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At least 307 records · Page 17

All-optical single-shot complete electric field measurement of extreme ultraviolet free electron laser pulses

Recent advances in ultrafast extreme ultraviolet (EUV) and x-ray light sources provide direct access to fundamental time and length scales for biology, chemistry, and materials physics. However, such light pulses are challenging to measure due to the need for femtosecond time resolution at difficult-to-detect wavelengths. Also, single-shot measurements are needed because severe pulse-to-pulse fluctuations are common. Here we demonstrate single-shot, complete field measurements by applying a novel version of frequency resolved optical gating. An EUV free electron laser beam creates a transient grating containing the pulse’s electric field information, which is read out with a 400 nm probe pulse. By varying the time delay between two copies of the EUV pump, rather than between the pump and the probe, we separate the needed coherent wave mixing from the slow incoherent response. Because this approach uses photoionization, it should be applicable from the vacuum ultraviolet to hard x rays.

36 MATERIALS SCIENCE↗

An Online Dynamic Amplitude-Correcting Gradient Estimation Technique to Align X-ray Focusing Optics

High-brightness X-ray pulses, as generated at synchrotrons and X-ray free electron lasers (XFELs), are used in a variety of scientific experiments. At these facilities, measurements often require optical equipment, e.g Compound Refractive Lenses (CRLs) to be precisely aligned and focused. The lateral alignment of CRLs to a beamline requires precise positioning along four axes: two translational, and the two rotational. At a synchrotron, alignment is often accomplished manually. However, XFEL beamlines present a beam brightness that fluctuates stochastically, making manual alignment a time-consuming endeavor. Automation using simplex or classic stochastic descent often fails, given the errant gradient estimates. Herein we present a dynamic-amplitude correction to the usual gradient based on the combination of a generalized finite difference stencil and a time-dependent sampling pattern. Intensity is recorded periodically, then used to normalize numerical derivatives against fluctuations. Error expectation is analyzed, and efficacy is demonstrated on classic benchmarks. We provide a proof of concept by laterally aligning optics on a simulated XFEL beamline using data recorded at both synchrotron and XFEL facilities.

97 MATHEMATICS AND COMPUTING↗

Generation of multiple attosecond sub-bursts in femtosecond pulse trains by long-wavelength driving lasers

High-order harmonics generated by a long intense femtosecond laser are known experimentally to create attosecond pulse trains (APTs). In the time domain, an APT consists of a sequence of sharp attosecond bursts that are equally separated by each half optical cycle. Here, in this work, we show that such well-known features can be modified when a longer wavelength driving laser is used. From our simulations, we show that multiple shorter attosecond sub-bursts exist in the femtosecond pulse train within each half optical cycle and the duration of each sub-burst scales approximately as $λ^{–2}_0$ with the driving laser wavelength λ 0 . We show that such sub-bursts can be found using quantitative rescattering model for harmonics generated from a single atom, and their origin is due to the interference of the quantum orbits from first two returns of the recombining electron. We further show that such sub-bursts can be phase matched under proper laser focusing condition and the position of the gas cell, thus, such new features should be observable experimentally.

47 OTHER INSTRUMENTATION↗

Optical phase conjugation in backward Raman amplification

Compression of an intense laser pulse using backward Raman amplification (BRA) in plasma, followed by vacuum focusing to a small spot size, can produce unprecedented ultrarelativistic laser intensities. The plasma density inhomogeneity during BRA, however, causes laser phase and amplitude distortions, limiting the pulse focusability. To solve the issue of distortion, we investigate the use of optical phase conjugation as the seed pulse for BRA. We show that the phase conjugated laser pulses can retain focusability in the nonlinear pump depletion regime of BRA, but not so easily in the linear amplification regime. This somewhat counterintuitive result is because the nonlinear pump depletion regime features a shorter amplification distance, and hence less phase distortion due to wave–wave interaction, than the linear amplification regime.

Jia, Qing↗

Roadmap on spatiotemporal light fields

Spatiotemporal sculpturing of light pulse with ultimately sophisticated structures represents a major goal of the everlasting pursue of ultra-fast information transmission and processing as well as ultra-intense energy concentration and extraction. It also holds the key to unlock new extraordinary fundamental physical effects. Traditionally, spatiotemporal light pulses are always treated as spatiotemporally separable wave packet as solution of the Maxwell’s equations. In the past decade, however, more generalized forms of spatiotemporally nonseparable solution started to emerge with growing importance for their striking physical effects. This roadmap intends to highlight the recent advances in the creation and control of increasingly complex spatiotemporally sculptured pulses, from spatiotemporally separable to complex nonseparable states, with diverse geometric and topological structures, presenting a bird’s eye viewpoint on the zoology of spatiotemporal light fields and the outlook of future trends and open challenges.

42 ENGINEERING↗

Nanoscale polarization transient gratings

Light manipulation at the nanoscale is essential both for fundamental science and modern technology. The quest to shorter lengthscales, however, requires the use of light wavelengths beyond the visible. In particular, in the extreme ultraviolet regime these manipulation capabilities are hampered by the lack of efficient optics, especially for polarization control. Here, we present a method to create periodic, polarization modulations at the nanoscale using a tailored configuration of the FERMI free electron laser and demonstrate its capabilities by comparing the dynamics induced by this polarization transient grating with those driven by a conventional intensity grating on a thin ferrimagnetic alloy. While the intensity grating signal is dominated by the thermoelastic response, the polarization grating excitation minimizes it, uncovering helicity-dependent responses previously undetected. We anticipate nanoscale polarization transient gratings to become useful for the study of physical, chemical and biological systems possessing chiral symmetry.

36 MATERIALS SCIENCE↗

Electron Spin Polarization in Large Electric Fields

This project investigated the effects of large electric fields on electron spin polarization in semiconductors, which is of interest for spin-based electronics (“spintronics”) and quantum information processing. It has been theoretically proposed that large electric fields could potentially preserve or amplify electron spin polarization, which would make it easier to generate, transport, and detect spin polarization in spin-based devices; however, previous measurements had not measured the response of electron spin polarization at large electric fields. During this project, methods to perform measurements of electron spin polarization at large electric fields were developed and performed using ultrafast time- and spatially-resolved magneto-optical spectroscopy, high-voltage pulses, and lock-in detection. The device geometry was engineered to reduce the threshold voltage required to reach the Gunn threshold, and the effect of optical illumination on the sample conductivity and Gunn oscillations was investigated. Electron spin polarization measurements were performed at electric fields up to and beyond the Gunn threshold for the device. The measurements showed that the electron spin polarization magnitude decreased with increasing electric field in the devices measured, and a spin amplification effect was not observed. However, these effects could potentially exist in a different material or in a material with a different doping concentration or in a different device geometry.

36 MATERIALS SCIENCE↗

Intrinsic optical bistability of photon avalanching nanocrystals

Optically bistable materials respond to a single input with two possible optical outputs, contingent on excitation history. Such materials would be ideal for optical switching and memory, but the limited understanding of intrinsic optical bistability (IOB) prevents the development of nanoscale IOB materials suitable for devices. Here we demonstrate IOB in Nd 3+ -doped KPb 2 Cl 5 avalanching nanoparticles, which switch with high contrast between luminescent and non-luminescent states, with hysteresis characteristic of bistability. Here we elucidate a non-thermal mechanism in which IOB originates from suppressed non-radiative relaxation in Nd 3+ ions and from the positive feedback of photon avalanching, resulting in extreme, >200th-order optical nonlinearities. The modulation of laser pulsing tunes the hysteresis widths, and dual-laser excitation enables transistor-like optical switching. This control over nanoscale IOB establishes avalanching nanoparticles for photonic devices in which light is used to manipulate light.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Atomic Force Microscope Active Optical Probe for Single-Molecule Imaging and Time-Resolved Optical Spectroscopy (DOE SBIR Phase II/IIA Final Report)

Actoprobe LLC reports on the results of its DOE SBIR Phase II/IIA project on the development of Atomic Force Microscope Active Optical Probe for Single-Molecule Imaging and Time-Resolved Optical Spectroscopy. While chemistry science and technology greatly benefit from Atomic Force Microscopy in surface characterization, time-resolved chemical imaging on the single-molecule level lags far behind. Current scanning probe microscopy only obtains information about mechanical but not optical/chemical properties. To address this problem, the Actoprobe LLC research team has proposed a novel class of Atomic Force Microscopy probes, Ultra-Fast Pulsed Active Atomic Force Microscopy Optical Probes (UFP AAOPs), that will allow ultrafast time-resolved optical and chemical imaging at the nanoscale. As envisioned, these unique optical probes will perform the functions of conventional Atomic Force Microscopy probes and, in addition, will simultaneously provide chemical information about molecular scale interactions. This innovation is accomplished by integrating an ultrafast pulsed Quantum Dot laser source into an Atomic Force Microscopy probe. This report describes our progress with the fabrication of an ultrafast micrometer-size semiconductor laser, based on “artificial atoms” - Quantum Dots, integrated with an Atomic Force Microscopy probe. In this Phase II/IIA project, we have demonstrated the feasibility of the UFP AAOP concept by fabricating a first prototype of the UFP AAOP. The excellent performance of the probe has been proven in terms of AFM and optical spatial resolution through rigorous tests. The UFP AAOP provides pulses with less than 4 ps duration and higher than 11 GHz repetition rate, and spatial resolution better than 300 nm at 1240 nm wavelength. Technically, it is possible to reduce the pulse width to less than 1 ps and to improve lateral resolution to ~ 0.5 nm, which implies the potential capability for the probe to characterize chemical compounds with single-molecule resolution. The UFP AAOP fabrication procedure has been developed for wafer-scale production of multiple devices, with the yield of the process estimated to be lower than 1% with the limited fabrication capabilities and equipment available for use in the research project. However, using high-volume production tools and special GaAs processing equipment, the yield can be significantly improved, theoretically to ~ 50%. Finally, economic feasibility and scale-up manufacturing potential were analyzed for UFP AAOP and found to be very promising. In summary, the Actoprobe team has successfully demonstrated the feasibility of the UFP AAOP concept.

36 MATERIALS SCIENCE↗

Effect of Auger recombination on transient optical properties in XUV and soft X-ray irradiated silicon nitride

Spatially encoded measurements of transient optical transmissivity became a standard tool for temporal diagnostics of free-electron-laser (FEL) pulses, as well as for the arrival time measurements in X-ray pump and optical probe experiments. The modern experimental techniques can measure changes in optical coefficients with a temporal resolution better than 10 fs. This, in an ideal case, would imply a similar resolution for the temporal pulse properties and the arrival time jitter between the FEL and optical laser pulses. However, carrier transport within the material and out of its surface, as well as carrier recombination may, in addition, significantly decrease the number of carriers. This would strongly affect the transient optical properties, making the diagnostic measurement inaccurate. Below we analyze in detail the effects of those processes on the optical properties of XUV and soft X-ray irradiated Si 3 N 4 , on sub-picosecond timescales. Si 3 N 4 is a wide-gap insulating material widely used for FEL pulse diagnostics. Theoretical predictions are compared with the published results of two experiments at FERMI and LCLS facilities, and with our own recent measurement. The comparison indicates that three body Auger recombination strongly affects the optical response of Si 3 N 4 after its collisional ionization stops. By deconvolving the contribution of Auger recombination, in future applications one could regain a high temporal resolution for the reconstruction of the FEL pulse properties measured with a Si 3 N 4 -based diagnostics tool.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Hard x-ray – optical four-wave mixing using a split-and-delay line

New, hard x-ray free electron lasers (FEL) produce intense femtosecond-to-attosecond pulses at angstrom wavelengths, giving access to the fundamental spatial and temporal scales of matter. These revolutionary light sources open the door to applying the suite of nonlinear, optical spectroscopy methods at hard x-ray photon energies. Nonlinear spectroscopy with hard x-rays can allow for measuring the coherence properties of short wavelength excitations with atomic specificity and for understanding how high energy excitations couple to other degrees of freedom in atomic, molecular or condensed-phase systems. As a step in this direction, here we present hard x-ray, optical four-wave mixing (4WM) measurements done at 9.8 keV at the split-and-delay line at the x-ray correlation spectroscopy (XCS) hutch of the Linac Coherent Light Source (LCLS). In this work, we create an x-ray transient grating (TG) from a pair of crossing x-ray beams and diffract optical laser pulses at 400 nm from the TG. The key technical advance here is being able to independently vary the delays of the x-ray pulses. Measurements were made in 3 different solid samples: bismuth germinate (BGO), zinc oxide (ZnO) and yttrium aluminum garnet (YAG). The resulting phase-matched, 4WM signal is measured in two different ways: by varying the x-ray, x-ray pulse delay which can reveal both material and light source coherence properties and also by varying the optical laser delay with respect to the x-ray TG to study how the x-ray excitation couples to the optical properties. Although no coherent 4WM signal was seen in these measurements, the absence of this signal gives important information on experimental requirements for detecting this in future work. Also, our laser-delay scans, although not a new measurement, were applied to different materials than in past work and reveal new examples x-ray induced lattice dynamics in solids. This work represents a key step towards extending nonlinear optics and time-resolved spectroscopy into the hard x-ray regime.

47 OTHER INSTRUMENTATION↗

High-repetition rate, CEP-stable shortwave infrared source with two-cycle pulses for field-resolved spectroscopy

We report on a passively carrier-envelope phase (CEP)-stable optical parametric amplifier generating two-cycle pulses at 2060 nm with energies of up to 2.25 µJ operating at a repetition rate of 400 kHz, specifically designed for applications in field-resolved spectroscopy. The measured pulse duration is 13.6 fs, resulting in two cycles of the carrier wave. Due to the robust CEP-stable front-end design, we achieve an open-loop CEP stability of 250 mrad (rms) and the capability for fast CEP modulation.

47 OTHER INSTRUMENTATION↗

Bayesian tomography of high-dimensional on-chip biphoton frequency combs with randomized measurements

Abstract Owing in large part to the advent of integrated biphoton frequency combs, recent years have witnessed increased attention to quantum information processing in the frequency domain for its inherent high dimensionality and entanglement compatible with fiber-optic networks. Quantum state tomography of such states, however, has required complex and precise engineering of active frequency mixing operations, which are difficult to scale. To address these limitations, we propose a solution that employs a pulse shaper and electro-optic phase modulator to perform random operations instead of mixing in a prescribed manner. We successfully verify the entanglement and reconstruct the full density matrix of biphoton frequency combs generated from an on-chip Si 3 N 4 microring resonator in up to an 8 × 8-dimensional two-qudit Hilbert space, the highest dimension to date for frequency bins. More generally, our employed Bayesian statistical model can be tailored to a variety of quantum systems with restricted measurement capabilities, forming an opportunistic tomographic framework that utilizes all available data in an optimal way.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

High repetition-rate pulse shaping of a spectrally broadened Yb femtosecond laser

We demonstrate compression and shaping of few cycle pulses from a high average power ytterbium laser system. The pulses from a commercial 20 W, 100 kHz Yb laser system are spectrally broadened in two-stages using cascaded, gas-filled, stretched hollow-core fibers and then compressed and shaped in an acousto-optic modulator-based pulse-shaper. The pulse-shaper allows for compression, characterization, and shaping all in one system, producing ∼10 fs pulses with 30 μ J of energy.

Codere, Julia↗

Mirrors for petawatt lasers: Design principles, limitations, and solutions

High intensity and high energy laser facilities place increasing demands on optical components, requiring large surface area optics with exacting specifications. Petawatt lasers are high energy, short-pulse laser systems generally based on chirped-pulse amplification, where an initial low energy short pulse is stretched, amplified, and then recompressed to produce fs to ps high-power laser pulses. In such petawatt lasers, the highest demands are placed on the final optics, including gratings which compress the pulses and mirrors which direct and focus the final high-power beams. The limiting factor in these optical components is generally laser-induced damage. Designing and fabricating these optical components to meet reflection, dispersion, and other requirements while meeting laser-induced damage requirements is the primary challenge discussed in this tutorial. We will introduce the reader to the technical challenges and tradeoffs required to produce mirrors for petawatt lasers and discuss current research directions.

47 OTHER INSTRUMENTATION↗

Real-time jitter correction in a photonic analog-to-digital converter

A real-time jitter meter is used to measure and digitally sample the pulse-to-pulse timing error in a laser pulse train. The jitter meter is self-referenced using a single-pulse delay line interferometer and measures timing jitter using optical heterodyne detection between two frequency channels of the pulse train. Jitter sensitivity down to 3×10 -10 fs 2 /Hz at 500 MHz has been demonstrated with a pulse-to-pulse noise floor of 1.6 fs. Furthermore, as a proof of principle, the digital correction of the output of a high-frequency photonic analog-to-digital converter (PADC) is demonstrated with an emulated jitter signal. Up to 23 dB of jitter correction, down to the noise floor of the PADC, is accomplished with radio-frequency modulation up to 40 GHz.

47 OTHER INSTRUMENTATION↗