Article
Chemistry, Physical
Kai Guther, Aron J. Cohen, Hongjun Luo, Ali Alavi
Summary: In this study, the application of similarity-transformed full configuration interaction quantum Monte Carlo based on the transcorrelated Hamiltonian in predicting the binding curve of the beryllium dimer has been demonstrated. By effectively addressing dynamic correlation beyond the basis set, accurate energies close to the complete basis set limit can be obtained with moderate basis sets and computational effort. The role of the Jastrow factor, its functional form, and potential sources for size consistency errors are discussed, leading to Jastrow forms that allow for high accuracy calculations of the vibrational spectrum of the beryllium dimer.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Ke Wang, Zhaoxuan Xie, Zhen Luo, Haibo Ma
Summary: The researchers have developed an automatic and efficient scheme for accurately constructing the bases for excitonic models, enabling black-box excited state structure calculations for large molecular systems. They introduced a new framework called block interaction product state (BIPS), where the bases are expressed as direct products of local states for each chromophore. Test calculations demonstrated that the BIPS framework accurately describes not only the excitation energies but also the properties of the low-lying excited states at a low computational cost.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Mechanics
Tie Wei, Daniel Livescu, Xiaofeng Liu
Summary: The study investigates the appropriate scales in planar turbulent wakes using a scaling patch approach. Proper scales for mean axial flow, mean transverse flow, and Reynolds shear stress are identified, and it is revealed that mean transverse flow plays an important role in the scaling and understanding of planar turbulent wakes.
Article
Chemistry, Physical
Soumi Haldar, Tamoghna Mukhopadhyay, Achintya Kumar Dutta
Summary: The article presents a novel and cost-effective approach to improve the CC2 model by using a second similarity transformation of the Hamiltonian to include higher-order terms. The newly developed ST-EOM-CC2 model shows significant improvement in excitation energies of Rydberg and charge-transfer excited states while retaining good performance for valence excited states.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Iryna Knysh, Jose D. J. Villalobos-Castro, Ivan Duchemin, Xavier Blase, Denis Jacquemin
Summary: The change of molecular dipole moment induced by photon absorption is important for interpreting optical spectra. While time-dependent density functional theory (TD-DFT) is commonly used to predict excited-state dipoles (mu(ES)), this study shows that the many-body Green's function Bethe-Salpeter equation (BSE) is a valuable alternative with decreased dependency on exchange-correlation functional. The BSE method is not only suitable for transition energies and oscillator strengths, but also for properties related to the excited-state density.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Zohreh Hashemi, Linn Leppert
Summary: In this study, the electronic structure and optical excitations of bacteriochlorophylls and chlorophylls were calculated using the GW+BSE method, showing excellent agreement with experimental data and overcoming some limitations of the TDDFT method.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Multidisciplinary
Hao Zhou, Ya-Juan Feng, Chao Wang, Teng Huang, Yi-Rong Liu, Shuai Jiang, Chun-Yu Wang, Wei Huang
Summary: Water, the most important molecule on Earth, presents challenges in identifying its precise microscopic structures, which can be addressed using a machine-learning water model for water nanoclusters. This model efficiently predicts structures and simulates vibrational spectra to verify atomic structures.
Article
Mathematics, Interdisciplinary Applications
Mohamed Guedda, Krisztian Hriczo, Laila Taourirte, Jihade Chaiboub, Gabriella Bognar
Summary: This paper explores a scale invariance theory through the study of a specific equation for coarsening of growing interfaces, demonstrating perpetual coarsening process and spatial periodic solutions. The findings provide detailed insights into the growth laws of interfacial width and mound lateral size, with analytical contributions aligning with previous results.
CHAOS SOLITONS & FRACTALS
(2022)
Article
Chemistry, Physical
Ashutosh Kumar, Ayush Asthana, Conner Masteran, Edward F. Vleev, Yu Zhang, Lukasz Cincio, Sergei Tretiak, Pavel A. Dub
Summary: This paper attempts to reduce the quantum resource requirements for molecular simulations on quantum computers while maintaining the desired accuracy. By using compact and balanced transcorrelated Hamiltonians to describe both the ground and excited states of molecular systems, and employing the VQE method and qEOM formalism, the number of required quantum gates and the deviations in excitation energies can be greatly reduced.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Engineering, Civil
Christian Malaga-Chuquitaype
Summary: This paper examines the seismic response scaling of degrading and non-degrading eccentric structures subjected to bidirectional earthquake action, finding that the duration of ground motion plays a fundamental role in defining the peak displacement response of structures. The study also highlights the significant impact of degradation on the structural response, as well as the emergence of self-similar response when orientationally consistent dimensionless parameters are selected.
EARTHQUAKE ENGINEERING & STRUCTURAL DYNAMICS
(2021)
Article
Chemistry, Physical
Jan Wilhelm, Patrick Seewald, Dorothea Golze
Summary: GW is an accurate method for computing electron addition and removal energies, but its conventional implementation has high computational cost, limiting its application to many systems. A low-scaling GW algorithm with improved accuracy was presented, demonstrating strong size-dependent variation in the fundamental gap of phosphorene nanosheets when applied.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Chemistry, Physical
Oliver J. Backhouse, Alejandro Santana-Bonilla, George H. Booth
Summary: The study demonstrates an efficient computational method based on fully self-consistent many-body perturbation theory for calculating the entire single-particle spectrum of correlated molecules. This method is capable of accurately characterizing spectral properties and has been successfully applied to resolving discrepancies in previous works on the antimalarial drug artemisinin.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Guilin Shen, Minggang Guo, Zhifan Wang, Fan Wang
Summary: Experimental excitation energies (EEs) of uranyl halides are relatively independent of the type of equatorial ligands, but the ligands have a significant effect on the electronic structure of uranyl. This study compares the EEs of uranyl chlorides and fluorides, finding that the number of ligands has a more pronounced effect on EEs than the type of ligands.
INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY
(2022)
Article
Engineering, Industrial
Rui Cong Gu, Yao Jiang, Yu Wei Liu, Ying Liu, Fan Liu, Jing Tao Wang
Summary: The size effect in equal-channel angular pressing (ECAP) was systematically investigated, showing stable and consistent microstructure recovery and mechanical property softening upon scaling up. Theoretical analyses indicated that the size effect in ECAP is inherently rooted in the laws of thermal physics.
JOURNAL OF MATERIALS PROCESSING TECHNOLOGY
(2021)
Article
Meteorology & Atmospheric Sciences
Baofeng Jiao, Lingkun Ran, Na Li, Ren Cai, Tao Qu, Yushu Zhou
Summary: Research on vertical motion in mesoscale systems is challenging, and a new form of generalized equations for vertical motion (Q(z)) and Omega (Q(p)) are derived. Analysis of a heavy rain event in southern Xinjiang shows that both Q(z) and Q(p) are closely related to radar reflectivity, vertical motion, and precipitation. Compared to classical quasigeostrophic and nongeostrophic Q vectors, Q(z) is more effective in indicating weak precipitation.
ADVANCES IN ATMOSPHERIC SCIENCES
(2023)
Article
Chemistry, Physical
Lucas Lang, Enrico Ravera, Giacomo Parigi, Claudio Luchinat, Frank Neese
Summary: This study elaborated on the derivation of the correct long-distance limit of pseudo-contact nuclear magnetic resonance chemical shifts from rigorous first-principles quantum mechanics, confirming the classical Kurland-McGarvey theory. The study also discussed the application of the point-dipole approximation (PDA) in approximate density functional theory and Hartree-Fock theories, and demonstrated how it is possible to overcome the previous assumption of a crude effective nuclear charge approximation by using the fully relativistic Dirac equation.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Rami Shafei, Dimitrios Maganas, Philipp Jean Strobel, Peter J. Schmidt, Wolfgang Schnick, Frank Neese
Summary: In this study, a computational protocol is developed to predict the absorption and emission spectral shapes of Eu2+-doped phosphors. The energy distribution and band shape of the emission spectrum are found to be related to the nature of the 4f-5d transitions in the absorption process. Simple descriptors are identified that show a strong correlation with the energy position and bandwidth of the experimental emission bands.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Frank Neese
Summary: The latest version 5.0 of the ORCA quantum chemistry program suite represents a significant improvement in performance, numerical robustness, functionality, and user friendliness.
WILEY INTERDISCIPLINARY REVIEWS-COMPUTATIONAL MOLECULAR SCIENCE
(2022)
Article
Chemistry, Physical
Nicolas O. Foglia, Dimitrios Maganas, Frank Neese
Summary: In this work, a time-dependent density functional theory (TD-DFT) scheme for computing optical spectroscopic properties in the framework of linearly and circularly polarized light is presented. The scheme can calculate absorption, circular dichroism, and magnetic circular dichroism spectra, and takes into account relativistic effects and random orientations of molecules.
JOURNAL OF CHEMICAL PHYSICS
(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)
Meeting Abstract
Biochemistry & Molecular Biology
Sinjini Bhattacharjee, Frank Neese, Dimitrios A. Pantazis
BIOCHIMICA ET BIOPHYSICA ACTA-BIOENERGETICS
(2022)
Article
Chemistry, Physical
Robert Izsak
Summary: A second quantized formulation for evaluating spin-dependent properties in the UHF basis is introduced in this article. The practical usage of this formulation is illustrated using the configuration interaction singles ansatz, and the results are compared to spin-restricted cases of the same ansatz. On a more tentative basis, the notion of quasi-spin-adaptation is also discussed, which ensures that the ansatz becomes spin-adapted as the unrestricted orbitals approach the restricted ones.
Article
Chemistry, Physical
Nick S. Blunt, Joan Camps, Ophelia Crawford, Robert Izsak, Sebastian Leontica, Arjun Mirani, Alexandra E. Moylett, Sam A. Scivier, Christoph Sunderhauf, Patrick Schopf, Jacob M. Taylor, Nicole Holzmann
Summary: Computational chemistry is crucial for the pharmaceutical industry, and quantum computing is a rapidly advancing technology that promises to revolutionize computational capabilities in chemical research. This article explores the potential applications of quantum computation in pharmaceutical problems, specifically in simulating molecules. The authors provide estimates of the quantum computational cost for simulating a protein-drug complex and highlight recent advancements in quantum algorithms that significantly reduce the required resources.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Robert Izsak, Aleksei V. Ivanov, Nick S. Blunt, Nicole Holzmann, Frank Neese
Summary: In this article, the different measures of electron correlation in wave function theory, density functional theory, and quantum information theory are briefly reviewed. The focus is then placed on a more traditional metric based on dominant weights in the full configuration solution and its behavior regarding the choice of N-electron and one-electron basis. The impact of symmetry is discussed, and the usefulness of distinguishing between determinants, configuration state functions, and configurations as reference functions is emphasized.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(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.
Article
Chemistry, Physical
M. Atanasov, N. Spiller, F. Neese
Summary: This study uses first principles calculations to simulate magnetic and spectroscopic data, providing an explanation for the stability of a mixed valence binuclear transition metal complex. The study also proposes a new model to interpret the magnetic behavior of the complex.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Andrew M. Teale, Trygve Helgaker, Andreas Savin, Carlo Adamo, Balint Aradi, Alexei Arbuznikov, Paul W. Ayers, Evert Jan Baerends, Vincenzo Barone, Patrizia Calaminici, Eric Cances, Emily A. Carter, Pratim Kumar Chattaraj, Henry Chermette, Ilaria Ciofini, T. Daniel Crawford, Frank De Proft, John F. Dobson, Claudia Draxl, Thomas Frauenheim, Emmanuel Fromager, Patricio Fuentealba, Laura Gagliardi, Giulia Galli, Jiali Gao, Paul Geerlings, Nikitas Gidopoulos, Peter M. W. Gill, Paola Gori-Giorgi, Andreas Gorling, Tim Gould, Stefan Grimme, Oleg Gritsenko, Hans Jorgen Aagaard Jensen, Erin R. Johnson, Robert O. Jones, Martin Kaupp, Andreas M. Koster, Leeor Kronik, Anna Krylov, Simen Kvaal, Andre Laestadius, Mel Levy, Mathieu Lewin, Shubin Liu, Pierre-Francois Loos, Neepa T. Maitra, Frank Neese, John P. Perdew, Katarzyna Pernal, Pascal Pernot, Piotr Piecuch, Elisa Rebolini, Lucia Reining, Pina Romaniello, Adrienn Ruzsinszky, Dennis R. Salahub, Matthias Scheffler, Peter Schwerdtfeger, Viktor N. Staroverov, Jianwei Sun, Erik Tellgren, David J. Tozer, Samuel B. Trickey, Carsten A. Ullrich, Alberto Vela, Giovanni Vignale, Tomasz A. Wesolowski, Xin Xu, Weitao Yang
Summary: This paper provides an informal review and discussion on the history, present status, and future of density-functional theory (DFT) by 70 workers in the field. The format of a roundtable discussion allowed participants to express their views through 302 individual contributions to a preset list of 26 questions. Supported by a bibliography of 777 entries, the paper offers a comprehensive snapshot of DFT in 2022.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
