Dmitriy Zusin

Generation of bright phase-matched circularly-polarized extreme ultraviolet high harmonics

Circularly-polarized extreme UV and X-ray radiation provides valuable access to the structural, electronic and magnetic properties of materials. To date, this capability was available only at large-scale X-ray facilities such as synchrotrons. Here we demonstrate the first bright, phase-matched, extreme UV circularly-polarized high harmonics and use this new light source for magnetic circular dichroism measurements at the M-shell absorption edges of Co. We show that phase matching of circularly-polarized harmonics is unique and robust, producing a photon flux comparable to the linearly polarized high harmonic sources that have been used very successfully for ultrafast element-selective magneto-optic experiments. This work thus represents a critical advance that makes possible element-specific imaging and spectroscopy of multiple elements simultaneously in magnetic and other chiral media with very high spatial and temporal resolution, using tabletop-scale setups.

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.

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:

Distinguishing attosecond electron–electron scattering and screening in transition metals

Significance Electron–electron interactions are among the fastest processes in materials that determine their fascinating properties, occurring on attosecond timescales on up (1 as = 10−18 s). The recent development of attosecond angle-resolved photoemission spectroscopy (atto-ARPES) using high harmonic generation has opened up the possibility of probing electron–electron interactions in real time. In this paper, we distinguish electron–electron screening and charge scattering in the time domain in individual energy bands within a solid. These results open up new possibilities for probing fundamental electron–electron interactions in a host of materials including magnetic, superconducting, and advanced quantum materials. Electron–electron interactions are the fastest processes in materials, occurring on femtosecond to attosecond timescales, depending on the electronic band structure of the material and the excitation energy. Such interactions can play a dominant role in light-induced processes such as nano-enhanced plasmonics and catalysis, light harvesting, or phase transitions. However, to date it has not been possible to experimentally distinguish fundamental electron interactions such as scattering and screening. Here, we use sequences of attosecond pulses to directly measure electron–electron interactions in different bands of different materials with both simple and complex Fermi surfaces. By extracting the time delays associated with photoemission we show that the lifetime of photoelectrons from the d band of Cu are longer by ∼100 as compared with those from the same band of Ni. We attribute this to the enhanced electron–electron scattering in the unfilled d band of Ni. Using theoretical modeling, we can extract the contributions of electron–electron scattering and screening in different bands of different materials with both simple and complex Fermi surfaces. Our results also show that screening influences high-energy photoelectrons (≈20 eV) significantly less than low-energy photoelectrons. As a result, high-energy photoelectrons can serve as a direct probe of spin-dependent electron–electron scattering by neglecting screening. This can then be applied to quantifying the contribution of electron interactions and screening to low-energy excitations near the Fermi level. The information derived here provides valuable and unique information for a host of quantum materials.

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.

X-Ray Magnetic Circular Dichroism Probed Using High Harmonics

We demonstrate the first generation and phase matching of circularly-polarized high harmonics, which are bright enough for X-ray magnetic circular dichroism measurements at the M absorption edges of the magnetic materials Fe, Co and Ni.

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.