Attosecond X-Ray Core-Level Chronoscopy of Aromatic Molecules

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 <a:math xmlns:a="http://www.w3.org/1998/Math/MathML" display="inline"> <a:mrow> <a:mi mathvariant="normal">N</a:mi> <a:mtext>−</a:mtext> <a:mn>1</a:mn> <a:mi>s</a:mi> </a:mrow> </a:math> and <d:math xmlns:d="http://www.w3.org/1998/Math/MathML" display="inline"> <d:mrow> <d:mi mathvariant="normal">C</d:mi> <d:mtext>−</d:mtext> <d:mn>1</d:mn> <d:mi>s</d:mi> </d:mrow> </d:math> 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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Journal
Physical Review X
Published
2025-11-14
DOI
https://doi.org/10.1103/dp5w-qxqc
Primary Topic
Laser-Matter Interactions and Applications
Type
article
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article

Attosecond X-Ray Core-Level Chronoscopy of Aromatic Molecules

Taran Driver, C. S. Trevisan, C. W. McCurdy, Xinxin Cheng et al.
Physical Review X
Laser-Matter Interactions and Applications
article

Attosecond X-Ray Core-Level Chronoscopy of Aromatic Molecules

Taran Driver, C. S. Trevisan, C. W. McCurdy, Xinxin Cheng, Hans Jakob Wörner, Agostino Marinelli, David Cesar, Matthias C. Hoffmann, Daniel Hammerland, Joseph Duris, Robert R. Lucchese, Peter Walter, River Robles, T. N. Rescigno, Ming‐Fu Lin, Jia-Bao Ji, Nicholas Sudar, Kirk A. Larsen, Saijoscha Heck, Anna L. Wang, Yuchen Liu, James Cryan, Kiyoshi Ueda, Xiaochun Gong, Meng Han, James M. Glownia, Razib Obaid, Thomas Wolf, Paris Franz, Zhaoheng Guo, Xiang Li, Jun Wang, Zhen Zhang, Jordan T. O’Neal, Andrei Kamalov
article en

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 <a:math xmlns:a="http://www.w3.org/1998/Math/MathML" display="inline"> <a:mrow> <a:mi mathvariant="normal">N</a:mi> <a:mtext>−</a:mtext> <a:mn>1</a:mn> <a:mi>s</a:mi> </a:mrow> </a:math> and <d:math xmlns:d="http://www.w3.org/1998/Math/MathML" display="inline"> <d:mrow> <d:mi mathvariant="normal">C</d:mi> <d:mtext>−</d:mtext> <d:mn>1</d:mn> <d:mi>s</d:mi> </d:mrow> </d:math> 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.

Physical Review XVol. 15(4)
Lawrence Berkeley National Laboratory (US), Kansas State University (US), Tohoku University (JP), California Maritime Academy (US), SLAC National Accelerator Laboratory (US), University of California System (US), ShanghaiTech University (CN), ETH Zurich (CH), École Polytechnique Fédérale de Lausanne (CH), Zhejiang University (CN), University of California, Davis (US)
Openalex Percentile: Top 73%
Laser-Matter Interactions and Applications
DOIOpen Access PDFOpenAlex
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