Table Of ContentSpringer Theses
Recognizing Outstanding Ph.D. Research
Daniela Rupp
Ionization and
Plasma Dynamics
of Single Large
Xenon Clusters in
Superintense XUV
Pulses
Springer Theses
Recognizing Outstanding Ph.D. Research
Aims and Scope
The series “Springer Theses” brings together a selection of the very best Ph.D.
theses from around the world and across the physical sciences. Nominated and
endorsed by two recognized specialists, each published volume has been selected
foritsscientificexcellenceandthehighimpactofitscontentsforthepertinentfield
of research. For greater accessibility to non-specialists, the published versions
includeanextendedintroduction,aswellasaforewordbythestudent’ssupervisor
explainingthespecialrelevanceoftheworkforthefield.Asawhole,theserieswill
provide a valuable resource both for newcomers to the research fields described,
and for other scientists seeking detailed background information on special
questions. Finally, it provides an accredited documentation of the valuable
contributions made by today’s younger generation of scientists.
Theses are accepted into the series by invited nomination only
and must fulfill all of the following criteria
(cid:129) They must be written in good English.
(cid:129) ThetopicshouldfallwithintheconfinesofChemistry,Physics,EarthSciences,
Engineeringandrelatedinterdisciplinary fields such asMaterials,Nanoscience,
Chemical Engineering, Complex Systems and Biophysics.
(cid:129) The work reported in the thesis must represent a significant scientific advance.
(cid:129) Ifthethesisincludespreviouslypublishedmaterial,permissiontoreproducethis
must be gained from the respective copyright holder.
(cid:129) They must have been examined and passed during the 12 months prior to
nomination.
(cid:129) Each thesis should include a foreword by the supervisor outlining the signifi-
cance of its content.
(cid:129) The theses should have a clearly defined structure including an introduction
accessible to scientists not expert in that particular field.
More information about this series at http://www.springer.com/series/8790
Daniela Rupp
Ionization and
Plasma Dynamics of
Single Large Xenon Clusters
in Superintense XUV Pulses
Doctoral Thesis accepted by
Technical University, Berlin, Germany
123
Author Supervisor
Dr. Daniela Rupp Prof. ThomasMöller
Institut für OptikundAtomare Physik Institut für OptikundAtomare Physik
Technische UniversitätBerlin Technische UniversitätBerlin
Berlin Berlin
Germany Germany
ISSN 2190-5053 ISSN 2190-5061 (electronic)
SpringerTheses
ISBN978-3-319-28647-1 ISBN978-3-319-28649-5 (eBook)
DOI 10.1007/978-3-319-28649-5
LibraryofCongressControlNumber:2015959932
©SpringerInternationalPublishingSwitzerland2016
Thisworkissubjecttocopyright.AllrightsarereservedbythePublisher,whetherthewholeorpart
of the material is concerned, specifically the rights of translation, reprinting, reuse of illustrations,
recitation, broadcasting, reproduction on microfilms or in any other physical way, and transmission
orinformationstorageandretrieval,electronicadaptation,computersoftware,orbysimilarordissimilar
methodologynowknownorhereafterdeveloped.
The use of general descriptive names, registered names, trademarks, service marks, etc. in this
publicationdoesnotimply,evenintheabsenceofaspecificstatement,thatsuchnamesareexemptfrom
therelevantprotectivelawsandregulationsandthereforefreeforgeneraluse.
The publisher, the authors and the editors are safe to assume that the advice and information in this
book are believed to be true and accurate at the date of publication. Neither the publisher nor the
authorsortheeditorsgiveawarranty,expressorimplied,withrespecttothematerialcontainedhereinor
foranyerrorsoromissionsthatmayhavebeenmade.
Printedonacid-freepaper
ThisSpringerimprintispublishedbySpringerNature
TheregisteredcompanyisSpringerInternationalPublishingAGSwitzerland
It is structure that we look for whenever we try to understand anything.
All science is built upon this search
Linus Pauling in The place of chemistry in the integration of sciences.
Main currents in modern thought, 7, 110 (1950)
’
Supervisor s Foreword
MorethanahundredyearsagoWilhelmConradRöntgendiscoveredanewtypeof
radiation, named by him as X rays. Already within the first years after invention
theydevelopedintoanextremelypowerfultoolwhichchangedprofoundlyawhole
branch of science.
Thanks to their short wavelength and the ability to transmit through matter,
X rays have developed into one of the most important diagnostic tools in science,
medicineandtechnology.Incontrasttohighpoweropticallasers,whichnowadays
are used for example for welding, X-ray sources are usually assumed to be weak;
wedon’tseeandfeelXrays.Now,withtheadventofX-raylasersbasedonparticle
accelerators, so called free-electron-lasers (FELs), X-ray beams and pulses with
power densities of up to 1018 W/cm2 have become available, many orders of
magnitude more intense than needed for welding. Thanks to their high intensity
they can beused for dynamicstudies of nanoscaleobjects onthenatural timescale
of molecular vibration and electron motion. On the other hand the focused X rays
cantransferallkindsofmatterintoaplasmastatewithinfemtoseconds.Therefore,
in order to make use of them, it is necessary to gain an understanding of their
interaction with matter, which can deviate from that at low doses.
This brings me to the topic of Daniela’s thesis. She has been studying the
interactionbetweenintenseshortwavelengthlightpulsesemittedfromanFEL,the
FLASH facility in Hamburg, with matter. As samples she uses large rare gas
clusters which have been established as model systems for light–matter interaction
sincetheirsizecanbeeasilyvariedandthustheyallowfordistinguishingbetween
atomic and condensed matter effects. A key aspect of Daniela’s work is the
investigation of single, individual clusters. This allows her to circumvent the
problem of averaging over cluster size and power densities und thus to generate
very meaningful experimental data. She could show how those clusters grow and
studied how the clusters transform into highly excited nanoplasma upon
vii
viii Supervisor’sForeword
illumination with intense light pulses. These future shaping results are not only
important for imaging of gas-phase nanoparticles but also for other fields ranging
from material science to bio- and plasma physics.
Berlin, Germany Prof. Thomas Möller
December 2015
Abstract
Inthisworkfundamentalmechanismsoftheinteractionbetweenmatterandstrong
short-wavelengthpulseshavebeeninvestigated.Fortheexperimentsultrashortand
highly intense light pulses in the extreme-ultraviolet spectral regime from the
Free-Electron Laser in Hamburg FLASH have been used. They provide access to
new fields of experiments such as imaging of single nanometer-sized structures.
Rare gas clusters in the gas phase were investigated as ideal model systems for
light–matter interaction. From the scattering patterns of individual clusters, their
size and shape as well as the power density they were exposed to can be deter-
mined. But also light-induced changes in the clusters on a femtosecond timescale
are encoded in the scattered light. By combining single cluster imaging with the
coincident measurement of ion spectra, it is possible to sort the single shot data
based on the information in the scattering patterns. Thus, the averaging of cluster
size distributions and FEL power density profiles which has been apparent in
virtuallyallpreviousstudiesonraregasclusterscanbeovercome.Thewell-defined
conditionsinthesingleshotdatasortedforclustersizeyielduniqueinsightintothe
nanoplasma dynamics.
Large xenon clusters with diameters of hundreds of nanometers up to microns
could be produced and investigated for the first time. Their scattering patterns
reveal a complex, hailstone-like structure, yielding new insight into cluster mor-
phology and growth mechanisms.
The characteristic energy distributions of the ions determined from the
time-of-flightspectraofverylargesinglexenonclustersindicatethatonlyionsfrom
the outermost atomic monolayer of the cluster explode off. At the same time, the
highly efficient recombination in the remaining, quasi-neutral nanoplasma allows
for most atoms in the cluster to return back to neutral state.
From the corresponding scattering patterns intensity profiles can be extracted.
Mie theory yields insight into the optical properties of the clusters. In the intensity
profilesoflargeclusters,modulationsareobservedwhichindicatethedevelopment
ix
x Abstract
of a core–shell system within the nanoplasma. The core and a shell that is up to
50 nm thick differ in the optical properties, yielding insight into ultrafast
rearrangements of the electronic structure of the cluster.
TheoriginalversionofthisthesiswasexaminedonMay30,2013.Forthisbook
some revisions have been made, in particular recent citations have been updated.
