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At least 1,099 records · Page 61

Probing ultra-fast processes with high dynamic range at 4th-generation light sources: Arrival time and intensity binning at unprecedented repetition rates

Here, understanding dynamics on ultrafast timescales enables unique and new insights into important processes in the materials and life sciences. In this respect, the fundamental pump-probe approach based on ultra-short photon pulses aims at the creation of stroboscopic movies. Performing such experiments at one of the many recently established accelerator-based 4th-generation light sources such as free-electron lasers or superradiant THz sources allows an enormous widening of the accessible parameter space for the excitation and/or probing light pulses. Compared to table-top devices, critical issues of this type of experiment are fluctuations of the timing between the accelerator and external laser systems and intensity instabilities of the accelerator-based photon sources. Existing solutions have so far been only demonstrated at low repetition rates and/or achieved a limited dynamic range in comparison to table-top experiments, while the 4th generation of accelerator-based light sources is based on superconducting radio-frequency technology, which enables operation at MHz or even GHz repetition rates. In this article, we present the successful demonstration of ultra-fast accelerator-laser pump-probe experiments performed at an unprecedentedly high repetition rate in the few-hundred-kHz regime and with a currently achievable optimal time resolution of 13 fs (rms). Our scheme, based on the pulse-resolved detection of multiple beam parameters relevant for the experiment, allows us to achieve an excellent sensitivity in real-world ultra-fast experiments, as demonstrated for the example of THz-field-driven coherent spin precession.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ultrafast carrier thermalization and trapping in silicon-germanium alloy probed by extreme ultraviolet transient absorption spectroscopy

Semiconductor alloys containing silicon and germanium are of growing importance for compact and highly efficient photonic devices due to their favorable properties for direct integration into silicon platforms and wide tunability of optical parameters. Here, we report the simultaneous direct and energy-resolved probing of ultrafast electron and hole dynamics in a silicon-germanium alloy with the stoichiometry Si0.25Ge0.75 by extreme ultraviolet transient absorption spectroscopy. Probing the photoinduced dynamics of charge carriers at the germanium M4,5-edge (∼30 eV) allows the germanium atoms to be used as reporter atoms for carrier dynamics in the alloy. The photoexcitation of electrons across the direct and indirect band gap into conduction band (CB) valleys and their subsequent hot carrier relaxation are observed and compared to pure germanium, where the Ge direct (ΔEgap,Ge,direct=0.8 eV) and Si0.25Ge0.75 indirect gaps (ΔEgap,Si0.25Ge0.75,indirect=0.95 eV) are comparable in energy. In the alloy, comparable carrier lifetimes are observed for the X, L, and Γ valleys in the conduction band. A midgap feature associated with electrons accumulating in trap states near the CB edge following intraband thermalization is observed in the Si0.25Ge0.75 alloy. The successful implementation of the reporter atom concept for capturing the dynamics of the electronic bands by site-specific probing in solids opens a route to study carrier dynamics in more complex materials with femtosecond and sub-femtosecond temporal resolution.

36 MATERIALS SCIENCE↗

Accounting for Debye sheath expansion for proud Langmuir probes in magnetic confinement fusion plasmas

A Child-Langmuir law-based method for accounting for Debye sheath expansion while fitting the current-voltage I-V characteristic of proud Langmuir probes (electrodes that extend into the volume of the plasma) is described. For Langmuir probes of a typical size used in tokamak plasmas, these new estimates of electron temperature and ion saturation current density values decreased by up to 60% compared to methods that did not account for sheath expansion. Changes to the collection area are modeled using the Child-Langmuir law and effective expansion perimeter l p , and the model is thus referred to as the “perimeter sheath expansion method.” l p is determined solely from electrode geometry, so the method may be employed without prior measurement of the magnitude of the sheath expansion effects for a given Langmuir probe and can be used for electrodes of different geometries. This method correctly predicts the non-saturating ΔI/ΔV slope for cold, low-density plasmas where sheath-expansion effects are strong, as well as for hot plasmas where ΔI/ΔV ~ 0, though it is shown that the sheath can still significantly affect the collection area in these hot conditions. The perimeter sheath expansion method has several advantages compared to methods where the non-saturating current is fitted: (1) It is more resilient to scatter in the I-V characteristics observed in turbulent plasmas. (2) It is able to separate the contributions to the ΔI/ΔV slope from sheath expansion to that of the high energy electron tail in high Te conditions. (3) It calculates the change in the collection area due to the Debye sheath for conditions where ΔI/ΔV ~ 0 and for V = V f .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Adaptation of a visible wavelength fluorescence microplate reader for discovery of near-infrared fluorescent probes

In this paper, we present an inexpensive, generalizable approach for modifying visible wavelength fluorescence microplate readers to detect emission in the near-infrared (NIR) I (650–950 nm) and NIR II (1000-1350 nm) tissue imaging windows. These wavelength ranges are promising for high sensitivity fluorescence-based cell assays and biological imaging, but the inaccessibility of NIR microplate readers is limiting development of the requisite, biocompatible fluorescent probes. Our modifications enable rapid screening of NIR candidate probes, using short pulses of UV light to provide excitation of diverse systems including dye molecules, semiconductor quantum dots, and metal clusters. To confirm the utility of our approach for rapid discovery of new NIR probes, we examine the silver cluster synthesis products formed on 375 candidate DNA strands that were originally designed to produce green-emitting, DNA-stabilized silver clusters. The fast, sensitive system developed here discovered DNA strands that unexpectedly stabilize NIR-emitting silver clusters.

47 OTHER INSTRUMENTATION↗

Conceptual design of extended magnetic probe set to improve 3D field detection in NSTX-U

Adding toroidal arrays of magnetic probes at the top and bottom of NSTX-U would improve both the detection of the multimodal plasma response to applied magnetic perturbations and the identification of the poloidal structure of unstable plasma modes, as well as contribute to the validation of MHD models, improve the understanding of the plasma response to external fields, and improve the error field correction. In this paper, the linear MHD code MARS-F/K has been used to identify poloidal locations that would improve the capability to measure stationary or near-stationary 3D fields that may result from the plasma response to external sources of non-axisymmetric fields. The study highlighted 6 poloidal positions where new arrays of both poloidal and radial magnetic field sensors would improve the poloidal resolution. Here, the proposed set of new arrays combined with the present ones is shown to be capable of measuring the poloidal structure of perturbations with n ≤ 6 and of detecting the multimodal plasma response. Assessment of the trade-off in the poloidal length of the probes leads to an ideal length between 10 cm and 30 cm. A method to configure the probes of a toroidal array based on the singular value decomposition condition number is proposed, and an ideal solution and a low-cost one are presented.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Utilization of outer-midplane collector probes with isotopically enriched tungsten tracer particles for impurity transport studies in the scrape-off layer of DIII-D (invited)

Triplet sets of replaceable graphite rod collector probes (CPs), each with collection surfaces on opposing faces and oriented normal to the magnetic field, were inserted at the outboard mid-plane of DIII-D to study divertor tungsten (W) transport in the Scrape-Off Layer (SOL). Each CP collects particles along field lines with different parallel sampling lengths (determined by the rod diameters and SOL transport) giving radial profiles from the main wall inward to R-R sep ~ 6 cm. The CPs were deployed in a first-of-a-kind experiment using two toroidal rings of distinguishable isotopically enriched, W-coated divertor tiles installed at 2 poloidal locations in the divertor. Post-mortem Rutherford backscatter spectrometry of the surface of the CPs provided areal density profiles of elemental W coverage. Higher W content was measured on the probe side facing along the field lines toward the inner target indicating higher concentration of W in the plasma upstream of the CP, even though the W-coated rings were in the outer target region of the divertor. Inductively coupled plasma mass spectroscopy validates the isotopic tracer technique through analysis of CPs exposed during L-mode discharges with the outer strike point on the isotopically enriched W coated-tile ring. The contribution from each divertor ring of W to the deposition profiles found on the mid-plane collector probes was able to be de-convoluted using a stable isotope mixing model. Furthermore the results provided quantitative information on the W source and transport from specific poloidal locations within the lower divertor region.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Using polarized positrons to probe physics beyond the standard model

A high intensity polarized positron beam, as part of the JLAB 12 GeV program and the proposed electron-ion collider (EIC), can provide a unique opportunity for testing the Standard Model (SM) and probing for new physics. The combination of high luminosity with polarized electrons and positrons incident on protons and deuterons can isolate important effects and distinguish between possible new physics scenarios in a manner that will complement current experimental efforts. Here, a comparison of cross sections between polarized electron and positron beams will allow for an extraction of the poorly known weak neutral current coupling combination 2C 3u - C 3d and would complement the proposed plan for a precision extraction of the combination 2C 2u - C d at the EIC. Precision measurements of these neutral weak couplings would constrain new physics scenarios including Leptoquarks, R-parity violating supersymmetry, and electron and quark compositeness. The dependence of the charged current cross section on the longitudinal polarization of the positron beam will provide an independent probe to test the chiral structure of the electroweak interactions. A polarized positron can probe charged lepton flavor violation (CLFV) through a search for e + → τ + transitions in a manner that is independent and complementary to the proposed e - → τ - search at the EIC. A positron beam incident on an electron in a stationary nuclear target will also allow for a dark-photon (A') search via the annihilation process e + + e - → A' + γ.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Fast sweeping probe system for characterization of spokes in E × B discharges

In this work, we developed a rapidly swept, back-to-back 100 kHz Langmuir probe system using a tunable compensating network to study the temporal evolution of low frequency oscillations in Penning discharges, Hall Thrusters, and other E × B discharges. Experimental validation of the probe system is performed at low and high sweeping frequencies in a stable Penning discharge. Then application of the probe system to measurements of plasma parameter fluctuations in a low frequency (4 kHz) rotating spoke and an analysis method using the Hilbert transform are shown. We proposs that the rotating spoke oscillation conducts approximately a third of the cross field current in our Penning device.

47 OTHER INSTRUMENTATION↗

Excited state dynamics of CH 2 I 2 and CH 2 BrI studied with UV pump VUV probe photoelectron spectroscopy

We compare the excited state dynamics of diiodomethane (CH 2 I 2 ) and bromoiodomethane (CH 2 BrI) using time resolved photoelectron spectroscopy. A 4.65 eV UV pump pulse launches a dissociative wave packet on excited states of both molecules and the ensuing dynamics are probed via photoionization using a 7.75 eV probe pulse. The resulting photoelectrons are measured with the velocity map imaging technique for each pump-probe delay. Our measurements highlight differences in the dynamics for the two molecules, which are interpreted with high-level ab initio molecular dynamics (trajectory surface hopping) calculations. Our analysis allows us to associate features in the photoelectron spectrum with different portions of the excited state wave packet represented by different trajectories. The excited state dynamics in bromoiodomethane are simple and can be described in terms of direct dissociation along the C–I coordinate, whereas the dynamics in diiodomethane involve internal conversion and motion along multiple dimensions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A combined multi-reference pump-probe simulation method with application to XUV signatures of ultrafast methyl iodide photodissociation

Here, UV pump-XUV/X-ray probe measurements have been successfully applied in the study of photo-induced chemical reactions. Although rich element-specific electronic structure information is accessible within XUV/X-ray (inner-shell) absorption spectra, it can be difficult to interpret the chemistry directly from the spectrum without supporting theoretical simulations. A multireference method to completely simulate UV pump-XUV/X-ray probe measurement has been developed and applied to study the methyl iodide photodissociation process. Multireference, fewest-switches surface hopping (FSSH) trajectories were used to explore the coupled electronic and ionic dynamics upon photoexcitation of methyl iodide. Interpretation of previous measurements is provided by associated multireference, restricted active space, inner-shell spectral simulations. This combination of multireference FSSH trajectories and XUV spectra provides an interpretation of transient features appearing in previous measurements within the first 100 fs after photoexcitation and validates the significant branching ratio in the final excited-state population. Finally, this methodology should prove useful for interpretation of the increasing number of inner-shell probe studies of molecular excited states or for directing new experiments toward interesting regions of the potential energy landscape.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Basic factors for acquiring, correcting, and interpreting probe current-voltage characteristic in moderate-collisional plasma for determining electron energy distribution

Methods for inferring the electron distribution function (EDF) from a probe current–voltage trace are reviewed for moderate-collisional plasma. The explicit accounting of particle collisions, modeling sheath depletion, and electron refilling processes are rarely performed when analyzing probe measurements, yet they are critical for regime validity, EDF-profile accuracy, and space potential quantification precision. Furthermore, the advantages, limitations, and utilization of large-area wall probes in moderate-collisional plasma, capable of highly resolved indications of energetic electrons in plasma, are outlined.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Axial proton probing of magnetic and electric fields inside laser-driven coils

In a laser-driven coil, a laser is used to eject electrons from a plate, which then draws a current through a loop. Diagnosing the field strength, geometry, and conditions within these loops has been one of the primary difficulties in fielding this type of target. In this paper, the diagnostic technique of axial proton probing with a mesh fiducial of a laser-driven coil is demonstrated. Multiple coil types were driven by a 1 ns, 1.25 kJ long pulse beam and probed several times. Here, this technique provides significantly more information than transverse probing on electric- and magnetic-field strength in the region of interest and shows in our experiment complex, non-uniform current path structures and charge distribution.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Ultrafast vibrational dynamics of a trigonal planar anionic probe in ionic liquids (ILs): A two-dimensional infrared (2DIR) spectroscopic investigation

A major impediment limiting the widespread application of ionic liquids (ILs) is their high shear viscosity. Incorporation of a tricyanomethanide (TCM - ) anion in ILs leads to low shear viscosity and improvement of several characteristics suitable for large scale applications. However, properties including interactions of TCM - with the local environment and dynamics of TCM - have not been thoroughly investigated. Herein, we have studied the ultrafast dynamics of TCM - in several imidazolium ILs using linear IR and two-dimensional infrared spectroscopy techniques. The spectral diffusion dynamics of the CN stretching modes of TCM - in all ILs exhibit a nonexponential behavior with a short time component of ~2 ps and a long time component spanning ~9 ps to 14 ps. The TCM - vibrational probe reports a significantly faster relaxation of ILs compared to those observed previously using linear vibrational probes, such as thiocyanate and selenocyanate. Our results indicate a rapid relaxation of the local ion-cage structure embedding the vibrational probe in the ILs. The faster relaxation suggests that the lifetime of the local ion-cage structure decreases in the presence of TCM - in the ILs. Linear IR spectroscopic results show that the hydrogen-bonding interaction between TCM - and imidazolium cations in ILs is much weaker. Shorter ion-cage lifetimes together with weaker hydrogen-bonding interactions account for the low shear viscosity of TCM - based ILs compared to commonly used ILs. In addition, this work demonstrates that TCM - can be used as a potential vibrational reporter to study the structure and dynamics of ILs and other molecular systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Excited state dynamics of cis , cis -1,3-cyclooctadiene: UV pump VUV probe time-resolved photoelectron spectroscopy

We present UV pump, vacuum ultraviolet probe time-resolved photoelectron spectroscopy measurements of the excited state dynamics of cis,cis-1,3-cyclooctadiene. A 4.75 eV deep UV pump pulse launches a vibrational wave packet on the first electronically excited state, and the ensuing dynamics are probed via ionization using a 7.92 eV probe pulse. The experimental results indicate that the wave packet undergoes rapid internal conversion to the ground state in under 100 fs. Comparing the measurements with electronic structure and trajectory surface hopping calculations, we are able to interpret the features in the measured photoelectron spectra in terms of ionization to several states of the molecular cation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

First application of a digital mirror Langmuir probe for real-time plasma diagnosis

We report for the first time, a digital Mirror Langmuir Probe (MLP) has successfully sampled plasma temperature, ion saturation current, and floating potential together on a single probe tip in real time in a radio-frequency driven helicon linear plasma device. This is accomplished by feedback control of the bias sweep to ensure a good fit to I–V characteristics with a high frequency, high power digital amplifier, and field-programmable gate array controller. Measurements taken by the MLP were validated by a low speed I–V characteristic manually collected during static plasma conditions. Plasma fluctuations, induced by varying the axial magnetic field($\widetilde{f}$ = 10 Hz), were also successfully monitored with the MLP. Further refinement of the digital MLP pushes it toward a turn-key system that minimizes the time to deployment and lessens the learning curve, positioning the digital MLP as a capable diagnostic for the study of low radio-frequency plasma physics. These demonstrations bolster confidence in fielding such digital MLP diagnostics in magnetic confinement experiments with high spatial and adequate temporal resolution, such as edge plasma, scrape-off layer, and divertor probes.

47 OTHER INSTRUMENTATION↗

Cryogenic probe for low-noise, high-frequency electronic measurements

The design and performance of a low-noise, modular cryogenic probe, which is applicable to a wide range of measurements over a broad range of working frequencies, temperatures, and magnetic fields, is presented. The design of the probe facilitates the exchange of sample holders and sample-stage amplifiers, which, combined with its characteristic low transmission and reflection loss, make this design suitable for high precision or low sensitivity measurements. The specific example of measuring the shot noise of magnetic tunnel junctions is discussed. We highlight various design characteristics chosen specifically to expand the applicability of the probe to measurement techniques such as nuclear magnetic resonance.

47 OTHER INSTRUMENTATION↗

Compact in situ probe for magnetotransport measurements of 2D materials under variable tensile strain

The recent development of freestanding oxide membranes has opened new opportunities for strain engineering of transition metal oxides beyond values accessible in bulk samples. While a number of studies have been performed with fixed strain, the ability to dynamically control the strain state during measurement would be greatly enabling. To this end, we present an in situ uniaxial strain probe optimized for transport measurements of tensile-strained 2D or quasi-2D materials down to 2 K. Utilizing a flexible polyimide substrate as the stress transfer medium, our platform simplifies the sample preparation process and allows precise alignment of strain fields relative to the crystalline axes. An in situ optical microscope monitors the macroscopic strain state operando and makes it possible to complete an entire magnetotransport study at cryogenic temperatures under continuous strain variations. We demonstrate the capabilities of the probe on a freestanding LaNiO 3 membrane, where we induce tensile strain up to 8% and observe a corresponding strong transport anisotropy. In view of the rapid developments in low-dimensional materials synthesis and the plethora of novel quantum phenomena they exhibit, this strain probe provides general instrumentation for examining and controlling these properties via strain.

2D materials↗

Probing autoionization decay lifetimes of the 4d−16ℓ core-excited states in xenon using attosecond noncollinear four-wave-mixing spectroscopy

The decay of core-excited states is a sensitive probe of autoionization dynamics and correlation effects in many-electron systems, occurring on ultrafast timescales. Xenon, with its dense manifold of autoionizing resonances that can be coupled with near-infrared light, provides a platform to investigate these processes. In this work, the autoionization decay lifetimes of 4d-16ℓ (ℓ = s, p, d, …) core-excited states in xenon atoms are probed with extreme ultraviolet (XUV) attosecond noncollinear four-wave-mixing (FWM) spectroscopy. The 4d{5/2,3/2}-16p XUV-bright states (optically dipole-allowed) exhibit decay lifetimes of ∼6 fs, which is consistent with spectator-type decay. In contrast, the 4d{5/2,3/2}-16s and 4d{5/2,3/2}-16d XUV-dark states (optically dipole forbidden) show longer decay lifetimes of ∼20 fs. Photoionization calculations confirm that all core-hole states with 4d character should decay via spectator channels in ≤6 fs, suggesting that the apparently longer dark-state decay times arise from an alternative mechanism. A few-level simulation of the FWM process shows that the inclusion of a nearby, longer-lived dark state can mimic the experimental FWM signal, suggesting population cycling with a second electronic state with non-4d character. Ab initio calculations support the presence of such multielectron excited states in the 60-70 eV range. These results demonstrate that FWM signals can encode coupled-state dynamics when probing complex systems, highlighting the importance of combining theoretical and experimental approaches to disentangle accurate core-level decay pathways and lifetimes.

Puskar, Nicolette G↗