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• W4386414030 abstract "We show that core-level x-ray absorption near edge structure (XANES) spectroscopy with attosecond soft x-ray (SXR) pulses [1] can image the flow of energy inside a material in real time [2]. We photoexcite graphite with a <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$11pm 1$</tex> fs pump pulse at 1850 nm, or with a <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$15pm 1$</tex> fs pulse at 800 nm, for various pump fluences between <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$2.8 pm$</tex> 0.2 <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$text{mJ}/text{cm}2$</tex> and <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$81pm 5 text{mJ}/text{cm}2$</tex> . Figure 1(a) shows the measured differential x-ray absorption <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$Deltamathrm{A}(mathrm{E})$</tex> (pumped minus unpumped) from which striking changes of up to 15% are immediately apparent. We identify these features as <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$pi$</tex> bonding state and as <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$pi^{*}$</tex> and <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$sigma^{*}$</tex> antibonding states. Attosecond-resolved measurement with a pump-probe delay step size of 0.6 fs show the buildup of coherent charge oscillations, i.e., polarization of the material. These oscillations occur at occupied states below and unoccupied states above the Fermi level predominantly at the pump carrier frequency. We identify the incoherent background due to the dephasing of coherent charge oscillation. This background rises within a few oscillations of the light field, signifying the ultrafast transfer of energy from the light field into the electron and hole excitation of the material. We find that ultrafast dephasing of the coherent carrier dynamics is governed by impact excitation (lE) for electrons, while holes exhibit a switchover from impact excitation to Auger heating (AH) already during the 11-fs duration of the infrared light field. We further analyze the coherent phonon signal by analyzing the oscillatory pattern exhibited by the <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$sigma^{*}$</tex> data with a short-time Fourier transform (STFT) analysis This analysis shows that already during and shortly after the laser excitation, coherent motion emerges over a broad range of frequencies. A comparison with the phonon dispersion from two-temperature-model molecular dynamics (TTM MD) simulations [4] [Fig. <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$1(mathrm{e})]$</tex> identifies them as the Raman-active <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$ulcorner-mathrm{E}2mathrm{g}$</tex> and the non-Raman-active K - A'1 SCOPs at <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$46.4pm 2.7$</tex> and 42.7 <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$pm 1.1$</tex> THz, respectively. The surprising early contribution from the (non-Raman-active) <tex xmlns:mml=http://www.w3.org/1998/Math/MathML xmlns:xlink=http://www.w3.org/1999/xlink>$mathrm{A}^{prime}1$</tex> mode originate from the very strong electron-SCOPs coupling, thus acting almost impulsively." @default.
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• W4386414030 date "2023-06-26" @default.
• W4386414030 modified "2023-10-18" @default.
• W4386414030 title "Attosecond Soft X-Ray Spectroscopy Reveals Energy Flow in a Semimetal" @default.
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• W4386414030 doi "https://doi.org/10.1109/cleo/europe-eqec57999.2023.10231494" @default.
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