Attosecond Delays in Molecular Photoionization
Open accessAbstract
We report measurements of energy-dependent photoionization delays between the two outermost valence shells of N_{2}O and H_{2}O. The combination of single-shot signal referencing with the use of different metal foils to filter the attosecond pulse train enables us to extract delays from congested spectra. Remarkably large delays up to 160 as are observed in N_{2}O, whereas the delays in H_{2}O are all smaller than 50 as in the photon-energy range of 20-40 eV. These results are interpreted by developing a theory of molecular photoionization delays. The long delays measured in N_{2}O are shown to reflect the population of molecular shape resonances that trap the photoelectron for a duration of up to ∼110 as. The unstructured continua of H_{2}O result in much smaller delays at the same photon energies. Our experimental and theoretical methods make the study of molecular attosecond photoionization dynamics accessible.
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Most recently, attosecond photoionization delays have been measured in molecules and high-harmonic spectroscopy has been developed to reconstruct charge migration in spatially oriented molecules on attosecond timescales.
“Most recently, attosecond photoionization delays have been measured in molecules [200] and highharmonic spectroscopy has been developed further to reconstruct charge migration in spatially oriented molecules on attosecond timescales [171].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [200]
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Attosecond interferometry of shape resonances in the recoil frame of CF 4
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Self-citationAttosecond Dynamics of Molecular Electronic Ring Currents
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RABBITT phase transition across the ionization threshold
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Wigner time delay in atomic photoionization
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Attosecond-Scale Streaking Methods for Strong-Field Ionization by Tailored Fields
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Attosecond pulse generation at ELI-ALPS 100 kHz repetition rate beamline
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Attosecond-resolved non-dipole photoionization dynamics
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Self-citationProbing electronic binding potentials with attosecond photoelectron wavepackets
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Angle-resolved studies of XUV–IR two-photon ionization in the RABBITT scheme
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Angularly resolved RABBITT using a second harmonic pulse
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Non-linear processes in the extreme ultraviolet
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Time Delays as Attosecond Probe of Interelectronic Coherence and Entanglement
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Attosecond metrology in circular polarization
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Spin–orbit-resolved spectral phase measurements around a Fano resonance
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Attosecond circular-dichroism chronoscopy of electron vortices
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Self-citationAttosecond delays in laser-assisted photodetachment from closed-shell negative ions
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Extracting attosecond delays from spectrally overlapping interferograms
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Attosecond photoionization delays in the vicinity of molecular Feshbach resonances
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Attosecond ionization time delays in strong-field physics
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Probing electronic decoherence with high-resolution attosecond photoelectron interferometry
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High harmonic generation-2ω attosecond stereo-photoionization interferometry in N2
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Attosecond delays between dissociative and non-dissociative ionization of polyatomic molecules
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Self-citationProper Time Delays Measured by Optical Streaking
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Analysis of RABITT time delays using the stationary multiphoton molecular R -matrix approach
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Resonant two-photon ionization of helium atoms studied by attosecond interferometry
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Probing Resonant Photoionization Time Delay by Self-Referenced Molecular Attoclock
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Self-citationTwo-Center Interference in the Photoionization Delays of Kr2
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Few-cycle high-harmonic generation in liquids: in-operando thickness measurement of flat microjets
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Self-citationAttosecond metrology of the two-dimensional charge distribution in molecules
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Attosecond Time Delay in Photoionization of Noble-Gas and Halogen Atoms
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Apparatus for attosecond transient-absorption spectroscopy in the water-window soft-X-ray region
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Self-citationRole of nuclear-electronic coupling in attosecond photoionization of H2
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Raman time-delay in attosecond transient absorption of strong-field created krypton vacancy
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Reconstruction of Nanoscale Near Fields by Attosecond Streaking
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Probing time delays and coherent imaging of multiphoton resonant ionization
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Revealing the Target Electronic Structure with Under-Threshold RABBITT
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Time delay in XUV/IR photoionization of H2O
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Wigner time delay in photodetachment
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Controlling photoionization using attosecond time-slit interferences
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Coulomb focusing in attosecond angular streaking
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Influence of nuclear dynamics on molecular attosecond photoelectron interferometry
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Energy-resolved attosecond interferometric photoemission from Ag(111) and Au(111) surfaces
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Resonant photoionization of O 2 up to the fourth ionization threshold
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Attosecond spectroscopy for filming the ultrafast movies of atoms, molecules and solids
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Full Characterization of a Molecular Cooper Minimum Using High-Harmonic Spectroscopy
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Attosecond physics and technology
Alexander, O., Ayuso, D., Matthews, M., Rego, L., Tisch, J. W. G., Weaver, B., & Marangos, J. P. (2025) · Applied Physics Letters · doi:10.1063/5.0251524 · Cited by 17 · see citing works
- Authors
- Huppert, M., Jordan, I., Baykusheva, D., von Conta, A., & Wörner, H. J.
- Affiliations
- ETH Zurich (CH)
- Venue
- Physical Review Letters
- Publisher
- American Physical Society (APS)
- Published
- 2016-08-22
- Volume
- 117
- Issue
- 9
- Pages
- 093001-093001
- ISSN
- 0031-9007 (ISSN-L)
- 1079-7114
- OpenAlex
- W2508703147
- Cited by
- 283
- References
- 45
- Citations by year
- 2026: 17 · 2025: 37 · 2024: 35 · 2023: 25 · 2022: 31 · 2021: 27 · 2020: 36 · 2019: 22 · 2018: 28 · 2017: 22 · 2016: 2
- FWCI
- 11.66
- Type
- journal article
- Language
- en
- Open access
- green
- arxiv.org
- Locations
- Physical Review Letters (publishedVersion)
- PubMed (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- arXiv (Cornell University)
- Funders
- European Research Council (307270-ATTOSCOPE)
- Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
- NCCR-MUST
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Atomic and Molecular Physics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Keywords
- molecular photoionization, N2O, water, shape resonances, photoelectron trapping, photoionization dynamics
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