89 research outputs found
Excited-State Response Theory Within the Context of the Coupled-Cluster Formalism
Time-dependent response theories are foundational to the development of
algorithms that determine quantum properties of electronic excited states of
molecules and periodic systems. They are employed in wave-function,
density-functional, and semiempirical methods, and are applied in an
incremental order: linear, quadratic, cubic, etc. Linear response theory is
known to produce electronic transitions from ground to excited state, and vice
versa. In this work, a linear-response approach, within the context of the
coupled cluster formalism, is developed to offer transition elements between
different excited states (including permanent elements), and related
properties. Our formalism, second linear response theory, is consistent with
quadratic response theory, and can serve as an alternative to develop and study
excited-state theoretical methods, including pathways for algorithmic
acceleration. This work also formulates an extension of our theory for general
propagations under non-linear external perturbations, where the observables are
given by linked expressions which can predict their time-evolution under
arbitrary initial states and could serve as a means of constructing general
state propagators. A connection with the physics of wavefunction theory is
developed as well, in which dynamical cluster operator amplitudes are related
to wavefunction linear superposition coefficients.Comment: 44 pages, 6 figures, submitted to Physical Review
Cluster Amplitudes and Their Interplay with Self-Consistency in Density Functional Methods
Density functional theory (DFT) provides convenient electronic structure
methods for the study of molecular systems and materials. Regular Kohn-Sham DFT
calculations rely on unitary transformations to determine the ground-state
electronic density, ground state energy, and related properties. However, for
dissociation of molecular systems into open-shell fragments, due to the
self-interaction error present in a large number of density functional
approximations, the self-consistent procedure based on the this type of
transformation gives rise to the well-known charge delocalization problem. To
avoid this issue, we showed previously that the cluster operator of
coupled-cluster theory can be utilized within the context of DFT to solve in an
alternative and approximate fashion the ground-state self-consistent problem.
This work further examines the application of the singles cluster operator to
molecular ground state calculations. Two approximations are derived and
explored: i), A linearized scheme of the quadratic equation used to determine
the cluster amplitudes, and, ii), the effect of carrying the calculations in a
non-self-consistent field fashion. These approaches are found to be capable of
improving the energy and density of the system and are quite stable in either
case. The theoretical framework discussed in this work could be used to
describe, with an added flexibility, quantum systems that display challenging
features and require expanded theoretical methods.Comment: 17 pages, 5 figures, 1 table, submitted to ChemPhysChe
Creating a three dimensional intrinsic electric dipole on rotated CrI bilayers
Two-dimensional (2D) materials are being explored as a novel multiferroic
platform. One of the most studied magnetoelectric multiferroic 2D materials are
antiferromagnetically-coupled (AFM) CrI bilayers. Neglecting magnetism,
those bilayers possess a crystalline point of inversion, which is only removed
by the antiparallel spin configuration among its two constituent monolayers.
The resultant intrinsic electric dipole on those bilayers has a magnitude no
larger than 0.04 pC/m, it points out-of-plane, and it reverts direction when
the--Ising-like--cromium spins are flipped (toward opposite layers {\em versus}
away from opposite layers). The combined presence of antiferromagnetism and a
weak intrinsic electric dipole makes this material a two-dimensional
magnetoelectric multiferroic. Here, we remove the crystalline center of
inversion of the bilayer by a relative rotation of its constituent
monolayers. This process {\em enhances} the out-of-plane intrinsic electric
dipole tenfold with respect to its magnitude in the non-rotated AFM bilayer and
also creates an even stronger and switchable in-plane intrinsic electric
dipole. The ability to create a three-dimensional electric dipole is important,
because it enhances the magnetoelectric coupling on this experimentally
accessible 2D material, which is explicitly calculated here as well.Comment: Accepted at PRB on May 1, 202
Beyond the molecular orbital conception of electronically excited states through the quantum theory of atoms in molecules
Evolución de la preparación física en el fútbol
The In the area of sport, has been being shown, one of the most important factors for the athlete to perform at its best is to have a good physical condition. Regardless of the technical improvement, medical support nutrition, new materials, etc.. physical training has in recent years experienced an extraordinary evolution in both quantity and quality. In recent decades, sports science have greatly evolved as a result of this progress are appearing in the physical preparation in football at all levels. In this article the main trends that have historically been being used to improve various physical qualities involving this sport, with the aim of achieving the best possible performance are analyzed.En el ámbito del deporte, ha venido siendo demostrado, que uno de los factores más importantes para que el deportista pueda rendir en las mejores condiciones es el de tener una buena preparación física. Independientemente del perfeccionamiento técnico, apoyo médico, nutrición, nuevos materiales, etc. la preparación física ha experimentado en los últimos años una evolución extraordinaria, tanto en cantidad como en calidad. En las últimas décadas las ciencias del deporte han evolucionado enormemente, producto de ello son los avances aparecidos en la preparación física en el fútbol a todos sus niveles. En este artículo se analizan las principales tendencias que históricamente han venido empleándose para la mejora de las diferentes cualidades físicas que implican la práctica de este deporte, con el objetivo de alcanzar el mejor rendimiento posible
Allelic Variation, Alternative Splicing and Expression Analysis of Psy1 Gene in Hordeum chilense Roem. et Schult
Background: The wild barley Hordeum chilense Roem. et Schult. is a valuable source of genes for increasing carotenoid content in wheat. Tritordeums, the amphiploids derived from durum or common wheat and H. chilense, systematically show higher values of yellow pigment colour and carotenoid content than durum wheat. Phytoene synthase 1 gene (Psy1) is considered a key step limiting the carotenoid biosynthesis, and the correlation of Psy1 transcripts accumulation and endosperm carotenoid content has been demonstrated in the main grass species. Methodology/Principal findings: We analyze the variability of Psy1 alleles in three lines of H. chilense (H1, H7 and H16) representing the three ecotypes described in this species. Moreover, we analyze Psy1 expression in leaves and in two seed developing stages of H1 and H7, showing mRNA accumulation patterns similar to those of wheat. Finally, we identify thirtysix different transcripts forms originated by alternative splicing of the 59 UTR and/or exons 1 to 5 of Psy1 gene. Transcripts function is tested in a heterologous complementation assay, revealing that from the sixteen different predicted proteins only four types (those of 432, 370, 364 and 271 amino acids), are functional in the bacterial system. Conclusions/Significance: The large number of transcripts originated by alternative splicing of Psy1, and the coexistence of functional and non functional forms, suggest a fine regulation of PSY activity in H. chilense. This work is the first analysis of H. chilense Psy1 gene and the results reported here are the bases for its potential use in carotenoid enhancement in duru
Differential clinical characteristics and prognosis of intraventricular conduction defects in patients with chronic heart failure
Intraventricular conduction defects (IVCDs) can impair prognosis of heart failure (HF), but their specific impact is not well established. This study aimed to analyse the clinical profile and outcomes of HF patients with LBBB, right bundle branch block (RBBB), left anterior fascicular block (LAFB), and no IVCDs. Clinical variables and outcomes after a median follow-up of 21 months were analysed in 1762 patients with chronic HF and LBBB (n = 532), RBBB (n = 134), LAFB (n = 154), and no IVCDs (n = 942). LBBB was associated with more marked LV dilation, depressed LVEF, and mitral valve regurgitation. Patients with RBBB presented overt signs of congestive HF and depressed right ventricular motion. The LAFB group presented intermediate clinical characteristics, and patients with no IVCDs were more often women with less enlarged left ventricles and less depressed LVEF. Death occurred in 332 patients (interannual mortality = 10.8%): cardiovascular in 257, extravascular in 61, and of unknown origin in 14 patients. Cardiac death occurred in 230 (pump failure in 171 and sudden death in 59). An adjusted Cox model showed higher risk of cardiac death and pump failure death in the LBBB and RBBB than in the LAFB and the no IVCD groups. LBBB and RBBB are associated with different clinical profiles and both are independent predictors of increased risk of cardiac death in patients with HF. A more favourable prognosis was observed in patients with LAFB and in those free of IVCDs. Further research in HF patients with RBBB is warranted
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