Low Energy Electron Reflection Research Articles

Surface structure of MOVPE-prepared As-modified Si(100) substrates

In the pursuit of high-efficiency tandem devices for solar energy conversion based on III-V-semiconductors, low-defect III-V nucleation on Si(100) substrates is essential. Here, hydrogen and arsenic are key ingredients in all growth processes with respect to industrially scalable metalorganic vapor phase epitaxy. Our study provides insight into Si(100) surface preparation for the initial stage of III-V nucleation. The samples investigated, prepared on substrates with different offcut angles, show single domain surfaces consisting of rows of preferentially buckled dimers. Low energy electron diffraction and reflection anisotropy spectroscopy confirm well-defined (1 × 2)/(2 × 1) majority domains. Fourier-transform infrared spectroscopy revealed hydrogen bonding to the surface dimers, while no impurities were found by XPS. Density functional theory calculations support the experimental results and reveal a novel surface motif of H-passivated Si-As mixed dimers.

Sensitivity to crystal stacking in low-energy electron microscopy

In this work we demonstrate the general characteristics of hcp and fcc stacking in low-energy electron reflectivity for transition metal surfaces, by following the restacking during homoepitaxial growth in real-time. For this purpose, the stacking of a model system, single-crystalline Ag islands during layer-by-layer growth at high temperature on O/W(110), is chosen. Multiple scattering calculations are used to model the relation between electron reflectivity and the crystal geometry. The changes in the electron reflectivity are shown to derive from the changes in the stacking sequence of the topmost surface layers. The results allow to distinguish between the hcp and fcc crystalline arrangements at a surface based on typical differences in the reflectivity curves, making the Ag results relevant for a variety of materials with hexagonal surface geometry. In particular, the multiplet structure within the first Bragg peak in the very low electron energy regime is identified with the fcc structure and thus it can be utilized as a fingerprint to determine the stacking sequence.

Spin-dependent electron reflection at W(110)

Spin-dependent reflection of low-energy electrons at the W(110) surface caused by spin–orbit interaction was studied experimentally and theoretically. Comprehensive information for a wide range of electron incidence angles and energies was collected via maps for the reflectivity, the spin-dependent reflection asymmetry, and the figure of merit of the spin separation. The experimental results are compared with calculations of the scattering process using a realistic surface potential barrier. The results are discussed in view of possible applications of W(110) as a scattering target in spin-polarization detectors. Possible working points for use in single- as well as multi-channel spin-polarization-detection devices are identified and discussed.

Space- and time-resolved UV-to-NIR surface spectroscopy and 2D nanoscopy at 1 MHz repetition rate.

We describe a setup for time-resolved photoemission electron microscopy with aberration correction enabling 3 nm spatial resolution and sub-20 fs temporal resolution. The latter is realized by our development of a widely tunable (215-970 nm) noncollinear optical parametric amplifier (NOPA) at 1 MHz repetition rate. We discuss several exemplary applications. Efficient photoemission from plasmonic Au nanoresonators is investigated with phase-coherent pulse pairs from an actively stabilized interferometer. More complex excitation fields are created with a liquid-crystal-based pulse shaper enabling amplitude and phase shaping of NOPA pulses with spectral components from 600 to 800 nm. With this system we demonstrate spectroscopy within a single plasmonic nanoslit resonator by spectral amplitude shaping and investigate the local field dynamics with coherent two-dimensional (2D) spectroscopy at the nanometer length scale ("2D nanoscopy"). We show that the local response varies across a distance as small as 33 nm in our sample. Further, we report two-color pump-probe experiments using two independent NOPA beamlines. We extract local variations of the excited-state dynamics of a monolayered 2D material (WSe2) that we correlate with low-energy electron microscopy (LEEM) and reflectivity measurements. Finally, we demonstrate the in situ sample preparation capabilities for organic thin films and their characterization via spatially resolved electron diffraction and dark-field LEEM.

Synthesis and stacking sequence characterization of h-BN/graphene heterostructures on Cu–Ni alloy

Novel properties are found in the vertically stacked graphene and hexagonal boron nitride (h-BN) heterostructures, the performances of which could crucially depend on the stacking sequence. Nevertheless, for most heterostructures fabricated by chemical vapor deposition (CVD), the stacking sequence is uncertain. Here we introduce a facile CVD method to synthesize the h-BN/graphene stacked heterostructures on Cu–Ni alloy substrate via subsequent formation of graphene grains underneath an h-BN-graphene in-plane heterostructure layer. An efficient and non-destructive method is developed to verify the stacking sequence by low-energy electron reflectivity (LEER) measurement. This work will facilitate both fabrication and characterization of van der Waals heterostructures (vdWHs) for the future research and applications.

Integrated modeling of plasma-dielectric interaction: kinetic boundary effects

Kinetic effects of plasma-dielectric interaction are studied theoretically with respect to the mechanisms of electron extraction from solids in response to ion and electron bombardment, coupled with plasma dynamics of a weakly emissive sheath. Emission coefficients of incident beams are first calculated by quantum mechanical as well as semi-classical approaches involving Auger neutralization, energy-dependent ejection due to primary beam, and reflection of low-energy electrons, which are then incorporated into a 1D1V simulation and plasma kinetic theory. Presheath with sheath structures are derived using fluid and kinetic theory regarding ion-induced emission, respectively. The Bohm criterion considering surface emission is evaluated as well. For electron-induced emission, it is found that sheath potential is no longer collinear with plasma electron temperature in our integrated model. Additionally, reflection of low-energy electrons is justified to have a minor impact on the floating sheath for low temperature half-bounded plasma under low pressure. The combined effects of both incident ions and electrons in bounded plasma are analyzed with symmetrical/asymmetrical emission yields at two boundaries. It is then proved that wall potential is barely affected by bulk plasma influx if emission coefficients are symmetrical, while emission due to transiting beam can drastically modify the sheath solution. Electron reflection also becomes more influential if secondary electrons have low initial energy. Finally, we summarize different roles of ion and electron in sheath structure. It is shown that ion-induced emission mitigates sheath potential but cannot reach critical emission on contrast to that of electron flux.

Electron reflection effects on particle and heat fluxes to positively charged dust subject to strong electron emission

A new model describing dust charging and heating in unmagnetized plasmas in the presence of large electron emission currents is presented. By accounting for the formation of a potential well due to trapped emitted electrons when the dust is positively charged, this model extends the so-called OML+ approach, thus far limited to thermionic emission, by including electron-induced emission processes, and in particular low-energy quasi-elastic electron reflection. Revised semi-analytical formulas for the current and heat fluxes associated with emitted electrons are successfully validated against particle-in-cell simulations and predict an overall reduction of dust heating by up to a factor of 2. When applied to tungsten dust heating in divertor-like plasmas, the new model predicts that the dust lifetime increases by up to 80%, as compared with standard orbital-motion-limited estimates.

Growth of h-BN on copper (110) in a LEEM

Hexagonal boron nitride (h-BN) was grown by borazine vapour deposition on single crystalline Cu (110) substrates at 740 °C. The growth was investigated in situ using a Low-Energy Electron Microscope (LEEM). Substrates were prepared ex situ by mechanical and electrochemical methods and once in the LEEM system, by annealing in a H2 atmosphere resulting in a reconstructed surface. Exposure to borazine vapour resulted in the nucleation of well-aligned trigonal h-BN islands, which merged to ribbons along surface steps, and into larger, more irregularly shaped features. A coverage of up to 60% was achieved with an exposure of 3900 L. A diffraction ring in the low energy electron diffraction pattern was observed with a preferential alignment along the Cu 〈 111 〉 directions of the underlying substrate. Low-energy electron reflectivity scans, as well as x-ray photoelectron and Raman spectroscopies, confirmed the presence of a partial monolayer of h-BN on the surface.

Thermal desorption and stability of cobalt phthalocyanine on Ag(100)

By performing work function change (ΔWF) measurements, we characterized thermal stability and desorption of cobalt phthalocyanine (CoPc) molecules on the Ag(100) surface from sub-monolayer to multilayer coverages. Based on the temperature dependence of the ΔWF we were able to determine the desorption temperature from multilayer. Obtained dependences of ΔWF and a low-energy electron reflectivity (R) for sub- and monolayer reveal that layers with contact with Ag(100) have higher thermal stability and their desorption is accompanied by decomposition of CoPc molecule. Exploring the time evolutions of the ΔWF at various temperatures allowed us to establish effective activation energies and effective frequency prefactors for processes occurring at various temperatures. The effective activation energies remain almost the same, from sub-monolayer to multilayer (2.97 eV – 2.62 eV), whereas the frequency prefactors vary from 1013 s−1 (monolayer) to 1024 s−1 (multilayer). For multilayer only desorption occurs, whereas for layers in contact with reactive Ag(100) surface (monolayer) the decomposition occurs at the same temperature range as desorption. Low-energy electron diffraction was used to describe CoPc molecular arrangements. To the best of our knowledge, we are the first who have observed (5 × 5)R ± 37° structure for CoPc on Ag(100).

Growth, thermal desorption and low dose ion bombardment damage of C60 films deposited on Cu(111)

Auger electron spectroscopy (AES), low energy electron diffraction (LEED) and reflection electron energy loss spectrometry (REELS) were used to characterize the growth and thermal stability of C60 films deposited on Cu(111). By means of LEED we found that while C60 grows in an ordered fashion up to the first monolayer (ML) at room temperature (RT), it turns amorphous beyond that point. On the other hand, when the substrate temperature is kept at 450 K, films up to two ML with crystalline structure are obtained. For substrate temperatures beyond 570 K thick films (more than 1 ML) do not grow at all. By using AES, we found that a thick C60 film starts to desorb at a temperature around 470 K but the first ML remains stable up to temperatures as high as 900 K. A ML with a better crystalline order is obtained after desorption than that growth with the substrate at RT or higher temperatures. When the substrate is heated at 970 K, the first ML is not fully removed but the C60 molecular structure is altered or molecules break up into smaller pieces. The ion induced damage on C60 on Cu(111) films was studied for typical ions, incoming energies and irradiation doses used in low energy ion scattering (LEIS) experiments. The D-value of C(KLL) Auger spectra, the π-plasmon of REELS and the evolution of the LEIS spectra, were monitored to characterize the damage caused to the film. We found that, at low doses (∼1014 ions cm−2), damage is only detectable for massive ions like Ar, but not for H and He in the 2–8 keV range.

Thickness characterization of atomically thin WSe2 on epitaxial graphene by low-energy electron reflectivity oscillations

In this work, low-energy electron microscopy is employed to probe structural as well as electronic information in few-layer WSe2 on epitaxial graphene on SiC. The emergence of unoccupied states in the WSe2–graphene heterostructures is studied using spectroscopic low-energy electron reflectivity. Reflectivity minima corresponding to specific WSe2 states that are localized between the monolayers of each vertical heterostructure are shown to reveal the number of layers for each point on the surface. A theory for the origin of these states is developed and utilized to explain the experimentally observed featured in the WSe2 electron reflectivity. This method allows for unambiguous counting of WSe2 layers, and furthermore may be applied to other two-dimensional transition metal dichalcogenide materials.

Tuning electronic transport in epitaxial graphene-based van der Waals heterostructures.

Two-dimensional tungsten diselenide (WSe2) has been used as a component in atomically thin photovoltaic devices, field effect transistors, and tunneling diodes in tandem with graphene. In some applications it is necessary to achieve efficient charge transport across the interface of layered WSe2-graphene, a semiconductor to semimetal junction with a van der Waals (vdW) gap. In such cases, band alignment engineering is required to ensure a low-resistance, ohmic contact. In this work, we investigate the impact of graphene electronic properties on the transport at the WSe2-graphene interface. Electrical transport measurements reveal a lower resistance between WSe2 and fully hydrogenated epitaxial graphene (EG(FH)) compared to WSe2 grown on partially hydrogenated epitaxial graphene (EGPH). Using low-energy electron microscopy and reflectivity on these samples, we extract the work function difference between the WSe2 and graphene and employ a charge transfer model to determine the WSe2 carrier density in both cases. The results indicate that WSe2-EG(FH) displays ohmic behavior at small biases due to a large hole density in the WSe2, whereas WSe2-EG(PH) forms a Schottky barrier junction.

Reduction of the Low-Energy Electron Reflectivity of Ag(100) upon Adsorption of Cobalt Phthalocyanine Molecules

Using the retarding field diode method for detection of the work function changes, we explore the low-energy electron (0 to 3 eV) reflectivity of Ag(100) covered with a layer of CoPc molecules. The molecular layer significantly reduces the electron reflectivity from the sample surface. The maximum of the sample current, which is associated with minimum of electron reflectivity is observed for 1 ML of CoPc. The reflectivity is diminished from above 50% for the clean sample to almost 20% for the coverage of 1 ML. Additionally, we show that the large change in reflectivity greatly influences the determination of changes in work function (Δϕ) when the retarding field diode method is used without normalization to the saturation currents of each I–V diode curve.

Measurements of low-energy electron reflection at a plasma boundary

It is demonstrated that low-energy (<3 eV) electron reflection from a solid surface in contact with a low-temperature plasma can have significant variation with time. An uncontaminated, i.e., “clean,” metallic surface (just after heating up to glow) in a plasma environment may have practically no reflection of low-energy incident electrons. However, a contaminated, i.e., “dirty,” surface (in some time after cleaning by heating) that has a few monolayers of absorbent can reflect low-energy incident electrons and therefore significantly affect the net electron current collected by the surface. This effect may significantly change plasma properties and should be taken into account in plasma experiments and models. A diagnostic method is demonstrated for measurements of low-energy electron absorption coefficient in plasmas with a mono-energetic electron group.

Low-energy electron reflection from Au-passivated Ir(0 0 1) for application in imaging spin-filters

We describe the principle, the preparation, and the calibration of a spin-polarizing electron mirror in multichannel spin polarimetry. We show data obtained by two independent devices (a goniometer-type LEED set-up and a momentum-microscope set-up) and compare them to the results of a relativistic multiple scattering theory. We also discuss the effects of misalignment and mosaic structure of the crystal. For multi-channel detection we find a 5000-fold increase of efficiency over a single-channel spin-detector. The lifetime of the detector is more than 6 months in ultra-high vacuum.

Inelastic effects in low-energy electron reflectivity of two-dimensional materials

A simple method is proposed for inclusion of inelastic effects (electron absorption) in computations of low-energy electron reflectivity (LEER) spectra. The theoretical spectra are formulated by matching of electron wavefunctions obtained from first-principles computations in a repeated vacuum–slab–vacuum geometry. Inelastic effects are included by allowing these states to decay in time in accordance with an imaginary term in the potential of the slab, and by mixing of the slab states in accordance with the same type of distribution as occurs in a free-electron model. LEER spectra are computed for various two-dimensional materials, including free-standing multilayer graphene, graphene on copper substrates, and hexagonal boron nitride on cobalt substrates.

Origin of chemical contrast in low-energy electron reflectivity of correlated multivalent oxides: The case of ceria

A combined experimental and theoretical study of the local chemistry of cerium oxide films and islands on Ru(0001) is presented. Based on intensity-voltage low-energy electron microscopy [$I(V)$-LEEM] and resonant x-ray photoemission spectroscopy, we establish a one-to-one correspondence between the local oxidation state of ${\mathrm{Ce}}^{3+}$ [cubic Ce${}_{2}$O${}_{3}$(111)] and ${\mathrm{Ce}}^{4+}$ [cubic CeO${}_{2}$(111)] and their respective spatially resolved $I(V)$ curves. Ab initio scattering theory explains the difference between the $I(V)$ curves in the low-energy range in terms of the ${k}_{\ensuremath{\parallel}}=0$ projected band structure arising from the different structure of the Ce 5d states in fully oxidized and reduced ceria. The theoretical analysis unambiguously attributes the LEEM contrast observed for chemically reduced cerium oxide to a variation in oxidation state on the nanometer scale, which is not present for the as-grown islands.

Formation of two-dimensional uranium silicide film and its electronic structure study

Uranium (U) deposition onto the Si (111) − 7×7 surface followed by annealing at 870K for 6min leads to the formation of 2D uranium silicide (USi1.67) film. The morphology and geometric structure have been studied by scanning tunneling microscopy (STM), low-energy electron diffraction (LEED) and reflection high energy electron diffraction (RHEED). The AlB2-type structure of USi1.67 epitaxial film is formed with a 1×1 periodicity. Morphologies of the crystalline USi1.67 film display triangular layered structures, and its electronic structure has been studied by a combination of angle-resolved photoemission spectroscopy (ARPES) and density functional theory calculations.

Low-energy electron reflectivity of graphene on copper and other substrates

The reflectivity of low energy electrons from graphene on copper substrates is studied both experimentally and theoretically. Well-known oscillations in the reflectivity of electrons with energies 0 - 8 eV above the vacuum level are observed in the experiment. These oscillations are reproduced in theory, based on a first-principles density functional description of interlayer states forming for various thicknesses of multilayer graphene. It is demonstrated that n layers of graphene produce a regular series of n-1 minima in the reflectance spectra, together with a possible additional minimum associated with an interlayer state forming between the graphene and the substrate. Both (111) and (001) orientations of the copper substrates are studied. Similarities in their reflectivity spectra arise from the interlayer states, whereas differences are found because of the different Cu band structures along those orientations. Results for graphene on other substrates, including Pt(111) and Ir(111), are also discussed.

Quantitative spin polarization analysis in photoelectron emission microscopy with an imaging spin filter

Using a photoelectron emission microscope (PEEM), we demonstrate spin-resolved electron spectroscopic imaging of ultrathin magnetic Co films grown on Cu(100). The spin-filter, based on the spin-dependent reflection of low energy electrons from a W(100) crystal, is attached to an aberration corrected electrostatic energy analyzer coupled to an electrostatic PEEM column. We present a method for the quantitative measurement of the electron spin polarization at 4 × 10³ points of the PEEM image, simultaneously. This approach uses the subsequent acquisition of two images with different scattering energies of the electrons at the W(100) target to directly derive the spin polarization without the need of magnetization reversal of the sample.