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"Gross, E."
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Ultrafast dynamics with the exact factorization
The exact factorization of the time-dependent electron–nuclear wavefunction has been employed successfully in the field of quantum molecular dynamics simulations for interpreting and simulating light-induced ultrafast processes. In this work, we summarize the major developments leading to the formulation of a trajectory-based approach, derived from the exact factorization equations, capable of dealing with nonadiabatic electronic processes, and including spin-orbit coupling and the non-perturbative effect of an external time-dependent field. This trajectory-based quantum-classical approach has been dubbed coupled-trajectory mixed quantum-classical (CT-MQC) algorithm, whose performance is tested here to study the photo-dissociation dynamics of IBr.
Graphic abstract
Journal Article
On the Mass of Atoms in Molecules: Beyond the Born-Oppenheimer Approximation
Describing the dynamics of nuclei in molecules requires a potential energy surface, which is traditionally provided by the Born-Oppenheimer or adiabatic approximation. However, we also need to assign masses to the nuclei. There, the Born-Oppenheimer picture does not account for the inertia of the electrons, and only bare nuclear masses are considered. Nowadays, experimental accuracy challenges the theoretical predictions of rotational and vibrational spectra and requires the participation of electrons in the internal motion of the molecule. More than 80 years after the original work of Born and Oppenheimer, this issue has still not been solved, in general. Here, we present a theoretical and numerical framework to address this problem in a general and rigorous way. Starting from the exact factorization of the electron-nuclear wave function, we include electronic effects beyond the Born-Oppenheimer regime in a perturbative way via position-dependent corrections to the bare nuclear masses. This maintains an adiabaticlike point of view: The nuclear degrees of freedom feel the presence of the electrons via a single potential energy surface, whereas the inertia of electrons is accounted for and the total mass of the system is recovered. This constitutes a general framework for describing the mass acquired by slow degrees of freedom due to the inertia of light, bounded particles; thus, it is applicable not only in electron-nuclear systems but in light-heavy nuclei or ions as well. We illustrate this idea with a model of proton transfer, where the light particle is the proton and the heavy particles are the oxygen atoms to which the proton is bounded. Inclusion of the light-particle inertia allows us to gain orders of magnitude in accuracy. The electron-nuclear perspective is adopted, instead, to calculate position-dependent mass corrections using density functional theory for a few polyatomic molecules at their equilibrium geometry. These data can serve as input for the computation of high-precision molecular spectra.
Journal Article
Electronic non-adiabatic states: towards a density functional theory beyond the Born-Oppenheimer approximation
A novel treatment of non-adiabatic couplings is proposed. The derivation is based on a theorem by Hunter stating that the wave function of the complete system of electrons and nuclei can be written, without approximation, as a Born-Oppenheimer (BO)-type product of a nuclear wave function, X(R), and an electronic one, ΦR(r), which depends parametrically on the nuclear configuration R. From the variational principle, we deduce formally exact equations for ΦR(r) and X(R). The algebraic structure of the exact nuclear equation coincides with the corresponding one in the adiabatic approximation. The electronic equation, however, contains terms not appearing in the adiabatic case, which couple the electronic and the nuclear wave functions and account for the electron-nuclear correlation beyond the BO level. It is proposed that these terms can be incorporated using an optimized local effective potential.
Journal Article
The optimal one dimensional periodic table: a modified Pettifor chemical scale from data mining
Starting from the experimental data contained in the inorganic crystal structure database, we use a statistical analysis to determine the likelihood that a chemical element A can be replaced by another B in a given structure. This information can be used to construct a matrix where each entry ( A , B ) is a measure of this likelihood. By ordering the rows and columns of this matrix in order to reduce its bandwidth, we construct a one-dimension ordering of the chemical elements, analogous to the famous Pettifor scale. The new scale shows large similarities with the one of Pettifor, but also striking differences, especially in what comes to the ordering of the non-metals.
Journal Article
A connectomic approach for subcallosal cingulate deep brain stimulation surgery: prospective targeting in treatment-resistant depression
Target identification and contact selection are known contributors to variability in efficacy across different clinical indications of deep brain stimulation surgery. A retrospective analysis of responders to subcallosal cingulate deep brain stimulation (SCC DBS) for depression demonstrated the common impact of the electrical stimulation on a stereotypic connectome of converging white matter bundles (forceps minor, uncinate fasciculus, cingulum and fronto-striatal fibers). To test the utility of a prospective connectomic approach for SCC DBS surgery, this pilot study used the four-bundle tractography 'connectome blueprint' to plan surgical targeting in 11 participants with treatment-resistant depression. Before surgery, targets were selected individually using deterministic tractography. Selection of contacts for chronic stimulation was made by matching the post-operative probabilistic tractography map to the pre-surgical deterministic tractography map for each subject. Intraoperative behavioral responses were used as a secondary verification of location. A probabilistic tract map of all participants demonstrated inclusion of the four bundles as intended, matching the connectome blueprint previously defined. Eight of 11 patients (72.7%) were responders and 5 were remitters after 6 months of open-label stimulation. At one year, 9 of 11 patients (81.8%) were responders, with 6 of them in remission. These results support the utility of a group probabilistic tractography map as a connectome blueprint for individualized, patient-specific, deterministic tractography targeting, confirming retrospective findings previously published. This new method represents a connectomic approach to guide future SCC DBS studies.
Journal Article
Balancing interfacial reactions to achieve long cycle life in high-energy lithium metal batteries
The rechargeable lithium metal battery has attracted wide attention as a next-generation energy storage technology. However, simultaneously achieving high cell-level energy density and long cycle life in realistic batteries is still a great challenge. Here we investigate the degradation mechanisms of Li || LiNi
0.6
Mn
0.2
Co
0.2
O
2
pouch cells and present fundamental linkages among Li thickness, electrolyte depletion and the structure evolution of solid–electrolyte interphase layers. Different cell failure processes are discovered when tuning the anode to cathode capacity ratio in compatible electrolytes. An optimal anode to cathode capacity ratio of 1:1 emerges because it balances well the rates of Li consumption, electrolyte depletion and solid–electrolyte interphase construction, thus decelerating the increase of cell polarization and extending cycle life. Contrary to conventional wisdom, long cycle life is observed by using ultra-thin Li (20 µm) in balanced cells. A prototype 350 Wh kg
−1
pouch cell (2.0 Ah) achieves over 600 long stable cycles with 76% capacity retention without a sudden cell death.
The development of Li metal batteries requires understanding of cell-level electrochemical processes. Here the authors investigate the interplay between electrode thickness, electrolyte depletion and solid–electrolyte interphase in practical pouch cells and demonstrate the construction of high-energy long-cycle Li metal batteries.
Journal Article
A Scoping Review of Empirical Asexuality Research in Social Science Literature
Research on asexuality as a part of the experience of human sexuality has increased over the last two decades. However, there has not yet been a systematic review of the extant literature on asexuality. This paper aims to provide a systematic scoping review of literature on asexuality with articles published in 2004 through August 2021. After a systematic search procedure, 48 studies were included. A codebook was developed to extract broad information about the literature on asexuality, including sampling techniques, research participant sociodemographics, and conceptualization of asexuality. Results of the review indicate that the research is currently split between qualitative and quantitative methods. The literature primarily relied on convenience sampling within asexual online communities. The primary online community was Asexual Visibility and Education Network (AVEN), which may have contributed to the majority of participants being White, presumptively cisgender, women between the ages of 20–30. Analysis of the overall literature scope demonstrates no support for asexuality as a medical condition (i.e., a disorder requiring treatment) and instead supports the need to recognize asexuality as a complex identity and sexual orientation. Implications for research are discussed, such as the need for additional research on the topic of human sexuality that includes asexuality as a sexual orientation as well as the need for more intersectional research within the literature.
Journal Article
Ultrafast laser induced local magnetization dynamics in Heusler compounds
The overarching goal of the field of femtomagnetism is to control, via laser light, the magnetic structure of matter on a femtosecond time scale. The temporal limits to the light-magnetism interaction are governed by the fact that the electron spin interacts indirectly with light, with current studies showing a laser induced global loss in the magnetic moment on a time scale of the order of a few 100 s of femtoseconds. In this work, by means of
ab-initio
calculations, we show that more complex magnetic materials - we use the example of the Heusler and half-Heusler alloys - allow for purely optical excitations to cause a significant change in the local moments on the order of 5 fs. This, being purely optical in nature, represents the ultimate mechanism for the short time scale manipulation of spins. Furthermore, we demonstrate that qualitative behaviour of this rich magnetic response to laser light can be deduced from the ground-state spectrum, thus providing a route to tailoring the response of some complex magnetic materials, like the Heuslers, to laser light by the well established methods for material design from ground-state calculations.
Journal Article