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@PHDTHESIS{Hilgers:1032226,
author = {Hilgers, Robin},
othercontributors = {Blügel, Stefan and Wortmann, Daniel and Assent, Ira and
Wuttig, Matthias},
title = {{P}rediction of {M}agnetic {M}aterials for {E}nergy and
{I}nformation {C}ombining {D}ata-{A}nalytics and
{F}irst-{P}rinciples {T}heory},
volume = {288},
school = {RWTH Aachen University},
type = {Dissertation},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2024-06074},
isbn = {978-3-95806-795-0},
series = {Reihe Schlüsseltechnologien / Key Technologies},
pages = {xv, 215},
year = {2024},
note = {First published with RWTH Aachen University; Dissertation,
RWTH Aachen University, 2024},
abstract = {The essential role of magnetic materials in information
technology and the corresponding energy consumption of data
storage centers is crucially underestimated in modern
society. Saving energy resources is the societal challenge
of the 21st century. One of the leading scientific
objectives is finding ways to reduce energy consumption and
make resource usage more efficient. This thesis aims to shed
light on possible contributions of materials science
simulations towards a green IT transformation by providing
workflows and best-practice guidelines for high-throughput
materials screening tasks. An instance of such a screening
task is the search for magnetic materials for the next
generation of storage and data processing devices. However,
as the simulation process itself is time-consuming, this
thesis explores not only the material phase space but also
the application opportunities for data science and machine
learning (ML) in the material’s property prediction
process. As a prime example of a complex magnetic material
property, which is a limiting quantity when it comes to
methodological applicability, the critical temperature
𝑇𝑐 of existing magnetic simulation data of Heusler
alloys will be predicted using ML models. The capability and
limitations of these models will be analyzed and discussed.
It is shown that it is possible to extract physical
relations and knowledge from trained ML models without any
prior knowledge of the underlying physics and system
mechanics. Whether a Heusler compound has a 𝑇𝑐 high
enough to be relevant for an application in magnetic data
storage and processing devices could be predicted with over
90 $\%$ accuracy using lightweight ML model algorithms on
typical materials science data set sizes. Beyond that, the
phenomenon of near half-metallicity in Heusler compounds was
examined, including the successful ML-based prediction of
compounds displaying this property which were not known to
be nearly half-metallic before (L21 Co2HfIn, XA Mn2TaGe, and
L21 Co2ScSn). This particular study used existing
first-principles data of full and inverse Heusler
compound’s spin-polarized density of states, in order to
screen publicly available structural and magnetic ab initio
data for compounds exhibiting near half-metallic properties.
The relations learned by the underlying ML models are
discussed and compared to a known physical model. It was
determined that ML models have the capability to extend and
complement known physical models and relations when applied
to existing (and potentially imperfect) data. Finally,
large-scale high-throughput ultrathin film simulations of
3𝑑 transition metal layers on face-centered cubic noble
metal substrates were performed to understand the magnetic
properties of these magnetic multilayer films, which are
predicted to represent well-suited host platforms for room
temperature stable Skyrmions and hence are considered
candidate materials for spintronics-based storage and data
processing device applications. Tailored to high-throughput
ab initio workflows, a scalable method—that increased the
overall convergence rate from 64.8 $\%$ to 94.3 $\%$ and
exhibited the potential to save up to 17 $\%$ of the
computational time required, as well as to reduce the number
of needed ab initio relaxation steps to relax a multilayer
film system by up to 29 $\%$ in this systematic study, while
being flexible enough also to be applicable to future use
cases—using the integration of batch learning into
high-throughput workflows, was developed. The use,
restrictions, implementation, starting conditions, and
benefits of ML-based techniques and explainable artificial
intelligence are discussed in depth in this thesis.},
cin = {PGI-1 / IAS-8},
cid = {I:(DE-Juel1)PGI-1-20110106 / I:(DE-Juel1)IAS-8-20210421},
pnm = {632 - Materials – Quantum, Complex and Functional
Materials (POF4-632) / HDS LEE - Helmholtz School for Data
Science in Life, Earth and Energy (HDS LEE)
(HDS-LEE-20190612)},
pid = {G:(DE-HGF)POF4-632 / G:(DE-Juel1)HDS-LEE-20190612},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
urn = {urn:nbn:de:0001-2501160959561.990566976222},
doi = {10.34734/FZJ-2024-06074},
url = {https://juser.fz-juelich.de/record/1032226},
}