Direct Observation of Band Gap Renormalization in Layered Indium Selenide.

Manipulation of intrinsic electronic structures by electron or hole doping in a controlled manner in van der Waals layered materials is the key to control their electrical and optical properties. Two-dimensional indium selenide (InSe) semiconductor has attracted attention due to its direct band gap and ultrahigh mobility as a promising material for optoelectronic devices. In this work, we manipulate the electronic structure of InSe by in situ surface electron doping and obtain a significant band gap renormalization of ∼120 meV directly observed by high-resolution angle resolved photoemission spectroscopy. This moderate doping level (carrier concentration of 8.1 × 1012 cm-2) can be achieved by electrical gating in field effect transistors, demonstrating the potential to design of broad spectral response devices.

Band Gap Renormalization, Carrier Multiplication, and Stark Broadening in Photoexcited Black Phosphorus.

We investigate black phosphorus by time- and angle-resolved photoelectron spectroscopy. The electrons excited by 1.57 eV photons relax down to a conduction band minimum within 1 ps. Despite the low band gap value, no relevant amount of carrier multiplication could be detected at an excitation density 3-6 × 1019 cm-3. In the thermalized state, the band gap renormalization is negligible up to a photoexcitation density that fills the conduction band by 150 meV. Astonishingly, a Stark broadening of the valence band takes place at an early delay time. We argue that electrons and holes with a high excess energy lead to inhomogeneous screening of near surface fields. As a consequence, the chemical potential is no longer pinned in a narrow impurity band.

Exciton Band Structure in Two-Dimensional Materials.

Low-dimensional materials differ from their bulk counterparts in many respects. In particular, the screening of the Coulomb interaction is strongly reduced, which can have important consequences such as the significant increase of exciton binding energies. In bulk materials the binding energy is used as an indicator in optical spectra to distinguish different kinds of excitons, but this is not possible in low-dimensional materials, where the binding energy is large and comparable in size for excitons of very different localization. Here we demonstrate that the exciton band structure, which can be accessed experimentally, instead provides a powerful way to identify the exciton character. By comparing the ab initio solution of the many-body Bethe-Salpeter equation for graphane and single-layer hexagonal boron nitride, we draw a general picture of the exciton dispersion in two-dimensional materials, highlighting the different role played by the exchange electron-hole interaction and by the electronic band structure. Our interpretation is substantiated by a prediction for phosphorene.

Dynamical effects in electron spectroscopy.

One of the big challenges of theoretical condensed-matter physics is the description, understanding, and prediction of the effects of the Coulomb interaction on materials properties. In electronic spectra, the Coulomb interaction causes a renormalization of energies and change of spectral weight. Most importantly, it can lead to new structures, often called satellites. These can be linked to the coupling of excitations, also termed dynamical effects. State-of-the-art methods in the framework of many-body perturbation theory, in particular, the widely used GW approximation, often fail to describe satellite spectra. Instead, approaches based on a picture of electron-boson coupling such as the cumulant expansion are promising for the description of plasmon satellites. In this work, we give a unified derivation of the GW approximation and the cumulant expansion for the one-body Green's function. Using the example of bulk sodium, we compare the resulting spectral functions both in the valence and in the core region, and we discuss the dispersion of quasi-particles and satellites. We show that self-consistency is crucial to obtain meaningful results, in particular, at large binding energies. Very good agreement with experiment is obtained when the intrinsic spectral function is corrected for extrinsic and interference effects. Finally, we sketch how one can approach the problem in the case of the two-body Green's function, and we discuss the cancellation of various dynamical effects that occur in that case.

Ab initio GW many-body effects in graphene.

We present an ab initio numerical many-body GW calculation of the band plot in freestanding graphene. We consider the full ionic and electronic structure introducing e-e interaction and correlation effects via a self-energy containing non-Hermitian and dynamical terms. With respect to the density-functional theory local-density approximation, the Fermi velocity is renormalized with an increase of 17%, in better agreement with the experiment. Close to the Dirac point the linear dispersion is modified by the presence of a kink, as observed by angle-resolved photoemission spectroscopy. We demonstrate that the kink is due to low-energy pi-->pi* single-particle excitations and to the pi plasmon. The GW self-energy does not open the band gap.

XMCD for monitoring exchange interactions. The role of the Gd 4f and 5d orbitals in metal-nitronyl nitroxide magnetic chains.

We report here the X-ray magnetic circular dichroism (XMCD) study at the Gd M(4,5)- and L(2,3)-edges of two linear magnetic chains involving Gd(III) cations bridged by nitronyl nitroxide radicals. This spectroscopy directly probes the magnetic moments of the 4f and 5d orbitals of the gadolinium ions. We compare macroscopic magnetic measurements and local XMCD signals. The M(4,5)-edges results are in agreement with the J values extracted from the fits of the SQUID magnetic measurements. The L(2,3)-edges signals show that the electronic density in the Gd 5d orbitals depends on the neighbors of the gadolinium cations. Nevertheless, the 5d orbitals do not seem to play any role in the superexchange pathway between radicals through the metal ion proposed to explain the particular magnetic exchange interactions between the radicals in these chains.