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@PHDTHESIS{Tesch:1026466,
      author       = {Tesch, Rebekka},
      title        = {{S}tructure and properties of electrochemical interfaces
                      from first principles simulations},
      volume       = {629},
      school       = {RWTH Aachen University},
      type         = {Dissertation},
      address      = {Jülich},
      publisher    = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
      reportid     = {FZJ-2024-03410},
      isbn         = {978-3-95806-753-0},
      series       = {Schriften des Forschungszentrums Jülich Reihe Energie $\&$
                      Umwelt / Energy $\&$ Environment},
      pages        = {xvi, 161},
      year         = {2024},
      note         = {Dissertation, RWTH Aachen University, 2024},
      abstract     = {The transition to a sustainable energy system relies on the
                      availability of high-performing and costeffective energy
                      storage and conversion devices, such as batteries, fuel
                      cells and electrolysers. The performance of these devices is
                      directly related to the properties of the employed
                      electrocatalyst materials. In order to develop
                      electrochemical devices that can respond to societal,
                      economical and environmental needs, catalyst materials must
                      be improved in terms of activity, long-term stability and
                      production cost. This requires significant progress in the
                      fundamental understanding of relevant electrochemical
                      processes. The majority of electrochemical processes take
                      place at the interface between a solid electrode and a
                      liquid electrolyte. Atomic-scale modeling is a powerful tool
                      that can yield important information on structural,
                      electronic and electrostatic properties of the interface.
                      However, self-consistently modeling the two parts of the
                      interface as well as their non-linear coupling is very
                      challenging. Existing computational methods are limited in
                      terms of accuracy and/or efficiency. The aim of this thesis
                      is to address some of the limitations of existing methods
                      and provide accurate computational methodologies for a
                      realistic description of the local reaction conditions at
                      the electrochemical interface and of the electrocatalytic
                      processes. We focus on two aspects: (1) the efficient and
                      accurate computation of the electronic structure of
                      materials with strongly correlated electrons, such as d- or
                      f -electrons, and (2) the self-consistentdescription of
                      phenomena at electrochemical interfaces, including the
                      effects of electrolyte species and electrode potential. For
                      these purposes, two methods have been studied in detail in
                      this thesis: (1) the DFT+U approach for the description of
                      strongly correlated electrons and (2) the recently developed
                      effective screening medium reference interaction site method
                      (ESM-RISM) for the description of electrochemical
                      interfaces. The conducted research enabled us to establish
                      an improved DFT+U approach for the computation of the
                      electronic structure of electrode materials. In this
                      methodology, we derive the Hubbard U parameter from an
                      existing first principles-based linear response method.
                      Additionally, we use Wannier projectors instead of standard
                      atomic orbitals projectors for more accurate counting of
                      orbital occupations. The resulting scheme provides an
                      improved electronic structure description of various d- and
                      f -materials and allows, for example, for enhanced studies
                      of catalytically active sites in oxide electrocatalysts.
                      These results indicate that a correct electronic structure
                      description is an important precondition for an accurate
                      computational modeling of electrochemical interfaces.},
      cin          = {IEK-13},
      cid          = {I:(DE-Juel1)IEK-13-20190226},
      pnm          = {899 - ohne Topic (POF4-899)},
      pid          = {G:(DE-HGF)POF4-899},
      typ          = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
      doi          = {10.34734/FZJ-2024-03410},
      url          = {https://juser.fz-juelich.de/record/1026466},
}