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At least 1,621 records · Page 90

Phonon-assisted nonlinear optical processes in ultrashort-pulse pumped optical parametric amplifiers

Optically active phonon modes in ferroelectrics such as potassium titanyl phosphate (KTP) and potassium titanyl arsenate (KTA) in the ~7–20 THz range play an important role in applications of these materials in Raman lasing and terahertz wave generation. Previous studies with picosecond pulse excitation demonstrated that the interaction of pump pulses with phonons can lead to efficient stimulated Raman scattering (SRS) accompanying optical parametric oscillation or amplification processes (OPO/OPA), and to efficient polariton-phonon scattering. In this work, we investigate the behavior of infrared OPAs employing KTP or KTA crystals when pumped with ~800-nm ultrashort pulses of duration comparable to the oscillation period of the optical phonons. We demonstrate that under conditions of coherent impulsive Raman excitation of the phonons, when the effective χ (2) nonlinearity cannot be considered instantaneous, the parametrically amplified waves (most notably, signal) undergo significant spectral modulations leading to an overall redshift of the OPA output. Furthermore, the pump intensity dependence of the redshifted OPA output, the temporal evolution of the parametric gain, as well as the pump spectral modulations suggest the presence of coupling between the nonlinear optical polarizations P NL of the impulsively excited phonons and those of parametrically amplified waves.

36 MATERIALS SCIENCE↗

Modeling of threshold and dynamics behavior of organic nanostructured lasers

Organic dye molecules offer significant potential as gain media in the emerging field of optical amplification and lasing at subwavelength scales. In this article, we investigate the laser dynamics in systems comprising subwavelength-structured cavities that incorporate organic dyes. To this end, we have developed a comprehensive theoretical framework able to accurately describe the interaction of organic molecules with any arbitrary photonic structure to produce single-mode lasing. The model provides explicit analytic expressions of the threshold and slope efficiency that characterize this class of lasers, and also the duration over which lasing action can be sustained before the dye photobleaches. Both the physical properties of the dyes and the optical properties of the cavities are considered. We also systematically studied the feasibility of achieving lasing action under continuous-wave excitation in optically pumped monolithic organic dye lasers. This study suggests routes to realize an organic laser that can potentially lase with a threshold of only a few W cm -2 . In conclusion, our work puts forward a theoretical formalism that could enable the advancement of nanostructured organic-based light emitting and sensing devices.

36 MATERIALS SCIENCE↗

Self-induced redox cycling coupled luminescence on nanopore recessed disk-multiscale bipolar electrodes

Self-induced redox cycling at nanopore ring-disk electrodes is coupled, through a bipolar electrode, to a remote fluorigenic reporter reaction. We present a new configuration for coupling fluorescence microscopy and voltammetry using self-induced redox cycling for ultrasensitive electrochemical measurements. An array of nanopores, each supporting a recessed disk electrode separated by 100 nm in depth from a planar multiscale bipolar top electrode, was fabricated using multilayer deposition, nanosphere lithography, and reactive-ion etching. Self-induced redox cycling was induced on the disk electrode producing ~30× current amplification, which was independently confirmed by measuring induced electrogenerated chemiluminescence from Ru(bpy) 3 2/3+ /tri-n-propylamine on the floating bipolar electrode. In this design, redox cycling occurs between the recessed disk and the top planar portion of a macroscopic thin film bipolar electrode in each nanopore. Electron transfer also occurs on a remote (mm-distance) portion of the planar bipolar electrode to maintain electroneutrality. This couples the electrochemical reactions of the target redox pair in the nanopore array with a reporter, such as a potential-switchable fluorescent indicator, in the cell at the distal end of the bipolar electrode. Oxidation or reduction of reversible analytes on the disk electrodes were accompanied by reduction or oxidation, respectively, on the nanopore portion of the bipolar electrode and then monitored by the accompanying oxidation of dihydroresorufin or reduction of resorufin at the remote end of the bipolar electrode, respectively. In both cases, changes in fluorescence intensity were triggered by the reaction of the target couple on the disk electrode, while recovery was largely governed by diffusion of the fluorescent indicator. Reduction of 1 nM of Ru(NH 3 ) 6 3+ on the nanoelectrode array was detected by monitoring the fluorescence intensity of resorufin, demonstrating high sensitivity fluorescence-mediated electrochemical sensing coupled to self-induced redox cycling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Redox cycling-based detection of phenazine metabolites secreted from Pseudomonas aeruginosa in nanopore electrode arrays

The opportunistic pathogen Pseudomonas aeruginosa (P. aeruginosa) produces several redox-active phenazine metabolites, including pyocyanin (PYO) and phenazine-1-carboxamide (PCN), which are electron carrier molecules that also aid in virulence. In particular, PYO is an exclusive metabolite produced by P. aeruginosa, which acts as a virulence factor in hospital-acquired infections and is therefore a good biomarker for identifying early stage colonization by this pathogen. Here, we describe the use of nanopore electrode arrays (NEAs) exhibiting metal–insulator–metal ring electrode architectures for enhanced detection of these phenazine metabolites. The size of the nanopores allows phenazine metabolites to freely diffuse into the interior and access the working electrodes, while the bacteria are excluded. Consequently, highly efficient redox cycling reactions in the NEAs can be accessed by free diffusion unhindered by the presence of bacteria. This strategy yields low limits of detection, i.e. 10.5 and 20.7 nM for PYO and PCN, respectively, values far below single molecule pore occupancy, e.g. at 10.5 nM < n pore > ~ 0.082 per nanopore – a limit which reflects the extraordinary signal amplification in the NEAs. Furthermore, experiments that compared results from minimal medium and rich medium show that P. aeruginosa produces the same types of phenazine metabolites even though growth rates and phenazine production patterns differ in these two media. Here, the NEA measurement strategy developed here should be useful as a diagnostic for pathogens generally and for understanding metabolism in clinically important microbial communities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Spin dynamics of [1,2- 13 C 2 ]pyruvate hyperpolarization by parahydrogen in reversible exchange at micro Tesla fields

Hyperpolarization of 13 C-pyruvate via Signal Amplification By Reversible Exchange (SABRE) is an important recent discovery because of both the relative simplicity of hyperpolarization and the central biological relevance of pyruvate as a biomolecular probe for in vitro or in vivo studies. Here, we analyze the [1,2- 13 C 2 ]pyruvate-SABRE spin system and its field dependence theoretically and experimentally. We provide first-principles analysis of the governing 4-spin dihydride- 13 C 2 Hamiltonian and numerical spin dynamics simulations of the 7-spin dihydride- 13 C 2 –CH 3 system. Furthermore, the analytical and the numerical results are compared to matching systematic experiments. With these methods we unravel the observed spin state mixing of singlet states and triplet states at microTesla fields and we also analyze the dynamics during transfer from micro-Tesla field to high field for detection to understand the resulting spectra from the [1,2- 13 C 2 ]pyruvate-SABRE system.

13C pyruvate↗

Population study of Galactic supernova remnants at very high γ -ray energies with H.E.S.S.

Shell-type supernova remnants (SNRs) are considered prime candidates for the acceleration of Galactic cosmic rays (CRs) up to the knee of the CR spectrum at E ≈ 3 × 10 15 eV. Our Milky Way galaxy hosts more than 350 SNRs discovered at radio wavelengths and at high energies, of which 220 fall into the H.E.S.S. Galactic Plane Survey (HGPS) region. Of those, only 50 SNRs are coincident with a H.E.S.S source and in 8 cases the very high-energy (VHE) emission is firmly identified as an SNR. The H.E.S.S. GPS provides us with a legacy for SNR population study in VHE γ-rays and we use this rich data set to extract VHE flux upper limits from all undetected SNRs. Overall, the derived flux upper limits are not in contradiction with the canonical CR paradigm. Assuming this paradigm holds true, we can constrain typical ambient density values around shell-type SNRs to n ≤ 7 cm -3 and electron-to-proton energy fractions above 10 TeV to ϵ ep ≤ 5 × 10 -3 . Furthermore, comparisons of VHE with radio luminosities in non-interacting SNRs reveal a behaviour that is in agreement with the theory of magnetic field amplification at shell-type SNRs.

79 ASTRONOMY AND ASTROPHYSICS↗

A finite-volume scheme for modeling compressible magnetohydrodynamic flows at low Mach numbers in stellar interiors

Fully compressible magnetohydrodynamic (MHD) simulations are a fundamental tool for investigating the role of dynamo amplification in the generation of magnetic fields in deep convective layers of stars. The flows that arise in such environments are characterized by low (sonic) Mach numbers ($\mathscr{M}$ son ≲ 10 –2 ). In these regimes, conventional MHD codes typically show excessive dissipation and tend to be inefficient as the Courant–Friedrichs–Lewy (CFL) constraint on the time step becomes too strict. In this work we present a new method for efficiently simulating MHD flows at low Mach numbers in a space-dependent gravitational potential while still retaining all effects of compressibility. The proposed scheme is implemented in the finite-volume SEVEN-LEAGUE HYDRO (SLH) code, and it makes use of a low-Mach version of the five-wave Harten–Lax–van Leer discontinuities (HLLD) solver to reduce numerical dissipation, an implicit–explicit time discretization technique based on Strang splitting to overcome the overly strict CFL constraint, and a well-balancing method that dramatically reduces the magnitude of spatial discretization errors in strongly stratified setups. The solenoidal constraint on the magnetic field is enforced by using a constrained transport method on a staggered grid. We carry out five verification tests, including the simulation of a small-scale dynamo in a star-like environment at $\mathscr{M}$ son ~ 10 –3 . We demonstrate that the proposed scheme can be used to accurately simulate compressible MHD flows in regimes of low Mach numbers and strongly stratified setups even with moderately coarse grids.

79 ASTRONOMY AND ASTROPHYSICS↗

Limits on the non-thermal emission of the WR–WR system Apep

Colliding-wind binaries (CWBs) constitute an emerging class of γ-ray sources powered by strong, dense winds in massive stellar systems. The most powerful of them are those binaries hosting a Wolf-Rayet (WR) star. Following the recent discovery of Apep – the closest known Galactic WR–WR binary – we discuss the non-detection of its putative high-energy emission by the Fermi Large Area Telescope (Fermi-LAT) in this Letter. The limits reported in the GeV regime can be used to set a lower limit on the magnetic field pressure density within the shocked wind-collision region (WCR), and to exclude Apep as a bright γ-ray emitting binary. Given that this WR–WR system is the most luminous CWB identified until now at radio wavelengths, this result proves unambiguously that non-thermal synchrotron emission is not a suitable identifier for the subset of γ-ray emitters in this class of particle accelerators. Rather, Apep could be an interesting case of study for magnetic field amplification in shocked stellar winds.

79 ASTRONOMY AND ASTROPHYSICS↗

Turbulent dynamo action and its effects on the mixing at the convective boundary of an idealized oxygen-burning shell

Convection is one of the most important mixing processes in stellar interiors. Hydrodynamic mass entrainment can bring fresh fuel from neighboring stable layers into a convection zone, modifying the structure and evolution of the star. Because flows in stellar convection zones are highly turbulent, multidimensional hydrodynamic simulations are fundamental to accurately capture the physics of mixing processes. Under some conditions, strong magnetic fields can be sustained by the action of a turbulent dynamo, adding another layer of complexity and possibly altering the dynamics in the convection zone and at its boundaries. In this study, we used our fully compressible S EVEN -L EAGUE H YDRO code to run detailed and highly resolved three-dimensional magnetohydrodynamic simulations of turbulent convection, dynamo amplification, and convective boundary mixing in a simplified setup whose stratification is similar to that of an oxygen-burning shell in a star with an initial mass of 25 M ⊙ . We find that the random stretching of magnetic field lines by fluid motions in the inertial range of the turbulent spectrum (i.e., a small-scale dynamo) naturally amplifies the seed field by several orders of magnitude in a few convective turnover timescales. During the subsequent saturated regime, the magnetic-to-kinetic energy ratio inside the convective shell reaches values as high as 0.33, and the average magnetic field strength is ∼10 10 G. Such strong fields efficiently suppress shear instabilities, which feed the turbulent cascade of kinetic energy, on a wide range of spatial scales. The resulting convective flows are characterized by thread-like structures that extend over a large fraction of the convective shell. The reduced flow speeds and the presence of magnetic fields with strengths up to 60% of the equipartition value at the upper convective boundary diminish the rate of mass entrainment from the stable layer by ≈20% as compared to the purely hydrodynamic case.

79 ASTRONOMY AND ASTROPHYSICS↗

Statistical analysis of high power microwave surface flashover delay times in nitrogen with metallic field enhancements

The physical mechanisms that contribute to atmospheric breakdown induced by high power microwaves (HPMs) are of particular interest for the further development of high power microwave systems and related technologies. For a system in which HPM is produced in a vacuum environment for the purpose of radiating into atmosphere, it is necessary to separate the atmospheric environment from the vacuum environment with a dielectric interface. Breakdown across this interface on the atmospheric side and plasma development to densities prohibiting further microwave propagation are of special interest. In this paper, the delay time between microwave application and plasma emergence is investigated. Various external parameters, such as UV illumination or the presence of small metallic points on the surface, provide sources for electron field emission and influence the delay time which yields crucial information on the breakdown mechanisms involved. Due to the inherent statistical appearance of initial electrons and the statistics of the charge carrier amplification mechanisms, the flashover delay times deviate by as much as {+-}50% from the average, for the investigated case of discharges in N{sub 2} at pressures of 60-140 Torr and a microwave frequency of 2.85 GHz with 3 {mu}s pulse duration, 50 ns pulse risetime, and MW/cm{sup 2} power densities. The statistical model described in this paper demonstrates how delay times for HPM surface flashover events can be effectively predicted for various conditions given sufficient knowledge about ionization rate coefficients as well as the production rate for breakdown initiating electrons.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Optical emission spectroscopy of the Linac4 and superconducting proton Linac plasma generators

CERN's superconducting proton Linac (SPL) study investigates a 50 Hz high-energy, high-power Linac for H{sup -} ions. The SPL plasma generator is an evolution of the DESY ion source plasma generator currently operated at CERN's Linac4 test stand. The plasma generator is a step towards a particle source for the SPL, it is designed to handle 100 kW peak RF-power at a 6% duty factor. While the acquisition of an integrated hydrogen plasma optical spectrum is straightforward, the measurement of a time-resolved spectrum requires dedicated amplification schemes. The experimental setup for visible light based on photomultipliers and narrow bandwidth filters and the UV spectrometer setup are described. The H{sub {alpha}}, H{sub {beta}}, and H{sub {gamma}} Balmer line intensities, the Lyman band and alpha transition were measured. A parametric study of the optical emission from the Linac4 ion source and the SPL plasma generator as a function of RF-power and gas pressure is presented. The potential of optical emission spectrometry coupled to RF-power coupling measurements for on-line monitoring of short RF heated hydrogen plasma pulses is discussed.

43 PARTICLE ACCELERATORS↗

Selective probe of the morphology and local vibrations at carbon nanoasperities

We introduce a way to selectively probe local vibration modes at nanostructured asperities such as tips of carbon nanohorns. Our observations benefit from signal amplification in surface-enhanced Raman scattering (SERS) at sites near a silver surface. We observe nanohorn tip vibration modes in the range 200-500 cm{sup -1}, which are obscured in regular Raman spectra. Ab initio density functional calculations assign modes in this frequency range to local vibrations at the nanohorn cap resembling the radial breathing mode of fullerenes. Careful interpretation of our SERS spectra indicates presence of caps with 5 or 6 pentagons, which are chemically the most active sites. Changes in the peak intensities and frequencies with time indicate that exposure to laser irradiation may cause structural rearrangements at the cap.

36 MATERIALS SCIENCE↗

Enhanced charge transfer by phenyl groups at a rubrene/C{sub 60} interface

Exciton dynamics at an interface between an electron donor, rubrene, and a C{sub 60} acceptor is studied by nonadiabatic quantum molecular dynamics simulation. Simulation results reveal an essential role of the phenyl groups in rubrene in increasing the charge-transfer rate by an order-of-magnitude. The atomistic mechanism of the enhanced charge transfer is found to be the amplification of aromatic breathing modes by the phenyl groups, which causes large fluctuations of electronic excitation energies. These findings provide insight into molecular structure design for efficient solar cells, while explaining recent experimental observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Impact of screening of resonant magnetic perturbations in three dimensional edge plasma transport simulations for DIII-D

The impact of resonant magnetic perturbations (RMPs) on the plasma edge can be analyzed in detail by three dimensional computer simulations, which take the underlying magnetic field structure as input. Previously, the 'vacuum approximation' has been used to calculate the magnetic field structure although plasma response effects may result in a screening (or even an amplification) of the external perturbations. Simulation results for an ITER similar shape plasma at the DIII-D tokamak are presented for the full vacuum perturbation field and an ad hoc screening case in comparison to the unperturbed configuration. It is shown that the RMP induced helical patterns in the plasma edge and on the divertor target shrink once screening is taken into account. However, a flat temperature profile is still found in the 'open field line domain' inside the separatrix, while the 'density pump out effect' found in the vacuum RMP case is considerably weakened.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

On the small-signal theory of stimulated Cherenkov emission in dielectric-lined waveguides

The growth characteristics of a two-dimensional Cherenkov free-electron laser (CFEL) in the small-signal low gain regime are studied for both single-electron and collective models. In the single-electron regime, for a thick enough beam, we prove that the gain of the CFEL can be increased by a factor of 2 than that obtained for an infinitely thin electron beam. Thus, the Cherenkov laser should be considered as a hybrid longitudinal/transverse free-electron laser device in general. In the collective-regime, we demonstrate the damping effects of Coulomb collisions among electrons on the amplification characteristics of a Cherenkov laser.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

High Bandwidth Differential Amplifier for Shock Experiments

We developed a high bandwidth differential amplifier for gas gun shock experiments. The circuit has a bandwidth up to 1 GHz, and is capable of measuring signals of ≤1.5 V with a common mode rejection of 250 V. Conductivity measurements of gas gun targets are measured by flowing high currents through the targets. The voltage is measured across the target using a technique similar to a four-point probe. Because of the design of the current source and load, the target voltage is approximately 250 V relative to ground. Since the expected voltage change in the target is < 1 V, the differential amplifier must have a large common mode rejection. Various amplifying designs are shown, although the increased amplification decreases bandwidth. Bench tests show that the amplifier can withstand significant common mode DC voltage and measure 10 ns, and 50 mV signals.

42 ENGINEERING↗