Article
Physics, Fluids & Plasmas
Shuai Zhang, Valentin V. Karasiev, Nathaniel Shaffer, Deyan I. Mihaylov, Katarina Nichols, Reetam Paul, R. M. N. Goshadze, Maitrayee Ghosh, Joshua Hinz, Reuben Epstein, Stefan Goedecker, S. X. Hu
Summary: In this study, a wide-range equation-of-state (EOS) table for a CH1.72O0.37N0.086 quaternary compound was constructed using density-functional theory molecular-dynamics calculations. The results show that the compression ratio of the C-H-O-N resin is larger than that of CH polystyrene due to the presence of oxygen and nitrogen. However, other properties are similar between CHON and CH. Furthermore, radiation hydrodynamic simulations show that CHON outperforms CH as the ablator for laser-direct-drive target designs.
Article
Chemistry, Physical
Baonan Jia, Feng Wei, Jinbo Hao, Zhengqin Zhao, Jiankang Peng, Ge Wu, Chunling Zhang, Xinhui Zhang, Gang Liu, Qi Zhang, Pengfei Lu
Summary: By using first-principles calculations, this study designed a defective MA(2)Z(4) monolayer family as highly efficient electrocatalysts for the HER. The study investigated their stability, electronic properties, and catalytic performance and found that vacancy regulation can enhance the catalytic activity. The study also demonstrated that the Volmer-Heyrovsky mechanism is preferred for the HER performance.
SUSTAINABLE ENERGY & FUELS
(2022)
Article
Chemistry, Physical
Mukesh Singh, Alok Shukla, Brahmananda Chakraborty
Summary: In this study, the hydrogen-storage properties of Zr-decorated g-graphyne monolayer were investigated using Density Functional Theory (DFT). The results predict that each Zr atom can adsorb up to seven H2 molecules with a hydrogen gravimetric density of 7.95 wt% and a desorption temperature of 574 K, making it suitable for fuel-cell applications. The strong attachment between decorated Zr atom and graphyne sheet is due to charge transfer, while hydrogen molecules adsorb on Zr decorated graphyne through Kubas type of interactions. The stability of Zr+g-graphyne was confirmed through ab-initio molecular dynamics simulations. Overall, these findings suggest that Zr functionalized on g-graphyne could be a promising solid-state hydrogen storage material.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Materials Science, Multidisciplinary
Haoran Zhu, Peixuan Liu, Xu Zuo, Bin Shao
Summary: This paper reveals that the antiferromagnetic ground state of CrOCl is determined by the competition of magnetic exchange interactions, and the adjustment of parameters can lead to the experimentally observed ground state.
Article
Physics, Multidisciplinary
Memoona Mehmood, Muhammad Nasir Rasul, Altaf Hussain, Muhammad Amir Rafiq, Muhammad Nadeem Khan, Faisal Iqbal
Summary: The crystal structure, electronic, bonding, and optical properties of monoclinic and trigonal phases of LiBaPO4 compound were investigated using density functional theory. The study revealed differences in the properties of the two phases, with the P-O bond showing the highest strength. Optical properties suggest that the trigonal phase may be suitable for photovoltaic applications.
Article
Physics, Applied
Yongchao Rao, C. Y. Zhao, Shenghong Ju
Summary: In this study, the thermal and electrical transport properties of diamond-cubic and metastable R8 phases of Si are comparatively studied. The results show that the metastable Si has lower lattice thermal conductivity and excellent electrical conductivity, leading to higher thermoelectric performance in n-type doping.
APPLIED PHYSICS LETTERS
(2022)
Article
Chemistry, Physical
Krishnamoorthy Arumugam, Ponnaih Ravindran
Summary: In this study, the magnetic properties of uranium monochalcogenides were investigated using density functional theory and various computational methods. The X-ray magnetic circular dichroism spectra were calculated and compared with experimental results. The effects of the Hubbard parameter on uranium's 5f electrons were also examined.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Meijuan Cheng, Xiaohong Shi, Shunqing Wu, Zi-Zhong Zhu
Summary: By performing first-principles calculations, the study investigated the linear and nonlinear optical properties of one-dimensional selenium and tellurium, and found that both materials exhibit significant linear and nonlinear optical responses. Selenium has a large second-harmonic generation coefficient, while tellurium shows a large linear electro-optic coefficient and shift current response.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Materials Science, Multidisciplinary
Jing Liu, Yuanchang Li
Summary: This study proposes a new design concept based on the unique feature of an excitonic insulator, negative exciton transition energy (E-t). Through first-principles calculations and experiments on one-dimensional organometallic wire, the viability of this concept is demonstrated. Substitutional doping allows for tuning the photon detection ability, providing wavelength selectivity, reduced thermal disturbance, and increased working temperature.
Article
Chemistry, Inorganic & Nuclear
Sung-Min Hyun, Kaleb A. Reid, Shaik Waseem Vali, Paul A. Lindahl, David C. Powers
Summary: This study describes a series of truncated 2-pyridylpyrrolide ligands that support mono- and binuclear Fe(II) complexes with a rare cis-divacant octahedral (CDO) geometry. These synthetic studies provide the structural basis to explore the implications of CDO geometry on Fe-catalyzed reactions.
INORGANIC CHEMISTRY
(2021)
Article
Materials Science, Multidisciplinary
Anatoly B. B. Belonoshko, Grigory S. S. Smirnov
Summary: Iron is the main component of Earth's core and exoplanetary cores. The crystal structure of iron under extreme conditions of high pressure and temperature is still unknown. Experimental data and simulations have contradictory results regarding the stability of different phases of iron. By using large-scale ab initio molecular dynamics simulations, this study compared the properties of iron phases at experimental conditions to provide a potential explanation for the experimental observations.
Article
Materials Science, Multidisciplinary
Alejandro Lopez-Bezanilla
Summary: Design principles are used to create dynamically stable transition metal, lanthanide, and actinide-based low-dimensional borides, predicting complex covalent heterostructures hosting Dirac states. Layered borides can be stacked in a layer-by-layer fashion to explore new physical properties and materials, with multiple Dirac states, highly dispersive electronic bands, and decoupled acoustic-optical phonon branches being studied.
PHYSICAL REVIEW MATERIALS
(2021)
Article
Materials Science, Multidisciplinary
Luis E. Gonzalez, David J. Gonzalez
Summary: The static and dynamic properties of several bulk liquid 4d transition metals near their respective melting points have been evaluated using ab-initio molecular dynamics simulations. The results demonstrate the existence of ordered structures and special collective excitations, and further study several transport coefficients.
INTERNATIONAL JOURNAL OF REFRACTORY METALS & HARD MATERIALS
(2022)
Article
Physics, Condensed Matter
Chongyang Fu, Weiqi Li, Chongyang Zeng, Le Zhang, Zeen Liu, Xiao Wu, Xiaojuan Ma
Summary: This study investigated the structural, electronic, and mechanical properties of the FeH binary compound under a pressure range of 0-300 GPa using first-principles calculations. It was found that FeH is stable within this pressure range based on mechanically stable criteria and phonon spectra. The study analyzed the electronic properties and observed metallic behavior under extreme pressure. Additionally, the study examined the elastic constants, bulk modulus, shear modulus, Vickers hardness, and Young's modulus, which were found to increase with pressure.
SOLID STATE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Junyi Liu, Xu Zhang, Gang Lu
Summary: In this work, the excited state dynamics in a WS2/graphene heterostructure are investigated through first-principles calculations, providing insights into the charge and energy transfer mechanisms. It is found that charge transfer is primarily driven by interlayer Auger-like processes due to strong electron-hole interactions, rather than direct interlayer excitations. The electron-phonon coupling is unable to compete with Auger processes due to phonon bottleneck. Additionally, the asymmetrical dynamics are attributed to the difference in density of states of the heterostructure.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Robert Izsak, Christoph Riplinger, Nick S. Blunt, Bernardo de Souza, Nicole Holzmann, Ophelia Crawford, Joan Camps, Frank Neese, Patrick Schopf
Summary: Quantum computers are expected to be useful in simulating strongly correlated chemical systems, but careful selection of orbital spaces is crucial. This study presents a scheme for automatically selecting an active space and combines quantum phase estimation and variational quantum eigensolver algorithms to accurately describe the environment. The protocol outlined here can be applied to chemical systems of any size, including those beyond the capabilities of classical computation.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Frank Neese
Summary: This paper describes the SHARK integral generation and digestion engine, which is based on the McMurchie/Davidson approach and utilizes an efficient BLAS algorithm. SHARK can handle various types of basis function integrals and features programming constructs that simplify workflows and avoid code duplication.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Bastiaan Kooij, Paul Varava, Farzaneh Fadaei-Tirani, Rosario Scopelliti, Dimitrios A. Pantazis, Gerard P. Van Trieste, David C. Powers, Kay Severin
Summary: In this study, we report the structural characterization of copper complexes with both bridging and terminal alkenylidene ligands. The complexes were obtained by irradiation of Cu-I complexes with N-heterocyclic diazoolefin ligands. The isolation and structural characterization of the complex with a terminal alkenylidene ligand were achieved through crystalline matrix isolation and in crystallo photolysis at low temperature.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Inorganic & Nuclear
Sofia Tzani, Michael Pissas, Vassilis Psycharis, Dimitrios A. Pantazis, Yiannis Sanakis, Catherine P. Raptopoulou
Summary: Two complexes were obtained by the reaction of methyl-2-pyridyl ketone with FeCl3.6H(2)O in various solvents. The molecular structures and physical properties of the two complexes are different.
DALTON TRANSACTIONS
(2023)
Article
Biochemistry & Molecular Biology
Anthony John Pastore, Alvaro Montoya, Manasi Kamat, Kari B. Basso, James S. Italia, Abhishek Chatterjee, Maria Drosou, Dimitrios A. Pantazis, Alexander Angerhofer
Summary: Oxalate decarboxylase is an acid stress response enzyme that converts oxalic acid into formate and carbon dioxide. The enzyme relies on binuclear Mn and long-range electron transfer facilitated by pi-stacked tryptophan dimers. Substituting one of the tryptophan residues with 5-hydroxytryptophan hinders electron transfer and suppresses enzymatic activity.
Article
Chemistry, Multidisciplinary
Matteo Capone, Abhishek Sirohiwal, Massimiliano Aschi, Dimitrios A. Pantazis, Isabella Daidone
Summary: Photosystem-II (PSII) is a multi-subunit protein complex that performs oxygenic photosynthesis by harvesting sunlight. Studying the processes following light excitation has been challenging due to spectral congestion, ultrafast nature, and multi-component behavior. Using advanced computational multiscale approaches, researchers have identified two possible primary pathways to radical-pair formation, with significantly different kinetics. The dominant pathway is fast (short-range), but the existence of a slower (long-range) alternative pathway suggests the evolution of redundancy for other purposes related to the formation of oxidative species in PSII that drives water oxidation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Yang Guo, Fabijan Pavosevic, Kantharuban Sivalingam, Ute Becker, Edward F. F. Valeev, Frank Neese
Summary: In this work, a linear scaling explicitly correlated N-electron valence state perturbation theory (NEVPT2-F12) is developed to reduce the computational scaling of the conventional NEVPT2-F12 to near-linear scaling using the idea of a domain-based local pair natural orbital (DLPNO). The excitation energies predicted by DLPNO-NEVPT2-F12 are as accurate as the exact NEVPT2-F12 results for low-lying excited states of organic molecules. The new algorithm is applied to study cluster models of rhodopsin and can handle systems with large basis functions and active spaces.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Maria Drosou, Gerard Comas-Vila, Frank Neese, Pedro Salvador, Dimitrios A. . Pantazis
Summary: Recent advancements in serial femtosecond crystallography have provided geometric models of distinct intermediates in the catalytic S-state cycle of the oxygen-evolving complex (OEC). However, the interpretation of these models is controversial due to discrepancies in the Mn4CaO5 cluster of the OEC.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Review
Chemistry, Multidisciplinary
Abhishek Sirohiwal, Dimitrios A. Pantazis
Summary: In this paper, the authors highlight the importance of quantum-chemistry based excited-state computations and large-scale molecular dynamics simulations in understanding the primary events of oxygenic photosynthesis. The research reveals the mechanism of charge separation in the primary enzyme of oxygenic photosynthesis and provides insights into the factors that enable photosynthesis beyond the red limit.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Simon L. Schumann, Simon Kotnig, Yury Kutin, Maria Drosou, Lukas M. Stratmann, Yana Streltsova, Alexander Schnegg, Dimitrios A. Pantazis, Guido H. Clever, Muege Kasanmascheff
Summary: In this study, the structure and conformational flexibility of a unimolecular GQ were investigated using electron-nuclear double resonance (ENDOR) experiments combined with Cu(II) and fluorine labeling. The successful application of the 19F-ENDOR methodology at 34 GHz overcame the limitations of higher-frequency spectrometers, providing both sensitivity and orientational resolution. This integrated study enhances our understanding of GQs and expands the methodological toolbox for studying other macromolecules.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Biochemistry & Molecular Biology
Ioannis Stylianakis, Nikolaos Zervos, Jenn-Huei Lii, Dimitrios A. Pantazis, Antonios Kolocouris
Summary: We conducted a study on 145 reference organic molecules used in computer-aided drug design. By using various force fields and computational methods, we calculated the conformational energies and barriers of these molecules. The results provide valuable insights into the stability of different conformers and can be utilized in drug design projects.
JOURNAL OF COMPUTER-AIDED MOLECULAR DESIGN
(2023)
Article
Chemistry, Multidisciplinary
Sinjini Bhattacharjee, Frank Neese, Dimitrios A. Pantazis
Summary: In this study, the triplet states within the Photosystem II reaction center (RC) were investigated using a multiscale quantum-mechanics/molecular-mechanics approach. The low-energy spectrum of excited singlet and triplet states, their properties, and the electrostatic modulation by the semiquinone Q(A)(-) were analyzed. The results provide a detailed understanding of the triplet states in the RC and contribute to the discussion on electron transfer, charge recombination, and photoprotection mechanisms in Photosystem II.
Article
Chemistry, Multidisciplinary
Maria Chrysina, Maria Drosou, Rebeca G. Castillo, Michael Reus, Frank Neese, Vera Krewald, Dimitrios A. Pantazis, Serena Debeer
Summary: This research investigates the water splitting enzyme in Photosystem II using high-energy resolution fluorescence detected X-ray absorption spectroscopy. By combining quantum chemical calculations and experimental data analysis, the geometric and electronic structures of different catalytic intermediates are determined, ruling out the presence of peroxo or oxyl radicals.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Ingolf Harden, Frank Neese, Giovanni Bistoni
Summary: This study investigates the aggregation process of chiral organocatalysts derived from phosphoric acids using high-level quantum mechanical calculations. The results show that the formation of catalyst dimers is possible and the aggregation process can significantly affect the stereo-controlling factors, reaction kinetics, and selectivity of the transformations.
Article
Chemistry, Multidisciplinary
Ingolf Harden, Frank Neese, Giovanni Bistoni
Summary: The formation of Bronsted acid aggregates in asymmetric organocatalytic reactions has a significant impact on the stereo-controlling factors of the transformations. This study uses high-level quantum mechanical calculations to investigate the influence of catalyst structure and reaction conditions on the spontaneity of the aggregation process, shedding light on its importance.