DOE OSTI · 3013756
Attosecond X-Ray Core-Level Chronoscopy of Aromatic Molecules
Abstract
Attosecond photoemission or photoionization delays are a unique probe of the structure and the electronic dynamics of matter. However, the spectral congestion of valence photoelectron spectra sets fundamental limits to the complexity of systems that can be studied, and the delocalization of valence electron wave functions blurs the spatial origin of the photoelectron wave packet. Using attosecond x-ray pulses from LCLS, we demonstrate the key advantages of measuring core-level delays: The photoelectron spectra remain atomlike, the measurements become element specific, and the observed scattering dynamics originate from a pointlike source when multicenter interference effects are negligible. We exploit these unique features to reveal the effects of changing functional groups (C-H vs N) and symmetry on attosecond scattering dynamics by measuring and calculating the photoionization delays between N−1𝑠 and C−1𝑠 core shells of a series of aromatic azabenzene molecules. Remarkably, the delays increase with the number of nitrogen atoms in the molecule and reveal multiple resonances. We identify two previously unknown mechanisms regulating the associated attosecond dynamics, namely the enhanced confinement of the trapped wave function with the replacement of C-H groups by N atoms and the decrease of the coupling strength among the photoemitted partial waves with increasing symmetry. This study demonstrates the unique opportunities opened by measurements of core-level photoionization delays for unraveling attosecond electron dynamics in complex matter.
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Ji, Jia-Bao [Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)] (ORCID:0000000182257544), Guo, Zhaoheng [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Ecole Polytechnique Federale Lausanne (EPFL) (Switzerland)], Driver, Taran [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000237616883), Trevisan, Cynthia S. [Cal Poly Maritime Academy, Vallejo, CA (United States)] (ORCID:0009000806786899), Cesar, David [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Cheng, Xinxin [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000175868240), Duris, Joseph [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000299301166), Franz, Paris L. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000327286283), Glownia, James [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000261727946), Gong, Xiaochun [Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Zhejiang Univ., Hangzhou (China)] (ORCID:0000000248266049), Hammerland, Daniel [Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)] (ORCID:0000000332803636), Han, Meng [Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Kansas State Univ., Manhattan, KS (United States)] (ORCID:0000000169526009), Heck, Saijoscha [Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)], Hoffmann, Matthias [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000235969853), Kamalov, Andrei [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0009000869090442), Larsen, Kirk A. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Li, Xiang [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000183384123), Lin, Ming-Fu [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Liu, Yuchen [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Davis, CA (United States)] (ORCID:0000000344251947), McCurdy, C. William [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Davis, CA (United States)], Obaid, Razib [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], O’Neal, Jordan T. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Rescigno, Thomas N. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000188911359), Robles, River R. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Sudar, Nicholas [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Walter, Peter [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Wang, Anna L. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Wang, Jun [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Wolf, Thomas J. A. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Zhang, Zhen [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Ueda, Kiyoshi [Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Tohoku Univ., Sendai (Japan); ShanghaiTech Univ. (China)] (ORCID:0000000180518966), Lucchese, Robert R. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Marinelli, Agostino [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Cryan, James P. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000277760919), Wörner, Hans Jakob [Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)] (ORCID:0000000288770872). 2025-11-14. Attosecond X-Ray Core-Level Chronoscopy of Aromatic Molecules. https://doi.org/10.1103/dp5w-qxqc
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