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Attosecond Photoelectron Metrology: from light to electrons

Ammitzböll, Mattias LU orcid (2025)
Abstract
The interaction between Extreme UltraViolet (XUV) Attosecond Pulse Trains (APT) and matter enables real-time investigation of electron dynamics on their natural time-scale. This is achieved by the addition of a weak InfraRed
(IR) field, which probes the ionization process. However, achieving the required temporal and spectral precision for such studies imposes stringent demands on the experimental setup. This thesis presents the development and implementation of a novel, ultra-stable, and flexible Mach-Zehnder interferometer for attosecond photoelectron metrology. The setup features active stabilization achieving < 13 attoseconds (RMS) temporal jitter and enables
photoelectron spectroscopy with an energy-resolution better than... (More)
The interaction between Extreme UltraViolet (XUV) Attosecond Pulse Trains (APT) and matter enables real-time investigation of electron dynamics on their natural time-scale. This is achieved by the addition of a weak InfraRed
(IR) field, which probes the ionization process. However, achieving the required temporal and spectral precision for such studies imposes stringent demands on the experimental setup. This thesis presents the development and implementation of a novel, ultra-stable, and flexible Mach-Zehnder interferometer for attosecond photoelectron metrology. The setup features active stabilization achieving < 13 attoseconds (RMS) temporal jitter and enables
photoelectron spectroscopy with an energy-resolution better than 80 meV for low-energy electrons.

Using this setup, two complementary experimental schemes have been employed. First, resonant two-photon ionization processes are investigated using the Reconstruction of Attosecond Beating By Interference of Twophoton
transitions (RABBIT) protocol. In helium, we measure phase variations as functions of angle and energy across the 3p, 4p, and 5p Rydberg series. Angular channel selection is achieved using cross-polarized pump and probe fields. In argon, we study the 3s−14p Fano resonance, resolving the spin-orbit (SO) splitting and observing phase variations that depend on the spectral width of the XUV pulse. These effects are interpreted by taking into
account the influence of final-state interactions.

Second, a new quantum state tomography protocol, KRAKEN (a Swedish acronym for Kvanttillstånds tomogRafi av AttoseKund ElektroNvågpaket), is introduced and experimentally demonstrated. KRAKEN enables
the reconstruction of the photoelectron density matrix, extending attosecond metrology to partially coherent or mixed quantum states. We show good agreement between KRAKEN measurements and theoretical predictions
for photoionization in helium and argon. The protocol is further extended with a poly-chromatic probe scheme (Poly-KRAKEN), which improves the efficiency and reduces the duration of the experimental measurement by exploiting both spectral and temporal domains simultaneously. (Less)
Please use this url to cite or link to this publication:
author
supervisor
opponent
  • Prof. Bourassin-Bouchet, Charles, Université Paris-Saclay, France.
organization
publishing date
type
Thesis
publication status
published
keywords
Attosecond, Photoionization, Quantum state tomography
pages
208 pages
publisher
Department of Physics, Lund University
defense location
Lecture Hall Rydbergsalen, Department of Physics, Professorsgatan 1, Faculty of Engineering LTH, Lund University, Lund.
defense date
2025-09-26 09:15:00
ISSN
0281-2762
0281-2762
ISBN
978-91-8104-636-6
978-91-8104-637-3
language
English
LU publication?
yes
id
f9b30ec9-cbad-4604-9d00-be7c49367159
date added to LUP
2025-09-02 11:20:04
date last changed
2025-09-05 03:33:27
@phdthesis{f9b30ec9-cbad-4604-9d00-be7c49367159,
  abstract     = {{The interaction between Extreme UltraViolet (XUV) Attosecond Pulse Trains (APT) and matter enables real-time investigation of electron dynamics on their natural time-scale. This is achieved by the addition of a weak InfraRed<br/>(IR) field, which probes the ionization process. However, achieving the required temporal and spectral precision for such studies imposes stringent demands on the experimental setup. This thesis presents the development and implementation of a novel, ultra-stable, and flexible Mach-Zehnder interferometer for attosecond photoelectron metrology. The setup features active stabilization achieving &lt; 13 attoseconds (RMS) temporal jitter and enables<br/>photoelectron spectroscopy with an energy-resolution better than 80 meV for low-energy electrons.<br/><br/>Using this setup, two complementary experimental schemes have been employed. First, resonant two-photon ionization processes are investigated using the Reconstruction of Attosecond Beating By Interference of Twophoton<br/>transitions (RABBIT) protocol. In helium, we measure phase variations as functions of angle and energy across the 3p, 4p, and 5p Rydberg series. Angular channel selection is achieved using cross-polarized pump and probe fields. In argon, we study the 3s−14p Fano resonance, resolving the spin-orbit (SO) splitting and observing phase variations that depend on the spectral width of the XUV pulse. These effects are interpreted by taking into<br/>account the influence of final-state interactions.<br/><br/>Second, a new quantum state tomography protocol, KRAKEN (a Swedish acronym for Kvanttillstånds tomogRafi av AttoseKund ElektroNvågpaket), is introduced and experimentally demonstrated. KRAKEN enables<br/>the reconstruction of the photoelectron density matrix, extending attosecond metrology to partially coherent or mixed quantum states. We show good agreement between KRAKEN measurements and theoretical predictions<br/>for photoionization in helium and argon. The protocol is further extended with a poly-chromatic probe scheme (Poly-KRAKEN), which improves the efficiency and reduces the duration of the experimental measurement by exploiting both spectral and temporal domains simultaneously.}},
  author       = {{Ammitzböll, Mattias}},
  isbn         = {{978-91-8104-636-6}},
  issn         = {{0281-2762}},
  keywords     = {{Attosecond; Photoionization; Quantum state tomography}},
  language     = {{eng}},
  month        = {{09}},
  publisher    = {{Department of Physics, Lund University}},
  school       = {{Lund University}},
  title        = {{Attosecond Photoelectron Metrology: from light to electrons}},
  url          = {{https://lup.lub.lu.se/search/files/226818180/Mattias_Ammitzb_ll_-WEBB.pdf}},
  year         = {{2025}},
}