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At least 271 records · Page 15

Ultrafast Dynamics of Excited Electronic States in Nitrobenzene Measured by Ultrafast Transient Polarization Spectroscopy

We investigate ultrafast dynamics of the lowest singlet excited electronic state in liquid nitrobenzene using ultrafast transient polarization spectroscopy, extending the well-known technique of optical Kerr effect spectroscopy to excited electronic states. The third-order nonlinear response of the excited molecular ensemble is measured using a pair of femtosecond pulses following a third femtosecond pulse that populates the S 1 excited state. By measuring this response, which is highly sensitive to details of the excited state character and structure, as a function of time delays between the three pulses involved, we extract the dephasing time of the wave packet on the excited state. The dephasing time, measured as a function of time delay after pump excitation, shows oscillations indicating oscillatory wave packet dynamics on the excited state. Finally, from the experimental measurements and supporting theoretical calculations, we deduce that the wave packet completely leaves the S 1 state potential energy surface after three traversals of the intersystem crossing between the singlet S 1 and triplet T 2 states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Magnetic structure and magnetoelectric properties of the spin-flop phase in LiFePO 4

We investigate the magnetic structure and magnetoelectric(ME) effect in the high-field phase of the antiferromagnet LiFePO 4 above the critical field of 31 T. A neutron diffraction study in pulsed magnetic fields reveals the propagation vector to be q = 0 for the high-field magnetic structure. Pulsed-field electric polarization measurements show that, at the critical field, the low-field off-diagonal ME coupling α ab is partially suppressed, and the diagonal element α bb emerges. These results are consistent with a spin-flop transition where the spin direction changes from primarily being along the easy b axis below the transition to being along a above. The persistence of off-diagonal ME tensor elements above the critical field suggests a lowering of the magnetic point-group symmetry and hence a more complex magnetic structure in the high-field phase. In addition, neutron diffraction measurements in low magnetic fields show no observable field-induced spin canting, which indicates a negligible Dzyaloshinskii-Moriya interaction. The observed spin-flop field supports the Hamiltonian recently deduced from inelastic neutron studies and indicates that the system is less frustrated and with a larger single-ion anisotropy than originally thought. Our results demonstrate the effectiveness of combining pulsed-field neutron diffraction and electric polarization measurements to elucidate the magnetic structures and symmetries at the highest attainable field strengths.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

In situ characterization of two unknown ultrashort laser pulses using four-wave mixing in gas

Accurate characterization of two ultrashort laser pulses is of great interest in many ultrafast pump-probe experiments. We demonstrate a method based on four-wave mixing (FWM) in a gas which could be easily implemented into many existing pump-probe setups with minimal modifications for accurate, in situ characterization of both unknown pulses. This technique is tested on pairs of unknown pulses at wavelengths of 400/800 nm, and 266/400 nm. We measured the spectrogram of the pulse generated through FWM of the two unknown pulses by scanning the delay between two unknown pulses. The retrieval algorithm converges to accurately predict the intensity and the phase profiles of both unknown pulses with a trace error of < 1% and the accuracy is verified using an independent pulse characterization device.

Nambu, Noa (ORCID:0000000197303400)↗

Quasi-Differential Neutron Scattering Measurements of 181 Ta and Teflon from 1.5 to 20 MeV [Slides]

This presentation covers motivation for the Experiments Performed. Secondly, it touches on upgrades to the Experimental Apparatus for Measurements. Thirdly, it presents quasi-Differential Experimental Methodology a) Pulse Shape Discrimination b) Validation Measurement of Carbon. The presentation concludes with Preliminary Results and Future Studies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Ultrashort Laser Pulse Shaping and Characterization for Tailored Electron Bunch Generation

Temporally shaped laser pulses are desirable in various applications including emittance reduction and beam-driven acceleration. Pulse shaping techniques enable flexible controls over the longitudinal distribution of electron bunches emitted from the photocathode. While direct manipulation and measurement of an ultrashort pulse can be challenging in the time domain, both actions can be performed in the frequency domain. In this paper, we report the study and development of laser shaper and diagnostics at Argonne Wakefield Accelerator (AWA). Simulations of the shaping process for several sought-after shapes are presented along with the temporal diagnosis. Status of the experiment at the AWA facility is also discussed.

43 PARTICLE ACCELERATORS↗

Electron-ion coincidence measurements of molecular dynamics with intense X-ray pulses

Molecules can sequentially absorb multiple photons when irradiated by an intense X-ray pulse from a free-electron laser. If the time delay between two photoabsorption events can be determined, this enables pump-probe experiments with a single X-ray pulse, where the absorption of the first photon induces electronic and nuclear dynamics that are probed by the absorption of the second photon. Here we show a realization of such a single-pulse X-ray pump-probe scheme on N 2 molecules, using the X-ray induced dissociation process as an internal clock that is read out via coincident detection of photoelectrons and fragment ions. By coincidence analysis of the kinetic energies of the ionic fragments and photoelectrons, the transition from a bound molecular dication to two isolated atomic ions is observed through the energy shift of the inner-shell electrons. Via ab-initio simulations, we are able to map characteristic features in the kinetic energy release and photoelectron spectrum to specific delay times between photoabsorptions. In contrast to previous studies where nuclear motions were typically revealed by measuring ion kinetics, our work shows that inner-shell photoelectron energies can also be sensitive probes of nuclear dynamics, which adds one more dimension to the study of light-matter interactions with X-ray pulses.

74 ATOMIC AND MOLECULAR PHYSICS↗

Measurement accuracy and spatial resolution of a distributed temperature sensor based on a two-pulse differential coherent reflectometer

We present a model and numerical simulation of a distributed temperature sensor based on a two-pulse differential coherent optical time-domain reflectometer (COTDR). The differential phase measured using a phase-sensitive Rayleigh reflectometer is shown to have a regular component, which is a linear function of temperature, and a random component, which is related to a random distribution of scattering centres in the fibre and restricts the accuracy of measurements of variations in temperature. Measurement accuracy can be improved by reducing the relative contribution of the random component via a decrease in pulse duration and/or an increase in the time delay between pulses. The spatial resolution of a differential two-pulse phase-sensitive reflectometer is shown to be determined by the time delay between pulses and to vary little with pulse duration. At a typical pulse duration (200 ns) and delay time (300 ns), the accuracy in measurements of variations in temperature in the 0.1-K range is 2 % and the spatial resolution is about 30 m. (fibre-optic sensors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Inferred UV fluence focal-spot profiles from soft x-ray pinhole-camera measurements on OMEGA

A method was developed with laser-irradiated Au planar foils to characterize the focal spot of UV laser beams on target at full energy from soft x-ray emission. A pinhole camera with a back-thinned charge-coupled–device detector and filtration with thin Be and Al foil filters provides images of the x-ray emission at photon energies <2 keV. This method requires a careful measurement of the relation between the applied UV fluence and the x-ray signal, which can be described by a power-law dependence. The measured exponent γ ~ 2 provides a dynamic range of ~25 for the inferred UV fluence. UV fluence profiles of selected beams were measured for 100-ps and 1-ns laser pulses and were compared to directly measured profiles from an UV equivalent-target-plane diagnostic. The inferred spot size and super-Gaussian order from the x-ray technique agree within several percent with the values measured with the direct UV measurements.

47 OTHER INSTRUMENTATION↗

Tailoring spectral properties for entangled photon generation

The linear intensity scaling of entangled two-photon absorption (ETPA) offers a fundamental mechanism to enable nonlinear optical spectroscopy and microscopy under a substantially lower excitation power than is currently feasible. However, the long data acquisition time and low signal-to-noise ratio in reported ETPA-based spectroscopic and microscopic studies prevent its widespread application. To gain the full potential of this novel quantum light approach, it is essential to optimize entangled photon generation for significantly enhanced ETPA responses. Here, we report a new quantum light source by combining entangled photon generation with free-space femtosecond pump-pulse shaping. Here, through measurements of singles and coincidence counts by varying the patterns applied to a spatial light modulator to control the spectral widths of the pump pulses, we reveal strong dependence of the singles and coincidence count rates as well as their ratios on the spectral widths of pump pulses. An optimal spectral width for the highest ratios between the coincidence photon and the signal or idler photon count rates is also determined. Identification of such optimal spectral widths for entangled photon generation in the presence of postgeneration spectral selection makes this quantum light source a promising choice for ETPA-based spectroscopy and imaging.

Photon pairs & parametric down-conversion↗

Challenges in Pulsed-Field Gradient Nuclear Magnetic Resonance on Magnetically Heterogeneous Interfaces: Sequence and Field-Dependent Apparent Diffusion Coefficients

It is well known that the internal gradient (gi) that exists within pores haunts the diffusion coefficient (D) as measured by the pulsed-field gradient (PFG) nuclear magnetic resonance (NMR). Several PFG-NMR methods developed to determine an accurate D were not successful. Then, the steady-state diffusion coefficient (Dapp,8) for the cation [C4mim]+ of [C4mim][Tf2N]; [1-butyl-3-methylimidazolium][bis(trifluoromethylsulfonyl)imde] ionic liquid confined in ordered mesoporous carbon (OMC) were determined by comparing Dapp,8 obtained from 1H PFG-NMR performed with three different stimulated echo sequences: STE, APFG, and MPFG under the two external magnetic field strength, B0 = 9.4 and 14.1 Tesla. The measured Dapp,8 which is an order of magnitude smaller than D of bulk [C4mim][Tf2N], is in good agreement between APFG and MPFG both in B0 = 9.4 and 14.1 Tesla. However, the strong gi artifact, which caused apparent diffusion coefficient (Dapp) depending strongly and weakly on B0 and temperature, respectively, in diffusion-time dependent Dapp, Dapp(?) obtained from a sequence with monopolar gradients (STE) was suppressed by using sequences employing bipolar gradients (APFG and MPFG) in the region of steady-state diffusion. But incompletely suppressed gi artifact resulting in the different behaviors of the early part of Dapp(?) between the sequences leads a ˜ 0.6 and 0.9 in MPFG and APFG, respectively, in the relationship between mean squared displacement and diffusion time: = 2Dta, where a = 0.5 and 1 for 1-dimensional single file diffusion and 3-dimensional bulk diffusion, respectively. The above observations clearly show that the diffusion behavior of ions/molecules within the pores and pore structure, such as the surface-to-volume ratio? (D?_app (?)=D_0 [1-4/(9vp) S/V v(D_0 ?)]) and tortuosity (T = D0/Dapp,8), are possible to be misunderstood, especially in the systems with a non-negligible gi. This work demonstrates that it may be necessary to test several PFG sequences under multiple external magnetic fields for the correct determination of the diffusion behavior of ions/molecules in the pores with a larger internal gradient, gi.

Han, Kee Sung↗

Plasma Mirrors For High Power Lasers: A new approach for high repetition rates combined with realistic PIC simulations

We describe a research program to develop high quality plasma mirrors for use with high repetition rate, high power laser facilities to greatly facilitate experiments in high energy density physics, particularly when using solid density targets. A system delivering ultrathin, free standing liquid crystal films that could handle PW class laser pulses was developed that preserved the laser beam image quality and improved pulse contrast by over two orders of magnitude. The pulse contrast improvement was measured using a high dynamic range cross-correlation. The system operated at a repetition rate of several PMs formed in situ per minute. Extension to 1 Hz repetition rates should be possible. As a practical application, a PM system was used to separate laser accelerated electrons from the ultrashort pulse drive laser so that the electron beam emittance could be directly measured. The 20 nm thick PMs did not contribute significantly to emittance degradation. It was also demonstrated that the films could operate in the difficult plasma and laser environment present for GeV laser based electron acceleration. PM operation is still not well understood and much work with PMs is done empirically. Accordingly, we also demonstrated a particle-in-cell based simulation technique that would model PM operation, tracking the PM operation from cold, neutral atoms to a hot dense plasma by accounting for multiphoton ionization, plasma collisionality, and the dynamically changing index of refraction. Simulations in 3D were compared to a 2D based approach that was comparable. Finally, we developed a simpler model that can predict the intensity at which a plasma mirror will have its peak reflectivity.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Non-premixed counterflow methane flames in DC/AC/NS electric fields

The response of counterflow diffusion flames to sub-breakdown DC and AC electric fields, as well as their superposition with ns pulse discharge waveforms, is studied in the plane-to-plane electrode geometry. Sub-breakdown DC and low-frequency AC electric fields cause the flame displacement toward the grounded electrode, in the direction of the applied field, indicating that the body force on the positive ions exceeds that on the electrons and negative ions. As the AC frequency increases, the flame response becomes less pronounced, due to the reduction of the electrohydrodynamic (EHD) body force impulse over the AC half-period. The electric field in the electrode gap is determined by ps Electric Field Induced Second Harmonic (E-FISH) generation, with absolute calibration using sub-breakdown ns pulses overlapped with the measured electric field waveform. The results show that the electric field distribution across the flame in the current saturation regime follows the Laplacian field. This indicates that the space charge density in the gap is too low to distort the applied DC or AC field, consistent with the kinetic modeling predictions. Combining a nanosecond pulse discharge with a sub-breakdown DC field generates a diffuse plasma across the entire gap. Time-resolved and spatially resolved measurements of the electric field in the discharge indicate the ionization wave propagation between the electrodes. The present results do not exhibit a detectable flame displacement enhancement by ns discharge pulses combined with a sub-breakdown field, observed previously. Kinetic modeling calculations show that the absence of this effect in the plane-to-plane geometry is due to the rapid plasma self-shielding. This indicates that alternative electrode geometries limiting the self-shielding would be more effective for the plasma / electric field enhanced flameholding and flame stabilization applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ion Number Density Quantification Utilizing Pulsing Frequency in Negative Differential Resistance (NDR) Regime of Microplasma Operation

A mathematical model is presented for quantifying the ion number density over a range of discharge current in microplasma discharges. The ion number density is determined from measured discharge voltage, current, pulsing frequency, and trace impurity that is injected into the system deliberately. Experiments are conducted in pure helium with nitrogen being introduced as the trace species. The ion number density is estimated over a range of discharge current and is compared with multidimensional simulation results.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Novel X-ray scanning technique for in-situ alignment of photo-detectors in the MEGII calorimeter

Here, we describe and show results of a novel technique to measure with high precision the positions of photodetectors installed in the upgraded liquid xenon calorimeter of the MEG II experiment. The measurement was done by detecting the signal in individual photo-detectors as the front surface of the calorimeter was scanned in axial (Z) and azimuthal (Φ) directions with a precisely controlled, thin, collimated beam of X-rays obtained from a 57 CoX-ray source. The measurements were made when the calorimeter was cold and operational, under which conditions they could not otherwise be made. This technique is used to check for changes in the photodetector positions due to the effects of cooling and thermal cycling of the support structure and to provide a reference between the positions of the operational photodetectors and alignment markers on the cryostat exterior. The use of an essentially monochromatic X-ray source allowed ancillary measurements of photodetector properties, including pulse shape, relative gain, and variation in response over the photodetector surface. Measurement uncertainties below 0.6mm in Z and 0.7 mrad in Φ have been achieved, well within the requirements for the MEG II performance.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

First operation of a multi-channel Q-Pix prototype: measuring transverse electron diffusion in a gas time projection chamber

We report measurements of the transverse diffusion of electrons in P-10 gas (90% Ar, 10% CH 4 ) in a laboratory-scale time projection chamber (TPC) utilizing a novel pixelated signal capture and digitization technique known as Q-Pix. The Q-Pix method incorporates a precision switched integrating transimpedance amplifier whose output is compared to a threshold voltage. Upon reaching the threshold, a comparator sends a 'reset' signal, initiating a discharge of the integrating capacitor. The time difference between successive resets is inversely proportional to the average current at the pixel in that time interval, and the number of resets is directly proportional to the total collected charge. We developed a 16-channel Q-Pix prototype fabricated from commercial off-the-shelf components and coupled them to 16 concentric annular anode electrodes to measure the spatial extent of the electron swarm that reaches the anode after drifting through the uniform field of the TPC. The swarm is produced at a gold photocathode using pulsed UV light. The measured transverse diffusion agrees with simulations in PyBoltz across a range of operating pressures (200–1500 Torr). These results demonstrate that a Q-Pix readout can successfully reconstruct the ionization topology in a TPC.

47 OTHER INSTRUMENTATION↗

The Planetary Ephemeris Program: Capability, Comparison, and Open Source Availability

We describe for the first time in scientific literature the Planetary Ephemeris Program (PEP), an open-source general-purpose astrometric data-analysis program. We discuss, in particular, the implementation of pulsar timing analysis, which was recently upgraded in PEP to handle more options. This implementation was done independently of other pulsar programs, with minor exceptions that we discuss. We illustrate the implementation of this capability by comparing the postfit residuals from the analyses of time-of-arrival observations by both PEP and Tempo2. The comparison shows substantial agreement: 22 ns rms differences for 1065 pulse time-of-arrival measurements for the millisecond pulsar in a binary system, PSR J1909-3744 (pulse period 2.947108 ms; full width half maximum of pulse 43 μs), for epochs in the interval from 2002 December to 2011 February.

42 ENGINEERING↗

Intrinsic spatial chirp of subcycle terahertz pulsed beams

Here, we present an analysis of spatial chirp in subcycle pulsed beams corroborated by spatiotemporal electro-optic sampling measurements of terahertz radiation. Modeling the subcycle pulsed beam as a superposition of monochromatic Gaussian beams, free-space propagation is shown to directly lead to lateral spatial chirp with the spectrum on-axis substantially bluer than the overall energy spectrum. The two-transverse + one-temporal dimensional profile of terahertz subcycle pulsed beams from organic crystals DSTMS and OH1 are measured and compared with observed spatiospectral correlations consistent with the model.

43 PARTICLE ACCELERATORS↗

Spectral and temporal dynamics of ultrashort pulses in a holmium-doped fibre amplifier

We have optimised a hybrid mode-locked holmium-doped fibre laser and a holmium-doped fibre amplifier for obtaining stable pulses as short as possible. Temporal and spectral characteristics of pulsed light have been measured as functions of pump power. Lasing has been achieved in the wavelength range 2066 – 2068 nm, with a full width at half maximum of the emission spectrum from 3 to 4 nm. The pulse duration does not exceed 1 ps and the pulse energy ranges from 0.2 to 0.5 nJ. To raise the pulse energy, holmium-doped fibre amplifiers based on two types of active fibre have been used. We have demonstrated a decrease in the width of the central part of the pulse autocorrelation function and considerable broadening of the spectrum of the pulses. The maximum average power at the amplifier output exceeds 200 mW. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗