| 1. |
- Chen, Cong, et al.
(author)
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Distinguishing attosecond electron-electron scattering and screening in transition metals
- 2017
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In: Proceedings of the National Academy of Sciences of the United States of America. - : National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 114:27, s. E5300-E5307
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Journal article (peer-reviewed)abstract
- 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 similar to 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 (approximate to 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.
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| 2. |
- Chen, Cong, et al.
(author)
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Tomographic reconstruction of circularly polarized high-harmonic fields : 3D attosecond metrology.
- 2016
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In: Science Advances. - : American Association for the Advancement of Science (AAAS). - 2375-2548. ; 2:2
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Journal article (peer-reviewed)abstract
- 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.
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| 3. |
- Fan, Tingting, et al.
(author)
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Bright circularly polarized soft X-ray high harmonics for X-ray magnetic circular dichroism
- 2015
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In: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 112:46, s. 14206-14211
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Journal article (peer-reviewed)abstract
- 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 mu m, 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 N-4,N-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.
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| 4. |
- Hickstein, Daniel D., et al.
(author)
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Direct Visualization of Laser-Driven Electron Multiple Scattering and Tunneling Distance in Strong-Field Ionization
- 2012
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In: Physical Review Letters. - 1079-7114. ; 109:7
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Journal article (peer-reviewed)abstract
- Using a simple model of strong-field ionization of atoms that generalizes the well-known 3-step model from 1D to 3D, we show that the experimental photoelectron angular distributions resulting from laser ionization of xenon and argon display prominent structures that correspond to electrons that pass by their parent ion more than once before strongly scattering. The shape of these structures can be associated with the specific number of times the electron is driven past its parent ion in the laser field before scattering. Furthermore, a careful analysis of the cutoff energy of the structures allows us to experimentally measure the distance between the electron and ion at the moment of tunnel ionization. This work provides new physical insight into how atoms ionize in strong laser fields and has implications for further efforts to extract atomic and molecular dynamics from strong-field physics.
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| 5. |
- Hickstein, Daniel D., et al.
(author)
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Non-collinear generation of angularly isolated circularly polarized high harmonics
- 2015
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In: Nature Photonics. - 1749-4885 .- 1749-4893. ; 9:11, s. 743-750
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Journal article (peer-reviewed)abstract
- We generate angularly isolated beams of circularly polarized extreme ultraviolet light through the first implementation of non-collinear high harmonic generation with circularly polarized driving lasers. This non-collinear technique offers numerous advantages over previous methods, including the generation of higher photon energies, the separation of the harmonics from the pump beam, the production of both left and right circularly polarized harmonics at the same wavelength and the capability of separating the harmonics without using a spectrometer. To confirm the circular polarization of the beams and to demonstrate the practicality of this new light source, we measure the magnetic circular dichroism of a 20 nm iron film. Furthermore, we explain the mechanisms of non-collinear high harmonic generation using analytical descriptions in both the photon and wave models. Advanced numerical simulations indicate that this non-collinear mixing enables the generation of isolated attosecond pulses with circular polarization.
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| 6. |
- Kfir, Ofer, et al.
(author)
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Generation of bright phase-matched circularly-polarized extreme ultraviolet high harmonics
- 2015
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In: Nature Photonics. - 1749-4885 .- 1749-4893. ; 9:2, s. 99-105
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Journal article (peer-reviewed)abstract
- Circularly-polarized extreme ultraviolet and X-ray radiation is useful for analysing the structural, electronic and magnetic properties of materials. To date, such radiation has only been available at large-scale X-ray facilities such as synchrotrons. Here, we demonstrate the first bright, phase-matched, extreme ultraviolet circularly-polarized high harmonics source. The harmonics are emitted when bi-chromatic counter-rotating circularly-polarized laser pulses field-ionize a gas in a hollow-core waveguide. We 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 linearly polarized high harmonic sources. This work represents a critical advance towards the development of table-top systems for element-specific imaging and spectroscopy of multiple elements simultaneously in magnetic and other chiral media with very high spatial and temporal resolution.
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| 7. |
- Kfir, Ofer, et al.
(author)
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Helicity-selective phase-matching and quasi-phase matching of circularly polarized high-order harmonics : towards chiral attosecond pulses
- 2016
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In: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 49:12
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Journal article (peer-reviewed)abstract
- Phase matching of circularly polarized high-order harmonics driven by counter-rotating bi-chromatic lasers was recently predicted theoretically and demonstrated experimentally. In that work, phase matching was analyzed by assuming that the total energy, spin angular momentum and linear momentum of the photons participating in the process are conserved. Here we propose a new perspective on phase matching of circularly polarized high harmonics. We derive an extended phase matching condition by requiring a new propagation matching condition between the classical vectorial bi-chromatic laser pump and harmonics fields. This allows us to include the influence of the laser pulse envelopes on phase matching. We find that the helicity dependent phase matching facilitates generation of high harmonics beams with a high degree of chirality. Indeed, we present an experimentally measured chiral spectrum that can support a train of attosecond pulses with a high degree of circular polarization. Moreover, while the degree of circularity of the most intense pulse approaches unity, all other pulses exhibit reduced circularity. This feature suggests the possibility of using a train of attosecond pulses as an isolated attosecond probe for chiral-sensitive experiments.
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