Attosecond streaking of atomic photoemission holds the promise to provide unprecedented information on the release time of the photoelectron. We show that attosecond streaking phase shifts indeed contain timing (or spectral phase) information associated with the Eisenbud-Wigner-Smith time delay matrix of quantum scattering. However, this is only accessible if the influence of the streaking infrared (IR) field on the emission process is properly accounted for. The IR probe field can strongly modify the observed streaking phase shift. We show that the part of the phase shift ("time shift") due to the interaction between the outgoing electron and the combined Coulomb and IR laser fields can be described classically. By contrast, the strong initial-state dependence of the streaking phase shift is only revealed through the solution of the time-dependent Schrödinger equation in its full dimensionality. We find a time delay between the hydrogenic 2s and 2p initial states in He + exceeding 20 as for a wide range of IR intensities and XUV energies.
We present a semiclassical two-step model for strong-field ionization that accounts for path interferences of tunnel-ionized electrons in the ionic potential beyond perturbation theory. Within the framework of a classical trajectory Monte Carlo representation of the phase-space dynamics, the model employs the semiclassical approximation to the phase of the full quantum propagator in the exit channel. By comparison with the exact numerical solution of the time-dependent Schrödinger equation for strong-field ionization of hydrogen, we show that for suitable choices of the momentum distribution after the first tunneling step, the model yields good quantitative agreement with the full quantum simulation. The two-dimensional photoelectron momentum distributions, the energy spectra, and the angular distributions are found to be in good agreement with the corresponding quantum results. Specifically, the model quantitatively reproduces the fanlike interference patterns in the low-energy part of the two-dimensional momentum distributions, as well as the modulations in the photoelectron angular distributions.
The propagation and transport of electrons in crystals is a fundamental process pertaining to the functioning of most electronic devices. Microscopic theories describe this phenomenon as being based on the motion of Bloch wave packets. These wave packets are superpositions of individual Bloch states with the group velocity determined by the dispersion of the electronic band structure near the central wavevector in momentum space. This concept has been verified experimentally in artificial superlattices by the observation of Bloch oscillations—periodic oscillations of electrons in real and momentum space. Here we present a direct observation of electron wave packet motion in a real-space and real-time experiment, on length and time scales shorter than the Bloch oscillation amplitude and period. We show that attosecond metrology (1 as = 10-18 seconds) now enables quantitative insight into weakly disturbed electron wave packet propagation on the atomic length scale without being hampered by scattering effects, which inevitably occur over macroscopic propagation length scales. We use sub-femtosecond (less than 10-15 seconds) extreme-ultraviolet light pulses to launch photoelectron wave packets inside a tungsten crystal that is covered by magnesium films of varied, well-defined thicknesses of a few ångströms. Probing the moment of arrival of the wave packets at the surface with attosecond precision reveals free-electron-like, ballistic propagation behaviour inside the magnesium adlayer—constituting the semi-classical limit of Bloch wave packet motion. Real-time access to electron transport through atomic layers and interfaces promises unprecedented insight into phenomena that may enable the scaling of electronic and photonic circuits to atomic dimensions. In addition, this experiment allows us to determine the penetration depth of electrical fields at optical frequencies at solid interfaces on the atomic scal
Upon impact on a solid surface, the potential energy stored in slow highly charged ions is primarily deposited into the electronic system of the target. By decelerating the projectile ions to kinetic energies as low as 150 x q eV, we find first unambiguous experimental evidence that potential energy alone is sufficient to cause permanent nanosized hillocks on the (111) surface of a CaF(2) single crystal. Our investigations reveal a surprisingly sharp and well-defined threshold of potential energy for hillock formation which can be linked to a solid-liquid phase transition.
High-harmonic generation by a highly non-linear interaction of infrared laser fields with matter allows for the generation of attosecond pulses in the XUV spectral regime. This process, well established for atoms, has been recently extended to the condensed phase. Remarkably well pronounced harmonics up to order ∼ 30 have been observed for dielectrics. We present the first ab-initio multiscale simulation of solid-state high-harmonic generation. We find that mesoscopic effects of the extended system, in particular the realistic sampling of the entire Brillouin zone, the pulse propagation in the dense medium, and the inhomogeneous illumination of the crystal have a strong effect on the formation of clean harmonic spectra. Our results provide a novel explanation for the formation of clean harmonics and have implications for a wide range of non-linear optical processes in dense media.PACS numbers: 42.65. Ky, 42.50.Hz, 72.20.Ht The generation of high harmonics (HHG) in the nonlinear interaction of intense ultrashort infrared (IR) laser pulses with matter has turned out to be a highly successful route towards the generation of attosecond pulses in the EUV and XUV spectral regimes [1][2][3][4]. It has become the workhorse of investigation of a vast array of electronic processes on the attosecond time scale [5]. Expanding the range of accessible photon energies and intensities faces, however, fundamental limitations. Experimental and theoretical investigations have established a scaling of the cut-off energy E cut ∝ λ 2 for HHG from atoms in the gas phase raising hopes to reach ever higher photon energies by increasing the wavelength λ of the driving laser pulse. However, the intensity in the cut-off region was found to scale unfavorably I cut ∝ λ −5.3 due to the large spatial dispersion of the electron wave packet upon return to its parent atom [6][7][8][9][10]. Propagation effects in gas filled capillaries have been found to partially offset this suppression at high λ [11].Extending HHG to the condensed phase promises to overcome some of these limitations to enable compact and brighter light sources and to open up the novel field of solid-state photonics on the attosecond scale. The recent observation of HHG in solids for intensities below the damage threshold [12][13][14][15][16][17][18] suggests opportunities for controlling electronic dynamics [16,17] and for an alloptical reconstruction of the band structure [19].The observed solid-state HHG substantially differs from the corresponding atomic spectra. For example, while for atoms the cut-off frequency ω HHG cut scales linearly with the (peak) intensity I 0 of the driving pulse [20,21] One major puzzle has remained so far unresolved: while many experiments display remarkably "clean" harmonic spectra with pronounced peaks near multiples of the driving frequency (odd multiples when inversion symmetry is preserved) all the way up to the cutoff frequency, corresponding simulations display a noisy spectrum lacking any clear harmonic structure over a wide range of fre...
We demonstrate that multiphoton-induced photoelectron emission from a gold surface caused by low-energy (unamplified) 4-fs, 750-nm laser pulses is sensitive to the timing of electric field oscillations with respect to the pulse peak. This observation confirms recent theoretical predictions and opens the door to measuring the absolute value of the carrier-envelope phase difference of few-cycle light pulses with a solid-state detector.
Attosecond science is based on electron dynamics driven by a strong optical electric field and has evolved beyond its original scope in gas-phase atomic and molecular physics to solid-state targets. In this review, we discuss a nanoscale attosecond physics laboratory that has enabled the first observations of strong-field-driven photoemission and recollision at a solid surface: laser-triggered metallic nanotips. In addition to the research questions of rather fundamental nature, femtosecond electron sources with outstanding beam qualities have resulted from this research, which has prompted follow-up application in the sensing of electric fields and lightwave electronics, ultrafast microscopy and diffraction, and fundamental matter-wave quantum optics. We review the theoretical and experimental concepts underlying near-field enhancement, photoemission regimes and electron acceleration mechanisms. Nanotips add new degrees of freedom to well known strong-field phenomena from atomic physics. For example, they enable the realization of a true sub-optical-cycle acceleration regime where recollision is suppressed. We also discuss the possibility of high-harmonic generation due to laser irradiation of metallic nanostructures.
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