Kevin M. Dorney

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.

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.

A new electron-ion coincidence 3D momentum-imaging method and its application in probing strong field dynamics of 2-phenylethyl-N, N-dimethylamine

We report the development of a new three-dimensional (3D) momentum-imaging setup based on conventional velocity map imaging to achieve the coincidence measurement of photoelectrons and photo-ions. This setup uses only one imaging detector (microchannel plates (MCP)/phosphor screen) but the voltages on electrodes are pulsed to push both electrons and ions toward the same detector. The ion-electron coincidence is achieved using two cameras to capture images of ions and electrons separately. The time-of-flight of ions and electrons are read out from MCP using a digitizer. We demonstrate this new system by studying the dissociative single and double ionization of PENNA (2-phenylethyl-N,N-dimethylamine). We further show that the camera-based 3D imaging system can operate at 10 kHz repetition rate.

High harmonics with spatially varying ellipticity

We present a method of producing ultrashort pulses of circularly polarized extreme ultraviolet (EUV) light through high-harmonic generation (HHG). HHG is a powerful tool for generating bright laser-like beams of EUV and soft x-ray light with ultrashort pulse durations, which are important for many spectroscopic and imaging applications in the materials, chemical, and nano sciences. Historically HHG was restricted to linear polarization; however, recent advances are making it possible to precisely control the polarization state of the emitted light simply by adjusting the driving laser beams and geometry. In this work, we gain polarization control by combining two spatially separated and orthogonally linearly polarized HHG sources to produce a far-field beam with a uniform intensity distribution, but with a spatially varying ellipticity that ranges from linearly to fully circularly polarized. This spatially varying ellipticity was characterized using EUV magnetic circular dichroism, which demonstrates that a high degree of circularity is achieved, reaching almost 100% near the magnetic M-edge of cobalt. The spatial modulation of the polarization facilitates measurements of circular dichroism, enabling us to measure spectrally resolved magnetic circular dichroism without the use of an EUV spectrometer, thereby avoiding the associated losses in both flux and spatial resolution, which could enable hyperspectral imaging of chiral systems. Through numerical simulations, we also show the generality of this scheme, which can be applied with either the discrete harmonic orders generated by many-cycle pulses or the high-harmonic supercontinua generated by few-cycle driving laser pulses. Therefore, this technique provides a promising route for the production of bright isolated attosecond pulses with circular polarization that can probe ultrafast spin dynamics in materials.

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.

Ionization Dynamics in Intense Two-Color Circularly Polarized Laser Fields

Ionization in intense two-color circularly polarized laser pulses is explored numerically and experimentally. Double ionization is enhanced with counterrotating fields, and diverse dynamics are uncovered that are impossible with linear polarization.

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