Momentum and energy dissipation of hot electrons in a Pb/Ag(111) quantum well system

The band structure of multilayer systems plays a crucial role for the ultrafast hot carrier dynamics at interfaces. Here, we study the energy- and momentum-dependent quasiparticle lifetimes of excited electrons in a highly ordered Pb monolayer film on Ag(111) prior and after the adsorption of a monolayer of 3,4,9,10-perylene-tetracarboxylic dianhydride (PTCDA). Using time-resolved two-photon momentum microscopy with femtosecond visible light pulses, we show that the electron dynamics of the Pb/Ag(111) quantum well system is largely dominated by two types of scattering processes: (i) isotropic intraband scattering processes within the quantum well state (QWS) and (ii) isotropic interband sca…

Influence of alkylphosphonic acid grafting on the electronic and magnetic properties of La2/3Sr1/3MnO3 surfaces

Self-assembled monolayers (SAMs) are highly promising materials for molecular engineering of electronic and spintronics devices thanks to their surface functionalization properties. In this direction, alkylphosphonic acids have been used to functionalize the most common ferromagnetic electrode in organic spintronics: La2/3Sr1/3MnO3 (LSMO). However, a study on the influence of SAMs grafting on LSMO electronic and magnetic properties is still missing. In this letter, we probe the influence of alkylphosphonic acids-based SAMs on the electronic and magnetic properties of the LSMO surface using different spectroscopies. We observe by X-ray photoemission and X-ray absorption that the grafting of …

Multiorbital exciton formation in an organic semiconductor

Harnessing the optoelectronic response of organic semiconductors requires a thorough understanding of the fundamental light-matter interaction that is dominated by the excitation of correlated electron-hole pairs, i.e. excitons. The nature of these excitons would be fully captured by knowing the quantum-mechanical wavefunction, which, however, is difficult to access both theoretically and experimentally. Here, we use femtosecond photoemission orbital tomography in combination with many-body perturbation theory to gain access to exciton wavefunctions in organic semiconductors. We find that the coherent sum of multiple electron-hole pair contributions that typically make up a single exciton c…

Spin-resolved low-energy and hard x-ray photoelectron spectroscopy of off-stoichiometric Co2MnSi Heusler thin films exhibiting a record TMR

Half-metallic Co2MnSi-based Heusler compounds have attracted attention because they yield very high tunnelling magnetoresistance (TMR) ratios. Record TMR ratios of 1995% (at 4.2 K) are obtained from off-stoichiometric Co2MnSi-based magnetic tunnel junctions. This work reports on a combination of band structure calculations and spin-resolved and photon-polarisation-dependent photoelectron spectroscopy for off-stoichiometric Heusler thin films with the composition Co2Mn1.30Si0.84. Co and Mn are probed by magnetic dichroism in angle-resolved photoelectron spectroscopy at the 2p core level. In contrast to the delocalised Co 3d states, a pronounced localisation of the Mn 3d states is deduced fro…

Interfacial States Cause Equal Decay of Plasmons and Hot Electrons at Gold-Metal Oxide Interfaces.

We compare the decay of plasmons and "conventional" hot electrons within the same series of gold/metal oxide interfaces. We found an accelerated decay of hot electrons at gold-metal oxide interfaces with decreasing band gap of the oxide material. The decay is accelerated by the increased phase space for electron scattering caused by additional interfacial states. Since plasmons decay faster within the same series of gold-metal oxide interfaces, we propose plasmons are able to decay into the same interfacial states as hot electrons. The similarity of plasmon damping to conventional hot electron decay implies that many classical surface analysis techniques and theoretical concepts are transfe…

Towards a full Heusler alloy showing room temperature half-metallicity at the surface

In this article we investigate the surface spin polarization in a 100 nm Co2Cr0.6Fe0.4Al (CCFA) film grown ex situ epitaxially on MgO(100) with a 10 nm Fe buffer layer by means of spin resolved photoemission. We show that a careful in situ preparation of the sample surface leads to values for the room temperature spin polarization up to 45% at the Fermi level. To our knowledge, this is the highest value measured so far at the surface region of a full Heusler alloy at room temperature.

Impact of local order and stoichiometry on the ultrafast magnetization dynamics of Heusler compounds

Nowadays, a wealth of information on ultrafast magnetization dynamics of thin ferromagnetic films exists in the literature. Information is, however, scarce on bulk single crystals, which may be especially important for the case of multi-sublattice systems. In Heusler compounds, representing prominent examples for such multi-sublattice systems, off-stoichiometry and degree of order can significantly change the magnetic properties of thin films, while bulk single crystals may be generally produced with a much more well-defined stoichiometry and a higher degree of ordering. A careful characterization of the local structure of thin films versus bulk single crystals combined with ultrafast demag…

Design of Molecular Spintronics Devices Containing Molybdenum Oxide as Hole Injection Layer

Back Cover: Mobilization upon Cooling (Angew. Chem. Int. Ed. 35/2021)

Mobilization upon Cooling

Abstract Phase transitions between different aggregate states are omnipresent in nature and technology. Conventionally, a crystalline phase melts upon heating as we use ice to cool a drink. Already in 1903, Gustav Tammann speculated about the opposite process, namely melting upon cooling. So far, evidence for such “inverse” transitions in real materials is rare and limited to few systems or extreme conditions. Here, we demonstrate an inverse phase transition for molecules adsorbed on a surface. Molybdenum tetraacetate on copper(111) forms an ordered structure at room temperature, which dissolves upon cooling. This transition is mediated by molecules becoming mobile, i.e., by mobilization up…

Enhancing Light Emission in Interface Engineered Spin-OLEDs through Spin-Polarized Injection at High Voltages

The quest for a spin-polarized organic light-emitting diode (spin-OLED) is a common goal in the emerging fields of molecular electronics and spintronics. In this device, two ferromagnetic (FM) electrodes are used to enhance the electroluminescence intensity of the OLED through a magnetic control of the spin polarization of the injected carriers. The major difficulty is that the driving voltage of an OLED device exceeds a few volts, while spin injection in organic materials is only efficient at low voltages. The fabrication of a spin-OLED that uses a conjugated polymer as bipolar spin collector layer and ferromagnetic electrodes is reported here. Through a careful engineering of the organic/…

Growth, domain structure, and atomic adsorption sites of hBN on the Ni(111) surface

One of the most important functionalities of the atomically thin insulator hexagonal boron nitride (hBN) is its ability to chemically and electronically decouple functional materials from highly reactive surfaces. It is therefore of utmost importance to uncover its structural properties on surfaces on an atomic and mesoscopic length scale. In this paper, we quantify the relative coverages of structurally different domains of a hBN layer on the Ni(111) surface using low-energy electron microscopy and the normal incidence x-ray standing wave technique. We find that hBN nucleates on defect sites of the Ni(111) surface and predominantly grows in two epitaxial domains that are rotated by ${60}^{…

Modification of the charge and magnetic order of a low dimensional ferromagnet by molecule-surface bonding

The ability to design and control the spin and charge order of low dimensional materials on the molecular scale offers an intriguing pathway towards the miniaturization of spintronic technology towards the nanometer scale. In this work, we focus on the adsorption induced modifications of the magnetic and electronic properties of a low dimensional ferromagnetic surface alloy after the adsorption of the prototypical organic molecule perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA). For this metal-organic interface, we observe the formation of a localized $\sigma$-like bond between the functional molecular groups and the surface alloy atoms. This strong chemical bonding coincides with a l…

Von geordneten zu mobilen Molekülen durch Kühlen

Phasenübergänge zwischen unterschiedlichen Aggregatzuständen sind in Natur und Technik allgegenwärtig. Üblicherweise schmilzt ein Kristall, wenn er erwärmt wird. Daher nutzen wir Eis, um einen Drink zu kühlen. Bereits im Jahre 1903 spekulierte Gustav Tammann über den umgekehrten Prozess des Schmelzens durch Kühlen. Bisher gibt es allerdings nur sehr wenige Beispiele für solche “inversen” Phasenübergänge, die meist auch auf extreme Bedingungen beschränkt sind. Hier zeigen wir einen inversen Phasenübergang von adsorbierten Molekülen auf einer Oberfläche. Molybdänacetat bildet bei Zimmertemperatur eine geordnete Struktur auf der (111)-Oberfläche von Kupfer, die sich beim Kühlen auflöst. Dieser…

Effects of post-growth annealing on structural and compositional properties of the Co2Cr0.6Fe0.4Al surface and its relevance for the surface electron spin polarization

In this study we investigate the influence of post-growth annealing on different Co2Cr0.6Fe0.4Al samples. We find strong changes in the geometric surface structure as well as in the element specific concentrations during the annealing process. These irreversible changes go in hand with characteristic changes in the electron spin polarization (ESP) at the surface: as observed in Cinchetti et al (2007 J. Phys. D: Appl. Phys. 40 1544), the iron buffered sample shows the largest spin polarization at the Fermi level. The latter remains positive as a consequence of the reduced density of states for the minority carriers due to the predicted minority gap, which can be clearly seen for all samples …

Time- and energy resolved photoemission electron microscopy-imaging of photoelectron time-of-flight analysis by means of pulsed excitations

Abstract The present work enlightens the developments in time- and energy resolved photoemission electron microscopy over the past few years. We describe basic principles of the technique and demonstrate different applications. An energy- and time-filtering photoemission electron microscopy (PEEM) for real-time spectroscopic imaging can be realized either by a retarding field or hemispherical energy analyzer or by using time-of-flight optics with a delay line detector. The latter method has the advantage of no data loss at all as all randomly incoming particles are measured not only by position but also by time. This is of particular interest for pump–probe experiments in the femtosecond an…

Spectroscopic evidence for a new type of surface resonance at noble metal surfaces

We investigated the surface and bulk properties of the pristine (110) surface of silver using threshold photoemission by excitation with light of 5.9 eV. Using a momentum microscope, we identified two distinct transitions along the $\overline{\mathrm{\ensuremath{\Gamma}}}\overline{\mathrm{Y}}$ direction of the crystal. The first one is a so far unknown surface resonance of the (110) noble-metal surface, exhibiting an exceptionally large bulk character that has so far been elusive in surface sensitive experiments. The second one stems from the well-known bulklike Mahan cone oriented along the $\mathrm{\ensuremath{\Gamma}}L$ direction inside the crystal but projected onto the (110)-surface cu…

Rücktitelbild: Von geordneten zu mobilen Molekülen durch Kühlen (Angew. Chem. 35/2021)

Spin scattering and spin-polarized hybrid interface states at a metal-organic interface

Spin scattering at the interface formed between metallic Fe and Cu-phthalocyanine molecules is investigated by spin-polarized scanning tunneling spectroscopy and spin-resolved photoemission. The results are interpreted using first-principles electronic structure theory. The combination of experimental and theoretical techniques allows us to shed light on the role of hybrid interface states for the spin scattering. We show that Cu-phthalocyanine acts, via hybrid interface states, as a local spin filter up to room temperature both below and above the Fermi energy, ${E}_{\mathrm{F}}$. At the same time, the molecule behaves as a featureless scattering barrier in a region of about 1 eV around ${…

Control of transport phenomena in magnetic heterostructures by wavelength modulation

We demonstrate the tuneablity of the ultrafast energy flow in magnetic/non-magnetic bilayer structures by changing the wavelength of the optical excitation. This is achieved by an advanced description of the temperature based $\mu$T-model that explicitly considers the wavelength- and layer-dependent absorption profile within multilayer structures. For the exemplary case of a Ni/Au bilayer, our simulations predict that the energy flow from Ni to Au is reversed when changing the wavelength of the excitation from the infrared to the ultraviolet spectral range. These predictions are fully supported by characteristic signatures in the magneto-optical Kerr traces of the Ni/Au model system. Our re…

Epitaxial film growth and magnetic properties ofCo2FeSi

We have grown thin films of the Heusler compound ${\mathrm{Co}}_{2}\mathrm{Fe}\mathrm{Si}$ by RF magnetron sputtering. On (100)-oriented MgO substrates we find fully epitaxial (100)-oriented and $L{2}_{1}$ ordered growth. On ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}(11\overline{2}0)$ substrates, the film growth is (110)-oriented, and several in-plane epitaxial domains are observed. The temperature dependence of the electrical resistivity shows a power law with an exponent of $7∕2$ at low temperatures. Investigation of the bulk magnetic properties reveals an extrapolated saturation magnetization of $5.0{\ensuremath{\mu}}_{B}∕\mathrm{f.u.}$ at $0\phantom{\rule{0.3em}{0ex}}\mathrm{K}$. The films on $…