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Time-Frequency Analysis in Attosecond Spectroscopy

Isinger, Marcus LU (2018)
Abstract
This thesis deals with ultrafast dynamics of electronic processes in rare gas atoms. The processes we explore include photoemission, where we time the emission of electrons moving away from the atomic core following ionization by a photon; and auto-ionization, where the atom spontaneously releases an electron wave-packet following photo-excitation. These processes occur on an attosecond and femtosecond time scale, respectively.
The experimental results presented in this thesis have been obtained with the interferometric technique named RABITT, which involves ionizing a target with a train of attosecond pulses and "probing" the event with a weak IR pulse. The attosecond pulse train is generated by focusing... (More)
This thesis deals with ultrafast dynamics of electronic processes in rare gas atoms. The processes we explore include photoemission, where we time the emission of electrons moving away from the atomic core following ionization by a photon; and auto-ionization, where the atom spontaneously releases an electron wave-packet following photo-excitation. These processes occur on an attosecond and femtosecond time scale, respectively.
The experimental results presented in this thesis have been obtained with the interferometric technique named RABITT, which involves ionizing a target with a train of attosecond pulses and "probing" the event with a weak IR pulse. The attosecond pulse train is generated by focusing an intense laser pulse of femtosecond duration into a gaseous medium. Through a well-known process called high-order harmonic generation, a broadband spectrum of phase locked frequencies are generated in the medium, resulting in a train of pulses with attosecond duration. The special characteristics of this spectrum allows for a quantum interferometer to be conceived by overlapping the train with a weaker replica of the femtosecond IR pulse. Information of the dynamics of the ionization process is imprinted in the interference fringes obtained by varying the delay between the APT and the IR pulse with attosecond precision.

In the six papers that this thesis is based on, we investigate three different rare gas systems: helium, neon and argon. We are able to tell which electron, released out of two different shells of neon, escapes first from their parent atom, with a precision of 10 attoseconds or better. In helium, we are able to follow the creation of a wave-packet created by absorption of an attosecond pulse in the vicinity of a resonance and time its decay. We pave the way towards accessing all available information about a similar wave-packet creation in argon, through an angle detection technique with attosecond precision. We then perform a detailed examination of the interferometric technique used in all six papers (RABITT) and determine its limitations in terms of time resolution.

The realization of this thesis work involved generating, from a fundamental frequency corresponding to a photon energy of 1.55 eV, high-order harmonics with photon energies exceeding 100 eV. It also involved developing a more stable optical interferometer, optimizing a 2 meter long time-of-flight electron spectrometer, developing scripts for treating and analyzing the data retrieved with the RABITT technique and creating a new interface for acquiring data from the spectrometers. (Less)
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author
supervisor
opponent
  • Professor Pfeifer, Thomas, Max Planck Institute for Nuclear Physics, Germany
organization
publishing date
type
Thesis
publication status
published
subject
keywords
Attosecond, Spectroscopy, Time-Frequency, High-order harmonic generation, Rabitt, Interferometry
edition
1st
pages
229 pages
publisher
Division of Atomic Physics, Department of Physics, Faculty of Engineering, LTH, Lund University
defense location
Rydbergsalen, Fysicum, Professorsgatan 1, Lund University, Faculty of Engineering LTH
defense date
2019-01-25 09:00:00
ISBN
978-91-7753-892-9
978-91-7753-893-6
project
Time-resolved studies of atoms and molecules using attosecond pulses of high energies and advanced electron spectrometers,
language
English
LU publication?
yes
id
78beb226-ae10-48cd-8674-7a3d4f495854
date added to LUP
2018-12-17 15:56:10
date last changed
2019-01-02 10:02:09
@phdthesis{78beb226-ae10-48cd-8674-7a3d4f495854,
  abstract     = {{This thesis deals with ultrafast dynamics of electronic processes in rare gas atoms. The processes we explore include <i>photoemission</i>, where we time the emission of electrons moving away from the atomic core following ionization by a photon; and <i>auto-ionization</i>, where the atom spontaneously releases an electron wave-packet following photo-excitation. These processes occur on an attosecond and femtosecond time scale, respectively.<br/> The experimental results presented in this thesis have been obtained with the interferometric technique named <i>RABITT</i>, which involves ionizing a target with a train of attosecond pulses and "probing" the event with a weak <i>IR </i>pulse. The attosecond pulse train is generated by focusing an intense laser pulse of femtosecond duration into a gaseous medium. Through a well-known process called high-order harmonic generation, a broadband spectrum of phase locked frequencies are generated in the medium, resulting in a train of pulses with attosecond duration. The special characteristics of this spectrum allows for a quantum interferometer to be conceived by overlapping the train with a weaker replica of the femtosecond <i>IR </i>pulse. Information of the dynamics of the ionization process is imprinted in the interference fringes obtained by varying the delay between the <i>APT </i>and the <i>IR </i>pulse with attosecond precision.<br/><br/> In the six papers that this thesis is based on, we investigate three different rare gas systems: <i>helium, neon</i> and <i>argon</i>. We are able to tell which electron, released out of two different shells of neon, escapes first from their parent atom, with a precision of 10 attoseconds or better. In helium, we are able to follow the creation of a wave-packet created by absorption of an attosecond pulse in the vicinity of a resonance and time its decay. We pave the way towards accessing all available information about a similar wave-packet creation in argon, through an angle detection technique with attosecond precision. We then perform a detailed examination of the interferometric technique used in all six papers (<i>RABITT</i>) and determine its limitations in terms of time resolution.<br/><br/> The realization of this thesis work involved generating, from a fundamental frequency corresponding to a photon energy of 1.55 eV, high-order harmonics with photon energies exceeding 100 eV. It also involved developing a more stable optical interferometer, optimizing a 2 meter long time-of-flight electron spectrometer, developing scripts for treating and analyzing the data retrieved with the <i>RABITT </i>technique and creating a new interface for acquiring data from the spectrometers.}},
  author       = {{Isinger, Marcus}},
  isbn         = {{978-91-7753-892-9}},
  keywords     = {{Attosecond; Spectroscopy; Time-Frequency; High-order harmonic generation; Rabitt; Interferometry}},
  language     = {{eng}},
  publisher    = {{Division of Atomic Physics, Department of Physics, Faculty of Engineering, LTH, Lund University}},
  school       = {{Lund University}},
  title        = {{Time-Frequency Analysis in Attosecond Spectroscopy}},
  url          = {{https://lup.lub.lu.se/search/files/55590077/Avhandling_inkl._omslag_UTAN_ARTIKLAR.pdf}},
  year         = {{2018}},
}