Daniel D. Hickstein

Bright circularly polarized soft x-ray high harmonics for x-ray magnetic circular dichroism

Significance The new ability to generate circularly polarized coherent (laser-like) beams of short wavelength high harmonics in a tabletop-scale setup is attracting intense interest worldwide. Although predicted in 1995, this capability was demonstrated experimentally only in 2014. However, all work to date (both theory and experiment) studied circularly polarized harmonics only in the extreme UV (EUV) region of the spectrum at wavelengths >18 nm. In this new work done in a broad international collaboration, we demonstrate the first soft X-ray high harmonics with circular polarization to wavelengths λ < 8 nm and the first tabletop soft X-ray magnetic circular dichroism (XMCD) measurements, and also uncover new X-ray light science that will inspire many more studies of circular high-harmonic generation (HHG). We demonstrate, to our knowledge, the first bright circularly polarized high-harmonic beams in the soft X-ray region of the electromagnetic spectrum, and use them to implement X-ray magnetic circular dichroism measurements in a tabletop-scale setup. Using counterrotating circularly polarized laser fields at 1.3 and 0.79 µm, we generate circularly polarized harmonics with photon energies exceeding 160 eV. The harmonic spectra emerge as a sequence of closely spaced pairs of left and right circularly polarized peaks, with energies determined by conservation of energy and spin angular momentum. We explain the single-atom and macroscopic physics by identifying the dominant electron quantum trajectories and optimal phase-matching conditions. The first advanced phase-matched propagation simulations for circularly polarized harmonics reveal the influence of the finite phase-matching temporal window on the spectrum, as well as the unique polarization-shaped attosecond pulse train. Finally, we use, to our knowledge, the first tabletop X-ray magnetic circular dichroism measurements at the N4,5 absorption edges of Gd to validate the high degree of circularity, brightness, and stability of this light source. These results demonstrate the feasibility of manipulating the polarization, spectrum, and temporal shape of high harmonics in the soft X-ray region by manipulating the driving laser waveform.

High flux coherent super-continuum soft X-ray source driven by a single-stage, 10mJ, Ti:sapphire amplifier-pumped OPA

We demonstrate the highest flux tabletop source of coherent soft X-rays to date, driven by a single-stage 10 mJ Ti:sapphire regenerative amplifier at 1 kHz. We first down-convert the laser to 1.3 µm using a parametric amplifier, before up-converting it to soft X-rays using high harmonic generation in a high-pressure, phase matched, hollow waveguide geometry. The resulting optimally phase matched broadband spectrum extends to 200 eV, with a soft X-ray photon flux of > 10(6) photons/pulse/1% bandwidth at 1 kHz, corresponding to > 10(9) photons/s/1% bandwidth, or approximately a three order-of-magnitude increase compared with past work. Finally, using this broad bandwidth X-ray source, we demonstrate X-ray absorption spectroscopy of multiple elements and transitions in molecules in a single spectrum, with a spectral resolution of 0.25 eV, and with the ability to resolve the near edge fine structure.

Dynamics of Strong-Field Double Ionization in Two-Color Counterrotating Fields.

The double ionization of helium in bichromatic, circularly polarized intense laser fields is analyzed with a classical ensemble approach. It is found that counterrotating fields produce significant nonsequential double-ion yield and drive novel ionization dynamics. It is shown that distinct pathways to ionization can be modified by altering the relative intensities of the two colors, allowing for unique control of strong-field processes. Electrons are observed to return to the ion at different angles from the angle of ionization, opening new possibilities for probing electronic and molecular structure on the ultrafast time scale.

Observation and control of shock waves in individual nanoplasmas.

Using an apparatus that images the momentum distribution of individual, isolated 100-nm-scale plasmas, we make the first experimental observation of shock waves in nanoplasmas. We demonstrate that the introduction of a heating pulse prior to the main laser pulse increases the intensity of the shock wave, producing a strong burst of quasimonoenergetic ions with an energy spread of less than 15%. Numerical hydrodynamic calculations confirm the appearance of accelerating shock waves and provide a mechanism for the generation and control of these shock waves. This observation of distinct shock waves in dense plasmas enables the control, study, and exploitation of nanoscale shock phenomena with tabletop-scale lasers.

Solvents Effects on Charge Transfer from Quantum Dots

To predict and understand the performance of nanodevices in different environments, the influence of the solvent must be explicitly understood. In this Communication, this important but largely unexplored question is addressed through a comparison of quantum dot charge transfer processes occurring in both liquid phase and in vacuum. By comparing solution phase transient absorption spectroscopy and gas-phase photoelectron spectroscopy, we show that hexane, a common nonpolar solvent for quantum dots, has negligible influence on charge transfer dynamics. Our experimental results, supported by insights from theory, indicate that the reorganization energy of nonpolar solvents plays a minimal role in the energy landscape of charge transfer in quantum dot devices. Thus, this study demonstrates that measurements conducted in nonpolar solvents can indeed provide insight into nanodevice performance in a wide variety of environments.

Materials Properties and Solvated Electron Dynamics of Isolated Nanoparticles and Nanodroplets Probed with Ultrafast Extreme Ultraviolet Beams

We present ultrafast photoemission measurements of isolated nanoparticles in vacuum using extreme ultraviolet (EUV) light produced through high harmonic generation. Surface-selective static EUV photoemission measurements were performed on nanoparticles with a wide array of compositions, ranging from ionic crystals to nanodroplets of organic material. We find that the total photoelectron yield varies greatly with nanoparticle composition and provides insight into material properties such as the electron mean free path and effective mass. Additionally, we conduct time-resolved photoelectron yield measurements of isolated oleylamine nanodroplets, observing that EUV photons can create solvated electrons in liquid nanodroplets. Using photoemission from a time-delayed 790 nm pulse, we observe that a solvated electron is produced in an excited state and subsequently relaxes to its ground state with a lifetime of 151 ± 31 fs. This work demonstrates that femotosecond EUV photoemission is a versatile surface-sensitive probe of the properties and ultrafast dynamics of isolated nanoparticles.

Mapping Nanoscale Absorption of Femtosecond Laser Pulses Using Plasma Explosion Imaging

We make direct observations of localized light absorption in a single nanostructure irradiated by a strong femtosecond laser field, by developing and applying a technique that we refer to as plasma explosion imaging. By imaging the photoion momentum distribution resulting from plasma formation in a laser-irradiated nanostructure, we map the spatial location of the highly localized plasma and thereby image the nanoscale light absorption. Our method probes individual, isolated nanoparticles in vacuum, which allows us to observe how small variations in the composition, shape, and orientation of the nanostructures lead to vastly different light absorption. Here, we study four different nanoparticle samples with overall dimensions of ∼100 nm and find that each sample exhibits distinct light absorption mechanisms despite their similar size. Specifically, we observe subwavelength focusing in single NaCl crystals, symmetric absorption in TiO2 aggregates, surface enhancement in dielectric particles containing a single gold nanoparticle, and interparticle hot spots in dielectric particles containing multiple smaller gold nanoparticles. These observations demonstrate how plasma explosion imaging directly reveals the diverse ways in which nanoparticles respond to strong laser fields, a process that is notoriously challenging to model because of the rapid evolution of materials properties that takes place on the femtosecond time scale as a solid nanostructure is transformed into a dense plasma.

Ultrafast electro-optic light with subcycle control

Making ultrafast cycles of light The ability to generate coherent optical frequency combs has had a huge impact on precision metrology, imaging, and sensing applications. On closer inspection, the broadband “white light” generated through the interaction of femtosecond mode-locked laser pulses is composed of billions or trillions of precisely spaced wavelengths of light. Carlson et al. demonstrate an alternative to the mode-locked laser approach—the electro-optic modulation of a continuous-wave laser light source can also generate optical frequency combs (see the Perspective by Torres-Company). The electro-optic modulation techniques can operate at much higher repetition rates than mode-locked lasers, which means they could potentially yield even more precise measurements. Science, this issue p. 1358; see also p. 1316 Electro-optic modulation of a continuous-wave laser is used to produce ultrafast and ultrastable optical frequency combs. Light sources that are ultrafast and ultrastable enable applications like timing with subfemtosecond precision and control of quantum and classical systems. Mode-locked lasers have often given access to this regime, by using their high pulse energies. We demonstrate an adaptable method for ultrastable control of low-energy femtosecond pulses based on common electro-optic modulation of a continuous-wave laser light source. We show that we can obtain 100-picojoule pulse trains at rates up to 30 gigahertz and demonstrate sub–optical cycle timing precision and useful output spectra spanning the near infrared. Our source enters the few-cycle ultrafast regime without mode locking, and its high speed provides access to nonlinear measurements and rapid transients.

Photonic-Chip Supercontinuum with Tailored Spectra for Counting Optical Frequencies

Supercontinuum generation using chip-integrated photonic waveguides is a powerful approach for spectrally broadening pulsed laser sources with very low pulse energies and compact form factors. When pumped with a mode-locked laser frequency comb, these waveguides can coherently expand the comb spectrum to more than an octave in bandwidth to enable self-referenced stabilization. However, for applications in frequency metrology and precision spectroscopy, it is desirable to not only support self-referencing, but also to generate low-noise combs with customizable broadband spectra. In this work, we demonstrate dispersion-engineered waveguides based on silicon nitride that are designed to meet these goals and enable precision optical metrology experiments across large wavelength spans. We perform a clock comparison measurement and report a clock-limited relative frequency instability of

Lorentz drift compensation in high harmonic generation in the soft and hard X-ray regions of the spectrum

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