Article
Chemistry, Multidisciplinary
Sascha Jahnigen, Katia Le Barbu-Debus, Regis Guillot, Rodolphe Vuilleumier, Anne Zehnacker
Summary: In this study, the effect of a twofold screw axis on the solid-state VCD spectrum was investigated using both experimental and theoretical analysis. It was found that the VCD spectrum can reflect the supramolecular chirality of the crystal.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Spectroscopy
Zhen Wang, Yugao Xu, Wenqin Li, Tao Lu, Gang Feng
Summary: In this study, the 1,4-pentadien-3-ol and its monohydrate were characterized using microwave spectroscopy and theoretical computations. The research revealed the characteristics of hydrogen bonds in the compounds.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2022)
Article
Biochemistry & Molecular Biology
Maxim V. Grigoriev, Leonid A. Solovyov, Anna V. Ruseikina, Aleksandr S. Aleksandrovsky, Vladimir A. Chernyshev, Dmitriy A. Velikanov, Alexander A. Garmonov, Maxim S. Molokeev, Aleksandr S. Oreshonkov, Nikolay P. Shestakov, Alexey V. Matigorov, Svetlana S. Volkova, Evgeniy A. Ostapchuk, Alexander V. Kertman, Thomas Schleid, Damir A. Safin
Summary: This work reports on the synthesis, crystal structure studies, and optical and magnetic properties of newly synthesized heterometallic quaternary selenides. The crystal structures were determined and the compounds were found to exhibit different magnetic properties. The optical band gaps were also measured and compared with calculated values.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Review
Chemistry, Multidisciplinary
Edward Ditler, Sandra Luber
Summary: Vibrational spectroscopy is an important experimental technique for characterizing molecules and materials, but the interpretation of experimental results can be challenging. Computational studies using molecular dynamics simulations provide a valuable tool for understanding and predicting experimental results. This review article summarizes the field of vibrational spectroscopy using first-principles molecular dynamics and highlights recent advances in simulation techniques.
WILEY INTERDISCIPLINARY REVIEWS-COMPUTATIONAL MOLECULAR SCIENCE
(2022)
Article
Chemistry, Physical
Juan J. J. Aucar, Alejandro F. F. Maldonado, Juan I. I. Melo
Summary: In this work, relativistic corrections to the electric field gradient (EFG) are presented, including spin-dependent corrections for the first time. The results show that these new corrections significantly improve the performance of the existing method and are in close agreement with calculations at the four-component Dirac-Hartree-Fock (4c-DHF) level. The accuracy of the EFG values obtained with this new method allows for the analysis of the electronic origin of relativistic effects using well-known nonrelativistic operators.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Materials Science, Coatings & Films
Petr Rehak, Jakub Ceska, Miroslav Cerny
Summary: Using a first-principles approach, the effect of oxygen as a substitutional impurity on the cohesion of three transition metal nitride multilayers was investigated. It was found that oxygen prefers to replace nitrogen atoms in interfacial planes and does not reduce the multilayer cohesion. In fact, in the AlN/TiN system, the presence of oxygen was found to increase the cohesion of the interface.
SURFACE & COATINGS TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Jeongjae Lee, Sunita Dey, Sian E. Dutton, Clare P. Grey
Summary: This study demonstrates an ab initio predictive synthesis strategy for producing multi-gram-scale MgVxOy phases relevant for Mg-ion battery cathodes. The characterization using Mg-25 solid-state NMR spectroscopy reveals the potential of Mg-25 NMR in studying reversible magnesiation and local charge distributions. The ab initio guided synthesis method is considered a step forward in targeting specific complex TM oxides with variable oxidation states of technological importance.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Jing Shang, Congxin Xia, Chun Tang, Chun Li, Yandong Ma, Yuantong Gu, Liangzhi Kou
Summary: The bending deformation of AgBiP2Se6 monolayers can manipulate the polarization direction and domain size, significantly improving the ferroelectric stability. This mechano-ferroelectric coupling represents a new mechanism for stabilization and polarization flip in 2D ferroelectrics, with potential applications in next-generation non-volatile storage devices.
NANOSCALE HORIZONS
(2021)
Article
Biochemistry & Molecular Biology
Natalia Grytsyk, Ludovic Richert, Pascal Didier, Dmytro Dziuba, Stefano Ciaco, Viola Mazzoleni, Thiebault Lequeu, Mattia Mori, Yitzhak Tor, Lara Martinez-Fernandez, Roberto Improta, Yves Mely
Summary: Time-resolved fluorescence anisotropy (TRFA) technique provides important information on the dynamics of biomolecules and their interaction with ligands. This study shows that thienoguanosine ((th)G), a fluorescent analogue of guanosine, overcomes the limitations of non-fluorescent natural nucleosides and serves as a unique reporter for investigating the rotational dynamics of dsDNA and protein/dsDNA complexes.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2022)
Article
Chemistry, Multidisciplinary
Guanping Li, Olaf Stefanczyk, Kunal Kumar, Yuuki Mineo, Koji Nakabayashi, Shin-ichi Ohkoshi
Summary: In this study, six new high-dimensional frameworks were successfully synthesized by self-assembly of Fe-II complexes of phenazine, quinoxaline, and 4,4'-trimethylenedipyridine with tetrahedral building blocks of [Hg-II(XCN)(4)](2-) (X=S or Se). Compounds 1, 3, and 3-Se exhibited intense sub-terahertz (sub-THz) absorbance, while compounds 1, 4, and 4-Se showed low-frequency Raman scattering. These findings suggest that heavy metal Fe-II-Hg-II systems are promising platforms for constructing sub-THz absorbers.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Qian-Rui Huang, Ryunosuke Shishido, Chih-Kai Lin, Chen-Wei Tsai, Jake A. Tan, Asuka Fujii, Jer-Lai Kuo
Summary: The study analyzed the infrared spectra of a series of asymmetric proton-bound dimers with protonated trimethylamine as the proton donor, revealing a red shift in the N-H+ stretching mode frequency as the proton affinity of acceptors increases. Despite the expected pattern, the observed band showed a peculiar splitting of around 300 cm(-1) with intensity resembling a two-level system. Theoretical investigation attributed this band splitting to strong coupling between the proton stretching mode and overtone states of proton bending modes, known as Fermi resonance, providing a general theoretical model linking the strong coupling to a quasi-two-level system intrinsic to proton motions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Ilya S. Sosulin, Mariia A. Lukianova, Anastasia D. Volosatova, Vladimir D. Drabkin, Svetlana V. Kameneva
Summary: Hydrogen bonding between saturated alkanes and HX is a unique type of interaction. Experimental and ab initio studies on the HCN...C2H6 complex show that only one structure is stabilized under experimental conditions, in good agreement with previous rotational spectroscopy studies.
JOURNAL OF MOLECULAR STRUCTURE
(2021)
Article
Chemistry, Applied
Thibault Pariat, Pauline M. Verite, Denis Jacquemin, Julien Massue, Gilles Ulrich
Summary: A dual-emissive fluorophore, HBBODipic, with an Excited-State Intramolecular Proton Transfer (ESIPT) process has been described. It has been used for generating panchromatic white-emission and ratiometric detection of substrates.
Article
Chemistry, Multidisciplinary
Helmut Poleschner, Konrad Seppelt
Summary: Thiiranium and seleniranium salts were synthesized from different starting materials and their reactions were investigated, revealing unexpected products due to attempts to cleave specific groups. The study highlights the complexity of reactions in this system.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Jens H. Tran, Philipp Traber, Bianca Seidler, Helmar Goerls, Stefanie Graefe, Martin Schulz
Summary: In this study, a novel copper complex with intense absorption properties in the visible and near-infrared (NIR) regions was developed. The absorption is attributed to low-energy metal-to-ligand charge-transfer bands, which arise from the destabilized copper-based donor states induced by the chelating anionic ligands. These findings provide a new route to achieving panchromatic absorption in Cu(I) complexes.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Biochemistry & Molecular Biology
Venkateswara Rao Mundlapati, Zeynab Imani, Gildas Goldsztejn, Eric Gloaguen, Valerie Brenner, Katia Le Barbu-Debus, Anne Zehnacker-Rentien, Jean-Pierre Baltaze, Sylvie Robin, Michel Mons, David J. Aitken
Summary: The study investigated the conformational preferences of S-methyl-L-cysteine, showing that single Cys(Me) residues adopt a specific conformation in gas phase and low polarity solution, while consecutive Cys(Me) residues form a regular type I beta-turn structure without specific interactions. The comparison with a thietane amino acid highlighted the significance of side chain flexibility for the conformational behavior of Cys(Me).
Article
Optics
Ariel Perez-Mellor, Katia Le Barbu-Debus, Valeria Lepere, Ivan Alata, Riccardo Spezia, Anne Zehnacker
Summary: The study on the protonated cyclic dipeptide cyclo histidine-phenylalanine reveals that stereochemical factors have a significant impact on the collision-induced dissociation processes, primarily due to proton mobility and the formation of different intermediate cyclic structures. This contrasts with the minor stereochemical effects observed for other cyclic dipeptides where the proton is carried by an amide CO.
EUROPEAN PHYSICAL JOURNAL D
(2021)
Article
Physics, Atomic, Molecular & Chemical
Ariel Perez-Mellor, Ivan Alata, Valeria Lepere, Riccardo Spezia, Anne Zehnacker-Rentien
Summary: This study investigates the structures and fragmentation properties of protonated cyclo (LTyr-LPro) and cyclo (LTyr-DPro) dipeptides based on a DKP ring using tandem mass spectrometry in a FT-ICR mass spectrometer. The results of CID and IRMPD spectroscopy are explained through quantum chemical calculations and chemical dynamics simulations, revealing distinct structural characteristics for different diastereomers. The protonated dimers of these dipeptides exhibit identical IR spectra, indicating a specific structure involving a strong interaction between subunits that is not sensitive to the absolute configuration of the residues.
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY
(2021)
Article
Chemistry, Physical
Jennifer Dupont, Valeria Lepere, Anne Zehnacker, Sebastian Hartweg, Gustavo A. Garcia, Laurent Nahon
Summary: Chirality and molecular conformation are crucial in molecular recognition, and valence-shell photoelectron circular dichroism (PECD) can sensitively detect them.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Jennifer Dupont, Regis Guillotb, Valeria Lepere, Anne Zehnacker
Summary: The structures of diastereomer diketopiperazine dipeptides cyclo(LTyr-LPhe) and cyclo-(DTyr-LPhe) were studied in the gas phase using resonance-enhanced two-photon ionization, IR/UV double resonance spectroscopy, and quantum chemical calculation. Both diastereomers exhibit two conformations with slight differences in weak CH···ir and NH···ir interactions. The crystal structure and vibrational circular dichroism spectrum were determined, with quantum chemical calculation shedding light on structural modifications between the gas phase and the solid state.
JOURNAL OF MOLECULAR STRUCTURE
(2022)
Article
Chemistry, Physical
Koki Yoshizawa, Keisuke Hirata, Shun-Ichi Ishiuchi, Masaaki Fujii, Anne Zehnacker
Summary: This study investigates the two diastereomers of the protonated diketopiperazine (DKP) dipeptide cyclo(Tyr-Tyr) using IR photodissociation spectroscopy and quantum chemical calculations. It is found that these diastereomers have similar structures with one folded ring over the DKP ring and the other extended in a trans geometry, forming a strong OH···π interaction. The neutral cyclo(LTyr-LTyr) dipeptide only exhibits a stacked geometry under supersonic expansion conditions, which is not observed in cyclo(LTyr-DTyr). In the protonated form, the strength of the OH···π interaction differs between the two diastereomers, resulting in significant differences in the nu(OH+) and protonated amide nu(NH) frequencies.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Sascha Jahnigen, Katia Le Barbu-Debus, Regis Guillot, Rodolphe Vuilleumier, Anne Zehnacker
Summary: In this study, the effect of a twofold screw axis on the solid-state VCD spectrum was investigated using both experimental and theoretical analysis. It was found that the VCD spectrum can reflect the supramolecular chirality of the crystal.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Zeynab Imani, Venkateswara Rao Mundlapati, Valerie Brenner, Eric Gloaguen, Katia Le Barbu-Debus, Anne Zehnacker-Rentien, Sylvie Robin, David J. Aitken, Michel Mons
Summary: The delta conformation, a local secondary structure in proteins, is stabilized by specific side-chain/backbone N-H interactions in derivatives of a cyclic amino acid with a sulphur atom in the gamma-position. This allows the delta conformation to compete with classical C5 and C7 hydrogen bonded conformers, expanding the range of small-molecule models beyond rigid proline-type compounds.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Koki Yoshizawa, Keisuke Hirata, Shun-ichi Ishiuchi, Masaaki Fujii, Anne Zehnacker
Summary: The structure of alkali metal complexes of cyclic dipeptide cyclo Tyr-Tyr was determined by IRPD and quantum chemical calculations. The structure of the complexes depends on the chirality of the tyrosine residues. For residues of identical chirality, the metal cation interacts with one amide oxygen and one aromatic ring, while for residues of opposite chirality, the metal cation interacts with both aromatic rings. The distance between the aromatic rings is influenced by the metal. UV photodissociation spectroscopy and analysis of the UV photo-fragments revealed the excited state deactivation processes, which are influenced by the chirality of the residues and the metal ion core. Na+ shows low-lying charge transfer states, leading to broadening of the electronic spectrum.
Article
Multidisciplinary Sciences
Etienne Rouquet, Madhusree Roy Chowdhury, Gustavo A. Garcia, Laurent Nahon, Jennifer Dupont, Valeria Lepere, Katia Le Barbu-Debus, Anne Zehnacker
Summary: An achiral chromophore can exhibit a chiral spectroscopic signature in the presence of a chiral environment. In this study, the asymmetric scattering of a photoelectron ejected from an achiral chromophore interacting with a chiral host was observed, indicating the induction of a chiroptical response within the electric dipole approximation. This induced chirality has important implications in structural and analytical studies, particularly in the field of laser-based PECD.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Taija L. Fischer, Margarethe Boedecker, Sophie M. Schweer, Jennifer Dupont, Valeria Lepere, Anne Zehnacker-Rentien, Martin A. Suhm, Benjamin Schroeder, Tobias Henkes, Diego M. Andrada, Roman M. Balabin, Haobam K. Singh, Himangshu P. Bhattacharyya, Manabendra Sarma, Silvan Kaser, Kai Topfer, Luis I. Vazquez-Salazar, Eric D. Boittier, Markus Meuwly, Giacomo Mandelli, Cecilia Lanzi, Riccardo Conte, Michele Ceotto, Fabian Dietrich, Vicente Cisternas, Ramachandran Gnanasekaran, Michael Hippler, Mahmoud Jarraya, Majdi Hochlaf, Narasimhan Viswanathan, Thomas Nevolianis, Gabriel Rath, Wassja A. Kopp, Kai Leonhard, Ricardo A. Mata
Summary: Vibrational spectroscopy in supersonic jet expansions is a powerful tool for benchmarking quantum chemical approaches. It provides potential benchmarking data for the critical analysis of procedures and unbiased testing opportunities. The results of the HyDRA blind challenge show promising predictive properties in both quantum mechanical approaches and machine learning strategies.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Arman Nejad, Ariel F. Perez Mellor, Manuel Lange, Ivan Alata, Anne Zehnacker, Martin A. Suhm
Summary: The hydrogen-bonded complexes formed between 2-naphthol (or beta-naphthol) and anisole were investigated using IR and UV absorption techniques. The experiments detected consistent hydrogen bonding between the OH group of 2-naphthol and the oxygen atom of anisole in different supersonic jet expansions. However, alternative hydrogen bonding to the aromatic ring of anisole was difficult to observe. The study highlights the importance of including three-body dispersion correction in theoretical calculations and suggests further investigations into related compounds.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Katia Le Barbu-Debus, Ariel Perez-Mellor, Valeria Lepere, Anne Zehnacker
Summary: The protonated dimers of diketopiperazine dipeptides were examined to investigate the influence of stereochemistry on their clustering propensity. The results showed that the chirality of the residue has a significant impact on the formation of beta sheet patterns observed in amyloid type aggregation.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Taija L. Fischer, Margarethe Boedecker, Anne Zehnacker-Rentien, Ricardo A. Mata, Martin A. Suhm
Summary: The procedure for the first HyDRA blind challenge for predicting water donor stretching vibrations in monohydrates of organic molecules is described. A training set of 10 monohydrates with known experimental data is presented, along with a test set of 10 monohydrates with unknown water donor vibrational wavenumbers. The rules for data submissions from computational chemistry groups are outlined, and the planned publication procedure after the challenge is discussed.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
