High-energy Peak Research Articles

One- and two-photon absorption spectra of the yellow fluorescent protein citrine: effects of intramolecular electron-vibrational coupling and intermolecular interactions

ABSTRACTBoth the vibrationally resolved and statistically averaged one-photon absorption (OPA) and two-photon absorption (TPA) spectra of the anionic form of chromophore (AC) in its micro-environment of yellow fluorescent protein (YFP) Citrine have been calculated. The result comparison has been made with those of the AC model compounds in vacuo and methanol solution, which allows us to allocate the individual contribution of the intramolecular electron-vibrational coupling, the electrostatic π-stacking interaction between Tyr203 and AC, and the interaction between AC and its micro-environment to the spectra. The results reveal that the non-Condon vibronic coupling effect is responsible for the blue shift of TPA absorption maximum compared with its OPA counterpart corresponding to S0 → S1, and that the π-stacking interaction between Tyr203 and AC alters the relative intensities of TPA maxima, which further enhances the higher-energy vibronic peaks and weakens the lowest-energy peak. The statically averaged OPA and TPA spectra calculated by quantum mechanics/molecular mechanics (QM/MM) methods based on Born–Oppenheimer molecular dynamics simulation largely deviate the experimental spectral lineshapes, which further verifies the significant contribution of non-Condon vibronic coupling effect on the spectra. The interaction of individual amino acid residue or water close to AC+Tyr203 has different effects on the spectra, which may increase/decrease the excitation energy depending on its position and electronic property.

Damage thresholds for blaze diffraction gratings and grazing incidence optics at an X-ray free-electron laser.

The Linac Coherent Light Source is upgrading its machine to high repetition rate and to extended ranges. Novel coatings, with limited surface oxidation, which are able to work at the carbon edge, are required. In addition, high-resolution soft X-ray monochromators become necessary. One of the big challenges is to design the mirror geometry and the grating profile to have high reflectivity (or efficiency) and at the same time survive the high peak energy of the free-electron laser pulses. For these reasons the experimental damage threshold, at 900 eV, of two platinum-coated gratings with different blazed angles has been investigated. The gratings were tested at 1° grazing incidence. To validate a model for which the damage threshold on the blaze grating can be estimated by calculating the damage threshold of a mirror with an angle of incidence identical to the angle of incidence on the grating plus the blaze angle, tests on Pt-coated substrates have also been performed. The results confirmed the prediction. Uncoated silicon, platinum and SiB3 (both deposited on a silicon substrate) were also investigated. In general, the measured damage threshold at grazing incidence is higher than that calculated under the assumption that there is no energy transport from the volume where the photons are absorbed. However, it was found that, for the case of the SiB3 coating, the grazing incidence condition did not increase the damage threshold, indicating that the energy transport away from the extinction volume is negligible.

Electronic and optical properties of 2H-perovskite related tantalum/niobium oxides

Quasi-one-dimensional oxides [Formula: see text] (A = Ba, Sr; [Formula: see text] = Na, Li and B = Ta, Nb) have been synthesized and found to display efficient photoluminescence. Their electronic and optical properties are calculated by using first-principles calculations. The modified Becke–Johnson exchange potential has been used to obtain accurate band gap. Our results reveal that alkali metal and alkaline-earth metal ions have very small contribution to the states around Fermi level, and for these compounds, the top valence bands and the conduction band bottom are dominated by O-2p and Nb/Ta-d states, respectively. All of these compounds have indirect band gap, with valence band maximum at K point and conduction band minimum at [Formula: see text] point. Optical absorption spectrum is characterized by two prominent peaks. The lower energy peak originates from electron transitions between Ta/Nb-[Formula: see text] and O-2p states, while the higher energy peak is determined by electron transitions between Ta/Nb-[Formula: see text] and O-2p. Despite the one-dimensional feature of the lattice structure, the electronic band structure and optical properties show three-dimensional character. We find that the band gap and optical absorption threshold are considerably larger than the energy of excitation light in the luminescence measurement. This indicates the important role of the in-gap states, which may be induced by the impurity or vacancy.

Asymmetrical quantum well degradation of InGaN/GaN blue laser diodes characterized by photoluminescence

The temperature, power, and voltage dependent photoluminescence spectra are studied in InGaN/GaN double quantum well blue laser diodes. Emissions from the two quantum wells can be distinguished at low temperature at low excitation power density due to the different built-in electric field in the two quantum wells. This finding is utilized to study the degradation of InGaN/GaN blue laser diodes. Two peaks are observed for the non-aged laser diode (LD), while one peak for the aged LD which performed 3200 h until no laser output is detected. The disappearance of the high energy peak in the photoluminescence spectra indicates a heavier degradation of the quantum well on the p-side, which agrees with our previous observation that both the linewidth and the potential fluctuation of InGaN quantum wells (QWs) reduced for the aged LDs.

Magnetic Susceptibility and Neutron Scattering of Graphene in Antiferromagnetic State: a Tight-Binding Approach

We address here a tight-binding model study of the frequency-dependent antiferromagnetic spin susceptibility for the graphene systems. The Hamiltonian consists of electron hopping up to the third-nearest-neighbors, substrate and impurity effects in presence of electron-electron interactions at A and B sub-lattices. To calculate susceptibility, we evaluate the two-particle electron Green’s function by using Zubarev’s Green’s function technique. The frequency-dependent antiferromagnetic susceptibility of the system is computed numerically by taking 1000 X 1000 grid points of the electron momentum. The susceptibility displays a sharp peak at the neutron momentum transfer energy at low energies and another higher-energy peak associated with the substrate-induced gap. The evolution of these two peaks are investigated by varying neutron wave vector, Coulomb correlation energy, substrate-induced gap, electron hopping integrals and A- and B-site electron-doping concentrations.

Organic-inorganic hybrid crystals, (2,4,6-CH3PyH)3Sb2Cl9 and (2,4,6-CH3PyH)3Bi2Cl9. Crystal structure characterization and tunneling of CH3 groups studied by 1H NMR and neutron spectroscopy

The crystal structures of (2,4,6-CH3PyH)3Sb2Cl9 (TMPCA) and (2,4,6-CH3PyH)3Bi2Cl9 (TMPCB) (Py – pyridine) have been determined at 100 K by the single crystal X-ray diffraction method. TMPCA and TMPCB crystallize in the monoclinic C2/c and triclinic P1 polar space group, respectively. In both cases the asymmetric part is comprised of three nonequivalent 2,4,6-trimethylpyridinium cations and a discrete M2Cl93− anion. The Bi2Cl93− moiety forms a face-sharing bi-octahedron, whereas in a case of Sb2Cl93− we deal with two pyramids connected by a corner. The inelastic neutron scattering spectra (INS) were recorded for TMPCA at low temperatures (4–50 K). Two peaks on each side of the central elastic line have been observed at ca. 4.8 and 2.9 μeV, the high energy peak exhibits an excitation energy value equal to ca. 6 meV. For TMPCA and TMPCB the 1H NMR spin–lattice relaxation times, T1, have been measured in the temperature region 15–410 K. The flattening of the T1 (spin–lattice) vs. reciprocal temperature, 1/T, dependence between 30 K and 15 K indicates the incoherent tunneling effect of the methyl group being treated as the quantum rotor. The conclusions drawn from the 1H NMR results as regards to the tunneling of the CH3 groups in the pyridinium cations are consistent with the tunneling peaks observed in the INS spectra.

Surface microstructure and chemistry of polyimide by single pulse ablation of picosecond laser

Polyimide (PI) surface was ablated by the single pulse of picosecond laser, and the effects of laser wavelength (λ=355nm and 1064nm) and fluence on surface microstructure and chemistry were explored. Scanning electron microscopy (SEM) analysis found that different surface microstructures, i.e., the concave of concentric ring and the convex of porous circular disk, were generated by 355nm and 1064nm picosecond laser ablation, respectively. X-ray photoelectron spectroscopy (XPS) characterization indicated that due to the high peak energy density of picosecond laser, oxygen and nitrogen from the ambient were incorporated into the PI surface mainly in the form of CO and CNC groups. Thus, both of the O/C and N/C atomic content ratios increased, but the increase caused by 1064nm wavelength laser was larger. It inferred that the differences of PI surface microstructures and chemistry resulted from different laser parameters were related to different laser-matter interaction effects. For 355nm picosecond laser, no obvious thermal features were observed and the probable ablation process of PI was mainly governed by photochemical effect; while for 1064nm picosecond laser, obvious thermal feature appeared and photothermal effect was thought to be dominant.

2D Raman band splitting in graphene: Charge screening and lifting of the K-point Kohn anomaly

Pristine graphene encapsulated in hexagonal boron nitride has transport properties rivalling suspended graphene, while being protected from contamination and mechanical damage. For high quality devices, it is important to avoid and monitor accidental doping and charge fluctuations. The 2D Raman double peak in intrinsic graphene can be used to optically determine charge density, with decreasing peak split corresponding to increasing charge density. We find strong correlations between the 2D1 and 2D2 split vs 2D line widths, intensities, and peak positions. Charge density fluctuations can be measured with orders of magnitude higher precision than previously accomplished using the G-band shift with charge. The two 2D intrinsic peaks can be associated with the “inner” and “outer” Raman scattering processes, with the counterintuitive assignment of the phonon closer to the K point in the KM direction (outer process) as the higher energy peak. Even low charge screening lifts the phonon Kohn anomaly near the K point for graphene encapsulated in hBN, and shifts the dominant intensity from the lower to the higher energy peak.

Analysis and Design of Coherent Combining of two Q-Switched Fiber Laser in Mach-Zehnder Type Cavity

Abstract In this work, we have developed an analytical model of an actively Q-switched Ytterbium-doped fiber laser by using two coupled cavities with amplifying fibers in Mach–Zehnder interferometer configuration. This oscillator system provides high peak power and high energy nanosecond pulse. The pulse energy is almost twice the energy of an individual fiber laser with a combining efficiency goes up 99%. This concept brings some novel perspectives for scaling the high energy and high peak power of nanosecond pulse fiber laser.

Origin of Superconductivity and Latent Charge Density Wave in NbS_{2}.

We elucidate the origin of the phonon-mediated superconductivity in 2H-NbS_{2} using the abinitio anisotropic Migdal-Eliashberg theory including Coulomb interactions. We demonstrate that superconductivity is associated with Fermi surface hot spots exhibiting an unusually strong electron-phonon interaction. The electron-lattice coupling is dominated by low-energy anharmonic phonons, which place the system on the verge of a charge density wave instability. We also provide definitive evidence for two-gap superconductivity in 2H-NbS_{2}, and show that the low- and high-energy peaks observed in tunneling spectra correspond to the Γ- and K-centered Fermi surface pockets, respectively. The present findings call for further efforts to determine whether our proposed mechanism underpins superconductivity in the whole family of metallic transition metal dichalcogenides.

Indium-incorporation enhancement of photoluminescence properties of Ga(In)SbBi alloys

Ga(In)SbBi alloys grown by molecular-beam epitaxy on GaSb substrates with up to 5.5% In and 1.8% Bi were studied by temperature- and power-dependent photoluminescence (PL) and compared to previous photoreflectance (PR) results. High energy and low energy PL peaks were observed and attributed respectively to Ga(In)SbBi bandgap-related emission and native acceptor-related emission. For GaSbBi below 100 K, the HE peak is at slightly lower energy than the bandgap determined from PR, indicating carrier localization. This phenomenon is significantly weaker in PL of GaInSbBi alloys, suggesting that the presence of indium improves the optical quality over that of GaSbBi.

Validation and uncertainty quantification of detector response functions for a 1″×2″ NaI collimated detector intended for inverse radioisotope source mapping applications

Abstract Detector response functions (DRFs) are often used for inverse analysis. We compute the DRF of a sodium iodide (NaI) nuclear material holdup field detector using the code named g03 developed by the Center for Engineering Applications of Radioisotopes (CEAR) at NC State University. Three measurement campaigns were performed in order to validate the DRF’s constructed by g03: on-axis detection of calibration sources, off-axis measurements of a highly enriched uranium (HEU) disk, and on-axis measurements of the HEU disk with steel plates inserted between the source and the detector to provide attenuation. Furthermore, this work quantifies the uncertainty of the Monte Carlo simulations used in and with g03, as well as the uncertainties associated with each semi-empirical model employed in the full DRF representation. Overall, for the calibration source measurements, the response computed by the DRF for the prediction of the full-energy peak region of responses was good, i.e. within two standard deviations of the experimental response. In contrast, the DRF tended to overestimate the Compton continuum by about 45–65% due to inadequate tuning of the electron range multiplier fit variable that empirically represents physics associated with electron transport that is not modeled explicitly in g03. For the HEU disk measurements, computed DRF responses tended to significantly underestimate (more than 20%) the secondary full-energy peaks (any peak of lower energy than the highest-energy peak computed) due to scattering in the detector collimator and aluminum can, which is not included in the g03 model. We ran a sufficiently large number of histories to ensure for all of the Monte Carlo simulations that the statistical uncertainties were lower than their experimental counterpart’s Poisson uncertainties. The uncertainties associated with least-squares fits to the experimental data tended to have parameter relative standard deviations lower than the peak channel relative standard deviation in most cases and good reduced chi-square values. The highest sources of uncertainty were identified as the energy calibration polynomial factor (due to limited source availability and NaI resolution) and the Ba-133 peak fit (only a very weak source was available), which were 20% and 10%, respectively.

Emergence of a Higher Energy Structure in Strong Field Ionization with Inhomogeneous Electric Fields.

Studies of strong field ionization have historically relied on the strong field approximation, which neglects all spatial dependence in the forces experienced by the electron after ionization. More recently, the small spatial inhomogeneity introduced by the long-range Coulomb potential has been linked to a number of important features in the photoelectron spectrum, such as Coulomb asymmetry, Coulomb focusing, and the low energy structure. Here, we demonstrate using midinfrared laser wavelength that a time-varying spatial dependence in the laser electric field, such as that produced in the vicinity of a nanostructure, creates a prominent higher energy peak. This higher energy structure (HES) originates from direct electrons ionized near the peak of a single half-cycle of the laser pulse. The HES is separated from all other ionization events, with its location and width highly dependent on the strength of spatial inhomogeneity. Hence, the HES can be used as a sensitive tool for near-field characterization in the "intermediate regime," where the electron's quiver amplitude is comparable to the field decay length. Moreover, the large accumulation of electrons with tuneable energy suggests a promising method for creating a localized source of electron pulses of attosecond duration using tabletop laser technology.

Power-Dependent Optical Property of Yb/Er: NaGdF4@Yb: NaGdF4@Yb:NaNdF4 Nanocrystals

In most of the reports on nanocrystal (NC) luminescent, the power depedence of luminescent intensity is studied using a continuous-wave laser with low power density, and the slopes of those different emission bands keep unchanged. In this paper, the up/down conversion of monodisperse Yb/Er: NaGdF4@Yb: NaGdF4@Yb: NaNdF4 NCs under the excitation of 800[Formula: see text]nm femtosecond laser was detected simultaneously by a home-built optical measurement setup. The power-dependent optical properties under the excitation of femtosecond laser are quite different from the normal situation, which is due to their high peak power and energy transfer processes: Nd[Formula: see text].

Microscopic theory of substrate-induced gap effect on real AFM susceptibility in graphene

We address here a tight-binding model study of frequency-dependent real part of antiferromagnetic susceptibility for the graphene systems. The Hamiltonian consists of electron hopping upto third nearest-neighbours, substrate and impurity effects in the presence of electron–electron interactions at A and B sublattices. To calculate susceptibility, we evaluate the two-particle electron Green’s function by using Zubarev’s Green’s function technique. The frequency-dependent real part of antiferromagnetic susceptibility of the system is computed numerically by taking $$1000 \times 1000$$ grid points of the electron momentum. The susceptibility displays a sharp peak at the neutron momentum transfer energy at low energies and another higher energy peak appearing at substrate-induced gap. The evolution of these two peaks is investigated by varying neutron wave vector, Coulomb correlation energy, substrate-induced gap, electron hopping integrals and A- and B-site electron doping concentrations.

Local strain-induced band gap fluctuations and exciton localization in aged WS2 monolayers

Optical properties of aged WS2 monolayers grown by CVD method on Si/SiO2 substrates are studied using temperature dependent photoluminescence and reflectance contrast spectroscopy. Aged WS2 monolayers have a typical surface roughness about 0.5 nm and, in addition, a high density of nanoparticles (nanocaps) with the base diameter about 30 nm and average height of 7 nm. The A-exciton of aged monolayer has a peak position at 1.951 eV while in as-grown monolayer the peak is at about 24 meV higher energy at room temperature. This red-shift is explained using local tensile strain concept, where strain value of 2.1% was calculated for these nanocap regions. Strained nanocaps have lower band gap energy and excitons will funnel into these regions. At T=10K a double exciton and trion peaks were revealed. The separation between double peaks is about 20 meV and the origin of higher energy peaks is related to the optical band gap energy fluctuations caused by random distribution of local tensile strain due to increased surface roughness. In addition, a wide defect related exciton band XD was found at about 1.93 eV in all aged monolayers. It is shown that the theory of localized excitons describes well the temperature dependence of peak position and halfwidth of the A-exciton band. The possible origin of nanocaps is also discussed.

A Model Study of Substrate Effect on the Neutron-Scattering Spectra of Ferromagnetic Ordered Graphene

Graphene as a possible new magnetic material has stimulated research interest for application in spintronic devices. Pristine graphene does not show magnetism due to equivalence of the two sub-lattices of carbon atoms. It is predicted that impurity effects, substrate-induced gap, and defects, are expected to produce in-equivalence in two carbon sub-lattices leading to magnetism. The spins on the same sub-lattices are found to exhibit ferromagnetic order and spins of different sub-lattices are found to exhibit anti-ferromagnetic order. We consider here impurity and substrate effects as the cause of generation of magnetism in graphene. We report here a microscopic tight-binding study of frequency-dependent neutron scattering spectra for ferromagnetic ordering in the graphene systems. The tight-binding Hamiltonian consists of electron hoppings upto third nearest neighbors and substrate and impurity effects in the presence of Coulomb interaction of electrons separately at two in-equivalent A and B sub-lattices of graphene. We calculate the two-particle electron Green’s functions by using Zubarev’s Green’s function technique. The frequency-dependent scattering intensity of the system is computed numerically. The spectra displays a sharp peak at the neutron momentum transfer energy at low energies and another higher-energy peak appearing at substrate-induced gap.

Mechanisms of the structural modification of Ti films by pulsed direct current and inductively coupled plasma-assisted pulsed direct current sputtering

Titanium (Ti) thin films have been deposited by direct current (dc), pulsed dc, and inductively coupled plasma (ICP)-assisted pulsed dc sputtering to investigate the effects of current pulsing and ICP assistance on film structure and properties. Ti thin films were deposited from a Ti target using Ar as a discharge gas. Ion energy was measured by energy-resolved mass spectrometry. The discharge plasma parameters were measured using a single probe with a time-resolved data acquisition system. The crystal structure was investigated by X-ray diffraction. Surface and cross-sectional morphologies were investigated by atomic force microscopy and scanning electron microscopy, respectively. The cross-sectional images demonstrated that the film structure changed from a coarse columnar structure with voids to a fine columnar structure. Changes in the roughness and crystallite sizes of the deposited Ti thin films indicated that the thin films were amorphized by the ICP-assisted sputtering, resulting in the smoothing of the film surface. Energy and mass analyses indicated that the energy fluxes to the substrate via Ar+ and Ti+ ions increased by more than four and two orders of magnitude, respectively, when ICP assistance was employed. This large difference in degree of enhancement generated by ICP assistance for Ar+ and Ti+ ions suggests different ionization efficiencies between gas-phase Ar and sputter-emitted energetic Ti, particularly in the ICP-assisted pulsed dc discharge. As a result of the increase in energy flux to the substrate, the mean energy transferred by both Ar+ and Ti+ ions per Ti metal particle (atom or ion) arriving at the substrate increased from approximately 40eV for dc sputtering to >104eV for ICP-assisted pulsed dc sputtering, and the mean energy transferred by Ti+ ions per Ti metal particle (atom or ion) arriving at the substrate increased from a few eV for dc sputtering to approximately 29–30eV for ICP-assisted pulsed dc sputtering. These increases in transferred energy reflect the formation of intense and broad high-energy peaks, as shown in the ion-energy spectra. It is shown that the formation of an additional high-energy peak to the single peak of the dc discharge results from the current pulsing, and that the further high-energy shift and splitting of the bimodal peaks result from the combination of the increase in plasma sheath potential to the grounded substrate and the increases in the electron density and electron temperature due to the subsequent ICP assistance to the pulsed dc discharge.

Core-hole-induced dynamical effects in the x-ray emission spectrum of liquid methanol.

We compute the x-ray emission spectrum of liquid methanol, with the dynamical effects that result from the creation of the core hole included in a semiclassical way. Our method closely reproduces a fully quantum mechanical description of the dynamical effects for relevant one-dimensional models of the hydrogen-bonded methanol molecules. For the liquid, we find excellent agreement with the experimental spectrum, including the large isotope effect in the first split peak. The dynamical effects depend sensitively on the initial structure in terms of the local hydrogen-bonding (H-bonding) character: non-donor molecules contribute mainly to the high-energy peak while molecules with a strong donating H-bond contribute to the peak at lower energy. The spectrum thus reflects the initial structure mediated by the dynamical effects that are, however, seen to be crucial in order to reproduce the intensity distribution of the recently measured spectrum.

The Fermi blazar sequence

We revisit the blazar sequence exploiting the complete, flux limited sample of blazars with known redshift detected by the Fermi satellite after 4 years of operations (the 3LAC sample). We divide the sources into gamma-ray luminosity bins, collect all the archival data for all blazars, and construct their spectral energy distribution (SED). We describe the average SED of blazars in the same luminosity bin through a very simple, completely phenomenological function consisting of two broken power laws connecting with a power law of fixed slope describing the radio emission. We do that separately for BL Lacs and for flat spectrum radio quasars (FSRQs) and also for all blazars together. The main results are: i) FSRQs display approximately the same SED as the luminosity increases, except for the fact that the relative importance of the high energy peak increases; ii) as a consequence, X-ray spectra of FSRQs become harder for larger luminosities; iii) BL Lacs form indeed a sequence: they become redder (i.e. the peak frequencies becomes smaller) for increasing luminosities, with a steeper gamma-ray slope and a larger dominance of the high energy peak; iv) for all blazars (BL Lacs+FSRQs) these properties becomes more prominent, as the highest luminosity bin is populated mostly by FSRQs and the lowest luminosity bin mostly by BL Lacs. This agrees with the original blazar sequence, although BL Lacs never have an average gamma-ray slope as hard as found in the original sequence. v) At high luminosities, a large fraction of FSRQs shows signs of thermal emission from the accretion disc, contributing in the optical-UV.