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At least 703 records · Page 39

Electronic structure evolution of fullerene on CH 3 NH 3 PbI 3

The thickness dependence of fullerene on CH 3 NH 3 PbI 3 perovskitefilm surface has been investigated by using ultraviolet photoemission spectroscopy (UPS), X-ray photoemission spectroscopy(XPS), and inverse photoemission spectroscopy (IPES). The lowest unoccupied molecular orbital and highest occupied molecular orbital (HOMO) can be observed directly with IPES and UPS. It is observed that the HOMO level in fullerene shifts to lower binding energy. The XPS results show a strong initial shift of core levels to lower binding energy in the perovskite, which indicates that electrons transfer from the perovskitefilm to fullerene molecules. Further deposition of fullerene forms C 60 solid, accompanied by the reduction of the electron transfer. As a result, the strongest electron transfer happened at 1/4 monolayer of fullerene.

36 MATERIALS SCIENCE↗

Itinerant electrons, local moments, and magnetic correlations in the pnictide superconductors CeFeAsO₁₋ x F x and Sr(Fe₁₋ x Co x )₂As₂

A direct and element-specific measurement of the local Fe spin moment has been provided by analyzing the Fe 3s core level photoemission spectra in the parent and optimally doped CeFeAsO₁₋ x F x (x = 0, 0.11) and Sr(Fe₁₋ x Co x )2As2 (x = 0, 0.10) pnictides. The rapid time scales of the photoemission process allowed the detection of large local spin moments fluctuating on a 10⁻¹⁵ s time scale in the paramagnetic, antiferromagnetic, and superconducting phases, indicative of the occurrence of ubiquitous strong Hund's magnetic correlations. The magnitude of the spin moment is found to vary significantly among different families, 1.3μ B in CeFeAsO and 2.1μB in SrFe₂As₂. Surprisingly, the spin moment is found to decrease considerably in the optimally doped samples, 0.9μ B in CeFeAsO₀.₈₉F₀.₁₁ and 1.3μ B in Sr(Fe₀.₉Co₀.₁)₂As₂. The strong variation of the spin moment against doping and material type indicates that the spin moments and the motion of itinerant electrons are influenced reciprocally in a self-consistent fashion, reflecting the strong competition between the antiferromagnetic superexchange interaction among the spin moments and the kinetic energy gain of the itinerant electrons in the presence of a strong Hund's coupling. By describing the evolution of the magnetic correlations concomitant with the appearance of superconductivity, these results constitute a fundamental step toward attaining a correct description of the microscopic mechanisms shaping the electronic properties in the pnictides, including magnetism and high-temperature superconductivity.

Vilmercati, Paolo↗

Surface localisation of laser photoelectron emission using Cu{sub 2}O and Ag film structures

A laser electron source localised on a photocathode surface was developed on the basis of Ag and Cu{sub 2}O thin films sequentially deposited by magnetron sputtering on a glass substrate. Photoemission of electrons under the action of the fourth (263 nm) harmonic of a femtosecond fibre laser was initiated from the surface of an Ag film deposited on the substrate surface. Photoelectron source localisation on the photocathode surface was provided by sputtering the Cu{sub 2}O copper oxide film on its surface, which significantly (about 50 times) reduced the photoemission efficiency, and by subsequent removal of the copper oxide layer in the photoemission spot with a diameter of ∼15 μm by means of focused second-harmonic radiation of a femtosecond fibre laser. In conducting research on the photocathode surface, a grid of photoemission spots was formed, which greatly facilitated the laser beam alignment with the photoemission spot. A decrease in the noises of ultrafast transmission electron microscope, associated with spatial fluctuations of the laser beam initiating pulsed photoelectron emission from the microscope photocathode when using a localised electron source on the basis of a structure of thin Cu{sub 2}O and Ag films, was experimentally demonstrated. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Bipolar charging of dust particles under ultraviolet radiation

The photoemission charging of dust particles under ultraviolet radiation from a xenon lamp has been investigated. The velocities of yttrium dust particles with a work function of 3.3 eV and their charges have been determined experimentally; the latter are about 400-500 and about 100 elementary charges per micron of radius for the positively and negatively charged fractions, respectively. The dust particle charging and the dust cloud evolution in a photoemission cell after exposure to an ultraviolet radiation source under the applied voltage have been simulated numerically. The photoemission charging of dust particles has been calculated on the basis of nonlocal and local charging models. Only unipolar particle charging is shown to take place in a system of polydisperse dust particles with the same photoemission efficiency. It has been established that bipolar charging is possible in the case of monodisperse particles with different quantum efficiencies. Polydispersity in this case facilitates the appearance of oppositely charged particles in a photoemission plasma.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Interferometric Plasmonic Lensing with Nanohole Arrays

Nonlinear photoemission electron microscopy (PEEM) of nanohole arrays in gold films maps propagating surface plasmons (PSPs) launched from lithographically patterned structures. Strong near field photoemission patterns are observed in the PEEM images, recorded following low angle of incidence irradiation of nanohole arrays with sub-15 fs laser pulses centered at 780 nm. The recorded photoemission patterns are attributed to constructive and destructive interferences between PSPs launched from the individual nanoholes which comprise the array. By exploiting the wave nature of PSPs, we demonstrate how varying the array geometry (hole diameter, pitch, and number of rows/columns) ultimately yields intense localized photoemission. Through a combination of PEEM and finite-difference time-domain simulations, we identify the optimal array geometry for efficient light coupling and interferometric plasmonic lensing. We show a preliminary application of inteferometric plasmonic lensing by enhancing the photoemission from the vertex of a gold triangle using nanohole array.

Gong, Yu↗

Silver nanorod arrays for photocathode applications

In this study, we explore the possibility of using plasmonic Ag nanorod arrays featuring enhanced photoemission as high-brightness photocathode material. Silver nanorod arrays are synthesized by the DC electrodeposition method and their dimensionality, uniformity, crystallinity and oxide/impurity content are characterized. These Ag nanorod arrays exhibit greatly enhanced two-photon photoemission under 400 nm femtosecond pulsed laser excitation. Plasmonic field enhancement in the array produces photoemission hot spots that are mapped using photoemission electron microscopy (PEEM). The relative photoemission enhancement of nanorod array hot spots relative to that of a flat Ag thin film is found to range between 102 and 3 x 10 3 .

14 SOLAR ENERGY↗

Revealing Hidden Orbital Pseudospin Texture with Time-Reversal Dichroism in Photoelectron Angular Distributions

We performed angle-resolved photoemission spectroscopy (ARPES) of bulk 2H-WSe 2 for different crystal orientations linked to each other by time-reversal symmetry. We introduce a new observable called time-reversal dichroism in photoelectron angular distributions (TRDAD), which quantifies the modulation of the photoemission intensity upon effective time-reversal operation. We demonstrate that the hidden orbital pseudospin texture leaves its imprint on TRDAD, due to multiple orbital interference effects in photoemission. Our experimental results are in quantitative agreement with both the tight-binding model and state-of-the-art fully relativistic calculations performed using the one-step model of photoemission. While spin-resolved ARPES probes the spin component of entangled spin-orbital texture in multiorbital systems, we unambiguously demonstrate that TRDAD reveals its orbital pseudospin texture counterpart.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Soft X-Ray Spectroscopic Study of Dense Strontium-Doped Lanthanum Manganite Cathodes for Solid Oxide Fuel Cell Applications

The evolution of the Mn charge state, chemical composition, and electronic structure of La{sub 0.8}Sr{sub 0.2}MnO{sub 3} (LSMO) cathodes during the catalytic activation of solid oxide fuel cell (SOFC) has been studies using X-ray spectroscopy of as-processed, exposed, and activated dense thin LSMO films. Comparison of O K-edge and Mn L{sub 3,2}-edge X-ray absorption spectra from the different stages of LSMO cathodes revealed that the largest change after the activation occurred in the Mn charge state with little change in the oxygen environment. Core-level X-ray photoemission spectroscopy and Mn L{sub 3} resonant photoemission spectroscopy studies of exposed and as-processed LSMO determined that the SOFC environment (800 C ambient pressure of O{sub 2}) alone results in La deficiency (severest near the surface with Sr doping >0.55) and a stronger Mn{sup 4+} contribution, leading to the increased insulating character of the cathode prior to activation. Meanwhile, O K-edge X-ray absorption measurements support Sr/La enrichment nearer the surface, along with the formation of mixed Sr{sub x}Mn{sub y}O{sub z} and/or passive MnO{sub x} and SrO species.

30 DIRECT ENERGY CONVERSION↗

Ultrafast dynamics in helium nanodroplets probed by femtosecond time-resolved EUV photoelectron imaging

The dynamics of electronically excited helium nanodroplets are studied by femtosecond time-resolved photoelectron imaging. EUV excitation into a broad absorption band centered around 23.8 eV leads to an indirect photoemission process that generates ultraslow photoelectrons. A 1.58 eV probe pulse transiently depletes the indirect photoemission signal for pump-probe time delays <200 fs and enhances the signal beyond this delay. The depletion is due to suppression of the indirect ionization process by the probe photon, which generates a broad, isotropically emitted photoelectron band. Similar time scales in the decay of the high energy photoelectron signal and the enhancement of the indirect photoemission signal suggest an internal relaxation process that populates states in the range of a lower energy droplet absorption band located just below the droplet ionization potential (IP {approx} 23.0 eV). A nearly 70% enhancement of the ultraslow photoelectron signal indicates that interband relaxation plays a more dominant role for the droplet de-excitation mechanism than photoemission.

74 ATOMIC AND MOLECULAR PHYSICS↗