Band structure renormalization at finite temperatures from first principles

In dieser Doktorarbeit untersuchen wir den Einfluss von Elektron-Phonon-Wechselwirkungen (EPW) auf die Bandlueckenrenormierung in kristallinen Festkoerpern bei endlichen Temperaturen. Das Hauptziel besteht darin, den Einfluss der Kernbewegung und der thermischen Ausdehnung des Gitters auf die Bandstruktur in einer Vielzahl von Materialien zu quantifizieren. Zu diesem Zweck wird der Temperatureinfluss auf das EPW in harmonischen Naeherungen unter Verwendung der stochastischen Abtastmethode und vollstaendig anharmonisch durch Durchführung von ab initio Molekulardynamiksimulationen (aiMD). Die Bandluecke bei endlichen Temperaturen wird aus der thermodynamisch gemittelten Spektralfunktion extrahiert, die unter Verwendung der Bandentfaltungstechnik berechnet wird. Waehrend die Verwendung von aiMD bereits fuer Berechnungen von EPW verwendet wurde, wurde die Kombination von aiMD und Bandentfaltung zur Behandlung der Bandluecken renormalisierung erst kuerzlich verwendet. In dieser Doktorarbeit haben wir eine verbesserte Bandentfaltungstechnik verwendet, um die Berechnung effektiv zu verwalten. Diese verbesserte Methode enthaelt mehrere methodische Neuerungen, die dazu dienen, den Rechenaufwand zu verringern und das statistische Rauschen in den Endergebnissen zu minimieren. Die aktualisierte Methode wurde gruendlich bewertet, dokumentiert und mit einer benutzerfreundlichen Oberflaeche gestaltet. Wir praesentieren eine umfassende Untersuchung der numerischen Aspekte der thermodynamischen Mittelung, der Schaetzung von Fehlerbalken und der Bewertung der Konvergenz in Bezug auf die Groesse der Simulationssuperzelle. Unser etabliertes Protokoll ermoeglicht die Berechnung der Bandlückenrenormierung bei endlichen Temperaturen, was in guter Uebereinstimmung mit frueheren theoretischen Studien und experimentellen Daten steht.In this thesis, we investigate the influence of electron-phonon interactions (EPI) on the band gap renormalization in crystalline solids at finite temperatures. The main goal is to identify the impact of the nuclear motion and the lattice thermal expansion on the band structure in a wide range of materials. For this purpose, the temperature influence on the EPI is calculated in the harmonic approximations by utilizing the stochastic sampling methodology and fully anharmonically, by performing ab initio molecular dynamics simulations (aiMD). The band gap at finite temperatures is extracted from the thermodynamically averaged spectral function, which is calculated using band-unfolding technique. While utilization of aiMD was already used for calculations of EPI the combination of aiMD and band-unfolding to treat the band gap renormalization was used only recently. In this thesis, we employed an improved band unfolding technique in order to effectively manage the calculations. This improved method incorporates several methodological innovations that serve to mitigate computational cost and minimize statistical noise in the final results. The updated method was thoroughly benchmarked, documented, and designed with a user-friendly interface. We present a comprehensive examination of the numerical aspects of thermodynamic averaging, the estimation of error bars, and the evaluation of convergence with respect to the size of the simulation supercell. Our established protocol enables the calculation of band gap renormalization at finite temperatures, which is in good agreement with prior theoretical studies and experimental data

The 2021 room-temperature superconductivity roadmap.

Designing materials with advanced functionalities is the main focus of contemporary solid-state physics and chemistry. Research efforts worldwide are funneled into a few high-end goals, one of the oldest, and most fascinating of which is the search for an ambient temperature superconductor (A-SC). The reason is clear: superconductivity at ambient conditions implies being able to handle, measure and access a single, coherent, macroscopic quantum mechanical state without the limitations associated with cryogenics and pressurization. This would not only open exciting avenues for fundamental research, but also pave the road for a wide range of technological applications, affecting strategic areas such as energy conservation and climate change. In this roadmap we have collected contributions from many of the main actors working on superconductivity, and asked them to share their personal viewpoint on the field. The hope is that this article will serve not only as an instantaneous picture of the status of research, but also as a true roadmap defining the main long-term theoretical and experimental challenges that lie ahead. Interestingly, although the current research in superconductor design is dominated by conventional (phonon-mediated) superconductors, there seems to be a widespread consensus that achieving A-SC may require different pairing mechanisms.In memoriam, to Neil Ashcroft, who inspired us all

Effects of Chlorine Mixing on Optoelectronics, Ion-Migration and Gamma-ray Detection In Bromide Perovskites

International audienceControlled anion-mixing in halide perovskites has been shown to be an effective route to precisely tuning optoelectronic properties, in order to achieve efficient photo- voltaic, light emission and radiation detection devices. However, an atomistic under- standing behind the precise mechanism impacting the performances of mixed halide perovskite devices, particularly as a radiation detector, is still missing. Combining high-level computational methods and multiple experiments, here we systematically investigate the effect of chlorine (Cl) incorporation on the optical and electronic prop- erties, structural stability, ion-migration as well as the γ-ray radiation detection ability of MAPbBr 3-x Cl x . We observe that precise halide mixing suppresses bromide ion mi- gration and consequently reduces the dark current by close to a factor of two, which significantly improves the resistance of the mixed-anion devices. Furthermore, reduced carrier effective masses and mostly unchanged exciton binding energies indicate en- hanced charge carrier transport for these perovskite alloys. At the atomistic level, modifications to ion migration and charge carrier transport properties improve elec- tronic properties and predominantly contribute to the better response and resolution in high-energy γ-ray detection with MAPbBr 3-x Cl x , as compared to MAPbBr 3 . This study provides a systematic approach to enhance the high-energy radiation detection ability of MAPbBr 3-x Cl x -based devices by understanding the atomistic properties un- derpinning performance

The 2021 Room-Temperature Superconductivity Roadmap

Designing materials with advanced functionalities is the main focus of contemporary solid-state physics and chemistry. Research efforts worldwide are funneled into a few high-end goals, one of the oldest, and most fascinating of which is the search for an ambient temperature superconductor (A-SC). The reason is clear: superconductivity at ambient conditions implies being able to handle, measure and access a single, coherent,macroscopic quantum mechanical state without the limitations associated with cryogenics and pressurization. This would not only open exciting avenues for fundamental research, but also pave the road for a wide range of technological applications, affecting strategic areas such as energy conservation and climate change. In this Roadmap we have collected contributions from many of the main actors working on superconductivity at high pressures, and asked them to share their personal viewpoint on the field. The hope is that this article will serve not only as an instantaneous picture of the status of research, but also as a true Roadmap defining the main long-term theoretical and experimental challenges that lie ahead. Interestingly, although the current research in superconductor design is dominated by conventional (phonon-mediated) superconductors, there seems to be a widespread consensus that achieving A-SC may require different pairing mechanisms

The 2021 Room-Temperature Superconductivity Roadmap

Last year, the report of Room-Temperature Superconductivity in high-pressure carbonaceous sulfur hydride marked a major milestone in the history of physics: one of the holy grails of condensed matter research was reached after more than one century of continuing efforts. This long path started with Neil Ashcroft's and Vitaly Ginzburg's visionary insights on high-temperature superconductivity in metallic hydrogen in the 60's and 70's, and has led to the current hydride fever, following the report of high-Tc high-pressure superconductivity in H3S in 2014. This Roadmap collects selected contributions from many of the main actors in this exciting chapter of condensed matter history. Key for the rapid progress of this field has been a new course for materials discovery, where experimental and theoretical discoveries proceed hand in hand. The aim of this Roadmap is not only to offer a snapshot of the current status of superconductor materials research, but also to define the theoretical and experimental obstacles that must be overcome for us to realize fully exploitable room temperature superconductors, and foresee future strategies and research directions. This means improving synthesis techniques, extending first-principles methods for superconductors and structural search algorithms for crystal structure predictions, but also identifying new approaches to material discovery based on artificial intelligence