Lukasz Plucinski

Probing bulk electronic structure with hard X-ray angle-resolved photoemission

Traditional ultraviolet/soft X-ray angle-resolved photoemission spectroscopy (ARPES) may in some cases be too strongly influenced by surface effects to be a useful probe of bulk electronic structure. Going to hard X-ray photon energies and thus larger electron inelastic mean-free paths should provide a more accurate picture of bulk electronic structure. We present experimental data for hard X-ray ARPES (HARPES) at energies of 3.2 and 6.0 keV. The systems discussed are W, as a model transition-metal system to illustrate basic principles, and GaAs, as a technologically-relevant material to illustrate the potential broad applicability of this new technique. We have investigated the effects of photon wave vector on wave vector conservation, and assessed methods for the removal of phonon-associated smearing of features and photoelectron diffraction effects. The experimental results are compared to free-electron final-state model calculations and to more precise one-step photoemission theory including matrix element effects.

Bulk electronic structure of the dilute magnetic semiconductor Ga1−xMnxAs through hard X-ray angle-resolved photoemission

A detailed understanding of the origin of the magnetism in dilute magnetic semiconductors is crucial to their development for applications. Using hard X-ray angle-resolved photoemission (HARPES) at 3.2 keV, we investigate the bulk electronic structure of the prototypical dilute magnetic semiconductor Ga(0.97)Mn(0.03)As, and the reference undoped GaAs. The data are compared to theory based on the coherent potential approximation and fully relativistic one-step-model photoemission calculations including matrix-element effects. Distinct differences are found between angle-resolved, as well as angle-integrated, valence spectra of Ga(0.97)Mn(0.03)As and GaAs, and these are in good agreement with theory. Direct observation of Mn-induced states between the GaAs valence-band maximum and the Fermi level, centred about 400u2009meV below this level, as well as changes throughout the full valence-level energy range, indicates that ferromagnetism in Ga(1-x)Mn(x)As must be considered to arise from both p-d exchange and double exchange, thus providing a more unifying picture of this controversial material.

A Closer Look Into Magnetism: Opportunities With Synchrotron Radiation

The unique properties of synchrotron radiation, such as broad energy spectrum, variable light polarization, and flexible time structure, have made it an enormously powerful tool in the study of magnetic phenomena and materials. The refinement of experimental techniques has led to many new research opportunities, keeping up with the challenges put up by modern magnetism research. In this contribution, we review some of the recent developments in the application of synchrotron radiation and particularly soft X-rays to current problems in magnetism, and we discuss future perspectives.

Robust surface electronic properties of topological insulators: Bi2Te3 films grown by molecular beam epitaxy

The surface electronic properties of the important topological insulator Bi2Te3 are shown to be robust under an extended surface preparation procedure, which includes exposure to atmosphere and subsequent cleaning and recrystallization by an optimized in situ sputter-anneal procedure under ultrahigh vacuum conditions. Clear Dirac-cone features are displayed in high-resolution angle-resolved photoemission spectra from the resulting samples, indicating remarkable insensitivity of the topological surface state to cleaning-induced surface roughness.

Electronic structure, surface morphology, and topologically protected surface states of Sb2Te3 thin films grown on Si(111)

We have performed a combined spectroscopy and microscopy study on surfaces of Sb2Te3/Si(111) thin films exposed to air and annealed under ultra-high vacuum conditions. Scanning tunneling microscopy images, with atomic resolution present in most areas of such processed surfaces, show a significant amount of impurities and defects. Scanning tunneling spectroscopy reveals the bulk band gap of ∼170u2009meV centered ∼65u2009meV above the Fermi level. This intrinsic p-type doping behavior is confirmed by high-resolution angle-resolved photoemission spectra, which show the dispersions of the lower Dirac cone and the spectral weight of the bulk valence bands crossing the Fermi level. Spin-polarized photoemission revealed up to ∼15% in-plane spin polarization for photoelectrons related to the topologically protected Dirac cone states near the Fermi level, and up to ∼40% for several states at higher binding energies. The results are interpreted using ab initio electronic structure simulations and confirm the robustness of ...

Energetic, spatial, and momentum character of the electronic structure at a buried interface : The two-dimensional electron gas between two metal oxides

The interfaces between two condensed phases often exhibit emergent physical properties that can lead to new physics and novel device applications and are the subject of intense study in many disciplines. We here apply experimental and theoretical techniques to the characterization of one such interesting interface system: the two-dimensional electron gas (2DEG) formed in multilayers consisting of SrTiO3 (STO) and GdTiO3 (GTO). This system has been the subject of multiple studies recently and shown to exhibit very high carrier charge densities and ferromagnetic effects, among other intriguing properties. We have studied a 2DEG-forming multilayer of the form [6 unit cells (u.c.) STO/3 u.c. of GTO](20) using a unique array of photoemission techniques including soft and hard x-ray excitation, soft x-ray angle-resolved photoemission, core-level spectroscopy, resonant excitation, and standing-wave effects, as well as theoretical calculations of the electronic structure at several levels and of the actual photoemission process. Standing-wave measurements below and above a strong resonance have been exploited as a powerful method for studying the 2DEG depth distribution. We have thus characterized the spatial and momentum properties of this 2DEG in detail, determining via depth-distribution measurements that it is spread throughout the 6 u.c. layer of STO and measuring the momentum dispersion of its states. The experimental results are supported in several ways by theory, leading to a much more complete picture of the nature of this 2DEG and suggesting that oxygen vacancies are not the origin of it. Similar multitechnique photoemission studies of such states at buried interfaces, combined with comparable theory, will be a very fruitful future approach for exploring and modifying the fascinating world of buried-interface physics and chemistry.

Realization of a vertical topological p-n junction in epitaxial Sb2Te3/Bi2Te3 heterostructures.

Three-dimensional (3D) topological insulators are a new state of quantum matter, which exhibits both a bulk band structure with an insulating energy gap as well as metallic spin-polarized Dirac fermion states when interfaced with a topologically trivial material. There have been various attempts to tune the Dirac point to a desired energetic position for exploring its unusual quantum properties. Here we show a direct experimental proof by angle-resolved photoemission of the realization of a vertical topological p–n junction made of a heterostructure of two different binary 3D TI materials Bi2Te3 and Sb2Te3 epitaxially grown on Si(111). We demonstrate that the chemical potential is tunable by about 200u2009meV when decreasing the upper Sb2Te3 layer thickness from 25 to 6 quintuple layers without applying any external bias. These results make it realistic to observe the topological exciton condensate and pave the way for exploring other exotic quantum phenomena in the near future.

Momentum-resolved electronic structure at a buried interface from soft X-ray standing-wave angle-resolved photoemission

Angle-resolved photoemission spectroscopy (ARPES) is a powerful technique for the study of electronic structure, but it lacks a direct ability to study buried interfaces between two materials. We address this limitation by combining ARPES with soft X-ray standing-wave (SW) excitation (SWARPES), in which the SW profile is scanned through the depth of the sample. We have studied the buried interface in a prototypical magnetic tunnel junction La0.7Sr0.3MnO3/SrTiO3. Depth-and momentum-resolved maps of Mn 3d eg and t2g states from the central, bulk-like and interface-like regions of La0.7Sr0.3MnO3 exhibit distinctly different behavior consistent with a change in the Mn bonding at the interface. We compare the experimental results to state-of-the-art density-functional and one-step photoemission theory, with encouraging agreement that suggests wide future applications of this technique.

Band structure evolution during the ultrafast ferromagnetic-paramagnetic phase transition in cobalt

Using spin- and time-resolved XUV photoemission, researchers monitor the band structure evolution of Co during its phase transition. The evolution of the electronic band structure of the simple ferromagnets Fe, Co, and Ni during their well-known ferromagnetic-paramagnetic phase transition has been under debate for decades, with no clear and even contradicting experimental observations so far. Using time- and spin-resolved photoelectron spectroscopy, we can make a movie on how the electronic properties change in real time after excitation with an ultrashort laser pulse. This allows us to monitor large transient changes in the spin-resolved electronic band structure of cobalt for the first time. We show that the loss of magnetization is not only found around the Fermi level, where the states are affected by the laser excitation, but also reaches much deeper into the electronic bands. We find that the ferromagnetic-paramagnetic phase transition cannot be explained by a loss of the exchange splitting of the spin-polarized bands but instead shows rapid band mirroring after the excitation, which is a clear signature of extremely efficient ultrafast magnon generation. Our result helps to understand band structure formation in these seemingly simple ferromagnetic systems and gives first clear evidence of the transient processes relevant to femtosecond demagnetization.

Direct Observation of the Band Gap Transition in Atomically Thin ReS2

ReS2 is considered as a promising candidate for novel electronic and sensor applications. The low crystal symmetry of this van der Waals compound leads to a highly anisotropic optical, vibrational, and transport behavior. However, the details of the electronic band structure of this fascinating material are still largely unexplored. We present a momentum-resolved study of the electronic structure of monolayer, bilayer, and bulk ReS2 using k-space photoemission microscopy in combination with first-principles calculations. We demonstrate that the valence electrons in bulk ReS2 are-contrary to assumptions in recent literature-significantly delocalized across the van der Waals gap. Furthermore, we directly observe the evolution of the valence band dispersion as a function of the number of layers, revealing the transition from an indirect band gap in bulk ReS2 to a direct gap in the bilayer and the monolayer. We also find a significantly increased effective hole mass in single-layer crystals. Our results establish bilayer ReS2 as an advantageous building block for two-dimensional devices and van der Waals heterostructures.