grooves reduce this frequency.
Article
Chemistry, Multidisciplinary
Francesca Peverini, Marco Bizzarri, Maurizio Boscardin, Lucio Calcagnile, Mirco Caprai, Anna Paola Caricato, Giuseppe Antonio Pablo Cirrone, Michele Crivellari, Giacomo Cuttone, Sylvain Dunand, Livio Fano, Benedetta Gianfelici, Omar Hammad, Maria Ionica, Keida Kanxheri, Matthew Large, Giuseppe Maruccio, Mauro Menichelli, Anna Grazia Monteduro, Francesco Moscatelli, Arianna Morozzi, Stefania Pallotta, Andrea Papi, Daniele Passeri, Marco Petasecca, Giada Petringa, Igor Pis, Gianluca Quarta, Silvia Rizzato, Alessandro Rossi, Giulia Rossi, Andrea Scorzoni, Cristian Soncini, Leonello Servoli, Silvia Tacchi, Cinzia Talamonti, Giovanni Verzellesi, Nicolas Wyrsch, Nicola Zema, Maddalena Pedio
Summary: This study investigates, for the first time, the damaging and recovering mechanisms of p-i-n detector devices based on hydrogenated amorphous silicon induced by a neutron source using high-resolution photoemission, soft X-ray absorption, and atomic force microscopy. Comparison of spectroscopic results on bare and irradiated samples reveals increased disorder and reduced Si-H bonds after irradiation, with partial recovery of the Si-H bonds observed after annealing.
Article
Multidisciplinary Sciences
Ihor Cherniukh, Gabriele Raino, Thilo Stoeferle, Max Burian, Alex Travesset, Denys Naumenko, Heinz Amenitsch, Rolf Erni, Rainer F. Mahrt, Maryna I. Bodnarchuk, Maksym V. Kovalenko
Summary: Through precise structural engineering, perovskite nanocrystals are co-assembled with other nanocrystal materials to form a range of binary and ternary perovskite-type superlattices that exhibit superfluorescence. These ABO3 superlattices, as well as the binary NaCl and AlB2 superlattice structures that we demonstrate, exhibit a high degree of orientational ordering of the CsPbBr3 nanocubes. They also exhibit superfluorescence – a collective emission that results in a burst of photons with ultrafast radiative decay (22 picoseconds) that could be tailored for use in ultrabright (quantum) light sources.
Article
Physics, Multidisciplinary
Shao-Hong Zhang, Zhe Zhou, Tian-Yang Fu, Yi-Yuan Xu, Jie-Yun Yan
Summary: This study investigates the optical absorption of semiconductor nanowires with hexagonal cross-sections, finding that the approximation of the hexagonal cross-section as a circular one depends on the energy levels considered. Only subbands corresponding to energy levels with hexagonal symmetry in the cross sections can be optically excited. These findings are important for the optical applications of nanowires based on their fine energy structures.
Article
Chemistry, Multidisciplinary
Elizabeth S. Foreman, Kara M. Kapnas, Craig Murray
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2016)
Article
Chemistry, Physical
Sara V. Tadayon, Elizabeth S. Foreman, Craig Murray
JOURNAL OF PHYSICAL CHEMISTRY A
(2018)
Article
Chemistry, Physical
Kara M. Kapnas, Benjamin W. Toulson, Elizabeth S. Foreman, Sarah A. Block, J. Grant Hill, Craig Murray
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2017)
Article
Chemistry, Physical
Benjamin W. Toulson, Kara M. Kapnas, Dmitry A. Fishman, Craig Murray
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2017)
Article
Chemistry, Physical
Benjamin W. Toulson, Dmitry A. Fishman, Craig Murray
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2018)
Article
Chemistry, Multidisciplinary
Wesley J. Transue, Matthew Nava, Maxwell W. Terban, Jing Yang, Matthew W. Greenberg, Gang Wu, Elizabeth S. Foreman, Chantal L. Mustoe, Pierre Kennepohl, Jonathan S. Owen, Simon J. L. Billinge, Heather J. Kulik, Christopher C. Cummins
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2019)
Article
Chemistry, Physical
Kara M. Kapnas, Craig Murray
JOURNAL OF CHEMICAL PHYSICS
(2020)
Article
Chemistry, Physical
Zachary A. Cornwell, Aaron W. Harrison, Craig Murray
Summary: The rate constants for the reactions between CH2OO and acetone, alpha-diketones, and beta-diketones were measured, showing faster reaction rates for alpha-diketones compared to beta-diketones with CH2OO. The results are consistent with previous measurements and provide insight into the reactivity of carbonyl compounds with Criegee intermediates.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Physical
Zachary A. Cornwell, Jonas J. Enders, Aaron W. Harrison, Craig Murray
Summary: Temperature-dependent rate constants for the reactions of CH2OO with acetone (Ac), biacetyl (BiAc), and acetylacetone (AcAc) have been measured. The reaction rates increase with decreasing temperature and follow linear Arrhenius plots. The calculations show that the reactions proceed via formation of an entrance channel complex followed by 1,3-dipolar cycloaddition. For the BiAc reaction, the rate limiting step appears to be rearrangement of a long-range van der Waals complex into the short-range complex that subsequently leads directly to the cycloaddition transition state with a very low energy barrier. The weak temperature dependence observed for AcAc is likely due to competition between two reaction pathways.
INTERNATIONAL JOURNAL OF CHEMICAL KINETICS
(2023)
Article
Chemistry, Physical
Kara M. Kapnas, Laura M. McCaslin, Craig Murray
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2019)
Article
Chemistry, Physical
Sergey Yu. Ketkov, Sheng-Yuan Tzeng, Elena A. Rychagova, Anton N. Lukoyanov, Wen-Bih Tzeng
Summary: Metallocenes, including methylcobaltocene, play important roles in various fields of chemistry. The ionization energy and vibrational structure of (Cp ')(Cp)Co can be influenced by introducing methyl substituents. The mass-analyzed threshold ionization spectrum and DFT calculations provide accurate information about the properties and transformations of (Cp ')(Cp)Co.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Review
Chemistry, Physical
Qifeng Mu, Jian Hu
Summary: Polymer mechanochemistry has experienced a renaissance due to the rapid development of mechanophores and principles governing mechanochemical transduction or material strengthening. It has not only provided fundamental guidelines for converting mechanical energy into chemical output, but also found applications in engineering and smart devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Da Hye Yang, Francesco Ricci, Fredrik L. Nordstrom, Na Li
Summary: Through systematic evaluation of the oiling-out behavior of procaine, we identified both stable and metastable liquid-liquid phase separation, and established phase diagrams to assist in rational selection of crystallization strategies.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Vikki Anand Varma, Simmie Jaglan, Mohd Yasir Khan, Sujin B. Babu
Summary: Designing engineering structures like nanocages, shells, and containers through self-assembly of colloids is a challenging problem. This work proposes a simple model for the subunit, which leads to the formation of monodispersed spherical cages or containers. The model with only one control parameter can be used to design cages with the desired radius.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Hainan Jiang, Yaolong He, Xiaolin Li, Zhiyao Jin, Huijie Yu, Dawei Li
Summary: The cycling lifespan and coulombic efficiency of lithium-ion batteries are crucial for high C-rate applications. The Li-ion concentration plays a crucial role in determining the mechanical integrity and structural stability of electrodes. This study focuses on graphite as the working electrode and establishes an experimental system to investigate the mechanical properties of composite graphite electrode at different C-rates. Considering the effect of Li-ion concentration in stress analysis is found to be significant.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Zhiye Wang, Yunchuan Li, Mingjun Sun
Summary: This study investigates the influence of intramolecular pi-pi interactions on the electronic transport capabilities of molecules. By designing and analyzing three pi-conjugated molecules, the researchers observe that different pi-conjugated structures have varying effects on electron transport. The findings provide a theoretical foundation for designing single-molecule electronic devices with multiple electron channels based on intramolecular pi-pi interactions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Yuandong Xu, Haoyang Feng, Chaoyang Dong, Yuqing Yang, Meng Zhou, Yajun Wei, Hui Guo, Yaqing Wei, Jishan Su, Yingying Ben, Xia Zhang
Summary: Hollow MoS2 cubes and spheres were successfully synthesized using a one-step hydrothermal method with the hard template method. The hollow MoS2 cubes exhibited higher specific capacitance and energy density compared to the hollow MoS2 spheres. The symmetrical supercapacitors assembled with these hollow structures showed good performance and high capacity retention after multiple cycles. These findings suggest that controlling the pore structure and surface characteristics of MoS2 is crucial for enhancing its electrochemical properties.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Ainhoa Oliden-Sanchez, Rebeca Sola-Llano, Joaquin Perez-Pariente, Luis Gomez-Hortiguela, Virginia Martinez-Martinez
Summary: The combination of photoactive molecules and inorganic structures is important for the development of advanced materials in optics. In this study, bulky dyes were successfully encapsulated in a zeolitic framework, resulting in emission throughout the visible spectrum.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Miaomiao Zhang, Cunyuan Pei, Qiqi Xiang, Lintao Liu, Zhongxu Dai, Huijuan Ma, Shibing Ni
Summary: The design of a solid electrolyte interphase (SEI) plays a crucial role in improving the electrochemical performance of anode materials. In this study, lithium difluoro(oxalate)borate (LiDFOB) is used as an electrolyte additive to form a protective SEI film on Li3VO4 (LVO) anodes. The addition of LiDFOB results in a dense, uniform, stable, and LiF-richer SEI, which enhances the Li-ion storage kinetics. The generated SEI also prevents further decomposition of the electrolyte and maintains the morphology of LVO anodes during charge/discharge processes. This work demonstrates the effectiveness of LiDFOB as a multi-functional additive for LiPF6 electrolytes and provides insights into SEI construction for high-performance LVO anodes.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
B. V. Andryushechkin, T. V. Pavlova, V. M. Shevlyuga
Summary: The atomic structure of the Ag(111)-p(4 x 4)-O phase was reexamined and two phases with the same periodicity were discovered. It was demonstrated that the accepted Ag6 model is incompatible with high-resolution oxygen-sensitive STM images.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
S. L. Romo-Avila, D. Marquez-Ruiz, R. A. Guirado-Lopez
Summary: In this study, we used density functional theory (DFT) calculations to investigate the interaction between model graphene oxide (GO) nanostructures and chlorine monoxide ClO. We aimed to understand the role of this highly oxidizing species in breaking C-C bonds and forming significant holes on GO sheets. Our results showed that C-C bonds in a single graphene oxide sheet can be broken through a simple mechanism involving the dissociation of two chemically attached ClO molecules. The formation of carbonyl groups and holes on the GO surface was also observed. This study provides important insights into the degradation of carbon nanotubes and the stability of GO during the myeloperoxidase (MPO) catalytic cycle.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Alberto Garcia-Fernandez, Birgit Kammlander, Stefania Riva, Hakan Rensmo, Ute B. Cappel
Summary: In this study, the X-ray stability of five different lead halide perovskite compositions (MAPbI3, MAPbCl3, MAPbBr3, FAPbBr3, CsPbBr3) was investigated using photoelectron spectroscopy. Different degradation mechanisms and resistance to X-ray were observed depending on the crystal composition. Overall, perovskite compositions based on the MA+ cation were found to be less stable than those based on FA+ or Cs+. Metallic lead formation was most easily observed in the chloride perovskite, followed by bromide, and very little in MAPbI3. Multiple degradation processes were identified for the bromide compositions, including ion migration, formation of volatile and solid products, as well as metallic lead. CsBr was formed as a solid degradation product on the surface of CsPbBr3.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Timofei Rostilov, Vadim Ziborov, Alexander Dolgoborodov, Mikhail Kuskov
Summary: The shock-loading behavior of nanomaterials is investigated in this study. It is found that shock compaction waves exhibit a distinct two-step structure, with the formation of faster precursor waves that travel ahead of the main compaction waves. The complexity of the shock Hugoniot curve of the tested nanomaterial is described, and the effect of initial porosity on the compressed states is demonstrated.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Sergey S. Nikitin, Alexander D. Koryakov, Elizaveta A. Antipinskaya, Alexey A. Markov, Mikhail V. Patrakeev
Summary: The stability of La1/3Sr2/3Fe1-xMnxO3-delta, a perovskite-type oxide, under reducing conditions is dependent on the manganese content. Increasing the manganese content leads to a decrease in stability. The behavior of iron and manganese in the oxide shows distinct differences, which can be attributed to the difference in the enthalpy of oxidation reactions. Additionally, the change in the La/Sr ratio affects the concentration of iron and manganese ions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Mosayeb Naseri, Shirin Amirian, Mehrdad Faraji, Mohammad Abdur Rashid, Maicon Pierre Lourenco, Venkataraman Thangadurai, D. R. Salahub
Summary: Inspired by the successful transfer of freestanding ultrathin films of SrTiO3 and BiFeO3, this study assessed the structural stability and investigated the electronic, optical, and thermoelectric properties of a group of two-dimensional perovskite-type materials called perovskenes. The findings revealed that these materials are wide bandgap semiconductors with potential application in UV shielding. Moreover, they exhibit better electrical and thermal conductivity at high temperatures, enabling efficient power generation in thermoelectric devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
