Article
Materials Science, Multidisciplinary
S. Kato, N. Nakajima, S. Yasui, S. Yasuhara, D. Fu, J. Adachi, H. Nitani, Y. Takeichi, A. Anspoks
Summary: For the first time, the dielectric response of a BaTiO3 thin film under an AC electric field was investigated using microsecond time-resolved X-ray absorption spectroscopy. The study revealed the correlated contributions of each constituent atom on the electronic states, with Ti 3d hybridizing with O 2p and Ti 4p, and Ba contributing to polarization reversal.
Article
Chemistry, Multidisciplinary
Ziyi Chen, Andrew G. Walsh, Xiao Wei, Manzhou Zhu, Peng Zhang
Summary: This study investigates the electronic properties of Ag-25(SR)(18) and Au-25(SR)(18) and develops a unique method to analyze the charge transfer behavior of nanoclusters. Experimental X-ray spectroscopy is used to demonstrate the bonding properties of silver nanoclusters, with the staple motif shown to have a significant impact on their electronic properties. The effective X-ray analysis techniques developed here provide new opportunities for the site-specific study of other nanoclusters.
Review
Energy & Fuels
Yangguang Hu, Chao Gao, Yujie Xiong
Summary: The time-resolved X-ray absorption technique plays a crucial role in understanding the mechanisms of photochemical reactions by capturing electronic and geometric changes in real time, providing guidance for designing advanced solar energy conversion systems.
Article
Chemistry, Physical
S. M. Kumawat, G. D. Dwivedi, T. W. Yen, D. Chandrasekhar Kakarla, A. Tiwari, S. J. Sun, H. D. Yang, H. Chou
Summary: In this work, the detailed structural, magnetic, dielectric, and transport properties, as well as electronic structure studies of a Mn2.4Ni0.6O4: system, are presented. The system exhibits a cubic crystal structure and ferrimagnetic transition at room temperature. Additionally, the system shows interesting transport behavior and a weakened semiconducting behavior at low temperatures.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Chemistry, Multidisciplinary
Lucia Velasco, Cunming Liu, Xiaoyi Zhang, Sergi Grau, Marcos Gil-Sepulcre, Carolina Gimbert-Surinach, Antonio Picon, Antoni Llobet, Serena DeBeer, Dooshaye Moonshiram
Summary: Nanosecond time-resolved X-ray and optical transient absorption spectroscopy were used to study three multimolecular photocatalytic systems with [Ru(bpy)3]2+ photoabsorber, ascorbic acid electron donor, and Co catalysts. The results reveal the complete mechanistic pathway of the Co-based photocatalysts in pure water and demonstrate that the protonation of the CoI intermediate can be enhanced through the introduction of terminal hydrogen containing amine substituents that function as efficient proton relays.
Article
Chemistry, Physical
Alexandre Mesquita, Elio Thizay Magnavita Oliveira, Hugo Bonette de Carvalho
Summary: Gadolinium-doped strontium titanate (Sr1-xGdxTiO3) is a perovskite structure material with interesting thermomechanical, termoelectrical, and electrochemical properties. X-ray absorption spectroscopy was used to analyze the local and electronic structure of Sr1-xGdxTiO3 samples, showing that increasing Gd content causes disorder and leads to a small displacement of Ti atoms. Changes in the XANES spectra at O K-edge for Sr1-xGdxTiO3 samples are influenced by the increase in Gd concentration.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Chemistry, Physical
Weifeng Huang, Jianxin Kang, Tingwen Chen, Dawei Pang, Lihua Wang, Hang Wei, Changchun Yang, Dongfeng Zhang, Lin Guo
Summary: Nickel based magnetic nanocrystals have wide applications in magnetic and catalytic fields. Tunable magnetic properties of nickel can be achieved through non-magnetic doping or phase transformation. This study presents a way to control the magnetism of Au@Ni-carbide magnetic materials by adjusting the amount of carbon in the Ni layer, and provides solid evidence for the carbonation process from fcc-Ni to Ni X C instead of phase transformation to hcp-Ni. Further investigation reveals that the magnetism of the hybrids is mainly contributed from the residual fcc-Ni.
Review
Chemistry, Physical
Francisco Zaera
Summary: Catalysis in industrial chemical processes has long been studied through various spectroscopic techniques like vibrational and X-ray spectroscopies, allowing for a molecular-level understanding of catalytic mechanisms. These techniques help researchers explore the intricate details of catalytic processes and advancements in the field.
JOURNAL OF CATALYSIS
(2021)
Article
Engineering, Environmental
Anshuman Satpathy, Jeffrey G. Catalano, Daniel E. Giammar
Summary: Adsorption and reduction of U(VI) on Fe(II)-bearing clay minerals can control uranium mobility in subsurface environments. The reduction of U(VI) was nearly complete at low sodium concentrations and both pH 3 and 6. At pH 6 and high sodium concentrations, U(VI) reduction was only 70%. Surface-bound U(VI) on unreduced montmorillonite was more easily extracted into solution with bicarbonate than surface-bound U(IV) generated by reduction. A nonelectrostatic surface complexation model was developed to interpret the equilibrium adsorption of U(IV) on Fe(II)-bearing montmorillonite as a function of pH and sodium concentration.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Materials Science, Ceramics
F. H. Bhat, G. Anjum, Ravi Kumar, Manzoor A. Malik, R. J. Choudhary, D. K. Shukla
Summary: Polycrystalline LaMn1-xCoxO3 (0.1 <= x <= 0.5) samples synthesized using conventional ceramic method exhibit strong magnetic properties with double transition and spin glass state. These characteristics are mainly influenced by the interactions between Co and Mn ions, showing significant magnetoresistance effects.
CERAMICS INTERNATIONAL
(2021)
Article
Chemistry, Physical
Beatriz Barata, Christele Legens, Elodie Devers, Olivier Delpoux, Laurent Barthe, Olga Roudenko, Valerie Briois
Summary: This paper describes and validates two cells designed to monitor the transformation of Mo based oxidic species during the preparation steps of a single hydrodesulfurization catalyst. The transformations occur during impregnation/maturation and drying. The in situ quick-EXAFS monitoring of the preparation steps provides quantitative results of Mo-speciation. Ex situ Raman spectroscopy is used as a complement. A two-step drying mechanism is proposed to explain the evolution of Mo-speciation during in situ drying.
Article
Chemistry, Physical
Worasarit Saengsui, Teerasak Tangkittimasak, Mantana Suwan, Nuchjarin Sangwong, Chalita Tangon, Narong Chanlek, Pattana Rakkwamsuk, Sitthisuntorn Supothina, Worawat Meevasana
Summary: Mg1-xCoxAl2O4, Zn1-xCoxFe2O4, and CrxSbxTi1-2xO2 pigment series with varying chemical constitution were prepared and structurally confirmed. Valence band maximum and Raman signal area were used to represent electronic and phononic absorption, respectively. The behavior of electronic and phononic absorption in near-infrared reflectance was trivial for Mg1-xCoxAl2O4 and Zn1-xCoxFe2O4, but nontrivial for CrxSbxTi1-2xO2. In CrxSbxTi1-2xO2, electronic absorption dominated at low doping regime, while phononic absorption played a dominance role at high doping regime. This nontrivial scenario provides insights into the reflective mechanism and paves the way for improving solar reflective pigment with color tuning.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Chemistry, Physical
Yogesh Kumar, S. Tripathi, Mangla Nand, R. Jangir, V. Srihari, A. Das, R. Singh, U. Deshpande, S. N. Jha, A. Arya
Summary: This study investigated the effect of Nd doping on the structural, optical, and electronic properties of lanthanum monazite structure. Pure and Nd-doped LaPO4 powders were prepared and analyzed for their composition, oxidation states, crystal structure, and bandgaps. The results confirmed the successful substitution of Nd in the LaPO4 matrix and provided insights into the local structure using extended X-ray absorption fine structure analysis.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Review
Chemistry, Physical
George E. Cutsail, Serena DeBeer
Summary: X-ray spectroscopy plays a significant role in catalysis research by providing essential electronic and geometric structural information. The development of dedicated synchrotron-based X-ray emission spectrometers has expanded experimental capabilities, offering more detailed data. There is a continuous demand for conventional XAS applications and the integration with more advanced techniques.
Article
Materials Science, Multidisciplinary
Ishan Pande, Sami Sainio, Jani Sainio, Ville Liljestrom, Hua Jiang, Tomi Laurila
Summary: This paper investigates the microstructure of carbon nanofibers (CNFs) grown on two different substrates and its correlation with surface chemistry. CNFs grown on Cr + Ni substrates show a slightly distorted herringbone-like structure, while those grown on Ti + Ni substrates have a relatively undefined structure. The latter possess a richer surface chemistry. These structure-chemistry correlations help tailor the features of CNFs for specific applications.
DIAMOND AND RELATED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Saikiran Kotaru, Sven Kahler, Maristella Alessio, Anna Krylov
Summary: The exchange coupling constants for a set of iron (III) binuclear and tetranuclear complexes are calculated using non-collinear spin-flip time-dependent density functional theory (NC-SF-TDDFT). The results show good agreement with experimentally derived values. The applicability of the Heisenberg model is explored by analyzing bonding patterns and natural orbitals (NO). The efficiency of the spin-flip protocol in computing exchange couplings and the utility of NO analysis in assessing the validity of effective spin Hamiltonians are demonstrated.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Pawel Wojcik, Eric R. Hudson, Anna Krylov
Summary: This study systematically investigates the diatomic radical-cations composed of a metal and a ligand, and finds that the electronic transitions in these cations for optical cycling are less effective compared to the successfully laser-cooled neutral molecules. Alternative transitions suitable for optical cycling are proposed, providing insights for the design of OCCs in charged or neutral molecules.
Article
Chemistry, Physical
Kaushik D. D. Nanda, Sahil Gulania, Anna I. I. Krylov
Summary: The equation-of-motion coupled-cluster singles and doubles method with double electron attachment (EOM-DEA-CCSD) is extended to calculate two-photon absorption (2PA) cross sections of diradicals and polyenes. The performance of this new implementation is compared with the CC3 quadratic response theory approach. The EOM-DEA-CCSD 2PA cross sections are comparable to the CC3 results for twisted ethene, but show large discrepancies for hexatriene, explained by configurational analysis of the 2PA channels.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Nayanthara K. Jayadev, Anthuan Ferino-Perez, Florian Matz, Anna I. Krylov, Jagau Thomas-C.
Summary: We conducted an ab initio computational study on the Auger electron spectrum of benzene. Using coupled-cluster theory and equation-of-motion coupled-cluster theory, we described the decaying nature of core-ionized states through two approaches and found that the computed spectra from both approaches agreed well with experimental Auger spectra. The Auger spectrum of benzene exhibits well-resolved peaks above 260 eV corresponding to final states with electrons removed from the highest occupied molecular orbitals.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Michael Epshtein, Bruno Nunes Cabral Tenorio, Marta L. Vidal, Valeriu Scutelnic, Zheyue Yang, Tian Xue, Anna I. Krylov, Sonia Coriani, Stephen R. Leone
Summary: Tabletop X-ray spectroscopy measurements and ab initio calculations are used to investigate the influence of the bromine atom on carbon core-valence transitions in the bromobenzene cation. The results show that replacing a hydrogen atom with a bromine atom in benzene shifts the transition energy in the X-ray spectrum. Moreover, the X-ray spectrum of the bromobenzene cation is dominated by two intense transitions, which are enhanced compared to the neutral bromobenzene.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Giovanni Li Manni, Ignacio Fdez. Galvan, Ali Alavi, Flavia Aleotti, Francesco Aquilante, Jochen Autschbach, Davide Avagliano, Alberto Baiardi, Jie J. Bao, Stefano Battaglia, Letitia Birnoschi, Alejandro Blanco-Gonzalez, Sergey I. Bokarev, Ria Broer, Roberto Cacciari, Paul B. Calio, Rebecca K. Carlson, Rafael Carvalho Couto, Luis Cerdan, Liviu F. Chibotaru, Nicholas F. Chilton, Jonathan Richard Church, Irene Conti, Sonia Coriani, Juliana Cuellar-Zuquin, Razan E. Daoud, Nike Dattani, Piero Decleva, Coen de Graaf, Mickael G. Delcey, Luca De Vico, Werner Dobrautz, Sijia S. Dong, Rulin Feng, Nicolas Ferre, Michael Filatov (Gulak), Laura Gagliardi, Marco Garavelli, Leticia Gonzalez, Yafu Guan, Meiyuan Guo, Matthew R. Hennefarth, Matthew R. Hermes, Chad E. Hoyer, Miquel Huix-Rotllant, Vishal Kumar Jaiswal, Andy Kaiser, Danil S. Kaliakin, Marjan Khamesian, Daniel S. King, Vladislav Kochetov, Marek Krosnicki, Arpit Arun Kumaar, Ernst D. Larsson, Susi Lehtola, Marie-Bernadette Lepetit, Hans Lischka, Pablo Lopez Rios, Marcus Lundberg, Dongxia Ma, Sebastian Mai, Philipp Marquetand, Isabella C. D. Merritt, Francesco Montorsi, Maximilian Morchen, Artur Nenov, Vu Ha Anh Nguyen, Yoshio Nishimoto, Meagan S. Oakley, Massimo Olivucci, Markus Oppel, Daniele Padula, Riddhish Pandharkar, Quan Manh Phung, Felix Plasser, Gerardo Raggi, Elisa Rebolini, Markus Reiher, Ivan Rivalta, Daniel Roca-Sanjuan, Thies Romig, Arta Anushirwan Safari, Aitor Sanchez-Mansilla, Andrew M. Sand, Igor Schapiro, Thais R. Scott, Javier Segarra-Marti, Francesco Segatta, Dumitru-Claudiu Sergentu, Prachi Sharma, Ron Shepard, Yinan Shu, Jakob K. Staab, Tjerk P. Straatsma, Lasse Kragh Sorensen, Bruno Nunes Cabral Tenorio, Donald G. Truhlar, Liviu Ungur, Morgane Vacher, Valera Veryazov, Torben Arne Voss, Oskar Weser, Dihua Wu, Xuchun Yang, David Yarkony, Chen Zhou, J. Patrick Zobel, Roland Lindh
Summary: This article describes the developments of the open-source OpenMolcas chemistry software environment since spring 2020, focusing on the novel functionalities in the stable branch and interfaces with other packages. These developments cover a wide range of topics in computational chemistry and provide an overview of the chemical phenomena and processes that OpenMolcas can address.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Plant Sciences
Chao Liang, Chi Ndi, Louise Kjaerulff, Susan Semple, Bevan Buirchell, Sonia Coriani, Birger Lindberg Moller, Dan Staerk
Summary: Extracts of Eremophila phyllopoda subsp. phyllopoda exhibited inhibitory activity against alpha-glucosidase and PTP1B. Through high-resolution profiling, 21 new serrulatane diterpenoids and five known furofuran lignans were identified. The structures were elucidated using HRMS and NMR spectroscopic data. The compounds showed potential as inhibitors for alpha-glucosidase and PTP1B.
JOURNAL OF NATURAL PRODUCTS
(2023)
Article
Chemistry, Physical
Anna Kristina Schnack-Petersen, Torsha Moitra, Sarai Dery Folkestad, Sonia Coriani
Summary: We have implemented a damped response framework in the open-source program eT for calculating resonant inelastic X-ray scattering (RIXS) at the CCSD and CC2 levels of theory. The framework can be extended to higher excitation methods and multilevel approaches. We compared the results with the frozen-core core-valence separated approach in Q-Chem and experimental data. The performance of the CC2 method was evaluated and found to be inferior to CCSD for X-ray absorption spectra, but comparable for RIXS spectra.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Sophie E. E. Canton, Mykola Biednov, Matyas Papai, Frederico A. A. Lima, Tae-Kyu Choi, Florian Otte, Yifeng Jiang, Paul Frankenberger, Martin Knoll, Peter Zalden, Wojciech Gawelda, Ahibur Rahaman, Klaus B. B. Moller, Christopher Milne, David J. J. Gosztola, Kaibo Zheng, Marius Retegan, Dmitry Khakhulin
Summary: Ultrafast optical absorption spectroscopy and X-ray emission spectroscopy were used to track the photoinduced spin-state switching of the prototypical complex [Co(terpy)(2)](2+) in solution phase. The study reveals that the complex undergoes ultrafast Jahn-Teller photoswitching between two different spin multiplicities on the femtosecond timescale.
Article
Chemistry, Physical
Anna Kristina Schnack-Petersen, Matyas Papai, Sonia Coriani, Klaus Braagaard Moller
Summary: The time-resolved x-ray absorption spectrum of BT-1T cation (BT-1T(+)) is simulated using trajectory surface hopping and quantum dynamics to investigate the charge transfer reaction. Static x-ray absorption spectra (XAS) of ground and excited states are calculated using time-dependent density functional theory and coupled cluster singles and doubles method, yielding consistent results. Small structural changes during the reaction have little impact on static XAS, thus enabling tr-XAS calculation based on state populations from nuclear dynamics simulation and a single set of static XAS calculations. This approach, applicable for investigating non-radiative decay processes near the Franck-Condon point in rigid molecules like BT-1T, saves computational resources.
STRUCTURAL DYNAMICS-US
(2023)
Article
Chemistry, Physical
Sonata Kvedaraviciute, David Carrasco-Busturia, Klaus B. Moller, Joigvan Magnus Haugaard Olsen
Summary: We propose a fully self-consistent polarizable embedding (PE) model that avoids unphysical boundary polarization by using the minimum-image convention (MIC) in induced electrostatics. This method provides a more physically accurate description of polarization throughout the molecular system. By comparing induced dipoles, electrostatic potentials, and optical properties of solute-solvent and biomolecular systems, we show that commonly used cutoff models, like the droplet model, have limitations in PE calculations due to unphysical polarization at the outer boundary.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Editorial Material
Chemistry, Physical
Anastassia N. Alexandrova, Julie S. Biteen, Sonia Coriani, Franz M. Geiger, Andrew A. Gewirth, Gillian R. Goward, Hua Guo, Libai Huang, Jian-Feng Li, Tim Liedl, Stephan Link, Zhi-Pan Liu, Sudipta Maiti, Andrew J. Orr-Ewing, David L. Osborn, Jim Pfaendtner, Benoit Roux, Friederike Schmid, J. R. Schmidt, William F. Schneider, Lyudmila V. Slipchenko, Gemma C. Solomon, Jeroen A. van Bokhoven, Veronique Van Speybroeck, Shen Ye, T. Daniel Crawford, Martin T. Zanni, Gregory V. Hartland, Joan-Emma Shea
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Editorial Material
Chemistry, Physical
Anastassia N. Alexandrova, Julie S. Biteen, Sonia Coriani, Franz M. Geiger, Andrew A. Gewirth, Gillian R. Goward, Hua Guo, Libai Huang, Jian-Feng Li, Tim Liedl, Stephan Link, Zhi-Pan Liu, Sudipta Maiti, Andrew J. Orr-Ewing, David L. Osborn, Jim Pfaendtner, Benoit Roux, Friederike Schmid, J. R. Schmidt, William F. Schneider, Lyudmila V. Slipchenko, Gemma C. Solomon, Jeroen A. van Bokhoven, Veronique Van Speybroeck, Shen Ye, T. Daniel Crawford, Martin T. Zanni, Gregory V. Hartland, Joan-Emma Shea
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Editorial Material
Chemistry, Physical
Anastassia N. Alexandrova, Julie S. Biteen, Sonia Coriani, Franz M. Geiger, Andrew A. Gewirth, Gillian R. Goward, Hua Guo, Libai Huang, Jian-Feng Li, Tim Liedl, Stephan Link, Zhi-Pan Liu, Sudipta Maiti, Andrew J. Orr-Ewing, David L. Osborn, Jim Pfaendtner, Benoit Roux, Friederike Schmid, J. R. Schmidt, William F. Schneider, Lyudmila V. Slipchenko, Gemma C. Solomon, Jeroen A. van Bokhoven, Veronique Van Speybroeck, Shen Ye, T. Daniel Crawford, Martin T. Zanni, Gregory V. Hartland, Joan-Emma Shea
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
