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  Attosecond soft X-ray spectroscopy reveals energy flow in a semimetal

Sidiropoulos, T. P. H., Palo, N. D., Rivas, D., Severino, S., Reduzzi, M., Sun, H.-W., et al. (2023). Attosecond soft X-ray spectroscopy reveals energy flow in a semimetal. In The European Conference on Lasers and Electro-Optics 2023.

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Item Permalink: https://hdl.handle.net/21.11116/0000-000E-6A24-3 Version Permalink: https://hdl.handle.net/21.11116/0000-000E-6BA3-2
Genre: Conference Paper

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 Creators:
Sidiropoulos, T. P. H.1, Author
Palo, N. Di1, Author
Rivas, D.E.1, Author
Severino, S.1, Author
Reduzzi, M.1, Author
Sun, H.-W.1, Author
Chien, Y.-H.1, Author
Nandy, B.1, Author
Bauerhenne, B.1, Author
Krylow, S.1, Author
Vasileiadis, T.1, Author
Danz, T.1, Author
Elliott, P.2, Author
Sharma, S.1, Author
Dewhurst, K.2, Author                 
Ropers, C.1, Author
Joly, Y.1, Author
Garcia, M. E.1, Author
Wolf, M.1, Author
Ernstorfer, R.1, Author
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Affiliations:
1External Organizations, ou_persistent22              
2Max Planck Institute of Microstructure Physics, Max Planck Society, ou_2415691              

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 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 11 ± 1 fs pump pulse at 1850 nm or with a 15 ± 1 fs pulse at 800 nm for various pump fluences between 2.8 ± 0.2 mJ/cm2 and 81 ± 5 mJ/cm2. Figure 1(a) shows the measured differential x-ray absorption ΔA(E) (pumped minus unpumped) from which striking changes of up to 15% are immediately apparent. We identify these features as π bonding state and as π* and σ* 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 (IE) 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 σ* 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.

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 Dates: 2023
 Publication Status: Issued
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Title: Conference on Lasers and Electro-Optics/Europe (CLEO/Europe 2023) and European Quantum Electronics Conference (EQEC 2023)
Place of Event: Munich, Germany
Start-/End Date: 2023-06-26 - 2023-06-30

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Title: The European Conference on Lasers and Electro-Optics 2023
Source Genre: Proceedings
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Pages: - Volume / Issue: - Sequence Number: cg_3_5 Start / End Page: - Identifier: ISBN: 979-8-3503-4599-5