Ruslan Ovsyannikov

Large Tunable Rashba Spin Splitting of a Two-Dimensional Electron Gas in Bi2Se3

We report a Rashba spin splitting of a two-dimensional electron gas in the topological insulator Bi(2)Se(3) from angle-resolved photoemission spectroscopy. We further demonstrate its electrostatic control, and show that spin splittings can be achieved which are at least an order-of-magnitude larger than in other semiconductors. Together these results show promise for the miniaturization of spintronic devices to the nanoscale and their operation at room temperature.

Efficient light emission from inorganic and organic semiconductor hybrid structures by energy-level tuning

The fundamental limits of inorganic semiconductors for light emitting applications, such as holographic displays, biomedical imaging and ultrafast data processing and communication, might be overcome by hybridization with their organic counterparts, which feature enhanced frequency response and colour range. Innovative hybrid inorganic/organic structures exploit efficient electrical injection and high excitation density of inorganic semiconductors and subsequent energy transfer to the organic semiconductor, provided that the radiative emission yield is high. An inherent obstacle to that end is the unfavourable energy level offset at hybrid inorganic/organic structures, which rather facilitates charge transfer that quenches light emission. Here, we introduce a technologically relevant method to optimize the hybrid structures energy levels, here comprising ZnO and a tailored ladder-type oligophenylene. The ZnO work function is substantially lowered with an organometallic donor monolayer, aligning the frontier levels of the inorganic and organic semiconductors. This increases the hybrid structures radiative emission yield sevenfold, validating the relevance of our approach.

Single bunch X-ray pulses on demand from a multi-bunch synchrotron radiation source

Synchrotron radiation facilities routinely operate in a multi-bunch regime, but applications relying on time-of-flight schemes require single bunch operation. Here we show that pulse picking by resonant excitation in a storage ring creates in addition to the multi-bunch operation a distinct and separable single bunch soft X-ray source. It has variable polarization, a photon flux of up to 10(7)-10(9)u2009phu2009s(-1)/0.1%BW at purity values of 10(4)-10(2) and a repetition rate of 1.25u2009MHz. The quasi-resonant excitation of incoherent betatron oscillations of electrons allows horizontal pulse separation at variable (also circular) polarization accessible for both, regular 30u2009ps pulses and ultrashort pulses of 2-3u2009ps duration. Combined with a new generation of angularly resolving electron spectrometers this creates unique opportunities for time-resolved photoemission studies as confirmed by time-of-flight spectra. Our pulse picking scheme is particularly suited for surface physics at diffraction-limited light sources promising ultimate spectral resolution.

Communication: Influence of graphene interlayers on the interaction between cobalt phthalocyanine and Ni(111)

The influence of graphene interlayers on electronic interface properties of cobalt phthalocyanine on Ni(111) is studied using both photoemission and X-ray absorption spectroscopy. A charge transfer associated with a redistribution of the d-electrons at the Co-atom of the phthalocyanine occurs at the interface to Ni(111). Even a graphene buffer layer cannot prevent the charge transfer at the interface to Ni(111); however, the detailed electronic situation is different.

Chemisorption, morphology, and structure of a n-type perylene diimide derivative at the interface with gold: influence on devices from thin films to single molecules.

We have investigated thin films of a perylene diimide derivative with a cyano-functionalized core (PDI-8CN2) deposited on Au(111) single crystals from the monolayer to the multilayer regime. We found that PDI-8CN2 is chemisorbed on gold. The molecules experience a thickness-dependent reorientation, and a 2D growth mode with molecular stepped terraces is achieved adopting low deposition rates. The obtained results are discussed in terms of their impact on field effect devices, also clarifying why the use of substrate/contact treatments, decoupling PDI-8CN2 molecules from the substrate/contacts, is beneficial for such devices. Our results also suggest that perylene diimide derivatives with CN bay-functionalization are very promising candidates for single-molecule electronic devices.

Partially Reversible Photoinduced Chemical Changes in a Mixed-Ion Perovskite Material for Solar Cells

Metal halide perovskites have emerged as materials of high interest for solar energy-to-electricity conversion, and in particular, the use of mixed-ion structures has led to high power conversion efficiencies and improved stability. For this reason, it is important to develop means to obtain atomic level understanding of the photoinduced behavior of these materials including processes such as photoinduced phase separation and ion migration. In this paper, we implement a new methodology combining visible laser illumination of a mixed-ion perovskite ((FAPbI3)0.85(MAPbBr3)0.15) with the element specificity and chemical sensitivity of core-level photoelectron spectroscopy. By carrying out measurements at a synchrotron beamline optimized for low X-ray fluxes, we are able to avoid sample changes due to X-ray illumination and are therefore able to monitor what sample changes are induced by visible illumination only. We find that laser illumination causes partially reversible chemistry in the surface region, including enrichment of bromide at the surface, which could be related to a phase separation into bromide- and iodide-rich phases. We also observe a partially reversible formation of metallic lead in the perovskite structure. These processes occur on the time scale of minutes during illumination. The presented methodology has a large potential for understanding light-induced chemistry in photoactive materials and could specifically be extended to systematically study the impact of morphology and composition on the photostability of metal halide perovskites.

Angle-resolved time-of-flight spectroscopy applied to multi-bunch operation at MAX-lab: a design study

Angle-resolved time-of-flight (ARTOF) spectrometers have found use in a number of applications, including ARPES. However, the fundamental requirement of an external start trigger matching the read-out time of the instrument limits its usability at many storage rings. Hitherto all reported experiments have been performed at storage rings capable of running in single-bunch mode. To eliminate this restriction, we propose a method where a pulsed electronic gate is introduced to allow for ARTOF usage at normal multi-bunch operation of the MAX II storage ring. This paper will show the working principle and outline the design for this technique.

Doping and oxidation effects under ambient conditions in copper surfaces: a “real-life” CuBe surface

Cu-Based materials are used in a variety of industrial applications from mechanics to electronics; thus, it is important to know the mechanisms occurring at their surfaces under ambient conditions. We investigate the CuBe surface by using a combination of soft X-ray spectroscopies, atomic force microscopy and first-principles calculations. We find that this surface behaves upon oxidation under ambient conditions very similarly to a pure copper surface: the oxidation process under ambient conditions leads to the formation of native Cu2O, while beryllium does not affect the electronic properties of the substrate. We have also investigated the role of mild annealing in ultra-high vacuum: after annealing, the CuBe surface shows the typical features of a metallic copper surface, with segregation of beryllium at the surface and its on-site oxidization. Our work elucidates the mechanisms leading to the real-life properties of this surface, accounting for its high performance in industrial applications.

Time-resolved soft X-ray absorption spectroscopy in transmission mode on liquids at MHz repetition rates

We present a setup combining a liquid flatjet sample delivery and a MHz laser system for time-resolved soft X-ray absorption measurements of liquid samples at the high brilliance undulator beamline UE52-SGM at Bessy II yielding unprecedented statistics in this spectral range. We demonstrate that the efficient detection of transient absorption changes in transmission mode enables the identification of photoexcited species in dilute samples. With iron(II)-trisbipyridine in aqueous solution as a benchmark system, we present absorption measurements at various edges in the soft X-ray regime. In combination with the wavelength tunability of the laser system, the set-up opens up opportunities to study the photochemistry of many systems at low concentrations, relevant to materials sciences, chemistry, and biology.

Effect of halide ratio and Cs+ addition on the photochemical stability of lead halide perovskites

Lead halide perovskite solar cells with multi-cation/mixed halide materials now give power conversion efficiencies of more than 20%. The stability of these mixed materials has been significantly improved through the addition of Cs+ compared to the original methylammonium lead iodide. However, it remains one of the most significant challenges for commercialisation. In this study, we use photoelectron spectroscopy (PES) in combination with visible laser illumination to study the photo-stability of perovskite films with different compositions. These include Bru2006:u2006I ratios of 50u2006:u200650 and 17u2006:u200683 and compositions with and without Cs+. For the samples without Cs and the 50u2006:u200650 samples, we found that the surface was enriched in Br and depleted in I during illumination and that some of the perovskite decomposed into Pb0, organic halide salts, and iodine. After illumination, both of these reactions were partially reversible. Furthermore, the surfaces of the films were enriched in organic halide salts indicating that the cations were not degraded into volatile products. With the addition of Cs+ to the samples, photo-induced changes were significantly suppressed for a 50u2006:u200650 bromide to iodide ratio and completely suppressed for perovskites with a 17u2006:u200683 ratio at light intensities exceeding 1 sun equivalent.