Article
Chemistry, Multidisciplinary
Jaya Mehara, Adarsh Koovakattil Surendran, Teun van Wieringen, Deeksha Setia, Cina Foroutan-Nejad, Michal Straka, Lubomir Rulisek, Jana Roithova
Summary: Gold(II) complexes are not commonly used in catalyzing chemical transformations due to their easy oxidation or reduction to more stable gold(III) or gold(I) complexes. In this study, we investigated the thermodynamics, stability, and spectral properties of [Au-II(L)(X)](+) complexes (L=ligand, X=halogen) in the gas phase. It was found that bidentate and tridentate ligands with nitrogen donor atoms are the best choices for stabilizing gaseous [Au-II(L)(X)](+) complexes. Quantum chemical calculations revealed that the molecular and electronic structures, as well as the spectroscopic properties, of the investigated gold(II) complexes are similar to those of stable copper(II) complexes.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Physical
Ikram Jomaa, Chaima Daghar, Noureddine Issaoui, Thierry Roisnel, Houda Marouani
Summary: This paper presents the crystal structure analysis and characterization of a new material, (C8H14N2)(ClO4)(2)·H2O, using single crystal X-ray diffraction. The compound crystallizes in the monoclinic system and exhibits extensive intermolecular interactions, including C-H···π interactions and hydrogen bonds, which contribute to its stability in the solid-state. The study also includes Hirshfeld surface analyses, DFT calculations, and molecular electrostatic potential inspection to further understand the molecule's properties and stability. (c) 2022 Elsevier B.V. All rights reserved.
JOURNAL OF MOLECULAR STRUCTURE
(2023)
Article
Engineering, Chemical
Yue Liu, Ji-Wei Wang, Jian Zhang, Ting-Ting Qi, Guang-Wen Chu, Hai-Kui Zou, Bao-Chang Sun
Summary: This study investigates the removal of NOx via non-thermal plasma reduction in a dielectric barrier discharge reactor. The results show that anaerobic conditions and higher discharge power contribute to a direct removal of NOx, with a maximum removal efficiency of up to 98.5% under optimized conditions. Adding NH3 favors the reduction of NOx to N-2 at lower discharge power. The study also reveals the role of reduced active species in the NOx removal mechanism during the non-thermal plasma reduction process.
FRONTIERS OF CHEMICAL SCIENCE AND ENGINEERING
(2022)
Article
Chemistry, Physical
Valdemir Ludwig, Alessandro Henrique de Lima, Lucas Modesto-Costa, Zelia M. Da Costa Ludwig, Joao Paulo Almeira de Mendonca, Welber Gianini Quirino, Fernando Sato
Summary: In this study, graphene oxide (GO) was synthesized and its vibrational properties were characterized for hydrated and lyophilized samples. Computational simulations showed a large polarization in the GO molecule due to strong hydrogen bonds formed between water molecules and oxygen functional groups. This led to broadening observed in the infrared and Raman spectra.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Chemistry, Physical
Dujuan Meng, Sophia Sagala, Adelia J. A. Aquino, Edward L. Quitevis
Summary: The study presented in the paper utilized optical heterodyne-detected Raman-induced Kerr effect spectroscopy (OHD-RIKES) and density functional theory (DFT) to investigate the low-frequency dynamics and picosecond reorientational dynamics of methyl methacrylate (MMA). The results show that the temperature dependence of the reorientational dynamics can be explained by a modified Debye-Stoke-Einstein equation, and the interpretation of the main band of the low-frequency reduced-Raman spectrum of poly(methyl methacrylate) (PMMA) is supported by the Kerr spectrum of MMA. The analysis suggests that the librational motion in PMMA is associated with the torsional motion of the methoxycarbonyl pendant group on the polymer chain.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Chemistry, Physical
Yangyu Zhou, Hao Liu, Xiaoyang Jin, Xiaopeng Xing, Xuefeng Wang, Guanjun Wang, Mingfei Zhou
Summary: A series of coinage metal complexes were generated in the gas phase using a laser-ablation device, with findings showing the differences and properties of bonding and interactions between metals and ligands among different metals.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
V. L. Diaz De Rosa, A. Gil Rebaza, M. L. Montes, M. A. Taylor, R. E. Alonso
Summary: Montmorillonite is a clay mineral commonly used for removing pollutants from wastewater. In this study, the sorption of strontium (Sr) on montmorillonite was investigated using an experimental and theoretical approach. It was found that Sr can be sorbed on both the external and internal surfaces of the clay, and the total specific surface area plays a crucial role in the sorption process. Nuclear magnetic resonance calculations were used to predict the sorption behavior of Sr.
APPLIED SURFACE SCIENCE
(2022)
Article
Spectroscopy
Neva Agarwala, Leyla Rohani, Gary Hastings
Summary: There is interest in incorporating substituted 1,4-naphthoquinones (NQs) into the A l binding site in photosystem I (PSI) photosynthetic protein complexes, as it alters the bioenergetics of electron transfer in PSI. Time-resolved FTIR studies have been conducted on PSI complexes with disubstituted NQs, comparing their absorption spectra in solution and through density functional theory (DFT) calculations. The calculated and experimental spectra agree well, aiding in making quantitative band assignments and predictions for time-resolved FTIR difference spectra.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2022)
Article
Chemistry, Organic
V. Anbu, T. Karthick, K. A. Vijayalakshmi
Summary: In this study, the spectroscopic characteristics and intermolecular interactions of 2,6-di-tert-butyl-p-cresol were analyzed. The results predicted its nonlinear optical properties and investigated its potential role in biological metabolism. DBPC was found to have drug-like properties and can permeate through the blood-brain barrier.
POLYCYCLIC AROMATIC COMPOUNDS
(2022)
Article
Chemistry, Applied
Raffaele Cucciniello, Michele Tomasini, Anna Russo, Laura Falivene, Angelita Gambuti, Martino Forino
Summary: Acetaldehyde plays a crucial role in determining certain properties of wine, and its reaction with flavonoids can significantly impact the color, astringency, and colloidal stability of the wine. A study investigated the reaction between acetaldehyde and catechin, revealing the formation of ethylidene-bridged catechins as initial products, which eventually dissociate to accumulate vinyl-catechins over time.
Article
Chemistry, Physical
Andrzej Eilmes, Wagner A. Alves
Summary: Measurements of the Far-IR and Raman spectra of 1:1 MACC-ether electrolytes were conducted in this study, revealing the major dimers [(mu-Cl)(2)Mg-2](2+) and [MgCl](+). A new IR band was identified in THF-based electrolytes, which may serve as a sensor. Additionally, the [(mu-Cl)(3)Mg-2](+) dimer was found in both 2:1 and 1:1 MACC-THF electrolytes, indicating the presence of electrochemically active species even at a 1:1 ratio.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Chemistry, Physical
Ariadne C. Catto, Marisa C. Oliveira, Renan A. P. Ribeiro, Waldir Avansi Jr, Luis F. da Silva, Elson Longo
Summary: This study investigates the ozone gas-sensing properties of hematite microrhombuses obtained via the hydrothermal method. Experimental results show the sensitivity and long-term stability of the microrhombuses towards O3 gas, while theoretical calculations highlight the importance of surfaces in the adsorption/desorption processes. The presence of (1 0 4) surfaces is found to enhance the sensitivity towards O3 molecules, confirming the experimental findings.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Reza Nematollahi, Bahareh Fahimirad, Rahimeh Eshaghi Malekshah, Ali Elhampour, Mohadese Piri, Majid M. Heravi
Summary: In this study, phosphorus-selenium doped carbon nitride was used to enhance the light absorption of pure carbon graphite nitride. The addition of silver nanoparticles created a surface plasmonic resonance effect, and the photocatalytic activity was improved by suppressing charge carriers' recombination. The synthesized photocatalyst showed enhanced degradation efficiency for the azo dye Rhodamine B under visible light irradiation. This study is rated 7 out of 10.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Biochemistry & Molecular Biology
Ximena Jaramillo-Fierro, John Ramon, Eduardo Valarezo
Summary: This study investigates the removal of cyanide species from aqueous solutions using the ZnTiO3/TiO2/H2O2/UVB system. The experimental results show that this system is effective in removing cyanide and has good detoxification effect.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Inorganic & Nuclear
Nobuaki Suzuki, Joohwi Lee, Yumi Masuoka, Shingo Ohta, Tetsuro Kobayashi, Ryoji Asahi
Summary: The study shows that KLTO exhibits good Li-ion conductivity and low activation energy, with Sn-doped KLTO demonstrating superior performance. However, further improvements in extrinsic doping and fabrication processes are necessary to enhance the performance of KLTO as a Li-ion solid electrolyte.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Tarcius N. Ramos, Benoit Champagne
Summary: The Sequential Quantum Mechanics/Molecular Mechanics scheme was used to systematically investigate the polarizability and first hyperpolarizability at the water-vacuum interface. It was found that the anisotropy of the polarizability increased, and there was an increase in the response of the first hyperpolarizability.
Article
Chemistry, Multidisciplinary
Bethany R. R. Hood, Yovan de Coene, Afonso V. V. Torre Do Vale Froes, Claire F. F. Jones, Pierre Beaujean, Vincent Liegeois, Fraser MacMillan, Benoit Champagne, Koen Clays, John Fielden
Summary: Electrochemically switched 2(nd) order non-linear optical responses have been demonstrated for the first time in polyoxometalates (POMs), with an arylimido-derivative showing a leading combination of high on/off contrast (94 %), high visible transparency, and cyclability.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Francois Mairesse, Lorenzo Maschio, Benoit Champagne
Summary: Using the CRYSTAL17 package, first-principles calculations were conducted to predict the values of chi((2)) for six historical NLO crystals. Various computational aspects were considered to ensure converged results, including lattice summations, k-points, electrostatic interactions, and atomic basis set size. The impact of HF exchange on the chi((2)) tensor components was also investigated.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Charlotte Bouquiaux, Frederic Castet, Benoit Champagne
Summary: The extensive collection of lipids found in cell membranes plays a significant role in the overall structure, dynamics, and properties of the membranes, as well as the biological processes occurring within them. This study focuses on investigating a range of saturated glycerophospholipids with varying headgroup structures using second harmonic generation (SHG) nonlinear optical (NLO) response analysis. The research reveals that the lipidic arrangement is strongly influenced by the hydrophilic head, while the hydrophobic region has less impact. Moreover, the computational approach provides insights into the relationship between lipid building blocks and the NLO responses of the embedded dye.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Organic
Abel Idrice Adjieufack, Benoit Champagne, Vincent Liegeois
Summary: Bonding evolution theory was used to elucidate the reaction mechanism of the intramolecular aza-Wittig reaction. The reaction involves the formation of a cycloadduct, decarboxylation, intramolecular [2+2] cycloaddition, and retro [2+2] cycloaddition. The rate-determining step is the formation of the cycloadduct and the reaction is exergonic, resulting in the formation of the aromatic benzothiazole.
SYNTHESIS-STUTTGART
(2023)
Editorial Material
Chemistry, Multidisciplinary
Tarcius N. Ramos, Benoit Champagne
Summary: This article investigates the interfacial selectivity of second harmonic generation at the water-vacuum interface through combining classical molecular dynamics and quantum chemistry simulations, distinguishing between bulk and interfacial contributions through calculated molecular first hyperpolarizability responses.
Article
Chemistry, Physical
Tarcius N. Ramos, Laura Le Bras, Yves L. Dory, Benoit Champagne
Summary: Targeting the use of second harmonic generation (SHG) as a bioimaging technique, the SHG first hyperpolarizabilities (beta) of assemblies of benzene-1,3,5-tricarboxamide derivatives were evaluated using density functional theory. The calculations revealed that the assemblies exhibit size-dependent SHG responses, with a maximum 18-times increase in beta HRS for B4 when going from monomer to pentamer. The presence of iodine atoms on the phenyl core enhanced the intrinsic SHG responses, and the side chains affected the relative orientation of dipole moment and first hyperpolarizability vectors.
Article
Chemistry, Physical
Andrea Bonvicini, Kayn A. Forbes, David L. Andrews, Benoit Champagne
Summary: This study presents the first computational quantum-chemistry implementation of hyper-Rayleigh scattering optical activity (HRS-OA), a nonlinear chiroptical phenomenon. The equations for simulating the differential scattering ratios of HRS-OA are derived based on the theory of quantum electrodynamics and the interactions of electric dipole, magnetic dipole, and electric quadrupole. Computation results of HRS-OA quantities for a chiral organic molecule (methyloxirane) using a broad range of atomic orbital basis sets are presented and analyzed, demonstrating the ability of HRS-OA to distinguish between enantiomers of the same chiral molecule.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Francois Mairesse, Benoit Champagne
Summary: The quantum treatment of electrons at the Kohn-Sham Density Functional Theory (DFT) level of approximation is used to optimize the structure of four organic and organo-metallic crystalline systems with nonlinear optical properties. The study addresses the lack of London-type interactions description in exchange-correlation functionals (XCFs) by employing the D* scheme, a variation of the D2 correction scaled for crystal solid state interactions. The performance and suitable scaling factors of the D* scheme are demonstrated for four representative XCFs.
INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY
(2023)
Article
Chemistry, Physical
Komlanvi Sevi Kaka, Pierre Beaujean, Frederic Castet, Benoit Champagne
Summary: Recent measurements of the third harmonic scattering responses of molecules have provided new insights into computing molecular second hyperpolarizabilities (gamma) and deducing structure-property relationships. This paper evaluates the second hyperpolarizability of the pi-nitroaniline molecule using various wavefunction and density functional theory methods. The results show that the MP2 scheme offers the best accuracy/cost ratio for computing static gamma, while density functional theory methods still face challenges in accurately computing gamma. Additionally, the double-hybrid B2-PLYP functional provides accurate estimates of static gamma values.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Andrea Bonvicini, Benoit Champagne
Summary: In this work, the expressions for the third-harmonic scattering optical activity (THS-OA) spectroscopic responses are derived by combining molecular quantum electrodynamics (QED) and response theory, allowing for their computational implementation. The study shows how the pure and mixed second hyperpolarizabilities can be obtained as specific cases of a generic cubic response function, enabling the calculation of THS-OA spectroscopy.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Andrea Bonvicini, Benoit Champagne
Summary: This paper discusses the theoretical formulation and computational procedure of linear and nonlinear molecular spectroscopies applied to isotropic samples. It introduces the concept of rotational averaging of Cartesian tensors and proposes a heuristic computational method for finding linearly independent fundamental isotropic Cartesian tensors.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Carmelo Naim, Raphael Vangheluwe, Isabelle Ledoux-Rak, Benoit Champagne, Claire Tonnele, Mireille Blanchard-Desce, Eduard Matito, Frederic Castet
Summary: The second-order nonlinear optical properties of four series of amphiphilic cationic chromophores have been investigated experimentally and theoretically. The theoretical methodology combining classical molecular dynamics and quantum chemical calculations provides a rational approach for designing SHG dyes based on EFISH measurements. The good agreement between experimental and theoretical results demonstrates the usefulness of this MD + QM scheme.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Charlotte Bouquiaux, Frederic Castet, Benoit Champagne
Summary: Lipid molecules play important roles in cell functions and their structural diversity is related to different fatty acids. The nature of fatty acids has an additive effect on the overall membrane structure. Nonlinear optical responses of an embedded chromophore can be used to study the local structure of cell membranes.
Article
Chemistry, Physical
Charlotte Bouquiaux, Pierre Beaujean, Tarcius N. Ramos, Frederic Castet, Vincent Rodriguez, Benoit Champagne
Summary: The solvent effects on the optical properties of an ANEP dye were studied using experimental and theoretical methods. Experimental measurements showed a decrease in the hyperpolarizablity of the dye in polar solvents, which was confirmed by theoretical calculations using different solvation models.
JOURNAL OF CHEMICAL PHYSICS
(2023)
