What is a crystal?

Almost 25 years have passed since Shechtman discovered quasicrystals, and 15 years since the Commission on Aperiodic Crystals of the International Union of Crystallography put forth a provisional definition of the term crystal to mean ``any solid having an essentially discrete diffraction diagram.'' Have we learned enough about crystallinity in the last 25 years, or do we need more time to explore additional physical systems? There is much confusion and contradiction in the literature in using the term crystal. Are we ready now to propose a permanent definition for crystal to be used by all? I argue that time has come to put a sense of order in all the confusion.Comment: Submitted to Zeitschrift fuer Kristallographi

The tensor hypercontracted parametric reduced density matrix algorithm: coupled-cluster accuracy with O(r^4) scaling

Tensor hypercontraction is a method that allows the representation of a high-rank tensor as a product of lower-rank tensors. In this paper, we show how tensor hypercontraction can be applied to both the electron repulsion integral (ERI) tensor and the two-particle excitation amplitudes used in the parametric reduced density matrix (pRDM) algorithm. Because only O(r) auxiliary functions are needed in both of these approximations, our overall algorithm can be shown to scale as O(r4), where r is the number of single-particle basis functions. We apply our algorithm to several small molecules, hydrogen chains, and alkanes to demonstrate its low formal scaling and practical utility. Provided we use enough auxiliary functions, we obtain accuracy similar to that of the traditional pRDM algorithm, somewhere between that of CCSD and CCSD(T).Comment: 11 pages, 1 figur

Equivariant pretheories and invariants of torsors

In the present paper we introduce and study the notion of an equivariant pretheory: basic examples include equivariant Chow groups, equivariant K-theory and equivariant algebraic cobordism. To extend this set of examples we define an equivariant (co)homology theory with coefficients in a Rost cycle module and provide a version of Merkurjev's (equivariant K-theory) spectral sequence for such a theory. As an application we generalize the theorem of Karpenko-Merkurjev on G-torsors and rational cycles; to every G-torsor E and a G-equivariant pretheory we associate a graded ring which serves as an invariant of E. In the case of Chow groups this ring encodes the information concerning the motivic J-invariant of E and in the case of Grothendieck's K_0 -- indexes of the respective Tits algebras.Comment: 23 pages; this is an essentially extended version of the previous preprint: the construction of an equivariant cycle (co)homology and the spectral sequence (generalizing the long exact localization sequence) are adde

A unified electrostatic and cavitation model for first-principles molecular dynamics in solution

The electrostatic continuum solvent model developed by Fattebert and Gygi is combined with a first-principles formulation of the cavitation energy based on a natural quantum-mechanical definition for the surface of a solute. Despite its simplicity, the cavitation contribution calculated by this approach is found to be in remarkable agreement with that obtained by more complex algorithms relying on a large set of parameters. Our model allows for very efficient Car-Parrinello simulations of finite or extended systems in solution, and demonstrates a level of accuracy as good as that of established quantum-chemistry continuum solvent methods. We apply this approach to the study of tetracyanoethylene dimers in dichloromethane, providing valuable structural and dynamical insights on the dimerization phenomenon

A note about the ground state of the H3+{\rm H}_3^+ hydrogen molecular ion

Three simple $7-, (7+3)-, 10-$parametric trial functions for the ${\rm H}_3^+$ molecular ion are presented. Each of them provides subsequently the most accurate approximation for the Born-Oppenheimer ground state energy among several-parametric trial functions. These trial functions are chosen following a criterion of physical adequacy and includes the electronic correlation in the exponential form $\sim\exp{(\gamma r_{12})}$, where $\gamma$ is a variational parameter. The Born-Oppenheimer energy is found to be $E=-1.340 34, -1.340 73, -1.341 59$\,a.u., respectively, for optimal equilateral triangular configuration of protons with the equilibrium interproton distance $R=1.65$\,a.u. The variational energy agrees in three significant digits (s.d.) with most accurate results available at present as well as for major expectation values.Comment: 12 pages, 1 figure, 3 table