A comprehensive, self-contained derivation of the one-body density matrices from single-reference excited-state calculation methods using the equation-of-motion formalism

In this contribution we review in a rigorous, yet comprehensive fashion the assessment of the one-body reduced density matrices derived from the most used single-reference excited-state calculation methods in the framework of the equation-of-motion formalism. Those methods are separated into two types: those which involve the coupling of a deexcitation operator to a single-excitation transition operator, and those which do not involve such a coupling. The case of many-body auxiliary wave functions for excited states is also addressed. For each of these approaches we were interested in deriving the elements of the one-body transition and difference density matrices, and to highlight their particular structure. This has been accomplished by applying a decomposition of integrals involving one-determinant quantum electronic states on which two or three pairs of second quantization operators can act. Such a decomposition has been done according to a corollary to Wick's theorem, which is brought in a comprehensive and detailed manner. A comment is also given about the consequences of using the equation-of-motion formulation in this context, and the two types of excited-state calculation methods (with and without coupling excitations to deexcitations) are finally compared from the point of view of the structure of their transition and difference density matrices

Theoretical Insights into the Topology of Molecular Excitons from Single-Reference Excited States Calculation Methods

This chapter gives an introduction to qualitative and quantitative topological analyses of molecular electronic transitions. Among the possibilities for qualitatively describing how the electronic structure of a molecule is reorganized upon light absorption, we chose to detail two of them, namely, the detachment/attachment density matrix analysis and the natural transition orbitals strategy. While these tools are often introduced separately, we decided to formally detail the connection existing between the two paradigms in the case of excited states calculation methods expressing any excited state as a linear combination of singly excited Slater determinants, written based on a single-reference ground state wave function. In this context, we show how the molecular exciton wave function plays a central role in the topological analysis of the electronic transition process

Definition of a linear equivalent model for a non-linear system with impacts

Modal characteristics of non-linear system are typically studied through response to harmonic excitation and using various definitions of non-linear modes. However, few results are available for systems under broadband excitation. The end objective sought here is to generate a linear system, in some sense equivalent to the non-linear system, whose modal characteristics evolve with a level of non-linearity. The considered application is the contact non-linearity found between the tubes of heat exchangers and their support plates. Such tubes, present in nuclear plants, participate to the nuclear safety and can be significantly excited by the fluid flow, so that their dynamic behavior is critical. The turbulent nature of the flow implies broadband excitation and the small gaps between the tubes and the support plate generate very significant non-linear behavior. The proposed equivalent linear system is based on a bilateral contact law whose stiffness and damping characteristics evolve with the amplitude of excitation. A non-linear model is first validated by correlation with experiments. It is then shown that three different indicators (bandwidth of main resonance, operational modal analysis of non-linear power spectral density and correlation of operational deflection shapes) lead to similar values of contact stiffness and damping in the equivalent linear model. This model is hus shown to be a very efficient tool to analyze the impact of the amplitude dependence of the non-linear behavior in the considered system

Definition of a linear equivalent model for a non-linear system with impacts

International audienceModal characteristics of non-linear system are typically studied through response to harmonic excitation and using various definitions of non-linear modes. However, few results are available for systems under broadband excitation. The end objective sought here is to generate a linear system, in some sense equivalent to the non-linear system, whose modal characteristics evolve with a level of non-linearity. The considered application is the contact non-linearity found between the tubes of heat exchangers and their support plates. Such tubes, present in nuclear plants, participate to the nuclear safety and can be significantly excited by the fluid flow, so that their dynamic behavior is critical. The turbulent nature of the flow implies broadband excitation and the small gaps between the tubes and the support plate generate very significant non-linear behavior. The proposed equivalent linear system is based on a bilateral contact law whose stiffness and damping characteristics evolve with the amplitude of excitation. A non-linear model is first validated by correlation with experiments. It is then shown that three different indicators (bandwidth of main resonance, operational modal analysis of non-linear power spectral density and correlation of operational deflection shapes) lead to similar values of contact stiffness and damping in the equivalent linear model. This model is hus shown to be a very efficient tool to analyze the impact of the amplitude dependence of the non-linear behavior in the considered system

Fibrillogenesis from nanosurfaces: multiphoton imaging and stereological analysis of collagen 3D self-assembly dynamics

International audienceThe assembly of proteins into fibrillar structures is an important process that concerns different biological contexts, including molecular medicine and functional biomaterials. Engineering of hybrid biomaterials can advantageously provide synergetic interactions of the biopolymers with an inorganic component to ensure specific supramolecular organization and dynamics. To this aim, we designed hybrid systems associating collagen and surface-functionalized silica particles and we built a new strategy to investigate fibrillogenesis processes in such multicomponents systems, working at the crossroads of chemistry, physics and mathematics. The self-assembly process was investigated by bimodal multiphoton imaging coupling second harmonic generation (SHG) and 2 photon excited fluorescence (2PEF). The in-depth spatial characterization of the system was further achieved using the three-dimensional analysis of the SHG/2PEF data via mathematical morphology processing. Quantitation of collagen distribution around particles offers strong evidence that the chemically induced confinement of the protein on the silica nanosurfaces has a key influence on the spatial extension of fibrillogenesis. This new approach is unique in the information it can provide on 3D dynamic hybrid systems and may be extended to other associations of fibrillar molecules with optically responsive nano-objects

The potential role of microbiota for controlling the spread of extended-spectrum beta-lactamase-producing Enterobacteriaceae (ESBL-PE) in neonatal population [version 1; referees: 2 approved]

The spread of extended-spectrum beta-lactamase-producing Enterobacteriaceae (ESBL-PE) in the hospital and also the community is worrisome. Neonates particularly are exposed to the risk of ESBL-PE acquisition and, owing to the immaturity of their immune system, to a higher secondary risk of ESBL-PE-related infection. Reducing the risk of acquisition in the hospital is usually based on a bundle of measures, including screening policies at admission, improving hand hygiene compliance, and decreasing antibiotic consumption. However, recent scientific data suggest new prevention opportunities based on microbiota modifications

Overview of the current use of levosimendan in France: a prospective observational cohort study

Abstract Background Following the results of randomized controlled trials on levosimendan, French health authorities requested an update of the current use and side-effects of this medication on a national scale. Method The France-LEVO registry was a prospective observational cohort study reflecting the indications, dosing regimens, and side-effects of levosimendan, as well as patient outcomes over a year. Results The patients included ( n = 602) represented 29.6% of the national yearly use of levosimendan in France. They were treated for cardiogenic shock ( n = 250, 41.5%), decompensated heart failure ( n = 127, 21.1%), cardiac surgery-related low cardiac output prophylaxis and/or treatment ( n = 86, 14.3%), and weaning from veno-arterial extracorporeal membrane oxygenation ( n = 82, 13.6%). They received 0.18 ± 0.07 µg/kg/min levosimendan over 26 ± 8 h. An initial bolus was administered in 45 patients (7.5%), 103 (17.1%) received repeated infusions, and 461 (76.6%) received inotropes and or vasoactive agents concomitantly. Hypotension was reported in 218 patients (36.2%), atrial fibrillation in 85 (14.1%), and serious adverse events in 17 (2.8%). 136 patients (22.6%) died in hospital, and 26 (4.3%) during the 90-day follow-up. Conclusions We observed that levosimendan was used in accordance with recent recommendations by French physicians. Hypotension and atrial fibrillation remained the most frequent side-effects, while serious adverse event potentially attributable to levosimendan were infrequent. The results suggest that this medication was safe and potentially associated with some benefit in the population studied