External paper

Mixtures of cations or halides with FAPbI3 (where FA is formamidinium) lead to high efficiency in perovskite solar cells (PSCs) but also to blue-shifted absorption and long-term stability issues caused by loss of volatile methylammonium (MA) and phase segregation. We report a deposition method using MA thiocyanate (MASCN) or FASCN vapor treatment to convert yellow d-FAPbI3 perovskite films to the desired pure a-phase. NMR quantifies MA incorporation into the framework.

We present a real-time ab initio description of optical orientation in bulk GaAs due to the coupling with an ultrashort circularly polarized laser source. The injection of spin-polarized electrons in the conduction band is correctly reproduced, and a nonvanishing spin polarization P parallel to the direction of propagation of the laser (z) emerges. A detailed analysis of the generation and the evolution of P(t) is given.

Antiferromagnetically coupled magnetic skyrmions are considered ideal candidates for high-density information carriers. This is due to the suppressed skyrmion Hall effect compared to conventional skyrmions and a smaller size due to the cancellation of some contributions to the magnetostatic dipolar fields. By means of systematic first-principles calculations based on density functional theory we search for suitable materials that can host antiferromagnetically coupled skyrmions.

Electrosorption of solvated species at metal electrodes is a most fundamental class of processes in interfacial electrochemistry. Here, we use its sensitive dependence on the electric double layer to assess the performance of ab initio thermodynamics approaches increasingly used for the first-principles description of electrocatalysis. We show analytically that computational hydrogen electrode calculations at zero net-charge can be understood as a first-order approximation to a fully grand canonical approach.

Bottom-up approaches exploiting on-surface synthesis reactions allow atomic-scale precision in the fabrication of graphene nanoribbons (GNRs); this is essential for their technological applications since their unique electronic and optical properties are largely controlled by the specific edge structure. By means of a combined experimental-theoretical investigation of some prototype GNRs, we show here that high-resolution electron energy-loss spectroscopy (HREELS) can be successfully employed to fingerprint the details of the GNR edge structure.

Electron-phonon interactions are key to understanding the dynamics of electrons in materials and can be modeled accurately from first principles. However, when electrons and holes form Coulomb-bound states (excitons), quantifying their interactions and scattering processes with phonons remains an open challenge. Here we show a rigorous approach for computing exciton-phonon (ex-ph) interactions and the associated exciton dynamical processes from first principles.

Time-resolved soft-x-ray photoemission spectroscopy is used to simultaneously measure the ultrafast dynamics of core-level spectral functions and excited states upon excitation of excitons in WSe2. We present a many-body approximation for the Green’s function, which excellently describes the transient core-hole spectral function. The relative dynamics of excited-state signal and core levels clearly show a delayed core-hole renormalization due to screening by excited quasifree carriers resulting from an excitonic Mott transition.

The nonequilibrium excitonic insulator (NEQ-EI) is an excited state of matter characterized by a finite density of coherent excitons and a time-dependent macroscopic polarization. The stability of this exciton superfluid as the density grows is jeopardized by the increased screening efficiency of the looser excitons. In this work we put forward a Hartree plus screened exchange scheme to predict the critical density at which the transition toward a free electron-hole plasma occurs.

Understanding the electronic energy landscape in metal halide perovskites is essential for further improvements in their promising performance in thin-film photovoltaics. Here, we uncover the presence of above-bandgap oscillatory features in the absorption spectra of formamidinium lead triiodide thin films.

We present an ab initio computational approach for the calculation of resonant Raman intensities, including both excitonic and nonadiabatic effects. Our diagrammatic approach, which we apply to two prototype, semiconducting layered materials, allows a detailed analysis of the impact of phonon-mediated exciton-exciton scattering on the intensities. In the case of bulk hexagonal boron nitride, this scattering leads to strong quantum interference between different excitonic resonances, strongly redistributing oscillator strength with respect to optical absorption spectra.