Article
Chemistry, Multidisciplinary
Seif Alwan, Yonatan Dubi
Summary: This study presents a theory for the CISS effect based on the interplay between spin-orbit interactions in the electrode, the chirality of the molecule, and spin-transfer torque at the molecule-electrode interface. The theory can qualitatively account for key experimental observations and provides a set of predictions that can be readily tested experimentally.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Yuki Sakai, Kana Matsuno, Takumi Nishikubo, Masayuki Fukuda, Shogo Wakazaki, Masahito Ikeda, Kazuki Takahashi, Zhao Pan, Lei Hu, Masaki Azuma
Summary: Two different mechanisms of negative thermal expansion (NTE) were observed in the solid solutions of perovskite-type oxides PbCrO3 and PbTiO3. For x <= 0.6, PbCr1-xTixO3 adopted a cubic structure similar to that of PbCrO3, while for x >= 0.7 a PbTiO3-type tetragonal structure was observed. The NTE observed at x <= 0.6 was caused by a cubic-to-cubic phase transition related to the rearrangement of Pb2+/Pb4+ in a charge glass structure. Despite the absence of intermetallic charge transfer, PbCrO3 exhibited a significant volume shrinkage of -2.5%. The NTE in the tetragonal phase was due to a ferroelectric-to-paraelectric phase transition, the same as in PbTiO3. By substituting Cr, the working temperature of PbTiO3 as an NTE material was effectively lowered while maintaining a large volume shrinkage of 0.6%.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Luming Yang, Julius J. Oppenheim, Mircea Dinca
Summary: This study discovered a new radical-bearing compound that can be used as a building block for molecule-based magnetic materials, and successfully achieved strong radical-mediated magnetic coupling.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Physical
Linyang Wang, Jiamin Sun, Maojun Deng, Chunhui Liu, Servet Ataberk Cayan, Korneel Molkens, Pieter Geiregat, Rino Morent, Nathalie De Geyter, Jeet Chakraborty, Pascal Van Der Voort
Summary: This study introduces two benzothiadiazole-based COFs with tunable electronic structures and electron affinities for photocatalytic H2O2 production. The triazine-containing TAPT-BT-COF exhibits outstanding charge separation and achieves high H2O2 production rate in pure water.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Physics, Multidisciplinary
X. Li, L. Inhester, S. J. Robatjazi, B. Erk, R. Boll, K. Hanasaki, K. Toyota, Y. Hao, C. Bomme, B. Rudek, L. Foucar, S. H. Southworth, C. S. Lehmann, B. Kraessig, T. Marchenko, M. Simon, K. Ueda, K. R. Ferguson, M. Bucher, T. Gorkhover, S. Carron, R. Alonso-Mori, J. E. Koglin, J. Correa, G. J. Williams, S. Boutet, L. Young, C. Bostedt, S. -K. Son, R. Santra, D. Rolles, A. Rudenko
Summary: The interaction between intense femtosecond x-ray pulses and molecules depends on a complex interplay of processes including multiple photoabsorptions, Auger decay, charge rearrangement, and nuclear motion. Experimental and theoretical studies on ionization and fragmentation of iodomethane demonstrate that the timing of ionization steps leading to specific reaction products is determined by pulse duration rather than energy or intensity. Short pulse durations enhance the yield of fragments with higher charge states, attributed to decreased charge transfer efficiency at larger internuclear separations during longer pulses.
PHYSICAL REVIEW LETTERS
(2021)
Article
Chemistry, Physical
Kelly M. Kopera, Harrison G. Tuckman, Grayson R. Hoy, Kristin L. Wustholz
Summary: In this study, factors influencing dispersive electron transfer kinetics in eosin-sensitized TiO2 were investigated by removing ensemble averaging and molecular aggregation effects. Statistical analysis revealed that the blinking dynamics of single eosin Y chromophores are best fit to lognormal distributions, and Monte Carlo simulations based on the Albery model successfully replicated this behavior. These findings suggest that both environmental heterogeneity and injection from multiple excited states play significant roles in governing kinetic dispersion in this system.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Multidisciplinary
Sheng Zhu, Xiaoxin Yang, Yixi Yao, Xinrui Zhang, Lan Li, Xiao Wang, Gaoyi Han, Yan Li
Summary: Carbon nanotubes are used to encapsulate and enhance the electrical properties of redox-active polyoxometalate molecular clusters, resulting in improved dispersion and capacity. This hybrid material achieves a high specific capacity of 328.6 F g(-1) at 10 mV s(-1) and retains 82.1% capacity at 500 mV s(-1). The assembled supercapacitor exhibits a maximum energy density of 33.4 Wh kg(-1) and long-term stability with 91.3% capacity retention over 10,000 cycles. This study highlights the potential of redox-driven encapsulation strategies in developing high-performance energy storage materials.
CELL REPORTS PHYSICAL SCIENCE
(2023)
Article
Chemistry, Applied
Muhammad Qasim, Maochang Liu, Liejin Guo
Summary: In this study, a P-doped-g-C3N4/Fe2P/red-P ternary composite was constructed through in-situ phosphorization of a Fe2O3@C/g-C3N4 heterojunction. The as-prepared composite exhibited significantly improved photocatalytic activity for pure water splitting under visible light irradiation without the need for noble metal additives. The optimized composite, containing 15 wt% Fe2P, showed the highest activity with a hydrogen production rate 107 and 39 times higher than that of pristine g-C3N4 and P-doped g-C3N4 respectively. Furthermore, this noble-metal-free photocatalyst achieved a solar-to-hydrogen conversion efficiency of about 0.2%.
Article
Chemistry, Physical
Yiqin Gong, Jianhua Shen, Yihua Zhu, Wei Yan, Jingrun Zhu, Lu Hou, Delong Xie, Chunzhong Li
Summary: In this study, short-chain conductive aromatic molecules were used to modify CsPbBr3 quantum dots and act as charge mediators for photocatalytic CO2 reduction, demonstrating higher potential than long-chain alkane or siloxane compounds. The electron consumption rate of the composite photocatalyst with aromatic mediators was significantly higher compared to alkane and siloxane ligands.
APPLIED SURFACE SCIENCE
(2021)
Article
Multidisciplinary Sciences
Jun Huang, Yanxia Chen, Michael Eikerling
Summary: This paper reveals that the surface-charging behaviors of the electrodes in an electrochemical cell are not independently described by their electric double-layer properties. Instead, they are correlated and determined by the electric double-layer and reaction kinetics of both electrodes. Two fundamental equations are derived to describe the correlated surface-charging behaviors, and approximate analytical solutions are provided for low and high current densities for better understanding. The implications of this conceptual analysis for theoretical and computational electrochemistry are discussed, and a strategy to modulate the activity of one electrode by tuning the electric double-layer parameters of the other electrode in a two-electrode electrochemical cell is demonstrated.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Chemistry, Medicinal
Jiali Guo, Ming Sun, Xueyan Zhao, Chaojie Shi, Haoming Su, Yanzhi Guo, Xuemei Pu
Summary: This study develops a graph neural network (GNN)-based deep learning framework to accurately predict the cocrystal density. The research considers three key factors of machine learning and finds that the stoichiometric ratios of molecules in cocrystals significantly influence prediction performances. Additionally, the complementarity of features is not suitable for enhancing molecular graph representation in cocrystal density prediction.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2023)
Article
Chemistry, Multidisciplinary
Yin Zhang, Xiang Lian, Wei Si, Jingjie Sha, Yunfei Chen
Summary: Understanding the origin of ionic conductance modulation in nanopore sensors is crucial for precise measurement of analytes on a single molecule level. Previous models focused on high ionic strength based on geometry and independent of applied voltage. However, our numerical simulations reveal that both electroosmotic flow and ionic concentration polarization are influenced by applied voltage, affecting ionic conductance. DNA translocation enhances the effects, resulting in voltage-dependent conductance blockades. These findings provide valuable insights for nanopore sensor design.
MATERIALS CHEMISTRY FRONTIERS
(2023)
Review
Chemistry, Applied
Vivek Anand, Roli Mishra, Yash Barot
Summary: This review discusses recent significant achievements in the field of white light emission through the application of pure organic molecules, addressing challenges and exploring novel synthetic and energy transfer approaches to overcome efficiency limitations.
Article
Chemistry, Physical
Rui Xia, Kangning Zhao, Jie Zheng, Tao Shen, Lei Zhang, Mark Huijben, Johan ten Elshof
Summary: Fast charging performance of electrode materials is crucial for batteries in portable devices and electric vehicles. This study proposes a new theoretical framework that can decouple the impacts of ohmic resistance, reaction rate, and ion diffusion on the fast charging properties of electrodes. The model is successfully validated using cyclic voltammetry data of four typical electrode materials. Surprisingly, it is found that the reaction rate is the limiting factor for the fast charging performance in all materials analyzed. The new model is believed to facilitate electrode design and accelerate the development of the next generations of fast-charging batteries.
ENERGY STORAGE MATERIALS
(2022)
Article
Chemistry, Applied
Qingfeng Zhai, Zhenhai Xia, Liming Dai
Summary: This review article discusses the recent advances in carbon-based metal-free electrocatalysts (C-MFECs) and how various strategies, such as heteroatom doping, defect doping, and molecular modification, can induce catalytic active sites to create efficient and multifunctional electrocatalysts. Theoretical research has shown that the catalytic activity in C-MFECs originates from the charge/spin redistributions induced by the change in electronic structures of doped carbon materials. The progress in the unified mechanistic understanding and the challenges and future perspectives in this field are also presented.
Article
Virology
Michaela Prochazkova, Tibor Fuzik, Danyil Grybchuk, Francesco Luca Falginella, Lucie Podesvova, Vyacheslav Yurchenko, Robert Vacha, Pavel Plevka
Summary: Leishmania parasites carrying Leishmania RNA virus 1 (LRV1) are more likely to cause severe disease, and the structure of the LRV1 capsid provides insights for developing new treatments.
JOURNAL OF VIROLOGY
(2021)
Article
Multidisciplinary Sciences
Miroslav Jurasek, Jitender Kumar, Petra Paclikova, Alka Kumari, Konstantinos Tripsianes, Vitezslav Bryja, Robert Vacha
Summary: The study investigated the impact of phosphorylation on the Dishevelled 3 protein's PDZ domain, revealing three major roles of phosphorylation: acting as a switch, affecting the binding groove conformation, and influencing the secondary binding site. The effects of phosphorylation were found to be non-additive and could potentially elucidate regulatory mechanisms in other PDZ domains.
SCIENTIFIC REPORTS
(2021)
Article
Multidisciplinary Sciences
Karel Skubnik, Lukas Sukenik, David Buchta, Tibor Fuzik, Michaela Prochazkova, Jana Moravcova, Lenka Smerdova, Antonin Pridal, Robert Vacha, Pavel Plevka
Summary: The Iflaviridae family consists of economically important viruses affecting western honeybees. These viruses induce genome release through conformational changes triggered by acidic pH, with different mechanisms for releasing genomes from their capsids.
Article
Chemistry, Medicinal
Ivo Kabelka, Radim Brozek, Robert Vacha
Summary: The study developed a new collective variable (CV) that accurately describes peptides translocating across membranes, incorporating peptide insertion, local membrane deformation, and peptide internal degrees of freedom related to its charged groups. By comparing different CVs and evaluating three common methods for free-energy calculations, the study showed that all of these components are necessary for an accurate description of peptide translocation. The developed CV allows for reliable and effective calculation of the free energy of peptide translocation, which could be useful in designing spontaneously translocating peptides.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2021)
Article
Chemistry, Physical
Man Thi Hong Nguyen, Ondrej Tichacek, Hector Martinez-Seara, Philip E. Mason, Pavel Jungwirth
Summary: The experiment observed that there are practically identical number densities in solutions of lithium and sodium chloride at equal molalities, which is attributed to the similar hydration and hydrogen bonding of Li+ and Na+ in the solution. On the other hand, the regular behavior of number density differences between NaCl and KCl solutions, as well as between LiCl and KCl solutions, showed lower number densities for larger cations.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Chemistry, Multidisciplinary
Yunfeng Hu, Phonemany Ounkham, Ondrej Marsalek, Thomas E. Markland, Bala Krishmoorthy, Aurora E. Clark
Summary: Nuclear quantum effects impact chemical reactivity and physicochemical properties, with shape metrics for ring polymers providing insight into atomic delocalization. Computational topology, specifically persistent homology, is used to describe the ensemble of shapes adopted by ring polymers. Wasserstein distances of Betti sequences in time characterize shape fluctuations, allowing for differentiation of atoms with different NQEs based on their dynamic properties.
FRONTIERS IN CHEMISTRY
(2021)
Article
Chemistry, Physical
Victor Cruces Chamorro, Carmelo Tempra, Pavel Jungwirth
Summary: This study investigates the small differences between heavy water and normal water, as well as the impact of zero-point vibrations on their physical and chemical properties, developing two classical molecular dynamics water models. These models accurately reproduce the differences in properties of water isotopes and can be used to simulate the behavior of biomolecules in heavy water.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Biology
Natalie Ben Abu, Philip E. Mason, Hadar Klein, Nitzan Dubovski, Yaron Ben Shoshan-Galeczki, Einav Malach, Veronika Prazienkova, Lenka Maletinska, Carmelo Tempra, Victor Cruces Chamorro, Josef Cvacka, Maik Behrens, Masha Y. Niv, Pavel Jungwirth
Summary: This study demonstrates that humans can distinguish heavy water from normal water by taste, with heavy water having a sweeter taste to humans but not to mice. Mechanistically, the sweet taste of heavy water is mediated by the human TAS1R2/TAS1R3 taste receptor.
COMMUNICATIONS BIOLOGY
(2021)
Article
Chemistry, Multidisciplinary
Ales Cahlik, Jack Hellerstedt, Jesus Mendieta-Moreno, Martin Svec, Vijai M. Santhini, Simon Pascal, Diego Soler-Polo, Sigurdur Erlingsson, Karel Vyborny, Pingo Mutombo, Ondrej Marsalek, Olivier Siri, Pavel Jelinek
Summary: In hydrogen-bonded systems, nuclear quantum effects have a significant impact on the material properties by enhancing the mechanical stability of molecular chains and creating distinctive electronic states. This offers opportunities for deeper understanding and utilization of these systems.
Article
Biochemistry & Molecular Biology
Ella Doron-Mandel, Indrek Koppel, Ofri Abraham, Ida Rishal, Terika P. Smith, Courtney N. Buchanan, Pabitra K. Sahoo, Jan Kadlec, Juan A. Oses-Prieto, Riki Kawaguchi, Stefanie Alber, Eitan Erez Zahavi, Pierluigi Di Matteo, Agostina Di Pizio, Didi-Andreas Song, Nataliya Okladnikov, Dalia Gordon, Shifra Ben-Dor, Rebecca Haffner-Krausz, Giovanni Coppola, Alma L. Burlingame, Pavel Jungwirth, Jeffery L. Twiss, Mike Fainzilber
Summary: Nucleolin is a multifunctional RNA Binding Protein (RBP) that can be found in various subcellular locations thanks to its glycine arginine rich (GAR) domain. This domain is responsible for driving subcellular localization through protein-protein interactions and mediating interactions with the plasma membrane. Additionally, the GAR domain plays a crucial role in nucleolin transport to axons and growth control of sensory neurons.
Article
Chemistry, Physical
Matti Javanainen, Hector Martinez-Seara, Christopher Kelly, Pavel Jungwirth, Balazs Fabian
Summary: Single-particle tracking experiments provide valuable information about the properties of biomembranes, revealing deviations from ideal Brownian motion such as confinement effects and anomalous diffusion. With advancements in experimental methods, anisotropic diffusion has the potential to play a significant role in understanding membrane structure and topology.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Vojtech Kostal, Krystof Brezina, Ondrej Marsalek, Pavel Jungwirth
Summary: Research on the benzene radical anion shows its intriguing properties as a metastable shape resonance in the gas phase, while being experimentally detectable and stable in solution, with solvation leading to stabilization. Explicit ionization calculations reveal the transition of the benzene radical anion from an unstable gas-phase ion to a completely solvated bound species.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Physical
Krystof Brezina, Vojtech Kostal, Pavel Jungwirth, Ondrej Marsalek
Summary: The study reveals the correspondence between the electronic and geometric structures of the benzene radical anion solvated in liquid ammonia, showing that the spatial character of the excess electron follows the Jahn-Teller distortions. Furthermore, decomposing the electronic density of states aids in understanding the contributions of the solute and the response of the solvent.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
H. Christian Schewe, Krystof Brezina, Vojtech Kostal, Philip E. Mason, Tillmann Buttersack, Dominik M. Stemer, Robert Seidel, Wilson Quevedo, Florian Trinter, Bernd Winter, Pavel Jungwirth
Summary: Valence band photoelectron spectroscopy measurements and electronic structure calculations were used to characterize the shifts in electron binding energies of benzene from gas to liquid phase, with the Born-Haber solvation model providing quantification. Despite the difference in polarity between liquid ammonia and benzene, the shifts were primarily determined by the electronic polarization response determined by the high frequency dielectric constant of the solvent.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)