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It has been extensively demonstrated through first principles quantum mechanics calculations that water exhibits strong hydrogen bond cooperativity. Classical molecular simulation and statistical mechanics methods typically assume pairwise…

Soft Condensed Matter · Physics 2017-05-24 Bennett D. Marshall

Alchemical perturbation density functional theory has been shown to be an efficient and computationally inexpensive way to explore chemical compound space. We investigate approximations made, in terms of atomic basis sets and perturbation…

Chemical Physics · Physics 2020-10-28 Giorgio Domenichini , Guido Falk von Rudorff , O. Anatole von Lilienfeld

We present an intuitive and general analytical approximation estimating the energy of covalent single and double bonds between participating atoms in terms of their respective nuclear charges with just three parameters, $[{E_\text{AB}…

Chemical Physics · Physics 2022-12-16 Michael J. Sahre , Guido Falk von Rudorff , O. Anatole von Lilienfeld

"Alchemical" interpolation paths, i.e.~coupling systems along fictitious paths that without realistic correspondence, are frequently used within materials and molecular modeling and simulation protocols for the estimation of relative…

Chemical Physics · Physics 2015-03-25 K. Y. Samuel Chang , O. Anatole von Lilienfeld

Molecular self-assembly plays a very important role in various aspects of technology as well as in biological systems. Governed by the covalent, hydrogen or van der Waals interactions - self-assembly of alike molecules results in a large…

We first argue that the covalent bond and the various closed-shell interactions can be thought of as symmetry broken versions of one and the same interaction, viz., the multi-center bond. We use specially chosen molecular units to show that…

Strongly Correlated Electrons · Physics 2017-06-16 Jon C. Golden , Vinh Ho , Vassiliy Lubchenko

The covalent-like characteristics of hydrogen bonds offer a new perspective on intermolecular interactions. Here, using density functional theory and post-Hartree-Fock methods, we reveal that there are two bonding molecular orbitals (MOs)…

Atomic and Molecular Clusters · Physics 2015-07-09 Bo Wang , Wanrun Jiang , Xing Dai , Yang Gao , Zhigang Wang , Rui-Qin Zhang

We provide a systematic test of empirical theories of covalent bonding in solids using an exact procedure to invert ab initio cohesive energy curves. By considering multiple structures of the same material, it is possible for the first time…

mtrl-th · Physics 2009-10-30 Martin Z. Bazant , Efthimios Kaxiras

The way atoms attach to each other defines the function(s), e.g., mechanical, optical, electronic, of a given material. The nature of the chemical bond is, therefore, one of the most fundamental issues in materials. Both ionic interactions,…

Materials Science · Physics 2019-07-10 Yevgeny Rakita , Thomas Kirchartz , Gary Hodes , David Cahen

Prior to recombination photons, electrons, and atomic nuclei rapidly scattered and behaved, almost, like a single tightly-coupled photon-baryon plasma. We investigate here the accuracy of the tight-coupling approximation commonly used to…

Cosmology and Nongalactic Astrophysics · Physics 2015-03-17 Francis-Yan Cyr-Racine , Kris Sigurdson

By judicious use of extrapolations to the 1-particle basis set limit and $n$-particle calibration techniques, total atomization energies of molecules with up to four heavy atoms can be obtained with calibration accuracy (1 kJ/mol or better,…

Chemical Physics · Physics 2007-05-23 Jan M. L. Martin

The "chemical bond" is a central concept in molecular sciences, but there is no consensus as to what a bond actually is. Therefore, a variety of bonding models have been developed, each defining the structure of molecules in a different…

Chemical Physics · Physics 2016-05-03 Amanda Morgenstern

Conjugated polymers are observed to aggregate in solution. To account for this observation we propose a inter-chain binding mechanism based on the intermolecular tunneling of the delocalized $\pi$-electrons occurring at points where the…

Soft Condensed Matter · Physics 2013-05-29 Jeremy D. Schmit , Alex J. Levine

We examine the influence of the main approximations employed in density-functional theory descriptions of the solid phase of molecular hydrogen near dissociation. We consider the importance of nuclear quantum effects on equilibrium…

Materials Science · Physics 2015-06-15 M. A. Morales , J. M. McMahon , C. Pierleoni , D. M. Ceperley

The hydrogen phase diagram has a number of unusual features which are generally well reproduced by density functional calculations. Unfortunately, these calculations fail to provide good physical insights into why those features occur. In…

Materials Science · Physics 2020-10-28 Hongxiang Zong , Heather Wiebe , Graeme J. Ackland

The van der Waals coefficients, from C_11 through to C_16 resulting from 2nd, 3rd and 4th order perturbation theory are estimated for the alkali (Li, Na, K and Rb) atoms. The dispersion coefficients are also computed for all possible…

Atomic Physics · Physics 2007-05-23 J. Mitroy , M. W. J. Bromley

The energy difference between two iso-electronic systems can be accurately approximated by the alchemical first order Hellmann-Feynmann derivative for the averaged Hamiltonian. This approximation is exact up to third order because…

Chemical Physics · Physics 2025-09-05 O. Anatole von Lilienfeld , Giorgio Domenichini

The relativistic second-order corrections at orders $m\alpha^6$ and $m\alpha^6(m/M)$ in hydrogen molecular ions are calculated. Convergence of numerical results is studied, which allows estimating the relative numerical uncertainty to be…

Atomic Physics · Physics 2025-06-30 Vladimir I. Korobov , Jean-Philippe Karr , Zhen-Xiang Zhong

The behaviour of molecules in space is to a large extent governed by where they freeze out or sublimate. The molecular binding energy is thus an important parameter for many astrochemical studies. This parameter is usually determined with…

Astrophysics of Galaxies · Physics 2022-10-05 Torben Villadsen , Niels F. W. Ligterink , Mie Andersen

Alchemical transformations showed that perturbation theory can be applied also to changes in the atomic nuclear charges of a molecule. The alchemical path that connects two different chemical species involves the conceptualization of a…

Chemical Physics · Physics 2024-03-27 Giorgio Domenichini
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