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Attosecond spectroscopy in condensed matter

Abstract

Comprehensive knowledge of the dynamic behaviour of electrons in condensed-matter systems is pertinent to the development of many modern technologies, such as semiconductor and molecular electronics, optoelectronics, information processing and photovoltaics. Yet it remains challenging to probe electronic processes, many of which take place in the attosecond (1 as = 10-18 s) regime. In contrast, atomic motion occurs on the femtosecond (1 fs = 10-15 s) timescale and has been mapped in solids in real time1,2 using femtosecond X-ray sources3. Here we extend the attosecond techniques4,5 previously used to study isolated atoms in the gas phase to observe electron motion in condensed-matter systems and on surfaces in real time. We demonstrate our ability to obtain direct time-domain access to charge dynamics with attosecond resolution by probing photoelectron emission from single-crystal tungsten. Our data reveal a delay of approximately 100 attoseconds between the emission of photoelectrons that originate from localized core states of the metal, and those that are freed from delocalized conduction-band states. These results illustrate that attosecond metrology constitutes a powerful tool for exploring not only gas-phase systems, but also fundamental electronic processes occurring on the attosecond timescale in condensed-matter systems and on surfaces.

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Figure 1: Experimental set-up.
Figure 2: Attosecond time-resolved photoemission spectra.
Figure 3: Evidence of delayed photoemission.

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Acknowledgements

We thank W. Hachmann for expeditious preparation of the XUV multilayer optical substrate. We acknowledge partial financial support by the Deutsche Forschungsgemeinschaft through the DFG Cluster of Excellence Munich Centre for Advanced Photonics, and through the SFB 613, and by the Volkswagen Stiftung Germany, and by the EURYI scheme award. P.M.E. acknowledges support from the Basque and Spanish Governments. R.K. acknowledges a fellowship from the Austrian Academy of Sciences and additional support from the Sofja Kovalevskaja Award of the Alexander von Humboldt Foundation. The apparatus to generate attosecond pulses was constructed at Technische Universität Wien, thanks to the support of the FWF.

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Correspondence to A. L. Cavalieri or F. Krausz or U. Heinzmann.

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Supplementary Information

The file contains additional description of the experimental apparatus, measurement technique, and data analysis, including Supplementary Figures 1-7 with Legends and Supplementary Table 1. (PDF 3368 kb)

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Cavalieri, A., Müller, N., Uphues, T. et al. Attosecond spectroscopy in condensed matter. Nature 449, 1029–1032 (2007). https://doi.org/10.1038/nature06229

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