Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites

Wang, Jun; Driver, Taran; Franz, Paris L.; Kolorenč, Přemysl; Thierstein, Emily; Robles, River R.; Isele, Erik; Guo, Zhaoheng; Cesar, David; Alexander, Oliver; Beauvarlet, Sandra; Borne, Kurtis; Cheng, Xinxin; DiMauro, Louis F.; Duris, Joseph; Glownia, James M.; Graßl, Martin; Hockett, Paul; Hoffman, Matthias; Kamalov, Andrei; Larsen, Kirk A.; Li, Siqi; Li, Xiang; Lin, Ming-Fu; Obaid, Razib; Rosenberger, Philipp; Walter, Peter; Wolf, Thomas J. A.; Marangos, Jon P.; Kling, Matthias F.; Bucksbaum, Philip H.; Marinelli, Agostino; Cryan, James P.

doi:10.1103/PhysRevX.15.011008

Title: Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites

Journal Article · 15 January 2025 · Physical Review. X

DOI: https://doi.org/10.1103/PhysRevX.15.011008 · OSTI ID:2502130

;

; Franz, Paris L.;

;

; Isele, Erik;

;

; Alexander, Oliver;

; Borne, Kurtis; Cheng, Xinxin; DiMauro, Louis F.;

;

The detailed understanding of electronic coherence in quantum systems requires measurements on the attosecond timescale. Attosecond x-ray pulses enable the study of electronic coherence in core-excited molecular systems. Here we report on the coherent motion of electrons in the 1,1-difluoroethylene ion following ionization of the $K$ shell of the two nonequivalent carbon sites with a subfemtosecond x-ray pulse. Using the angular streaking technique to track the Auger-Meitner decay, we observe temporal modulations of the emission, indicating the electronic coherence of the core-excited ionic states, and extract a $6.5 \pm 0.8 fs$ average lifetime of the core-level vacancies. A quantum-mechanical model is employed to interpret the measurement, and we find the observed temporal modulations are independent of charge density oscillations. This work opens a new regime of coherent electronic motion, beyond charge migration, where electronic coherence manifests in the nonlocal quantum correlation between atomic sites while charge density oscillation is absent. Our results broaden the landscape of electronic coherence in molecular systems. Published by the American Physical Society 2025

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Research Organization:: SLAC

Sponsoring Organization:: USDOE Office of Science (SC); USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2502130

Journal Information:: Physical Review. X, Journal Name: Physical Review. X Journal Issue: 1 Vol. 15; ISSN PRXHAE; ISSN 2160-3308

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (48)

Core-electron binding energies for gaseous atoms and molecules Jolly, W. L.; Bomben, K. D.; Eyermann, C. J. Atomic Data and Nuclear Data Tables, Vol. 31, Issue 3 https://doi.org/10.1016/0092-640X(84)90011-1	journal	November 1984
30.4-nm He(II) Photoelectron spectra of organic molecules Bieri, Gerhard; Åsbrink, Leif; Von Niessen, Wolfgang Journal of Electron Spectroscopy and Related Phenomena, Vol. 23, Issue 2 https://doi.org/10.1016/0368-2048(81)80036-9	journal	January 1981
Ultrafast Charge Migration Following Valence Ionization of 4-Methylphenol: Jumping over the Aromatic Ring ^† Kuleff, Alexander I.; Lünnemann, Siegfried; Cederbaum, Lorenz S. The Journal of Physical Chemistry A, Vol. 114, Issue 33 https://doi.org/10.1021/jp101256n	journal	August 2010
Electronic Control of Initial Nuclear Dynamics Adjacent to a Conical Intersection Vacher, Morgane; Meisner, Jan; Mendive-Tapia, David The Journal of Physical Chemistry A, Vol. 119, Issue 21 https://doi.org/10.1021/jp509774t	journal	December 2014
Using coherence to enhance function in chemical and biophysical systems Scholes, Gregory D.; Fleming, Graham R.; Chen, Lin X. Nature, Vol. 543, Issue 7647 https://doi.org/10.1038/nature21425	journal	March 2017
Attosecond molecular dynamics: fact or fiction? Lépine, Franck; Ivanov, Misha Y.; Vrakking, Marc J. J. Nature Photonics, Vol. 8, Issue 3 https://doi.org/10.1038/nphoton.2014.25	journal	February 2014
Tunable isolated attosecond X-ray pulses with gigawatt peak power from a free-electron laser Duris, Joseph; Li, Siqi; Driver, Taran Nature Photonics https://doi.org/10.1038/s41566-019-0549-5	journal	December 2019
Experimental demonstration of attosecond pump–probe spectroscopy with an X-ray free-electron laser Guo, Zhaoheng; Driver, Taran; Beauvarlet, Sandra Nature Photonics, Vol. 18, Issue 7 https://doi.org/10.1038/s41566-024-01419-w	journal	April 2024
Terawatt-scale attosecond X-ray pulses from a cascaded superradiant free-electron laser Franz, Paris; Li, Siqi; Driver, Taran Nature Photonics, Vol. 18, Issue 7 https://doi.org/10.1038/s41566-024-01427-w	journal	May 2024
Clocking Auger electrons Haynes, D. C.; Wurzer, M.; Schletter, A. Nature Physics, Vol. 17, Issue 4 https://doi.org/10.1038/s41567-020-01111-0	journal	January 2021
Decoherence and revival in attosecond charge migration driven by non-adiabatic dynamics Matselyukh, Danylo T.; Despré, Victor; Golubev, Nikolay V. Nature Physics, Vol. 18, Issue 10 https://doi.org/10.1038/s41567-022-01690-0	journal	August 2022
Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine Månsson, Erik P.; Latini, Simone; Covito, Fabio Communications Chemistry, Vol. 4, Issue 1 https://doi.org/10.1038/s42004-021-00510-5	journal	May 2021
Onset of ionic coherence and ultrafast charge dynamics in attosecond molecular ionisation Ruberti, M. Physical Chemistry Chemical Physics, Vol. 21, Issue 32 https://doi.org/10.1039/C9CP03074C	journal	January 2019
Quantum coherence in molecular photoionization Ruberti, Marco; Patchkovskii, Serguei; Averbukh, Vitali Physical Chemistry Chemical Physics, Vol. 24, Issue 33 https://doi.org/10.1039/D2CP01562E	journal	January 2022
Core‐level binding‐energy shifts in small molecules Davis, D. W.; Banna, M. S.; Shirley, D. A. The Journal of Chemical Physics, Vol. 60, Issue 1 https://doi.org/10.1063/1.1680774	journal	January 1974
Two-dimensional charged particle image inversion using a polar basis function expansion Garcia, Gustavo A.; Nahon, Laurent; Powis, Ivan Review of Scientific Instruments, Vol. 75, Issue 11 https://doi.org/10.1063/1.1807578	journal	November 2004
A co-axial velocity map imaging spectrometer for electrons Li, S.; Champenois, E. G.; Coffee, R. AIP Advances, Vol. 8, Issue 11 https://doi.org/10.1063/1.5046192	journal	November 2018
Detecting coherent core-hole wave-packet dynamics in N ₂ by time- and angle-resolved inner-shell photoelectron spectroscopy Inhester, Ludger; Greenman, Loren; Rudenko, Artem The Journal of Chemical Physics, Vol. 151, Issue 5 https://doi.org/10.1063/1.5109867	journal	August 2019
Charge-induced chemical dynamics in glycine probed with time-resolved Auger electron spectroscopy Schwickert, David; Ruberti, Marco; Kolorenč, Přemysl Structural Dynamics, Vol. 9, Issue 6 https://doi.org/10.1063/4.0000165	journal	November 2022
Recent developments in the general atomic and molecular electronic structure system Barca, Giuseppe M. J.; Bertoni, Colleen; Carrington, Laura The Journal of Chemical Physics, Vol. 152, Issue 15 https://doi.org/10.1063/5.0005188	journal	April 2020
Fano-ADC(2,2) method for electronic decay rates Kolorenč, P.; Averbukh, V. The Journal of Chemical Physics, Vol. 152, Issue 21 https://doi.org/10.1063/5.0007912	journal	June 2020
Unified Theory of Auger Electron Emission Åberg, T. Physica Scripta, Vol. T41 https://doi.org/10.1088/0031-8949/1992/T41/013	journal	January 1992
The spectroscopy of the geminal ethylene difluoride (1,1-C ₂ H ₂ F ₂ ): the HeI, threshold and constant ion state photoelectron spectroscopies Locht, R.; Dehareng, D.; Leyh, B. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 45, Issue 11 https://doi.org/10.1088/0953-4075/45/11/115101	journal	May 2012
Angular streaking and sideband formation in rotating terahertz and far-infrared fields Kazansky, A. K.; Sazhina, I. P.; Nosik, V. L. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 50, Issue 10 https://doi.org/10.1088/1361-6455/aa69e9	journal	April 2017
Angular streaking of Auger-electrons by THz field Kazansky, A. K.; Sazhina, I. P.; Kabachnik, N. M. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 52, Issue 4 https://doi.org/10.1088/1361-6455/aafa33	journal	January 2019
Photon energy-resolved velocity map imaging from spectral domain ghost imaging Wang, Jun; Driver, Taran; Allum, Felix New Journal of Physics, Vol. 25, Issue 3 https://doi.org/10.1088/1367-2630/acc201	journal	March 2023
On the Angular Distribution in Nuclear Reactions and Coincidence Measurements Yang, C. N. Physical Review, Vol. 74, Issue 7 https://doi.org/10.1103/PhysRev.74.764	journal	October 1948
Absolute oscillator strengths from K -shell electron-energy-loss spectra of the fluoroethenes and 1,3-perfluorobutadiene McLaren, R.; Clark, S. A. C.; Ishii, I. Physical Review A, Vol. 36, Issue 4 https://doi.org/10.1103/PhysRevA.36.1683	journal	August 1987
Core Ionization Initiates Subfemtosecond Charge Migration in the Valence Shell of Molecules Kuleff, Alexander I.; Kryzhevoi, Nikolai V.; Pernpointner, Markus Physical Review Letters, Vol. 117, Issue 9 https://doi.org/10.1103/PhysRevLett.117.093002	journal	August 2016
On-the-Fly ab initio Semiclassical Evaluation of Electronic Coherences in Polyatomic Molecules Reveals a Simple Mechanism of Decoherence Golubev, Nikolay V.; Begušić, Tomislav; Vaníček, Jiří Physical Review Letters, Vol. 125, Issue 8 https://doi.org/10.1103/PhysRevLett.125.083001	journal	August 2020
Experimental Control of Quantum-Mechanical Entanglement in an Attosecond Pump-Probe Experiment Koll, Lisa-Marie; Maikowski, Laura; Drescher, Lorenz Physical Review Letters, Vol. 128, Issue 4 https://doi.org/10.1103/PhysRevLett.128.043201	journal	January 2022
Core-Hole Coherent Spectroscopy in Molecules Rodríguez-Cuenca, Emilio; Picón, Antonio; Oberli, Solène Physical Review Letters, Vol. 132, Issue 26 https://doi.org/10.1103/PhysRevLett.132.263202	journal	June 2024
Attosecond Streak Camera Itatani, J.; Quéré, F.; Yudin, G. L. Physical Review Letters, Vol. 88, Issue 17 https://doi.org/10.1103/PhysRevLett.88.173903	journal	April 2002
Quantum Theory of Attosecond XUV Pulse Measurement by Laser Dressed Photoionization Kitzler, Markus; Milosevic, Nenad; Scrinzi, Armin Physical Review Letters, Vol. 88, Issue 17 https://doi.org/10.1103/PhysRevLett.88.173904	journal	April 2002
Continuous-variable quantum state tomography of photoelectrons Laurell, H.; Finkelstein-Shapiro, D.; Dittel, C. Physical Review Research, Vol. 4, Issue 3 https://doi.org/10.1103/PhysRevResearch.4.033220	journal	September 2022
Quantifying Decoherence in Attosecond Metrology Bourassin-Bouchet, C.; Barreau, L.; Gruson, V. Physical Review X, Vol. 10, Issue 3 https://doi.org/10.1103/PhysRevX.10.031048	journal	August 2020
Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule Barillot, T.; Alexander, O.; Cooper, B. Physical Review X, Vol. 11, Issue 3 https://doi.org/10.1103/PhysRevX.11.031048	journal	September 2021
New tools for calibrating diffraction setups Kieffer, J.; Valls, V.; Blanc, N. Journal of Synchrotron Radiation, Vol. 27, Issue 2 https://doi.org/10.1107/S1600577520000776	journal	February 2020
Compact realization of all-attosecond pump-probe spectroscopy Kretschmar, Martin; Svirplys, Evaldas; Volkov, Mikhail Science Advances, Vol. 10, Issue 8 https://doi.org/10.1126/sciadv.adk9605	journal	February 2024
Generation of entanglement using a short-wavelength seeded free-electron laser Nandi, Saikat; Stenquist, Axel; Papoulia, Asimina Science Advances, Vol. 10, Issue 16 https://doi.org/10.1126/sciadv.ado0668	journal	April 2024
Ultrafast Probing of Core Hole Localization in N2 Schoffler, M. S.; Titze, J.; Petridis, N. Science, Vol. 320, Issue 5878 https://doi.org/10.1126/science.1154989	journal	May 2008
Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses Calegari, F.; Ayuso, D.; Trabattoni, A. Science, Vol. 346, Issue 6207 https://doi.org/10.1126/science.1254061	journal	October 2014
Attosecond coherent electron motion in Auger-Meitner decay Li, Siqi; Driver, Taran; Rosenberger, Philipp Science, Vol. 375, Issue 6578 https://doi.org/10.1126/science.abj2096	journal	January 2022
Attosecond-pump attosecond-probe x-ray spectroscopy of liquid water Li, Shuai; Lu, Lixin; Bhattacharyya, Swarnendu Science, Vol. 383, Issue 6687 https://doi.org/10.1126/science.adn6059	journal	March 2024
The Generalization of Student's Ratio Hotelling, Harold The Annals of Mathematical Statistics, Vol. 2, Issue 3 https://doi.org/10.1214/aoms/1177732979	journal	August 1931
Bootstrap Methods: Another Look at the Jackknife Efron, B. The Annals of Statistics, Vol. 7, Issue 1 https://doi.org/10.1214/aos/1176344552	journal	January 1979
Time-resolved pump-probe experiments at the LCLS Glownia, James M.; Cryan, J.; Andreasson, J. Optics Express, Vol. 18, Issue 17 https://doi.org/10.1364/OE.18.017620	journal	January 2010
Compact single-shot soft X-ray photon spectrometer for free-electron laser diagnostics Larsen, Kirk A.; Borne, Kurtis; Obaid, Razib Optics Express, Vol. 31, Issue 22 https://doi.org/10.1364/OE.502105	journal	October 2023