Structural dynamics at surfaces by ultrafast reflection high-energy electron diffraction.

Many fundamental processes of structural changes at surfaces occur on a pico- or femtosecond timescale. In order to study such ultrafast processes, we have combined modern surface science techniques with fs-laser pulses in a pump-probe scheme. Grazing incidence of the electrons ensures surface sensitivity in ultrafast reflection high-energy electron diffraction (URHEED).

Interplay of Kinetic Limitations and Disintegration: Selective Growth of Hexagonal Boron Nitride and Borophene Monolayers on Metal Substrates.

The CVD growth of bielemental 2D-materials by using molecular precursors involves complex formation kinetics taking place at the surface and sometimes also subsurface regions of the substrate. Competing microscopic processes fundamentally limit the parameter space for optimal growth of the desired material. Kinetic limitations for diffusion and nucleation cause a high density of small domains and grain boundaries.

Dimer Coupling Energies of the Si(001) Surface.

The coupling energies between the buckled dimers of the Si(001) surface were determined through analysis of the anisotropic critical behavior of its order-disorder phase transition. Spot profiles in high-resolution low-energy electron diffraction as a function of temperature were analyzed within the framework of the anisotropic two-dimensional Ising model. The validity of this approach is justified by the large ratio of correlation lengths, ξ_{∥}^{+}/ξ_{⊥}^{+}=5.

Quantitative determination of the electric field strength in a plasmon focus from ponderomotive energy shifts.

Spectroscopic photoemission microscopy is used to detect and quantify a ponderomotive shift in the energy of electrons that are emitted from a surface plasmon polariton focus. The focus is formed on an atomically flat Au(111) surface by an Archimedean spiral and is spatiotemporally separated from the circularly polarized light pulse used to excite the spiral. A spectroscopic analysis of electrons emitted from the focus exhibits a peaked above-threshold electron emission spectrum.

Broad background in electron diffraction of 2D materials as a signature of their superior quality.

An unusually broad bell-shaped component (BSC) has been previously observed in surface electron diffraction on different types of 2D systems. It was suggested to be an indicator of uniformity of epitaxial graphene (Gr) and hexagonal boron nitride (hBN). In the current study we use low-energy electron microscopy and micro-diffraction to directly relate the BSC to the crystal quality of the diffracting 2D material.

Violation of Boltzmann Equipartition Theorem in Angular Phonon Phase Space Slows down Nanoscale Heat Transfer in Ultrathin Heterofilms.

Heat transfer through heterointerfaces is intrinsically hampered by a thermal boundary resistance originating from the discontinuity of the elastic properties. Here, we show that with shrinking dimensions the heat flow from an ultrathin epitaxial film through atomically flat interfaces into a single crystalline substrate is significantly reduced due to violation of Boltzmann equipartition theorem in the angular phonon phase space. For films thinner than the phonons mean free path, we find phonons trapped in the film by total internal reflection, thus suppressing heat transfer.

Segregation-Enhanced Epitaxy of Borophene on Ir(111) by Thermal Decomposition of Borazine.

Like other 2D materials, the boron-based borophene exhibits interesting structural and electronic properties. While borophene is typically prepared by molecular beam epitaxy, we report here on an alternative way of synthesizing large single-phase borophene domains by segregation-enhanced epitaxy. X-ray photoelectron spectroscopy shows that borazine dosing at 1100 °C onto Ir(111) yields a boron-rich surface without traces of nitrogen.

Equilibrium shape of single-layer hexagonal boron nitride islands on iridium.

Large, high-quality layers of hexagonal boron nitride (hBN) are a prerequisite for further advancement in scientific investigation and technological utilization of this exceptional 2D material. Here we address this demand by investigating chemical vapor deposition synthesis of hBN on an Ir(111) substrate, and focus on the substrate morphology, more specifically mono-atomic steps that are always present on all catalytic surfaces of practical use. From low-energy electron microscopy and atomic force microscopy data, we are able to set up an extended Wulff construction scheme and provide a clear elaboration of different interactions governing the equilibrium shapes of the growing hBN islands that deviate from the idealistic triangular form.

Temperature-Controlled Rotational Epitaxy of Graphene.

When graphene is placed on a crystalline surface, the periodic structures within the layers superimpose and moiré superlattices form. Small lattice rotations between the two materials in contact strongly modify the moiré lattice parameter, upon which many electronic, vibrational, and chemical properties depend. While precise adjustment of the relative orientation in the degree- and sub-degree-range can be achieved via careful deterministic transfer of graphene, we report on the spontaneous reorientation of graphene on a metallic substrate, Ir(111).

Imaging the Nonlinear Plasmoemission Dynamics of Electrons from Strong Plasmonic Fields.

We use subcycle time-resolved photoemission microscopy to unambiguously distinguish optically triggered electron emission (photoemission) from effects caused purely by the plasmonic field (termed "plasmoemission"). We find from time-resolved imaging that nonlinear plasmoemission is dominated by the transverse plasmon field component by utilizing a transient standing wave from two counter-propagating plasmon pulses of opposite transverse spin. From plasmonic foci on flat metal surfaces, we observe highly nonlinear plasmoemission up to the fifth power of intensity and quantized energy transfer, which reflects the quantum-mechanical nature of surface plasmons.

Short-range surface plasmonics: Localized electron emission dynamics from a 60-nm spot on an atomically flat single-crystalline gold surface.

We experimentally and theoretically visualize the propagation of short-range surface plasmon polaritons using atomically flat single-crystalline gold platelets on silicon substrates. We study their excitation and subfemtosecond dynamics via normal-incidence two-photon photoemission electron microscopy. By milling a plasmonic disk and grating structure into a single-crystalline gold platelet, we observe nanofocusing of the short-range surface plasmon polariton.

To tilt or not to tilt: correction of the distortion caused by inclined sample surfaces in low-energy electron diffraction.

Low-energy electron diffraction (LEED) is a widely employed technique for the structural characterization of crystalline surfaces and epitaxial adsorbates. For technical reasons the accessible reciprocal space is limited at a given primary electron energy E. This limitation may be overcome by sweeping E to observe higher diffraction orders decisively enhancing the quantitative examination.

Atomistic picture of charge density wave formation at surfaces.

We used ultrafast electron diffraction and density-functional theory calculations to gain insight into the charge density wave (CDW) formation on In/Si(111). Weak excitation by a femtosecond-laser pulse results in the melting of the CDW. The immediate freezing is hindered by a barrier for the motion of atoms during the phase transition: The melted CDW constitutes a long-lived, supercooled phase and is strong evidence for a first-order transition.

Interplay of wrinkles, strain, and lattice parameter in graphene on iridium.

Following graphene growth by thermal decomposition of ethylene on Ir(111) at high temperatures we analyzed the strain state and the wrinkle formation kinetics as function of temperature. Using the moiré spot separation in a low energy electron diffraction pattern as a magnifying mechanism for the difference in the lattice parameters between Ir and graphene, we achieved an unrivaled relative precision of ±0.1 pm for the graphene lattice parameter.

Atomically smooth p-doped silicon nanowires catalyzed by aluminum at low temperature.

Silicon nanowires (SiNWs) are powerful nanotechnological building blocks. To date, a variety of metals have been used to synthesize high-density epitaxial SiNWs through metal-catalyzed vapor phase epitaxy. Understanding the impact of the catalyst on the intrinsic properties of SiNWs is critical for precise manipulation of the emerging SiNW-based devices.

Electronic acceleration of atomic motions and disordering in bismuth.

The development of X-ray and electron diffraction methods with ultrahigh time resolution has made it possible to map directly, at the atomic level, structural changes in solids induced by laser excitation. This has resulted in unprecedented insights into the lattice dynamics of solids undergoing phase transitions. In aluminium, for example, femtosecond optical excitation hardly affects the potential energy surface of the lattice; instead, melting of the material is governed by the transfer of thermal energy between the excited electrons and the initially cold lattice.

Au stabilization and coverage of sawtooth facets on Si nanowires grown by vapor-liquid-solid epitaxy.

Si nanowires grown in UHV by Au-catalyzed vapor-liquid-solid epitaxy are known to exhibit sidewalls with {112}-type orientation that show faceting. To understand the origin of the faceting, Au induced faceting on Si(112) surfaces was studied in situ by spot-profile-analyzing low-energy electron diffraction. With increasing Au coverage at 750 degrees C, the Si(112) surface undergoes various morphological transformations until, at a critical Au coverage of about 3.

Femtosecond X-ray measurement of coherent lattice vibrations near the Lindemann stability limit.

The study of phase-transition dynamics in solids beyond a time-averaged kinetic description requires direct measurement of the changes in the atomic configuration along the physical pathways leading to the new phase. The timescale of interest is in the range 10(-14) to 10(-12) s. Until recently, only optical techniques were capable of providing adequate time resolution, albeit with indirect sensitivity to structural arrangement.