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We introduce an extreme ultraviolet (XUV)-beamline designed for the time-resolved investigation and coherent control of attosecond (as) electron dynamics in atoms and molecules by polarization-shaped as-laser pulses. Shaped as-pulses are generated through high-harmonic generation (HHG) of tailored white-light supercontinua (WLS) in noble gases. The interaction of shaped as-pulses with the sample is studied using velocity map imaging (VMI) techniques to achieve the differential detection of photoelectron wave packets. The instrument consists of the WLS-beamline, which includes a hollow-core fiber compressor and a home-built 4f polarization pulse shaper, and the high-vacuum XUV-beamline, which combines an HHG-stage and a versatile multi-experiment vacuum chamber equipped with a home-built VMI spectrometer. The VMI spectrometer allows the detection of photoelectron wave packets from both the multiphoton ionization (MPI) of atomic or molecular samples by the tailored WLS-pulses and the single-photon ionization (SPI) by the shaped XUV-pulses. To characterize the VMI spectrometer, we studied the MPI of xenon atoms by linearly polarized WLS pulses. To validate the interplay of these components, we conducted experiments on the SPI of xenon atoms with linearly polarized XUV-pulses. Our results include the reconstruction of the 3D photoelectron momentum distribution (PMD) and initial findings on the coherent control of the PMD by tuning the spectrum of the XUV-pulses with the spectral phase of the WLS. Our results demonstrate the performance of the entire instrument for HHG-based photoelectron imaging spectroscopy with prototypical shaped pulses. Perspectively, we will employ polarization-tailored WLS-pulses to generate polarization-shaped as-pulses. [ABSTRACT FROM AUTHOR]

Sagittally focusing x-ray crystal spectrometers with elliptical profiles in the meridional (x-ray dispersion) plane are proposed for plasma diagnostics in experiments accompanied by high neutron yields. The spectrometers feature a variable sagittal radius of curvature to ensure the sagittal focusing of rays for each photon energy in a chosen detection plane. The detector is placed after the ray crossing point at the second ellipse focus, and the source-to-detector distance is maximized to reduce the neutron-induced background. The elliptical shape imposes a limitation on the spectrometer geometry such that the influence of the source size on the spectral resolution can be avoided only for a demagnifying spectrometer (the source-to-crystal distance is larger than that of crystal-to-detector). Hence, two designs are proposed. The first design, featuring high magnification and limited spectral resolution can be suitable for x-ray continuum spectroscopy. The second design of high demagnification is optimized for spectral resolution, and can be used for time-resolved spectroscopy of plasma's characteristic emission lines using streak cameras. The key performance characteristics of the two designs are verified using ray tracing. [ABSTRACT FROM AUTHOR]

We present the development of a versatile apparatus for 6.2 eV laser-based time and angle-resolved photoemission spectroscopy with micrometer spatial resolution (time-resolved μ-ARPES). With a combination of tunable spatial resolution down to ∼11 μm, high energy resolution (∼11 meV), near-transform-limited temporal resolution (∼280 fs), and tunable 1.55 eV pump fluence up to 3 mJ/cm2, this time-resolved μ-ARPES system enables the measurement of ultrafast electron dynamics in exfoliated and inhomogeneous materials. We demonstrate the performance of our system by correlating the spectral broadening of the topological surface state of Bi2Se3 with the spatial dimension of the probe pulse, as well as resolving the spatial inhomogeneity contribution to the observed spectral broadening. Finally, after in situ exfoliation, we performed time-resolved μ-ARPES on a ∼30 μm flake of transition metal dichalcogenide WTe2, thus demonstrating the ability to access ultrafast electron dynamics with momentum resolution on micro-exfoliated materials. [ABSTRACT FROM AUTHOR]

Parametric superfluorescence (PSF), which originated from the optical amplification of vacuum quantum noise, is the primary noise source of femtosecond fluorescence non-collinear optical parametric amplification spectroscopy (FNOPAS). It severely affects the detection limit of FNOPAS to collect the femtosecond time-resolved spectra of extremely weak fluorescence. Here, we report the development of femtosecond fluorescence conical optical parametric amplification spectroscopy (FCOPAS), aimed at effectively suppressing the noise fluctuation from the PSF background. In contrast to traditional FNOPAS configurations utilizing lateral fluorescence collection and dot-like parametric amplification, FCOPAS employs an innovative conical fluorescence collection and ring-like amplification setup. This design enables effective cancellation of noise fluctuation across the entire PSF ring, resulting in an approximate order of magnitude reduction in PSF noise compared to prior FNOPAS outcomes. This advancement enables the resolution of transient fluorescence spectra of 4-dicyanomethylene-2-methyl-6-p-dimethylaminostyryl-4H-pyran (DCM) dye molecules in ethanol, even at an optically dilute concentration of 10−6 mol/l, with significantly enhanced signal-to-noise ratios. This improvement will be significant for extremely weak fluorescence detection on the femtosecond time scale. [ABSTRACT FROM AUTHOR]

A noncollinear optical parametric amplifier (NOPA) can produce few-cycle femtosecond laser pulses that are ideally suited for time-resolved optical spectroscopy measurements. However, the nonlinear-optical process giving rise to ultrabroadband pulses is susceptible to spatiotemporal dispersion problems. Here, we detail refinements, including chirped-pulse amplification (CPA) and pulse-front matching (PFM), that minimize spatiotemporal dispersion and thereby improve the properties of ultrabroadband pulses produced by a NOPA. The description includes a rationale behind the choices of optical and optomechanical components, as well as assessment protocols. We demonstrate these techniques using a 1 kHz, second-harmonic Ti:sapphire pump configuration, which produces ∼5-fs duration pulses that span from about 500 to 800 nm with a bandwidth of about 200 THz. To demonstrate the utility of the CPA-PFM-NOPA, we measure vibrational quantum beats in the transient–absorption spectrum of methylene blue, a dye molecule that serves as a reference standard. [ABSTRACT FROM AUTHOR]

A time-resolved electron paramagnetic resonance (TREPR) method with 40 ns time resolution and a high sensitivity suitable for the detection of short-lived radicals under thermal equilibrium is developed. The key is the introduction of a new detection technique named ultrawide single sideband phase sensitive detection (U-PSD) to the conventional continuous-wave EPR, which remarkably enhanced the sensitivity for the detection of broadband transient signals compared with the direct detection protocol. By repeatedly triggering a transient kinetic event f(t) (e.g., by laser flash photolysis) under a 100 kHz magnetic field modulation with precise phase control, this technique can build an ultrawide single sideband modulated signal. After single sideband demodulation, the flicker noise-suppressed signal f(t) with wide bandwidth is recovered. A U-PSD TREPR spectrometer prototype has been built, which integrated timing sequence control, laser flash excitation, data acquisition systems, and the U-PSD algorithm with a conventional continuous-wave EPR. It exhibited excellent performance in monitoring a model transient radical system, laser flash photolysis of benzophenone in isopropanol. Both the intense chemically induced dynamic electron polarization signals and the much weaker thermal equilibrium EPR signals of the generated acetone ketyl radical and benzophenone ketyl radical were clearly observed within a wide timescale ranging from sub-microsecond to milliseconds. This prototype validated the feasibility of the U-PSD technique and demonstrated its superior performance in studying complex photochemical systems containing various transient radicals, which complements the established TREPR techniques and provides a powerful tool for deep mechanistic understandings, such as in photoredox catalysis and artificial photosynthesis. [ABSTRACT FROM AUTHOR]

We describe a setup of time-, spin-, and angle-resolved photoemission spectroscopy (tr-SARPES) employing a 10.7 eV (λ = 115.6 nm) pulse laser at a 1 MHz repetition rate as a probe photon source. This equipment effectively combines the technologies of a high-power Yb:fiber laser, ultraviolet-driven harmonic generation in Xe gas, and a SARPES apparatus equipped with very-low-energy-electron-diffraction spin detectors. A high repetition rate (1 MHz) of the probe laser allows experiments with the photoemission space-charge effects significantly reduced, despite a high flux of 1013 photons/s on the sample. The relatively high photon energy (10.7 eV) also brings the capability of observing a wide momentum range that covers the entire Brillouin zone of many materials while ensuring high momentum resolution. The experimental setup overcomes the low efficiency of spin-resolved measurements, which gets even more severe for the pump-probed unoccupied states, and affords the opportunity to investigate ultrafast electron and spin dynamics of modern quantum materials with energy and time resolutions of 25 meV and 360 fs, respectively. [ABSTRACT FROM AUTHOR]

Significant information on the dynamics of the plasma constituents in Hall effect thrusters can be obtained using minimally intrusive techniques, such as laser-induced fluorescence (LIF) diagnostics. Indeed, LIF provides an excellent tool to determine the ion velocity distribution function with high spatial resolution. Even in a steady-state operation, recording time-resolved maps of the velocity distribution is relevant due to persisting time-dependent features of the thruster discharge. One of the preeminent phenomena that render the ion velocity distribution to be time dependent is commonly attributed to the breathing mode, characterized by pronounced oscillations in the discharge current. The goal of this work is to propose a new technique for plasma dynamic studies based on LIF spectroscopy with phase-resolution during the breathing period. For this purpose, the Hilbert transform is used to define the instantaneous phase of oscillation of the thruster current. Ion velocity distribution modification over assigned phases of oscillation is measured simultaneously and in real-time thanks to a fully numerical analysis of the data. [ABSTRACT FROM AUTHOR]

The implementation of attosecond photoelectron–photoion coincidence spectroscopy for the investigation of atomic and molecular dynamics calls for a high-repetition-rate driving source combined with experimental setups characterized by excellent stability for data acquisition over time intervals ranging from a few hours up to a few days. This requirement is crucial for the investigation of processes characterized by low cross sections and for the characterization of fully differential photoelectron(s) and photoion(s) angular and energy distributions. We demonstrate that the implementation of industrial-grade lasers, combined with a careful design of the delay line implemented in the pump–probe setup, allows one to reach ultrastable experimental conditions leading to an error in the estimation of the time delays of only 12 as over an acquisition time of 6.5 h. This result opens up new possibilities for the investigation of attosecond dynamics in simple quantum systems. [ABSTRACT FROM AUTHOR]

Atomic force microscopy (AFM) is an analytical surface characterization tool that reveals the surface topography at a nanometer length scale while probing local chemical, mechanical, and even electronic sample properties. Both contact (performed with a constant deflection of the cantilever probe) and dynamic operation modes (enabled by demodulation of the oscillation signal under tip–sample interaction) can be employed to conduct AFM-based measurements. Although surface topography is accessible regardless of the operation mode, the resolution and the availability of the quantified surface properties depend on the mode of operation. However, advanced imaging techniques, such as frequency modulation, to achieve high resolution, quantitative surface properties are not implemented in many commercial systems. Here, we show the step-by-step customization of an atomic force microscope. The original system was capable of surface topography and basic force spectroscopy measurements while employing environmental control, such as temperature variation of the sample/tip, etc. We upgraded this original setup with additional hardware (e.g., a lock-in amplifier with phase-locked loop capacity, a high-voltage amplifier, and a new controller) and software integration while utilizing its environmental control features. We show the capabilities of the customized system with frequency modulation-based topography experiments and automated voltage and/or distance spectroscopy, time-resolved AFM, and two-dimensional force spectroscopy measurements under ambient conditions. We also illustrate the enhanced stability of the setup with active topography and frequency drift corrections. We believe that our methodology can be useful for the customization and automation of other scanning probe systems. [ABSTRACT FROM AUTHOR]

Time-resolved angle-resolved photoemission spectroscopy (Tr-APRES) gives direct insight into electron dynamics by providing temporal-, energy-, and momentum-resolved information in one experiment. A major obstacle to using high harmonic generation (HHG) probe pulses for photoemission spectroscopy is the low conversion efficiency, that is, the low flux of probe photons. We use a Yb-KGW based duo-laser source with an oscillator to pump two separate amplifiers and generate two synchronized pulsed laser sources with average energies of 7.5 and 6 W. By using the multiplate continuum method and chirped mirrors, the resulting flux of HHG photons at 33–70 eV can be increased 50-fold (up to 1011 photons/s) by using post-compressed 30 fs pulses compared with the photon flux generated by the fundamental 190 fs pulses. Moreover, pulses from the 6 W amplifier are used to pump an optical parametric amplifier that can vary the wavelengths for photoexcitation. The system performance is demonstrated by applying Tr-ARPES to single-crystal graphite. The front tilt broadening is significantly suppressed by the off-plane mounted conical grating, leading to a 184 fs temporal resolution that is mainly limited by the pump pulse. The energy resolution is 176 meV. [ABSTRACT FROM AUTHOR]

We report on the development of a diagnostic to measure the time-resolved column density and Doppler temperature of atomic vapors produced by laser ablation. The diagnostic is based on the strong frequency dependence of the atomic susceptibility near an electronic transition in the interrogated atomic species. Interference on the face of a fast photodetector between the several frequency components present in a sinusoidally phase-modulated probe beam will produce a time signature uniquely determined by the column density of atoms in the probed atomic state and the Doppler temperature of the atomic vapor. With the extensive, high precision atomic spectroscopy data available in the literature, it is possible to model the vapor and extract the desired parameters through comparison of the model result with the experimental data. [ABSTRACT FROM AUTHOR]

A recently presented chemical vapor deposition (CVD) method involves using plasma electrons as reducing agents for deposition of metals. The plasma electrons are attracted to the substrate surface by a positive substrate bias. Here, we present how a standard quartz crystal microbalance (QCM) system can be modified to allow applying a DC bias to the QCM sensor to attract plasma electrons to it and thereby also enable in situ growth monitoring during the electron-assisted CVD method. We show initial results from mass gain evolution over time during deposition of iron films using the biased QCM and how the biased QCM can be used for process development and provide insight into the surface chemistry by time-resolving the CVD method. Post-deposition analyses of the QCM crystals by cross-section electron microscopy and high-resolution x-ray photoelectron spectroscopy show that the QCM crystals are coated by an iron-containing film and thus function as substrates in the CVD process. A comparison of the areal mass density given by the QCM crystal and the areal mass density from elastic recoil detection analysis and Rutherford backscattering spectrometry was done to verify the function of the QCM setup. Time-resolved CVD experiments show that this biased QCM method holds great promise as one of the tools for understanding the surface chemistry of the newly developed CVD method. [ABSTRACT FROM AUTHOR]

Developing a widely tunable vacuum ultraviolet (VUV) source with a sub-100 fs pulse duration is critical for ultrafast pump–probe techniques such as time- and angle-resolved photoemission spectroscopy (TrARPES). While a tunable probe source with a photon energy of 5.3–7.0 eV has been recently implemented for TrARPES by using a KBe2BO3F2 (KBBF) device, the time resolution of 280–320 fs is still not ideal, which is mainly limited by the duration of the VUV probe pulse generated by the KBBF device. Here, by designing a new KBBF device, which is specially optimized for fs applications, an optimum pulse duration of 55 fs is obtained after systematic diagnostics and optimization. More importantly, a high time resolution of 81–95 fs is achieved for TrARPES measurements covering the probe photon energy range of 5.3–7.0 eV, making it particularly useful for investigating the ultrafast dynamics of quantum materials. Our work extends the application of the KBBF device to ultrafast pump–probe techniques with the advantages of both a widely tunable VUV source and ultimate time resolution. [ABSTRACT FROM AUTHOR]

High-precision x-ray imaging diagnostics of hotspot at the stagnation stage are essential for regulating implosion asymmetry and retrieving physical implosion parameters. With regard to 10–20 keV energy band imaging, existing diagnostic instruments such as Kirkpatrick–Baez microscopes and pinhole cameras are insufficient in terms of spatial resolution and collection efficiency. The situation is even worse when high-speed, time-resolved imaging diagnostics are performed by coupling framing cameras or line-of-sight imagers. This article presents the basic principles and optical system design of a 17.48 keV modified Wolter x-ray microscope, to resolve the problems encountered in high-energy imaging diagnostics. The proposed optical configuration offers a better spatial resolution, greater depth of field, and preliminary compliance with the requirements of high precision optical processing techniques. The spatial resolution is better than 1 µm in a field range ±150 µm, and is better than 3 µm in a total field of view ∼408 µm in diameter. The geometric solid angle is calculated as 3.0 × 10−5 sr and is estimated to be 1.2 × 10−6 sr, considering the reflectivity of the double mirrors. The proposed microscope is expected to effectively improve spatial resolution and signal-to-noise ratio for high-energy imaging diagnostics. [ABSTRACT FROM AUTHOR]

A 790-nm-driven high-harmonic generation source with a repetition rate of 6 kHz is combined with a toroidal-grating monochromator and a high-detection-efficiency photoelectron time-of-flight momentum microscope to enable time- and momentum-resolved photoemission spectroscopy over a spectral range of 23.6–45.5 eV with sub-100 fs time resolution. Three-dimensional (3D) Fermi surface mapping is demonstrated on graphene-covered Ir(111) with energy and momentum resolutions of ≲100 meV and ≲0.1 Å−1, respectively. The tabletop experiment sets the stage for measuring the kz-dependent ultrafast dynamics of 3D electronic structure, including band structure, Fermi surface, and carrier dynamics in 3D materials as well as 3D orbital dynamics in molecular layers. [ABSTRACT FROM AUTHOR]

The time-resolving magnetic recoil spectrometer (MRSt) is a transformative diagnostic that will be used to measure the time-resolved neutron spectrum from an inertial confinement fusion implosion at the National Ignition Facility (NIF). It uses a CD foil on the outside of the hohlraum to convert fusion neutrons to recoil deuterons. An ion-optical system positioned outside the NIF target chamber energy-disperses and focuses forward-scattered deuterons. A pulse-dilation drift tube (PDDT) subsequently dilates, un-skews, and detects the signal. While the foil and ion-optical system have been designed, the PDDT requires more development before it can be implemented. Therefore, a phased plan is presented that first uses the foil and ion-optical systems with detectors that can be implemented immediately—namely CR-39 and hDISC streak cameras. These detectors will allow the MRSt to be commissioned in an intermediate stage and begin collecting data on a reduced timescale, while the PDDT is developed in parallel. A CR-39 detector will be used in phase 1 for the measurement of the time-integrated neutron spectra with excellent energy-resolution, necessary for the energy calibration of the system. Streak cameras will be used in phase 2 for measurement of the time-resolved spectrum with limited spectral coverage, which is sufficient to diagnose the time-resolved ion temperature. Simulations are presented that predict the performance of the streak camera detector, indicating that it will achieve excellent burn history measurements at current yields, and good time-resolved ion-temperature measurements at yields above 3 × 1017. The PDDT will be used for optimal efficiency and resolution in phase 3. [ABSTRACT FROM AUTHOR]

EXPANSE, an EXPanded Angle Neutron Spin Echo instrument, has been proposed and selected as one of the first suite of instruments to be built at the Second Target Station of the Spallation Neutron Source at the Oak Ridge National Laboratory. This instrument is designed to address scientific problems that involve high-energy resolution (neV–μeV) of dynamic processes in a wide range of materials. The wide-angle detector banks of EXPANSE provide coverage of nearly two orders of magnitude in scattering wavenumbers, and the wide wavelength band affords approximately four orders of magnitude in Fourier times. This instrument will offer unique capabilities that are not available in the currently existing neutron scattering instruments in the United States. Specifically, EXPANSE will enable direct measurements of slow dynamics in the time domain over wide Q-ranges simultaneously and will also enable time-resolved spectroscopic studies. The instrument is expected to contribute to a diverse range of science areas, including soft matter, polymers, biological materials, liquids and glasses, energy materials, unconventional magnets, and quantum materials. [ABSTRACT FROM AUTHOR]

Understanding thermal transport at the microscale to the nanoscale is crucially important for a wide range of technologies ranging from device thermal management and protection systems to thermal-energy regulation and harvesting. In the past decades, non-contact optical methods, such as time-domain and frequency-domain thermoreflectance, have emerged as extremely powerful and versatile thermal metrological techniques for the measurement of material thermal conductivities. Here, we report the measurement of thermal conductivity of thin films of CH3NH3PbI3 (MAPbI3), a prototypical metal-halide perovskite, by developing a time-resolved optical technique called vibrational-pump visible-probe (VPVP) spectroscopy. The VPVP technique relies on the direct thermal excitation of MAPbI3 by femtosecond mid-infrared optical pump pulses that are wavelength-tuned to a vibrational mode of the material, after which the time dependent optical transmittance across the visible range is probed in the ns to the μs time window using a broadband pulsed laser. Using the VPVP method, we determine the thermal conductivities of MAPbI3 thin films deposited on different substrates. The transducer-free VPVP method reported here is expected to permit spectrally resolving and spatiotemporally imaging of the dynamic lattice temperature variations in organic, polymeric, and hybrid organic–inorganic semiconductors. [ABSTRACT FROM AUTHOR]

This paper reports on the assembly of a compact, low-cost, pulsed-power facility used for plasma studies. The construction uses two modules placed on opposite sides of the test chamber to minimize the system impedance and improve access to test samples. The stored energy is 1 kJ with a peak current of 135 kA and a 1592 ns quarter-period time. Up until now, an imploding conical-wire array has been studied by using time-integrated (visible) imaging, and time-resolved laser imaging, providing a measure of the plasma jet speed in the range of 170 km/s. Our future plans will continue to investigate high-energy-density plasmas that are relevant to the space environment, fusion, and spectroscopy. [ABSTRACT FROM AUTHOR]

Time- and angle-resolved photoemission spectroscopy (TrARPES) is a powerful technique for capturing the ultrafast dynamics of charge carriers and revealing photo-induced phase transitions in quantum materials. However, the lack of widely tunable probe photon energy, which is critical for accessing the dispersions at different out-of-plane momentum kz in TrARPES measurements, has hindered the ultrafast dynamics investigation of 3D quantum materials, such as Dirac or Weyl semimetals. Here, we report the development of a TrARPES system with a highly tunable probe photon energy from 5.3 to 7.0 eV. The tunable probe photon energy is generated by the fourth harmonic generation of a tunable wavelength femtosecond laser source by combining a β-BaB2O4 crystal and a KBe2BO3F2 crystal. A high energy resolution of 29–48 meV and time resolution of 280–320 fs are demonstrated on 3D topological materials ZrTe5 and Sb2Te3. Our work opens up new opportunities for exploring ultrafast dynamics in 3D quantum materials. [ABSTRACT FROM AUTHOR]

We present the design, integration, and operation of the novel vacuum ultraviolet (VUV) beamline installed at the free-electron laser (FEL) FLASH. The VUV source is based on high-order harmonic generation (HHG) in gas and is driven by an optical laser system synchronized with the timing structure of the FEL. Ultrashort pulses in the spectral range from 10 to 40 eV are coupled with the FEL in the beamline FL26, which features a reaction microscope (REMI) permanent endstation for time-resolved studies of ultrafast dynamics in atomic and molecular targets. The connection of the high-pressure gas HHG source to the ultra-high vacuum FEL beamline requires a compact and reliable system, able to encounter the challenging vacuum requirements and coupling conditions. First commissioning results show the successful operation of the beamline, reaching a VUV focused beam size of about 20 µm at the REMI endstation. Proof-of-principle photo-electron momentum measurements in argon indicate the source capabilities for future two-color pump–probe experiments. [ABSTRACT FROM AUTHOR]

We present the development of a multi-resolution photoemission spectroscopy (MRPES) setup, which probes quantum materials in energy, momentum, space, and time. This versatile setup integrates three light sources in one photoemission setup and can conveniently switch between traditional angle-resolved photoemission spectroscopy (ARPES), time-resolved ARPES (trARPES), and micrometer-scale spatially resolved ARPES. It provides a first-time all-in-one solution to achieve an energy resolution of < 4 meV, a time resolution of < 35 fs, and a spatial resolution of ∼ 10 μm in photoemission spectroscopy. Remarkably, we obtain the shortest time resolution among the trARPES setups using solid-state nonlinear crystals for frequency upconversion. Furthermore, this MRPES setup is integrated with a shadow-mask assisted molecular beam epitaxy system, which transforms the traditional photoemission spectroscopy into a quantum device characterization instrument. We demonstrate the functionalities of this novel quantum material testbed using FeSe/SrTiO3 thin films and MnBi4Te7 magnetic topological insulators. [ABSTRACT FROM AUTHOR]

We present a two-color Kerr microscopy system based on two electronically synchronized erbium-fiber laser oscillators with independently tunable emission energies spanning most of the visible spectrum. Combining a spatial resolution below 2 μm and sub-ps time resolution with high sensitivity and cryogenic sample temperatures, it is ideally suited for studying spin and valley dynamics in a wide range of two-dimensional materials. We illustrate its capabilities by studying a monolayer of the common semiconducting transition metal disulfide MoS2. [ABSTRACT FROM AUTHOR]

We present a table-top extreme ultraviolet (XUV) beamline for measuring time- and frequency-resolved XUV-excited optical luminescence (XEOL) with additional femtosecond-resolution XUV transient absorption spectroscopy functionality. XUV pulses are generated via high-harmonic generation using a near-infrared pulse in a noble gas medium and focused to excite luminescence from a solid sample. The luminescence is collimated and guided into a streak camera where its spectral components are temporally resolved with picosecond temporal resolution. We time-resolve XUV-excited luminescence and compare the results to luminescence decays excited at longer wavelengths for three different materials: (i) sodium salicylate, an often used XUV scintillator; (ii) fluorescent labeling molecule 4-carbazole benzoic (CB) acid; and (iii) a zirconium metal oxo-cluster labeled with CB, which is a photoresist candidate for extreme-ultraviolet lithography. Our results establish time-resolved XEOL as a new technique to measure transient XUV-driven phenomena in solid-state samples and identify decay mechanisms of molecules following XUV and soft-x-ray excitation. [ABSTRACT FROM AUTHOR]

Rapid compression machines (RCMs) are used to simulate a single stroke of an internal combustion engine. After a high-speed compression process, a high-pressure and low-to-intermediate temperature condition can be obtained, under which ignition processes are usually studied. With the help of different diagnostic methods, the detailed speciation information of the ignition process can be quantified. In this study, the molecular beam mass spectrometry (MBMS) diagnostic method was applied on an RCM to realize time-resolved concentration profile measurements. To realize the combination between RCM and MBMS, particle dampers were adopted to suppress the vibrations of the RCM, and a novel flexible interface was designed to maintain a high vacuum, which ensured the safe and effective operation of a high-repetition-rate time-of-flight mass spectrometer (HRR-TOF-MS). The detailed configuration of this diagnostic method is presented, and the data acquisition system and data analysis method are described. The arrangement was validated through the investigation of the well-studied decomposition of 1,3,5-trioxane at temperatures between 697 and 777 K at 10 bars. The measured concentration profiles of 1,3,5-trioxane and formaldehyde were in good agreement with previous experimental and theoretical calculation results. The experimental results showed that the newly developed RCM coupled with the HRR-TOF-MS has advantages in time-resolved speciation measurements at low-to-intermediate temperatures and high pressures, and it can be applied in low-temperature combustion chemical kinetics studies. [ABSTRACT FROM AUTHOR]

Here, we report our newly built table-top ultrafast extreme ultraviolet (EUV) photoemission electron microscope. The coherent ultrafast EUV light is served by a single order harmonic, which is generated by the interaction between the intense 800-nm femtosecond laser and noble gases in the hollow core fiber. The required order of the harmonic is selected out by a single grating in the off-plane mount and focused on the sample in the ultrahigh vacuum chamber of the photoemission electron microscope. Using metal gold and copper samples, the spatial resolution is calibrated to be better than 50 nm and the energy resolution is calibrated to be better than 300 meV. This microscope provides an advanced tool for studying electron dynamics covering the full Brillouin zone of solid materials with ultrahigh time, space, and energy resolution. [ABSTRACT FROM AUTHOR]

The impurity radiation from the divertor region of the EAST tokamak is dominantly in the wavelength range of vacuum ultraviolet (VUV) due to the elevated edge electron temperature. A space-resolved VUV spectroscopy is developed to measure impurity radiation in the divertor region. An eagle-type VUV spectrometer with a focal length of 1 m is adopted in this system, equipped with a spherical grating and a charged-coupled device (CCD) detector. The performance of the VUV spectrometer is preliminarily tested on a synchrotron radiation facility. The wavelength calibration is conducted near 65 nm. It is found that the wavelength range observed by the CCD detector is about 11.07 nm around the central wavelength of about 65 nm. With a linear dispersion of 0.0053 nm/pixel, it is possible to measure the ion temperature lower than 20 eV at the edge region by analyzing the Doppler broadening of a carbon line. These test results show that the performance of the VUV spectrometer is capable of measuring divertor radiation and analyzing the ion temperature of edge impurity ions. [ABSTRACT FROM AUTHOR]

Achieving a high time resolution is highly desirable for revealing the electron dynamics and light-induced phenomena in time- and angle-resolved photoemission spectroscopy (TrARPES). Here, we identify key factors for achieving the optimum time resolution, including laser bandwidth and optical component induced chirp. A full diagnostic scheme is constructed to characterize the pulse duration and chirp of the fundamental beam, second harmonic, and fourth harmonic, and prism pairs are used to compensate for the chirp. Moreover, by using a Sb2Te3 film as a test sample, we can achieve a high test efficiency for the time resolution during the optimization process. An optimized time resolution of 81 fs is achieved in our TrARPES system with a high repetition rate tunable from 76 to 4.75/n MHz. [ABSTRACT FROM AUTHOR]

Structures, kinetics, and chemical reactivities at interfaces and surfaces are key to understanding many of the fundamental scientific problems related to chemical, material, biological, and physical systems. These steady-state and dynamical properties at interfaces and surfaces require even-order techniques with time-resolution and spectral-resolution. Here, we develop fourth-order interface-/surface-specific two-dimensional electronic spectroscopy, including both two-dimensional electronic sum frequency generation (2D-ESFG) spectroscopy and two-dimensional electronic second harmonic generation (2D-ESHG) spectroscopy, for structural and dynamics studies of interfaces and surfaces. The 2D-ESFG and 2D-ESHG techniques were based on a unique laser source of broadband short-wave IR from 1200 nm to 2200 nm from a home-built optical parametric amplifier. With the broadband short-wave IR source, surface spectra cover most of the visible light region from 480 nm to 760 nm. A translating wedge-based identical pulses encoding system (TWINs) was introduced to generate a phase-locked pulse pair for coherent excitation in the 2D-ESFG and 2D-ESHG. As an example, we demonstrated surface dark states and their interactions of the surface states at p-type GaAs (001) surfaces with the 2D-ESFG and 2D-ESHG techniques. These newly developed time-resolved and interface-/surface-specific 2D spectroscopies would bring new information for structure and dynamics at interfaces and surfaces in the fields of the environment, materials, catalysis, and biology. [ABSTRACT FROM AUTHOR]

Time-of-flight-based momentum microscopy has a growing presence in photoemission studies, as it enables parallel energy- and momentum-resolved acquisition of the full photoelectron distribution. Here, we report table-top extreme ultraviolet time- and angle-resolved photoemission spectroscopy (trARPES) featuring both a hemispherical analyzer and a momentum microscope within the same setup. We present a systematic comparison of the two detection schemes and quantify experimentally relevant parameters, including pump- and probe-induced space-charge effects, detection efficiency, photoelectron count rates, and depth of focus. We highlight the advantages and limitations of both instruments based on exemplary trARPES measurements of bulk WSe2. Our analysis demonstrates the complementary nature of the two spectrometers for time-resolved ARPES experiments. Their combination in a single experimental apparatus allows us to address a broad range of scientific questions with trARPES. [ABSTRACT FROM AUTHOR]

Here, we present an integrated ultra-high vacuum apparatus—named MBE-Cluster —dedicated to the growth and in situ structural, spectroscopic, and magnetic characterization of complex materials. Molecular Beam Epitaxy (MBE) growth of metal oxides, e.g., manganites, and deposition of the patterned metallic layers can be fabricated and in situ characterized by reflection high-energy electron diffraction, low-energy electron diffraction, Auger electron spectroscopy, x-ray photoemission spectroscopy, and azimuthal longitudinal magneto-optic Kerr effect. The temperature can be controlled in the range from 5 K to 580 K, with the possibility of application of magnetic fields H up to ±7 kOe and electric fields E for voltages up to ±500 V. The MBE-Cluster operates for in-house research as well as user facility in combination with the APE beamlines at Sincrotrone-Trieste and the high harmonic generator facility for time-resolved spectroscopy. [ABSTRACT FROM AUTHOR]

Laser enhanced field evaporation of surface atoms in laser-assisted Atom Probe Tomography (APT) can simultaneously excite photoluminescence in semiconductor or insulating specimens. An atom probe equipped with appropriate focalization and collection optics has been coupled with an in situ micro-photoluminescence (μPL) bench that can be operated during APT analysis. The photonic atom probe instrument we have developed operates at frequencies up to 500 kHz and is controlled by 150 fs laser pulses tunable in energy in a large spectral range (spanning from deep UV to near IR). Micro-PL spectroscopy is performed using a 320 mm focal length spectrometer equipped with a CCD camera for time-integrated and with a streak camera for time-resolved acquisitions. An example of application of this instrument on a multi-quantum well oxide heterostructure sample illustrates the potential of this new generation of tomographic atom probes. [ABSTRACT FROM AUTHOR]

To facilitate the development of molten salt reactor technologies, a fundamental understanding of the physical and chemical properties of molten salts under the combined conditions of high temperature and intense radiation fields is necessary. Optical spectroscopic (UV–Vis–near IR) and electrochemical techniques are powerful analytical tools to probe molecular structure, speciation, thermodynamics, and kinetics of solution dynamics. Here, we report the design and fabrication of three custom-made apparatus: (i) a multi-port spectroelectrochemical furnace equipped with optical spectroscopic and electrochemical instrumentation, (ii) a high-temperature cell holder for time-resolved optical detection of radiolytic transients in molten salts, and (iii) a miniaturized spectroscopy furnace for the investigation of steady-state electron beam effects on molten salt speciation and composition by optical spectroscopy. Initial results obtained with the spectroelectrochemical furnace (i) and high-temperature cell holder (ii) are reported. [ABSTRACT FROM AUTHOR]

We present a compact setup for spin-, time-, and angle-resolved photoemission spectroscopy. A 10 kHz titanium sapphire laser system delivers pulses of 20 fs duration, which drive a high harmonic generation-based source for ultraviolet photons at 21 eV for photoemission. The same laser also excites the sample for pump–probe experiments. Emitted electrons pass through a hemispherical energy analyzer and a spin-filtering element. The latter is based on spin-polarized low-energy electron diffraction on an Au-passivated iridium crystal. The performance of the measurement system is discussed in terms of the resolution and efficiency of the spin filter, which are higher than those for Mott-based techniques. [ABSTRACT FROM AUTHOR]

A newly constructed high-repetition-rate shock tube designed for kinetic studies of high-temperature reactions using spectroscopic methods is described. The instrument operates at a 0.2-Hz cycle rate with a high reproducibility of reaction conditions that permits extensive signal averaging to improve the quality of kinetic trace data. The density and temperature of the gas behind the reflected shock wave are examined by probing the product formation from reference reactions. Two types of experimental techniques are implemented: transient absorption spectroscopy and time-resolved laser-induced fluorescence. Both methods are shown to be suitable for kinetic measurements of elementary reactions, as illustrated by their application in thermal decomposition reactions of the benzyl radicals and trifluoromethane. [ABSTRACT FROM AUTHOR]

We report a novel experimental technique to investigate ultrafast dynamics in photoexcited molecules by probing the 3rd-order nonlinear optical susceptibility. A non-collinear 3-pulse scheme is developed to probe the ultrafast dynamics of excited electronic states using the optical Kerr effect. Optical homodyne and optical heterodyne detections are demonstrated to measure the 3rd-order nonlinear optical response for the S1 excited state of liquid nitrobenzene, which is populated by 2-photon absorption of a 780 nm 40 fs excitation pulse. [ABSTRACT FROM AUTHOR]

Performing time- and angle-resolved photoemission (tr-ARPES) spectroscopy at high momenta necessitates extreme ultraviolet laser pulses, which are typically produced via high harmonic generation (HHG). Despite recent advances, HHG-based setups still require large pulse energies (from hundreds of μJ to mJ) and their energy resolution is limited to tens of meV. Here, we present a novel 11 eV tr-ARPES setup that generates a flux of 5 × 1010 photons/s and achieves an unprecedented energy resolution of 16 meV. It can be operated at high repetition rates (up to 250 kHz) while using input pulse energies down to 3 µJ. We demonstrate these unique capabilities by simultaneously capturing the energy and momentum resolved dynamics in two well-separated momentum space regions of a charge density wave material ErTe3. This novel setup offers the opportunity to study the non-equilibrium band structure of solids with exceptional energy and time resolutions at high repetition rates. [ABSTRACT FROM AUTHOR]

A multichannel spectroscopic diagnostic based on the Stark effect on helium lines was developed and implemented in IShTAR (Ion Cyclotron Sheath Test ARrangement) to measure the spatial distribution of electric fields across the radio frequency sheaths of the ion cyclotron antenna. Direct measurements of the DC electric fields in the antenna sheaths are an important missing component in understanding the antenna-plasma edge interactions in magnetically confined fusion plasmas since they will be used to benchmark theoretical models against real antenna operation. Along with the high-resolution Czerny-Turner monochromator and a detector with an intensifier, the hardware relies on the 2 chained set of linear-to-linear fiber bundles that provide seven optical channels capable of resolving an 8.4 mm region in the vicinity of the antenna's box. The diagnostic is supported with local helium gas puff, enabling it to operate in nonhelium plasmas. Spatially resolved electric field was measured for two discharge configurations, one with and one without the ICRF antenna. The results show a clear difference in the shape of the DC electric field's spatial profile for the two cases studied, with the elevated values when the ICRF antenna was operating. This demonstrates the ability of the diagnostic to measure even small relative changes in the intensity of the electric field. [ABSTRACT FROM AUTHOR]

We describe a setup for time-resolved photoemission electron microscopy with aberration correction enabling 3 nm spatial resolution and sub-20 fs temporal resolution. The latter is realized by our development of a widely tunable (215–970 nm) noncollinear optical parametric amplifier (NOPA) at 1 MHz repetition rate. We discuss several exemplary applications. Efficient photoemission from plasmonic Au nanoresonators is investigated with phase-coherent pulse pairs from an actively stabilized interferometer. More complex excitation fields are created with a liquid-crystal-based pulse shaper enabling amplitude and phase shaping of NOPA pulses with spectral components from 600 to 800 nm. With this system we demonstrate spectroscopy within a single plasmonic nanoslit resonator by spectral amplitude shaping and investigate the local field dynamics with coherent two-dimensional (2D) spectroscopy at the nanometer length scale ("2D nanoscopy"). We show that the local response varies across a distance as small as 33 nm in our sample. Further, we report two-color pump–probe experiments using two independent NOPA beamlines. We extract local variations of the excited-state dynamics of a monolayered 2D material (WSe2) that we correlate with low-energy electron microscopy (LEEM) and reflectivity measurements. Finally, we demonstrate the in situ sample preparation capabilities for organic thin films and their characterization via spatially resolved electron diffraction and dark-field LEEM. [ABSTRACT FROM AUTHOR]

We present a conceptually new, slit-based slice imaging technique for ion-imaging experiments, offering a way for high slice resolution imaging in the polarization plane of an ionizing laser pulse. In the present method, a mechanically adjustable slit is installed in the drift region of the flight of the ions so that only a thin central slice of a three-dimensionally expanding ion cloud (Newton sphere) passes through the slit. The sliced cloud is then projected onto a two-dimensional position-sensitive ion detector installed parallel to the slice plane. Compared to the conventional two-dimensional imaging, the present "space-slice imaging" scheme has two principle novelties: (1) The slit acts as an ideal gate for the slicing, and a slice resolution of 1% or higher can be achieved, in principle, using submillimeter slit width for a typical a few-centimeter ion cloud. (2) The imaging plane can be automatically parallel to the polarization plane of a laser pulse regardless of the state of polarization, resulting in a hitherto unrealized "camera angle." We developed a space-slice ion imaging apparatus to realize and validate the present scheme. To evaluate its performance, we carried out the Coulomb explosion imaging of the N2 molecule. By adjusting slit width, slicing up to approximately 0.33% was achieved without remarkable image distortion. The polarization-dependent imaging shows that the ejection angles of ions can be directly read from the observed images obtained with any polarization states. The present imaging measurements in the laser polarization plane opens new avenues for the study of laser-induced dynamics; these dynamics cannot be fully characterized with the existing two-dimensional setups. As an example, we applied the present approach to the time-resolved imaging of a laser-driven rotational wave packet of N2, using a circularly polarized exploding pulse as an isotropic probe in the imaging plane. We successfully observed clear time-dependent images containing full spatiotemporal information of the wave packet dynamics. Details of the concept, design, and operation of our apparatus are presented in the present paper. [ABSTRACT FROM AUTHOR]

We report a time-resolved normal-incidence photoemission electron microscope with an imaging time-of-flight detector using ∼7-fs near-infrared laser pulses and a phase-stabilized interferometer for studying ultrafast nanoplasmonic dynamics via nonlinear photoemission from metallic nanostructures. The interferometer's stability (35 ± 6 as root-mean-square from 0.2 Hz to 40 kHz) as well as on-line characterization of the driving laser field, which is a requirement for nanoplasmonic near-field reconstruction, is discussed in detail. We observed strong field enhancement and few-femtosecond localized surface plasmon lifetimes at a monolayer of self-assembled gold nanospheres with ∼40 nm diameter and ∼2 nm interparticle distance. A wide range of plasmon resonance frequencies could be simultaneously detected in the time domain at different nanospheres, which are distinguishable already within the first optical cycle or as close as about ±1 fs around time-zero. Energy-resolved imaging (microspectroscopy) additionally revealed spectral broadening due to strong-field or space charge effects. These results provide a clear path toward visualizing optically excited nanoplasmonic near-fields at ultimate spatiotemporal resolution. [ABSTRACT FROM AUTHOR]

We present the development of a time- and angle-resolved photoemission spectroscopy based on a Yb-based femtosecond laser and a hemispherical electron analyzer. The energy of the pump photon is tunable between 1.4 and 1.9 eV, and the pulse duration is around 30 fs. We use a KBe2BO3F2 nonlinear optical crystal to generate probe pulses, of which the photon energy is up to 6.7 eV, and obtain an overall time resolution of 1 ps and energy resolution of 18 meV. In addition, β-BaB2O4 crystals are used to generate alternative probe pulses at 6.05 eV, giving an overall time resolution of 130 fs and energy resolution of 19 meV. We illustrate the performance of the system with representative data on several samples (Bi2Se3, YbCd2Sb2, and FeSe). [ABSTRACT FROM AUTHOR]

Measuring bound-state quantum dynamics, excited and driven by strong fields, is achievable by time-resolved absorption spectroscopy. Here, a vacuum beamline for spectroscopy in the attosecond temporal and extreme ultraviolet (XUV) spectral range is presented, which is a tool for observing and controlling nonequilibrium electron dynamics. In particular, we introduce a technique to record an XUV absorption signal and the corresponding reference simultaneously, which greatly improves the signal quality. The apparatus is based on a common beam path design for XUV and near-infrared (NIR) laser light in a vacuum. This ensures minimal spatiotemporal fluctuations between the strong NIR laser and the XUV excitation and reference beams, while the grazing incidence optics enable broadband spectral coverage. The apparatus combines high spectral and temporal resolution together with an increase in sensitivity to weak absorption signatures by an order of magnitude. This opens up new possibilities for studying strong-field-driven electron dynamics in bound systems on their natural attosecond time scale. [ABSTRACT FROM AUTHOR]

A new system which combines two independent diagnostic devices on the same line of sight is used to measure the X-ray spectrum in the 50-1000 eV regime. The first device is an array of six channels of time-resolved X-ray diodes (XRD's), arranged to cover the spectral band with low spectral resolution (λ/Δλ ∼ 3). The second device is a time-integrated sinusoidal transmission grating spectrometer (STGS) with a wide spectral range coverage and moderate spectral resolution (λ/Δλ ∼ 30). The spectral band of each XRD can be tuned by selecting a cathode, an x-ray mirror, and a filter. The novel sinusoidal shape of the STGS allows acquisition of a pure first-order spectrum without contribution of high dispersion orders, resulting in a higher accuracy spectrum measurement. The system described here has recently been used [Y. Ehrlich et al., Rev. Sci. Instrum. 88, 043507 (2017)] to demonstrate an improved unfolding algorithm of an XRD-acquired spectrum, achieved by experimental information gathered from the STGS measurement. [ABSTRACT FROM AUTHOR]

Optical Kerr gating technique has been employed to investigate the life history of relativistic electrons in solids by temporally gating their Cherenkov emission. Mega-ampere currents of relativistic electrons are created during ultra-intense (2 × 1019 W/cm2) laser-solid interactions. In order to measure the lifetime of these relativistic electrons in solids, we temporally gate their Cherenkov emission using an optical Kerr gate (OKG). The OKG is induced in a nonlinear medium, namely, carbon-di-sulphide (CS2), with a measured gate-width (FWHM) of 2 ps. The gate femtosecond laser pulse is synchronized with the intense interaction pulse generating relativistic electrons. The arrival time of the gate laser pulse on the CS2 cell is varied with the help of a delay stage. We find that Cherenkov emission from relativistic electrons created with a ultra-short laser pulse (25 fs) lives as long as 120 ps, a few thousand times that of the incident light pulse. [ABSTRACT FROM AUTHOR]

Pulses of I o i (10 SP 11 sp ) neutrons may be feasible for single-shot thermometry on other loading platforms, with significant challenges in loading over an adequate area and in protecting the laser source and the detector. Compared with LANSCE experiments using spallation neutrons, laser-accelerated neutrons with a lower initial mean energy do mean that the moderator can be slightly smaller for the same luminosity per neutron. Several further orders of magnitude increase in neutron production are needed before short-pulse laser facilities could usefully perform single-shot NRS thermometry on laser-loaded samples. [Extracted from the article]

This report highlights the combination of the FluoTime 300 photoluminescence spectrometer with a FluoMic add-on as a powerful tool for photophysical research and applications, yielding spectral, temporal, and spatial information on a wide range of samples. The steady-state and time-resolved measurement capabilities of this combination are demonstrated reflecting a broad range of applications. [ABSTRACT FROM AUTHOR]

This paper deals with the development and construction of an apparatus for time-resolved tunable diode laser absorption spectroscopy (LAS) for the diagnostics of pulsed plasma. A detailed description of the extension of a progressive method of laser absorption spectroscopy in continuous regime to a direct triggering method of the time-resolved laser absorption spectroscopy (TR-LAS) is presented. The main advantage of the developed method is its capability to measure the time evolution of the whole absorption profile with a preset time resolution, which can be less than 1 μs. Therefore, the presented method of repetitive sampling applied onLASin plasma processes is capable of simultaneous measurement of the density and kinetic temperature of selected particles. Its appropriate applications are to periodical processes in technological plasma, namely pulsed plasma discharges. The developed method of TR-LAS was applied to measurements of the temporal evolution of density and kinetic temperature of argon metastable species during high-power impulse magnetron sputtering of titanium and titanium dioxide thin films. [ABSTRACT FROM AUTHOR]

To perform the femtosecond pump-probe spectroscopy under high pressure and low temperature, we constructed a measurement system with a piston cylinder type pressure cell installing an optical fiber bundle. The applied pressure was achieved to 6 kbar and the cell was cooled down to 15 K. Several demonstrations revealed that broadening and change of polarization of pulse (duration of ~120 fs) owing to the dispersions in the fiber bundle are much small indicating that those have little influence on the measurement of carrier relaxation dynamics. In the measurements of κ-(BEDT-TTF)2Cu(NCS)2 under 1.3 kbar at 43 K, we have successfully detected the polarization anisotropy of the carrier relaxation dynamics and estimated the decay time in the same way as the normal measurement. [ABSTRACT FROM AUTHOR]