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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Student Support for the “Frontiers in Attosecond & Ultrafast X-ray Science” School

The new millennium witnessed two revolutionary breakthroughs in ultrafast x-ray science: table-top XUV sources based on high harmonic generation in gases ushered in the attosecond era while facility-based x-ray free-electron lasers opened the path for intense, femtosecond hard x-rays. This award requested scholarship funds for a 2019 and 2023 School whose prime objective was the training of young scientists in these emerging complementary areas both relevant to DOE BES mission. The school entitled the “Frontiers of Attosecond and Ultrafast X-ray Science (FAXS)” (http://www.erice-attosecond.it/) was the second and fourth in a series, which began in 2017. The two Schools were held during March 10-16, 2019 and March 26-31, 2023 at the Ettore Majorana Foundation and Centre for Scientific Culture (http://www.ccsem.infn.it/) in Erice, Sicily. The DOE funds supported the registration fee for young scientists (graduate students and postdocs) from US institutions. The registration fees included School participation, lodging and meals over the duration of the School. Note, the third addition of the School was held in 2022 as a virtual event due to the pandemic, DOE funds were not necessary for this event. The FAXS School is a course of the 62th and 63rd International School of Quantum Electronics under the directorship of Prof. Diederik Wiersma (University of Florence). The Directors for the FAXS School are Louis DiMauro (The Ohio State University, USA) and Mauro Nisoli (Politecnico di Milano, Italy). The FAXS School program consisted of approximately 10 lectures by leading experts in attosecond and x-ray science (see attached list). Most lecturers delivered a series of three 1-hour lectures. The lecturers were required to spend the full 5 days at the school so to promote interaction with the students. The Erice Majorana Center venue accommodated ~75 young scientists. The registration fee covered the cost of participating in the school, lodging and meals for the entire duration of the school. The schedule consisted of lectures every morning and afternoon except for one afternoon that was reserved for an archaeological excursion. Every evening had a student/postdoc poster session and social gatherings at the Majorana Center to encourage further interaction of all participants and lecturers. The two FAXS Schools attracted an international group of young scientists. The DOE funds supported the registration fee for 11 students/postdocs from US institutions (5 supported in 2019 and 6 supported in 2023). The management of the DOE fellowships were administered through the Research Foundation of The Ohio State University. FAXS scholarships for European students/postdocs were provided by European funding sources administered by co-Director, Prof. Nisoli. All students/postdocs were encouraged to present a poster. Travel expenses to the FAXS School were the responsibility of the student/postdoc home institution.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2014

Electron pair emission detected by time-of-flight spectrometers: Recent progress

We present results for electron coincidence spectroscopy using two time-of-flight (ToF) spectrometers. Excited by electron impact, the energy and momentum distribution of electron pairs emitted from the Cu(111) surface are resolved and a spectral feature related to the Shockley surface state is identified. By combining the two ToF spectrometers with a high-order harmonic generation light source, we demonstrate double photoemission spectroscopy in the laboratory that required synchrotron radiation in the past. Utilizing this setup, we report results for (γ,2e) on NiO(001) on Ag(001) excited with light at 30 eV photon energy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Toward ultrafast soft x-ray spectroscopy of organic photovoltaic devices

Novel ultrafast x-ray sources based on high harmonic generation and at x-ray free electron lasers are opening up new opportunities to resolve complex ultrafast processes in condensed phase systems with exceptional temporal resolution and atomic site specificity. In this perspective, we present techniques for resolving charge localization, transfer, and separation processes in organic semiconductors and organic photovoltaic devices with time-resolved soft x-ray spectroscopy. We review recent results in ultrafast soft x-ray spectroscopy of these systems and discuss routes to overcome the technical challenges in performing time-resolved x-ray experiments on photosensitive materials with poor thermal conductivity and low pump intensity thresholds for nonlinear effects.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2026

Redirection and reshaping of intense extreme-ultraviolet radiation

The goal to control short-wavelength radiation for the investigation and manipulation of ultrafast dynamics in quantum systems coevolves with the growing availability of extreme-ultraviolet (XUV) and x-ray sources from high-harmonic generation and free-electron lasers. Here, we present an XUV spatio-spectral phase modulator based on an intense XUV laser beam propagating through an optically thick resonant target, introducing dispersion profile variations around the resonance both perpendicular to and along the laser propagation direction. The resulting dipole radiation gets spectrally reshaped and becomes more divergent as compared to the original beam in the far field. As an experimental demonstration, the intense-XUV–induced double-peak off-axis structure in the far-field spectrum obtained at the Free-Electron Laser in Hamburg (FLASH) shows indications of the underlying XUV-driven Rabi dynamics and resonant pulse propagation effects. The presented work highlights a ubiquitous phenomenon occurring when an intense laser beam passes through a resonant medium.

He, Yu [Max-Planck-Institut für Kernphysik, Heidel↗
DOE OSTI2021

Removal of correlated background in a high-order harmonic transient absorption spectra with principal component regression

We demonstrate a 40x mean noise power reduction (NPR) in core-to-valence extreme ultraviolet (XUV) femtosecond transient absorption spectroscopy with a high harmonic generation (HHG) light source. An adaptive iteratively reweighted principal component regression (airPCR) is used to analyze and suppress spectrally correlated HHG intensity fluctuations. The technique requires significantly less user input and leads to a higher mean NPR than a previously introduced edge-pixel PCR method that relies on the manual identification of signal-free spectral regions. Both techniques are applied in a time-resolved XUV absorption study of the 2 snp 1 P o ( n ≥ 2) autoionizing Rydberg states of helium, demonstrating sub-10 −3 optical density sensitivity.

Faccialà, Davide (ORCID:0000000250720394)↗
NASA NTRS1985

Efficient frequency conversion of laser sources in nonlinear crystals

The use of nonlinear crystals to extend the frequency range of solid-state laser sources is proposed. The harmonic generation of high-average-power laser sources and CW-laser-sources nonlinear crystals is considered. The development of Nd:YAG pumped parametric oscillators and optical parametric amplifiers using LiNbO3 or AgGaS2 is studied. The LiNbO3 oscillator has tunable output over the 1.4-4.0 micron range and is applicable for remote sensing measurements of molecules and of humidity and temperature; AgGaS2 oscillators provide the potential for 3-15 micron infrared generation. Advances in material synthesis techniques related to the design and synthesis of nonlinear media are discussed. Various procedures for the synthesis of nonlinear crystals are described.

Byer, R. L.↗
DOE OSTI2024

Wavelength scaling and multicolor operation of a plasma-driven attosecond x-ray source via harmonic generation

The generation of high-power coherent soft x-ray pulses of sub-100 as duration and 10 nm wavelength using beams from a GeV energy plasma wakefield accelerator has been recently investigated in Emma []. As a future upgrade to this concept, this contribution investigates scaling to shorter x-ray wavelengths by cascading undulators tuned to higher harmonics of the fundamental. We present two simulation studies for plasma-driven attosecond harmonic generation schemes with final photon wavelengths of 2 and 0.40 nm. We demonstrate in these schemes that using undulators with retuned fundamental frequencies can produce GW-scale pulses of sub-nm radiation with tens of attosecond-scale pulse lengths, an order of magnitude shorter than current state-of-the-art attosecond x-ray free electron lasers (XFELs). This multipulse multicolor operation will be broadly applicable to attosecond pump-probe experiments. Published by the American Physical Society 2024

43 PARTICLE ACCELERATORS↗
DOE OSTI2015

HELIOS—A laboratory based on high-order harmonic generation of extreme ultraviolet photons for time-resolved spectroscopy

In this paper, we present the HELIOS (High Energy Laser Induced Overtone Source) laboratory, an in-house high-order harmonic generation facility which generates extreme ultraviolet (XUV) photon pulses in the range of 15-70 eV with monochromatized XUV pulse lengths below 35 fs. HELIOS is a source for time-resolved pump-probe/two-color spectroscopy in the sub-50 fs range, which can be operated at 5 kHz or 10 kHz. An optical parametric amplifier is available for pump-probe experiments with wavelengths ranging from 240 nm to 20 000 nm. The produced XUV radiation is monochromatized by a grating in the so-called off-plane mount. Together with overall design parameters, first monochromatized spectra are shown with an intensity of 2 ⋅ 10{sup 10} photons/s (at 5 kHz) in the 29th harmonic, after the monochromator. The XUV pulse duration is measured to be <25 fs after monochromatization.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Detection of the keto-enol tautomerization in acetaldehyde, acetone, cyclohexanone, and methyl vinyl ketone with a novel VUV light source

The discovery of enols in combustion environments and our atmosphere has garnered increasing attention to the many unanswered questions surrounding enol chemistry. The scarcity of experimental data concerning these enols renders combustion and atmospheric models with a lack of constraining parameters, leading to varying computational predictions. Experimental detection is difficult because mass spectrometry, a powerful tool for probing a wide variety of species, cannot distinguish between enols and their thermodynamically favorable ketone isomers. A solution to this ambiguity is to use tunable vacuum ultraviolet (VUV) light from a synchrotron to identify the presence of the enol by its lower ionization energy compared to the isomer. We present a tabletop-scale VUV light source that implements highly cascaded harmonic generation, a new regime of cascaded nonlinear optics, to provide a set of spectral lines spaced by 1.2 eV. We demonstrate that the variety of photon energies available allows us to detect the keto-enol tautomerization of four aldehydes and ketones. By combining this novel VUV light source with an established microreactor, we first revisit the formation of vinyl alcohol from acetaldehyde and confirm that the observed isomerization is indeed unimolecular. Secondly, we observe the thermal tautomerization of acetone to propen-2-ol for the first time. Finally, we observe the thermal tautomerization of cyclohexanone to 1-cyclohexenol and methyl vinyl ketone to 2-hydroxybutadiene, where the results are in good agreement with those reported at a synchrotron. Furthermore, our measurements can be used to constrain models, inform future experimental studies of enol reactivity, and potentially enhance current understanding of combustion and environmental chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Attosecond light science and its application for probing quantum materials

In this paper, we review the development and application of coherent short wavelength light sources implemented using the high harmonic generation (HHG) process. The physics underlying HHG brought quantum physics into the domain of attosecond time-scales for the first time. Here, the observation and manipulation of electron dynamics on such short time-scales—a capability not conceived—of just a few decades ago—is becoming both more-and-more sophisticated and useful as a route to achieve exquisite control over short wavelength light. New experimental techniques are enabling HHG light sources to provide new insights into fundamental quantum interactions in materials, making it possible for the first time to capture the fastest charge, spin, photon and phonon interactions and to achieve diffraction-limited imaging at short wavelengths.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

A simple electron time-of-flight spectrometer for ultrafast vacuum ultraviolet photoelectron spectroscopy of liquid solutions

We present a simple electron time of flight spectrometer for time resolved photoelectron spectroscopy of liquid samples using a vacuum ultraviolet (VUV) source produced by high-harmonic generation. The field free spectrometer coupled with the time-preserving monochromator for the VUV at the Artemis facility of the Rutherford Appleton Laboratory achieves an energy resolution of 0.65 eV at 40 eV with a sub 100 fs temporal resolution. A key feature of the design is a differentially pumped drift tube allowing a microliquid jet to be aligned and started at ambient atmosphere while preserving a pressure of 10⁻¹ mbar at the micro channel plate detector. The pumping requirements for photoelectron (PE) spectroscopy in vacuum are presented, while the instrument performance is demonstrated with PE spectra of salt solutions in water. The capability of the instrument for time resolved measurements is demonstrated by observing the ultrafast (50 fs) vibrational excitation of water leading to temporary proton transfer.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Table-top extreme ultraviolet second harmonic generation

The lack of available table-top extreme ultraviolet (XUV) sources with high enough fluxes and coherence properties has limited the availability of nonlinear XUV and x-ray spectroscopies to free-electron lasers (FELs). Here, we demonstrate second harmonic generation (SHG) on a table-top XUV source by observing SHG near the Ti M 2,3 edge with a high-harmonic seeded soft x-ray laser. Furthermore, this experiment represents the first SHG experiment in the XUV. First-principles electronic structure calculations suggest the surface specificity and separate the observed signal into its resonant and nonresonant contributions. The realization of XUV-SHG on a table-top source opens up more accessible opportunities for the study of element-specific dynamics in multicomponent systems where surface, interfacial, and bulk-phase asymmetries play a driving role.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Bright, single helicity, high harmonics driven by mid-infrared bicircular laser fields

High-harmonic generation (HHG) is a unique tabletop light source with femtosecond-to-attosecond pulse duration and tailorable polarization and beam shape. Here, we use counter-rotating femtosecond laser pulses of 0.8 µm and 2.0 μm to extend the photon energy range of circularly polarized high-harmonics and also generate single-helicity HHG spectra. By driving HHG in helium, we produce circularly polarized soft x-ray harmonics beyond 170 eV—the highest photon energy of circularly polarized HHG achieved to date. In an Ar medium, dense spectra at photon energies well beyond the Cooper minimum are generated, with regions composed of a single helicity—consistent with the generation of a train of circularly polarized attosecond pulses. Finally, we show theoretically that circularly polarized HHG photon energies can extend beyond the carbon K edge, extending the range of molecular and materials systems that can be accessed using dynamic HHG chiral spectro-microscopies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Bright high-repetition-rate source of narrowband extreme-ultraviolet harmonics beyond 22 eV

Novel table-top sources of extreme-ultraviolet light based on high-harmonic generation yield unique insight into the fundamental properties of molecules, nanomaterials or correlated solids, and enable advanced applications in imaging or metrology. Extending high-harmonic generation to high repetition rates portends great experimental benefits, yet efficient extreme-ultraviolet conversion of correspondingly weak driving pulses is challenging. In this article, we demonstrate a highly-efficient source of femtosecond extreme-ultraviolet pulses at 50-kHz repetition rate, utilizing the ultraviolet second-harmonic focused tightly into Kr gas. In this cascaded scheme, a photon flux beyond ≈3 × 10 13 s -1 is generated at 22.3 eV, with 5 × 10 -5 conversion efficiency that surpasses similar harmonics directly driven by the fundamental by two orders-of-magnitude. The enhancement arises from both wavelength scaling of the atomic dipole and improved spatio-temporal phase matching, confirmed by simulations. Finally, spectral isolation of a single 72-meV-wide harmonic renders this bright, 50-kHz extreme-ultraviolet source a powerful tool for ultrafast photoemission, nanoscale imaging and other applications.

36 MATERIALS SCIENCE↗
DOE OSTI2015

The Physics of Gain Mechanisms in a Self-Amplified Spontaneous Emission Free-Electron Laser

This is the final report for the DoE BES contract DE-FG02-07ER46272. This grant began under a title that gives its history in a few words: The Physics of Gain Mechanisms in a Self-Amplified Spontaneous Emission Free-Electron Laser. At the time of adopting this name, the UCLA Particle Beam Physics Laboratory (PBPL) was at the forefront of the first demonstrations of SASE FEL, giving the experimental basis for the 4th generation X-ray light source now exemplified by the LCLS, a remarkable generation of machines that have revolutionize nanoscale and ultrafast science. The grant title indicates that physical aspects of the FEL are of interest, and implies that progress requires comprehensive investigations. These aspects include: the physics and technology of high brightness electron beam generation, phase space manipulations, advanced beam diagnostics, state-of-the-art undulators, studies of FEL mode characteristics, as well as the introduction of new theoretical models and start-to-end simulations, all yielding a deep understanding of the SASE FEL. The latest period (2010-13) of BES grant support has been the most productive yet for the UCLA PBPL, and the extensive list of accomplishments is illustrative of our central contributions to advanced FEL research. We give a concise overview here and review our research results in further detail below. In FEL and ultrafast beam physics, we have experimentally investigated: production of helical beams and FEL modes with orbital angular momentum; chirp-taper single-spike FEL gain; new FROG techniques optimized for FEL, introduced coherent imaging of beam profiles using transition radiation; and demonstrated a next generation cryoundulator. We have performed deep theoretical studies of these phenomena and other advanced FEL physics concepts, such as the space-charge amplifier. In high brightness beams, we have: introduced a new class of hybrid photoinjector for <100 fs beam production; developed new approaches to self-shaped ellipsoidal beams; used nonlinear plasma oscillations to create beam pulse trains; tested new plasmonic, high quantum efficiency cathodes, and developed new methods of beam measurement with um spatial/sub-fs temporal resolution. In ultrafast imaging, we have: developed advanced electro-optic timing systems, performed the 1st pump-probe study using single shot UED, demonstrated continuously time-resolved UED with RF deflection; made initial use of inverse Compton scattering (ICS) X-ray sources in application through single-shot inline phase contrast imaging, established single-shot X-ray diffraction, and observed ICS high harmonic generation and redshifting due to nonlinear effects. In 5th generation light source research, we have developed the techniques of narrowband, very high power coherent Cerenkov radiation sources based on dielectric wakefield devices. This work is represented by numerous publications in leading journals: e.g. Nature Physics, Physical Review Letters, Applied Physics Letters. The PBPL program’s influence on the field also extends to organization of the electron beam applications community; we have organized the first international UED workshops and the initial two meetings dedicated to 5th generation light source.

43 PARTICLE ACCELERATORS↗
DOE OSTI2014

High resolution coherent diffractive imaging with a table-top extreme ultraviolet source

We demonstrate a resolution of 45 nm with a sample size down to 3 μm × 3 μm is achieved in a short exposure time of 2 s, from the diffraction pattern generated by a table-top high harmonic source at around 30 nm. By using a narrow-bandwidth focusing mirror, the diffraction pattern's quality is improved and the required exposure time is significantly reduced. In order to obtain a high quality of the reconstructed image, the ratio of the beam size to the sample size and the curvature of the focused beam need to be considered in the reconstruction process. This new experimental scheme is very promising for imaging sub-10 nm scale objects with a table-top source based on a small inexpensive femtosecond laser system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Ultrafast Dynamics of Molecules on Surfaces Studied with Time-Resolved XUV Photoelectron Spectroscopy (Final Report)

In this project we set out to make technical advances in time-resolved photoemission from surfaces and study molecule-surface charge transfer processes. Combining a novel light source developed at Stony Brook with a new type of time-of-flight photoemission electron microscope (TOF k-mic) developed in Mainz, Germany, we achieved the former goal. Our light source, based on cavity-enhanced high harmonic generation at 61 MHz repetition rate, enables ultrafast time-resolved photoemission experiments to be conducted with orders of magnitude higher photocurrents than otherwise possible. Critically, this provides the high dynamic range necessary to study perturbatively excited samples, such that one can study the intrinsic dynamics of electrons and holes as they would occur in a device. Combining our light source with the TOF k-mic, we’ve achieved an overall improvement in data rate of time- and angle-resolved photoemission (tr-ARPES) of approximately four orders of magnitude over the previous state-of-the-art using kHz-repetition rate sources and conventional hemispherical electron analyzers. This new instrument is now being used in experiments on 2D materials and organic semiconductors.

74 ATOMIC AND MOLECULAR PHYSICS↗