Matching emission centers of electrons and photons in current-carrying silver nanoparticle films.

Current flow through a nanoparticle film (two-dimensional ensemble of small tunnel-coupled metal particles on a dielectric substrate) is accompanied by electron and photon emission. It has a localized character (originates from emission centers). With an increase in applied voltage, the number of emission centers increases, and with further increase, some of them may burn out. In dark conditions, photon emission centers are visible with a bare eye. To visualize electron emission centers, emission electron microscopy is used. The conducted measurements allow comparison of the number and relative positions of electron and photon emission centers. It is shown that electrons and photons are emitted from the same centers.

Near-Edge X-ray Absorption Fine Structure Investigation of the Quasi-One-Dimensional Organic Conductor (TMTSF)2PF6.

We present high-resolution near-edge X-ray absorption fine structure (NEXAFS) measurements at the P L2/3 edges, F K edge, C K edge, and Se M2/3 edges of the quasi-one-dimensional (1D) conductor and superconductor (TMTSF)2PF6. NEXAFS allows probing the donor and acceptor moieties separately; spectra were recorded between room temperature (RT) and 30 K at normal incidence. Spectra taken around RT were also studied as a function of the angle (θ) between the electric field of the X-ray beam and the 1D conducting direction. In contrast with a previous study of the S L2/3-edges spectra in (TMTTF)2AsF6, the Se M2/3 edges of (TMTSF)2PF6 do not exhibit a well-resolved spectrum. Surprisingly, the C K-edge spectra contain three well-defined peaks exhibiting strong and nontrivial θ and temperature dependence. The nature of these peaks as well as those of the F K-edge spectra could be rationalized on the basis of first-principles DFT calculations. Despite the structural similarity, the NEXAFS spectra of (TMTSF)2PF6 and (TMTTF)2AsF6 exhibit important differences. In contrast with the case of (TMTTF)2AsF6, the F K-edge spectra of (TMTSF)2PF6 do not change with temperature despite stronger donor-anion interactions. All these features reveal subtle differences in the electronic structure of the TMTSF and TMTTF families of salts.

Microscopic origin of the charge transfer in single crystals based on thiophene derivatives: A combined NEXAFS and density functional theory approach.

We have investigated the charge transfer mechanism in single crystals of DTBDT-TCNQ and DTBDT-F4TCNQ (where DTBDT is dithieno[2,3-d;2',3'-d'] benzo[1,2-b;4,5-b']dithiophene) using a combination of near-edge X-ray absorption spectroscopy (NEXAFS) and density functional theory calculations (DFT) including final state effects beyond the sudden state approximation. In particular, we find that a description that considers the partial screening of the electron-hole Coulomb correlation on a static level as well as the rearrangement of electronic density shows excellent agreement with experiment and allows to uncover the details of the charge transfer mechanism in DTBDT-TCNQ and DTBDT-F4 TCNQ, as well as a reinterpretation of previous NEXAFS data on pure TCNQ. Finally, we further show that almost the same quality of agreement between theoretical results and experiment is obtained by the much faster Z+1/2 approximation, where the core hole effects are simulated by replacing N or F with atomic number Z with the neighboring atom with atomic number Z+1/2.

Donor-anion interactions at the charge localization and charge ordering transitions of (TMTTF)2AsF6 probed by NEXAFS.

High-resolution near-edge X-ray absorption fine structure (NEXAFS) measurements at the As M-edge, F K-edge and S L-edge of the Fabre salt (TMTTF)2AsF6 were performed from room temperature (RT) to 90 K, allowing to reach the charge localization regime below Tρ ≈ 230 K and to cross the charge ordering (CO) transition at TCO ≈ 102 K. The F K-edge and S L-edge spectra exhibit several transitions which have been indexed on the basis of first-principles DFT calculations. Upon cooling from RT significant energy shifts up to +0.8 eV and -0.4 eV were observed in transitions exhibited by the F 1s and S 2p spectra respectively, while the As 3p doublet does not show a significant shift. Opposite energy shifts found in the F 1s and S 2p spectra reflect substantial thermal changes in the electronic environment of F atoms of the anion and S atoms of TMTTF. The changes found around the charge localization crossover suggest an increase of the participation of the S d orbitals in the empty states of TMTTF as well as an increase of the strength of donoranion interactions. A new F 1s pre-edge signal detected upon entry into the CO phase is a clear fingerprint of the symmetry breaking occurring at TCO. We propose that this new transition is caused by a substantial mixing between the HOMO of the AsF6(-) anion and the unoccupied part of the TMTTF HOMO conduction band. Analysis of the whole spectra also suggests that the loss of the inversion symmetry associated with the CO is due to an anion displacement increasing the strength of SF interactions. Our data show unambiguously that anions are not, as previously assumed, innocent spectators during the electronic modifications experienced by the Fabre salts upon cooling. In particular the interpretation of the spectra pointing out a thermally dependent mixing of anion wave functions with those of the TMTTF chains demonstrates for the first time the importance of anion-donor interactions.

Quantitative measurements of magnetic stray field dynamics of Permalloy particles in a photoemission electron microscopy.

By example of a Permalloy particle (40 × 40 µm(2) size, 30 nm thickness) we demonstrate a procedure to quantitatively investigate the dynamics of magnetic stray fields during ultrafast magnetization reversal. The measurements have been performed in a time-resolving photoemission electron microscope using the X-ray magnetic circular dichroism. In the particle under investigation, we have observed a flux-closure-dominated magnetic ground structure, minimizing the magnetic stray field outside the sample. A fast magnetic field pulse introduced changes in the micromagnetic structure accompanied with an incomplete flux closure. As a result, stray fields arise along the edges of domains, which cause a change of contrast and an image deformation of the particles geometry (curvature of its edge). The magnetic stray fields are calculated from a deformation of the X-ray magnetic circular dichroism (XMCD) images taken after the magnetic field pulse in a 1 ns interval. These measurements reveal a decrease of magnetic stray fields with time. An estimate of the lower limit of the domain wall velocity yields about 2 × 10(3) m s(-1).

Measurement of potential distribution function on object surface by using an electron microscope in the mirror operation mode.

The quantitative theory of image contrast in an electron microscope in the mirror operation mode is given in this paper. This theory permits us to calculate the potential distribution on the object surface from the current density distribution on the microscope screen. The potential distribution results in image formation on the screen. Local electric fields existing on the object surface lead to a perturbation of electron trajectories above the object and to a redistribution of the current density on the screen, causing image contrast. Using the quantitative correlation between these fields and the function of current density distribution on the screen, it is possible to calculate the magnitude of these microfields as well. As illustration, a measured potential distribution on an object surface with spiral structures of adsorbates was analysed. These structures are formed during reaction of CO oxidation on Pt(110). The value of the measured contact potential difference comprised a few hundredths of volt.

Electronic structure of large disc-type donors and acceptors.

Searching for new pi-conjugated charge-transfer systems, the electronic structure of a new acceptor-donor pair derived from coronene (C(24)H(12)) was investigated by ultraviolet photoelectron spectroscopy (UPS). The acceptor coronene-hexaone (C(24)H(6)O(6), in the following abbreviated as COHON) and the donor hexamethoxycoronene (C(30)H(24)O(6), abbreviated as HMC) were adsorbed as pure and mixed phases on gold substrates. At low coverage, COHON adsorption leads to the appearance of a charge-transfer induced interface state 1.75 eV below the Fermi energy. At multilayer coverage the photoemission intensity of the interface state drops and the valence spectrum of neutral COHON appears. The sample work function decreases from 5.3 eV (clean Au) to 4.8 eV (monolayer) followed by an increase to 5.6 eV (multilayer). The formation of a significant interface dipole due to charge-transfer at the metal-organic interface is possibly accompanied by a change in molecular orientation. HMC on Au exhibits no interface state and the sample work function decreases monotonically to ca. 4.8 eV (multilayer). The UPS spectra of individual donor and acceptor multilayers show good agreement with density functional theory modeling. In donor/acceptor mixed films the photoemission signal of the donor (acceptor) shifts to higher (lower) binding energy. This trend is predicted by the calculation and is anticipated when charge is transferred from donor to acceptor. We propose that mixed films of COHON and HMC constitute a weak charge-transfer system.

High-pass energy-filtered photoemission electron microscopy imaging of dopants in silicon.

Differently doped areas in silicon can show strong electron-optical contrast in dependence on the dopant concentration and surface conditions. Photoemission electron microscopy is a powerful surface-sensitive technique suitable for fast imaging of doping-induced contrast in semiconductors. We report on the observation of Si (100) samples with n- and p-type doped patterns (with the dopant concentration varied from 10(16) to 10(19) cm(-3)) on a p- and n-type substrate (doped to 10(15) cm(-3)), respectively. A high-pass energy filter of the entire image enabled us to obtain spectroscopic information, i.e. quantified photo threshold and related photoyield differences depending on the doping level. Measurements have confirmed the possibility of resolving areas at a high contrast even with the lowest dopant concentration when employing the energy filter. The influence of electron absorption phenomena on contrast formation is discussed.

Spin texture of time-reversal symmetry invariant surface states on W(110).

We find in the case of W(110) previously overlooked anomalous surface states having their spin locked at right angle to their momentum using spin-resolved momentum microscopy. In addition to the well known Dirac-like surface state with Rashba spin texture near the -point, we observe a tilted Dirac cone with circularly shaped cross section and a Dirac crossing at 0.28 × within the projected bulk band gap of tungsten. This state has eye-catching similarities to the spin-locked surface state of a topological insulator. The experiments are fortified by a one-step photoemission calculation in its density-matrix formulation.

Anomalous d-like surface resonances on Mo(110) analyzed by time-of-flight momentum microscopy.

The electronic surface states on Mo(110) have been investigated using time-of-flight momentum microscopy with synchrotron radiation (hν=35 eV). This novel angle-resolved photoemission approach yields a simultaneous acquisition of the E-vs-k spectral function in the full surface Brillouin zone and several eV energy interval. (kx,ky,EB)-maps with 3.4 Å(-1) diameter reveal a rich structure of d-like surface resonances in the spin-orbit induced partial band gap. Calculations using the one-step model in its density matrix formulation predict an anomalous state with Dirac-like signature and Rashba spin texture crossing the bandgap at Γ¯ and EB=1.2 eV. The experiment shows that the linear dispersion persists away from the Γ¯-point in an extended energy- and k∥-range. Analogously to a similar state previously found on W(110) the dispersion is linear along H¯-Γ¯-H¯ and almost zero along N¯-Γ¯-N¯. The similarity is surprising since the spin-orbit interaction is 5 times smaller in Mo. A second point with unusual topology is found midway between Γ¯ and N¯. Band symmetries are probed by linear dichroism.

Growth of rodlike silver nanoparticles by vapor deposition of small clusters.

A beam of silver clusters of 3 nm average diameter is produced by the gas-aggregation technique and deposited onto the NaCl (100) surface. Subsequent agglomeration leads in part to the growth of rodlike particles with the structure of truncated decahedra of typical dimensions 70 nm long and 10 nm diameter and a fivefold symmetry, as shown in the picture. A growth mechanism is inferred from a detailed analysis of electron microscopy data.

Imaging spin filter for electrons based on specular reflection from iridium (001).

As Stern-Gerlach type spin filters do not work with electrons, spin analysis of electron beams is accomplished by spin-dependent scattering processes based on spin-orbit or exchange interaction. Existing polarimeters are single-channel devices characterized by an inherently low figure of merit (FoM) of typically 10⁻4-10⁻³. This single-channel approach is not compatible with parallel imaging microscopes and also not with modern electron spectrometers that acquire a certain energy and angular interval simultaneously. We present a novel type of polarimeter that can transport a full image by making use of k-parallel conservation in low-energy electron diffraction. We studied specular reflection from Ir (001) because this spin-filter crystal provides a high analyzing power combined with a "lifetime" in UHV of a full day. One good working point is centered at 39 eV scattering energy with a broad maximum of 5 eV usable width. A second one at about 10 eV shows a narrower profile but much higher FoM. A relativistic layer-KKR SPLEED calculation shows good agreement with measurements.

Self-trapping of magnetic oscillation modes in Landau flux-closure structures.

We investigated the magnetodynamics in rectangular Permalloy platelets by means of time-resolved x-ray photoemission microscopy. 10 nm thick platelets of size 16 x 32 microm were excited by an oscillatory field along the short side of the sample with a fundamental frequency of 500 MHz and considerable contributions of higher harmonics. Under the influence of the oscillatory field, the Néel wall in the initial classical Landau pattern shifts away from the center, corresponding to an induced magnetic moment perpendicular to the exciting field. This phenomenon is explained by a self-trapping effect of the dominating spin-wave mode when the system is excited just below the resonance frequency. The basic driving mechanism is the maximization of entropy.

Peculiarities of imaging one- and two-dimensional structures using an electron microscope in the mirror operation mode.

Measurements performed in an electron microscope with the mirror operation mode are most sensitive to local electric fields and geometrical roughness of any kind of the object being studied. The object with a geometrical relief is equivalent to a smooth surface with an effective distribution of microfields. Electrons forming the image interact with the local microfields for an extended time: during approach to the object, deceleration and acceleration away from the object. As a result, the electron trajectories can be strongly distorted, and the contrast changes essentially, leading to image deformation of details of the object under investigation and to lowering of the resolution. These effects are theoretically described and are illustrated by experiments. An analysis of these effects enables the real size and the shape of the object involved to be reconstructed.

Use of emission electron microscope for potential mapping in semiconductor microelectronics.

An emission electron microscope was used for visualization and measurement of the distribution of electric fields and potentials on the surface under study. The contrast of microfields is caused by the fact that slow-moving electrons emitted from the object surface are deflected by these fields. The measurements were performed on a p-n junction to which a voltage was applied. It is shown that the type of contrast from the p-n junction can be reversed depending on the position of the contrast aperture restricting the electron beam. The same result was obtained by means of a computer simulation.

Measurement of the electric field distribution and potentials on the object surface in an emission electron microscope without restriction of the electron beams.

An emission electron microscope without restriction of the electron beams was used to visualize and measure the distribution of electric fields and potentials on the surface under study. Investigations of this kind can be performed in an emission electron microscope without any aperture diaphragm. The potentialities of this method have been demonstrated using measurements with a silicon p-n junction to which a voltage has been applied in the reverse direction. The quantitative analysis becomes more complicated if the specimen is characterized by a heterogeneous intensity distribution of the electron emission from different areas of its surface. In the latter case two images obtained at different accelerating voltages (i.e. different voltages of the microscope extractor) provide the information necessary for an analysis of electric field and potential distributions.

Imaging of three-dimensional objects in emission electron microscopy.

Under investigation by emission electron microscopy, the shape and size of three-dimensional objects are distorted because of the appearance of a characteristic potential relief and a possible contact potential difference between the particles and the substrate. An estimation of these effects for spherical particles is made. It is shown that the apparent size of particles observed in an emission electron microscope (EEM) could be increased as well as decreased depending on the relation between the work functions of the particle and the substrate. The corresponding formulae are given and several possibilities are shown which permit us to determine from the EEM image the real size of particles and their work function relative to the substrate.