Christian Gentry

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.

Tomographic reconstruction of circularly polarized high-harmonic fields: 3D attosecond metrology

Circularly polarized attosecond pulse trains in the EUV region were reconstructed using 3D attosecond metrology. Bright, circularly polarized, extreme ultraviolet (EUV) and soft x-ray high-harmonic beams can now be produced using counter-rotating circularly polarized driving laser fields. Although the resulting circularly polarized harmonics consist of relatively simple pairs of peaks in the spectral domain, in the time domain, the field is predicted to emerge as a complex series of rotating linearly polarized bursts, varying rapidly in amplitude, frequency, and polarization. We extend attosecond metrology techniques to circularly polarized light by simultaneously irradiating a copper surface with circularly polarized high-harmonic and linearly polarized infrared laser fields. The resulting temporal modulation of the photoelectron spectra carries essential phase information about the EUV field. Utilizing the polarization selectivity of the solid surface and by rotating the circularly polarized EUV field in space, we fully retrieve the amplitude and phase of the circularly polarized harmonics, allowing us to reconstruct one of the most complex coherent light fields produced to date.

Critical behavior within 20 fs drives the out-of-equilibrium laser-induced magnetic phase transition in nickel

High-harmonic spectroscopies reveal that fast energy transfer within 20 fs triggers ultrafast magnetic phase transition in Ni. It has long been known that ferromagnets undergo a phase transition from ferromagnetic to paramagnetic at the Curie temperature, associated with critical phenomena such as a divergence in the heat capacity. A ferromagnet can also be transiently demagnetized by heating it with an ultrafast laser pulse. However, to date, the connection between out-of-equilibrium and equilibrium phase transitions, or how fast the out-of-equilibrium phase transitions can proceed, was not known. By combining time- and angle-resolved photoemission with time-resolved transverse magneto-optical Kerr spectroscopies, we show that the same critical behavior also governs the ultrafast magnetic phase transition in nickel. This is evidenced by several observations. First, we observe a divergence of the transient heat capacity of the electron spin system preceding material demagnetization. Second, when the electron temperature is transiently driven above the Curie temperature, we observe an extremely rapid change in the material response: The spin system absorbs sufficient energy within the first 20 fs to subsequently proceed through the phase transition, whereas demagnetization and the collapse of the exchange splitting occur on much longer, fluence-independent time scales of ~176 fs. Third, we find that the transient electron temperature alone dictates the magnetic response. Our results are important because they connect the out-of-equilibrium material behavior to the strongly coupled equilibrium behavior and uncover a new time scale in the process of ultrafast demagnetization.

Tomographic Reconstruction of Circularly Polarized High Harmonic Fields: 3D Attosecond Metrology

Using laser-dressed photoelectron spectroscopy from solids, we completely characterized the circularly polarized harmonics, allowing us to reconstruct the complex 3D waveform of the circularly polarized attosecond pulse train.

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.

Heisenberg vs. stoner: Probing the microscopic picture of ultrafast demagnetization using high harmonics

We uncover the multiple mechanisms underlying laser-driven demagnetization in cobalt using a tabletop high harmonic source. Ultrafast magnon excitation, as well as a transient reduction of the exchange splitting, are both important on femtosecond timescales.

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.

Influence of microscopic and macroscopic effects on attosecond pulse generation using two-color laser fields

Attosecond pulses and pulse trains generated by high-order harmonic generation are finding broad applications in advanced spectroscopies and imaging, enabling sub-femtosecond electron dynamics to be probed in atomic, molecular and material systems. To date, isolated attosecond pulses have been generated either by using very short few-cycle driving pulses, or by using temporal and polarization gating, or by taking advantage of phase-matching gating. Here we show that by driving high harmonics with a two-color linearly polarized laser field, the temporal window for time-gated phase matching is shorter than for the equivalent singe-color driving laser. As a result, we can generate quasi-isolated attosecond pulses with a peak width of ∼ 450 as using relatively long 26 femtosecond laser pulses. Our experimental data are in good agreement with theoretical simulations, and show that the phase matching window decreases by a factor of 4 - from four optical cycles in the case of a single-color fundamental driving laser, to one optical cycle in the case of two-color (ω-2ω) laser drivers. Finally, we also demonstrate that by changing the relative delay between the two-color laser fields, we can control the duration of the attosecond bursts from 450 as to 1.2 fs.

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.

3D Characterization of Attosecond Pulse Trains with Circular Polarization

Using laser-dressed photoelectron spectroscopy from solids, we fully characterize circularly polarized harmonics for the first time to reconstruct the complex 3D waveform of a circularly polarized attosecond pulse train.