Tingting Fan

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.

Helicity-Selective Phase-Matching and Quasi-Phase matching of Circularly Polarized High-Order Harmonics: Towards Chiral Attosecond Pulses

Author(s): Kfir, O; Grychtol, P; Turgut, E; Knut, R; Zusin, D; Fleischer, A; Bordo, E; Fan, T; Popmintchev, D; Popmintchev, T; Kapteyn, H; Murnane, M; Cohen, O | Abstract:

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.

Phase matching of noncollinear sum and difference frequency high harmonic generation above and below the critical ionization level

We experimentally investigate phase matching of high harmonic generation in a noncollinear geometry and demonstrate phase matching above critical ionization using noncollinear high-order-difference-frequency generation, which provides a route to maximize the generated photon energies.

Generation of bright soft X-ray harmonics with circular polarization for X-ray magnetic circular dichroism

We present the first circularly polarized harmonics in the soft X-ray region and the physics underlying it. This source enables the first X-ray magnetic circular dichroism measurements in rare earth elements on tabletop.

Bright Soft X-ray High Harmonic Generation with Circular Polarization for X-ray Magnetic Circular Dichroism

We present the first circularly polarized soft X-ray harmonics to photon energies >160eV. Bright phase matched beams are used to characterize important materials with intrinsic perpendicular magnetic anisotropy on tabletop for the first time