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Timestamp: 2019-04-23 00:58:48+00:00

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Attosecond photoelectron streaking spectroscopy allows time-resolved electron dynamics with a temporal resolution approaching the atomic unit of time. Studies have been performed in numerous systems, including atoms, molecules, and surfaces, and the quest for ever higher temporal resolution called for ever wider spectral extent of the attosecond pulses. For typical experiments relying on attosecond pulses with a duration of 200 as, the time-bandwidth limitation for a Gaussian pulse implies a minimal spectral bandwidth larger than 9 eV translating to a corresponding spread of the detected photoelectron kinetic energies. Here, by utilizing a specially tailored narrowband reflective XUV multilayer mirror, we explore experimentally the minimal spectral width compatible with attosecond time-resolved photoelectron spectroscopy while obtaining the highest possible spectral resolution. The validity of the concept is proven by recording attosecond electron streaking traces from the direct semiconductor gallium arsenide (GaAs), with a nominal bandgap of 1.42 eV at room temperature, proving the potential of the approach for tracking charge dynamics also in these technologically highly relevant materials that previously have been inaccessible to attosecond science.
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Fig. 1. (a) Measured spectral reflectivity profile (solid orange) of the realized Mo/B4C multilayer mirror, its fit (dotted blue), the target profile centered at 112 eV (dashed gray), and the corresponding simulated GD (dashed red) within the bandwidth of ΔE=1.8 eV. The multilayer design parameters are listed bottom left. (b) Small inset depicts the complete spectral range of the normalized measured reflectivity profile indicating a high suppression of lower and higher frequency components (no filter transmission profile included).
Fig. 2. (a) + (b) Mirror picture without and with delaminating multilayer coating. (c) Simulated reflectivity dependence on the gamma ratio γ=dMo/d and the number of periods N for the Mo/B4C material system centered at 112 eV. The corresponding spectral bandwidths in the eV unit are additionally depicted as black contour lines.
Fig. 3. Unstreaked photoelectron spectra of the gallium 3d peak measured with a broadband (FWHM=5 eV) multilayer mirror (blue) and with the narrowband (FWHM=1.8 eV) Mo/B4C mirror (red). The circles and squares, respectively, represent the data points, whereas the solid lines depict the corresponding Gaussian fit. The convolution (black) of our TOF ∼1% energy resolution, the mirror, and the gallium 3d spectrum (green) from  agrees with our measurement.
Fig. 4. (a) Measured and (b) retrieved electron streaking on GaAs. The white line in (b) depicts the retrieved vector potential A(t) of the NIR. (c) Retrieved photoelectron wave packet intensity (solid blue) and GD (dashed red) in the spectral domain. (d) Intensity and phase in the temporal domain. (e) Calculated electric field of the NIR (solid red), the envelope (solid blue), and the simulated XUV pulse (purple).

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