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@PHDTHESIS{Heber:625263,
author = {Heber, Michael},
othercontributors = {Rossnagel, Kai and Kärtner, Franz},
title = {{S}tudies on ultrafast dynamics in correlated electron
systems with time- and angle-resolved photoemission
spectroscopy},
school = {University of Hamburg},
type = {Dissertation},
address = {Hamburg},
reportid = {PUBDB-2025-01079},
pages = {102},
year = {2024},
note = {Dissertation, University of Hamburg, 2024},
abstract = {Angle-resolved photoemission spectroscopy (ARPES) is a
potent technique for studying the electronic band structure
of condensed matter. The use of the pump-probe technique
extends ARPES into the time domain, allowing the electron
dynamics to be observed on an ultrafast timescale. High
harmonic generation (HHG) sources and free electron lasers
(FELs) generate extreme ultraviolet (EUV) or X-ray pulses
that have a temporal width of 100 fs or less. HHG converts
optical or infrared laser radiation into the EUV, whereas in
the FEL, relativistic electrons emit coherent synchrotron
radiation in an alternating magnetic field. The FEL FLASH
(Free electron LASer Hamburg) is a high-repetition-rate FEL
that extends the photon energy into the soft X-ray range.
Electron spectrometers with high detection efficiency are
essential because the repetition rate of the pump and probe
source frequently constrains time-resolved (tr-)ARPES
measurements. Therefore, time-of-flight photoelectron
spectrometers with a 3D detection scheme are best suited for
this purpose. The tr-ARPES setups, the wide-angle
photoelectron spectrometer WESPE and the momentum microscope
HEXTOF, are based on the time-of-flight technique and
designed for the plane grating beamline PG2 at FLASH. In
this thesis I present the time resolved studies on three
different quantum materials.Frequently, the momentum
microscope is also paired with a HHG source. In the first
scientific application of this thesis, a sample of pristine
graphene on iridium(111) is investigated to evaluate the
potential of this laboratory-based experimental setup. The
results demonstrate a sub-100 fs time resolution and a field
of view larger than the first Brillouin zone. The
multispectral nature of the HHG spectrum enables measurement
of kz-dependent ARPES signal which were used to reconstruct
a tomogram of the Fermi surface of iridium.The Dirac cone is
not a unique feature of Graphene. It also appears as a
characteristic feature of the surface state of topological
insulators, which were investigated in the second experiment
chapter. Despite being insulating in the bulk, topological
insulators possess an intriguing conducting topological
state at the surface. The topological insulator bismuth
selenide (Bi2Se3) was investigated using the HEXTOF setup.
Tr-ARPES data was obtained for the topological surface
state, and tr-XPS data was obtained for the Bi 4d and Se 3d
core levels. Our study aimed to explore the electron
dynamics at high pump fluences within the topological
surface state, as well as to examine the robustness of the
state itself. Even at fluences that result in surface
ablation, our experiments have demonstrated that the
topological surface state remains intact, and its dynamics
maintain their characteristics.The last scientific case in
this thesis deals with a heavy fermionic system, where 4f
and 5f electrons interact with conduction band electrons,
forming quasi-particles in the band structure. Thulium
selenide (TmSe) is a heavy fermionic system with mixed
valence character on the Tm site. The Tm 4f electrons
hybridize with the electrons in the conduction band,
resulting in the formation of a heavy fermion multiplet in
the PES spectra near the Fermi level. When TmSe is doped
with tellurium, the lattice expands, causing a transition
from the mixed valence state to a predominantly divalent
state. The dynamics of the 3H6 multiplet peak shows a
dependence on the Te concentration. In the mixed valence
state, a delayed long-lasting dynamic is observed.This
thesis not only demonstrates how versatile and powerful
tr-ARPES is for the study of condensed/quantum matter in
general, but also explicitly shows that recent developments
in momentum microscope instrumentation can satisfy a wide
range of needs, paving the way to a “one fits
all”-design which includes besides time and angle also
spin resolution.},
cin = {U HH / DOOR ; HAS-User / $XFEL_E2_SXP$},
cid = {$I:(DE-H253)U_HH-20120814$ / I:(DE-H253)HAS-User-20120731 /
$I:(DE-H253)XFEL_E2_SXP-20240106$},
pnm = {6G2 - FLASH (DESY) (POF4-6G2) / 6G3 - PETRA III (DESY)
(POF4-6G3) / PHGS, VH-GS-500 - PIER Helmholtz Graduate
School $(2015_IFV-VH-GS-500)$},
pid = {G:(DE-HGF)POF4-6G2 / G:(DE-HGF)POF4-6G3 /
$G:(DE-HGF)2015_IFV-VH-GS-500$},
experiment = {EXP:(DE-H253)F-PG2-20150101 / EXP:(DE-H253)P-P04-20150101},
typ = {PUB:(DE-HGF)11},
urn = {urn:nbn:de:gbv:18-ediss-122082},
doi = {10.3204/PUBDB-2025-01079},
url = {https://bib-pubdb1.desy.de/record/625263},
}