A Theoretical Introduction to Stimulated Resonant Inelastic X-ray Scattering up to the Quadrupole Order

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http://urn.fi/URN:NBN:fi:hulib-202009254143
Title: A Theoretical Introduction to Stimulated Resonant Inelastic X-ray Scattering up to the Quadrupole Order
Author: Rasola, Miika
Contributor: University of Helsinki, Faculty of Science
Publisher: Helsingin yliopisto
Date: 2020
Language: eng
URI: http://urn.fi/URN:NBN:fi:hulib-202009254143
http://hdl.handle.net/10138/319633
Thesis level: master's thesis
Degree program: Teoreettisten ja laskennallisten menetelmien maisteriohjelma
Master's Programme in Theoretical and Computational Methods
Magisterprogrammet i teoretiska och beräkningsmetoder
Specialisation: ei opintosuuntaa
no specialization
ingen studieinriktning
Discipline: none
Abstract: Resonant inelastic X-ray scattering (RIXS) is one of the most powerful synchrotron based methods for attaining information of the electronic structure of materials. Novel ultra-brilliant X-ray sources, X-ray free electron lasers (XFEL), offer new intriguing possibilities beyond the traditional synchrotron based techniques facilitating the transition of X-ray spectroscopic methods to the nonlinear intensity regime. Such nonlinear phenomena are well known in the optical energy range, less so in X-ray energies. The transition of RIXS to the nonlinear region could have significant impact on X-ray based materials research by enabling more accurate measurements of previously observed transitions, allowing the detection of weakly coupled transitions on dilute samples and possibly uncovering completely unforeseen information or working as a platform for novel intricate methods of the future. The nonlinear RIXS or stimulated RIXS (SRIXS) on XFEL has already been demonstrated in the simplest possible proof of concept case. In this work a comprehensive introduction to SRIXS is presented from a theoretical point of view starting from the very beginning, thus making it suitable for anyone with the basic understanding of quantum mechanics and spectroscopy. To start off, the principles of many body quantum mechanics are revised and the configuration interactions method for representing molecular states is introduced. No previous familiarity with X-ray matter interaction or RIXS is required as the molecular and interaction Hamiltonians are carefully derived, based on which a thorough analysis of the traditional RIXS theory is presented. In order to stay in touch with the real world, the basic experimental facts are recapped before moving on to SRIXS. First, an intuitive picture of the nonlinear process is presented shedding some light onto the term \textit{stimulated} while introducing basic terminology and some X-ray pulse schemes along with futuristic theoretical examples of SRIXS experiments. After this, a careful derivation of the Maxwell-Liouville-von Neumann theory up to quadrupole order is presented for the first time ever. Finally, the chapter is concluded with a short analysis of the experimental status quo on XFELs and some speculation on possible transition metal samples where SRIXS in its current state could be applied to observe quadrupole transitions advancing the field remarkably.
Subject: nonlinear X-ray spectroscopy
RIXS
Stimulated RIXS
XFEL
SASE


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