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Zhang et al. J. Mater. Inf. 2026, 6, 11 Page 3 of 17

thereby significantly reducing thermal conductivity [29,31] . On the other hand, K in ceramics predominantly
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depends on intrinsic factors, including bond strength, lattice rigidity, and phase stability, along with extrinsic
toughening mechanisms such as crack deflection, bridging, and stress-induced phase transformations [32-34] .
Controlled introduction of structural distortions and interfaces is known to activate these toughening
mechanisms, thereby improving fracture resistance in brittle oxide ceramics [23,24,35] . Despite these advances, a
comprehensive, systematic understanding of the individual contributions of different RE elements to the
delicate balance between low κ and high K in zirconate and tantalate systems remains elusive. Clarifying
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these relationships is essential for rationally optimizing and designing advanced TBC materials with tailored
thermomechanical properties.

Traditional experimental approaches to thermal barrier material discovery, typically grounded in empirical
trial-and-error methodologies , face significant limitations when applied to the vast compositional space of
[36]
RE oxides. The high cost, long cycle times and difficulty in isolating intrinsic structure–property
relationships hinder the ability of these methods to identify high-performance candidates efficiently [37-39] .
Moreover, most existing studies focus on individual compositions, lacking a systematic cross-comparison of
the full RE series. Addressing these challenges requires an integrated strategy that can both explore broad
chemical design spaces and uncover the underlying physical principles governing thermomechanical
performance . Advances in high-throughput computational methods combined with data-driven analyses
[40]
have emerged as powerful tools for the accelerated discovery and rational design of complex,
multicomponent materials [3,41,42] . By systematically computing material properties across broad chemical
spaces using first-principles calculations and subsequently analyzing the resulting large datasets, these
approaches enable the identification of key physical parameters and governing principles that link
atomic-scale features to macroscopic behavior . For instance, such approaches have identified correlations
[43]
between ionic charge and thermal conductivity in perovskite oxides and quantified the impact of severe
[44]
lattice distortion on K in ceramics by linking it to local bonding environments and macroscopic
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elastic/plastic properties [26,27] . In addition, they have revealed how atomic bonding distortions directly
influence phonon scattering and reduce thermal conductivity in RE oxides [13,27] .

In this work, the present work systematically investigates and compares structural stability, κ , K , and
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bonding characteristics in RE Zr O (pyrochlore/defect fluorite) and RE TaO (Weberite-type/defect fluorite)
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oxides across 17 RE elements (RE = Sc, Y, La ~ Lu). Although RE TaO and RE Zr O oxides differ in
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stoichiometry and crystal symmetry, both systems feature BO (B = Ta or Zr) octahedra and distorted RE
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coordination polyhedra derived from fluorite-related frameworks. These structural analogies, together with
shared controlling factors such as RE ionic radius (r ), bond distortion and electronic distribution, support
RE3+
a unified structure–property comparison across both families. By employing a high-throughput calculations
approach combined with data-driven analytics, this study generates an extensive dataset encompassing
formation energy (E form ), equilibrium volume (V 0), lattice parameters, bond characteristics, thermal
conductivities, and K . Subsequent correlation analyses and dimensionality reduction techniques identify
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key atomic-scale descriptors, including ionic radius, bond-length heterogeneity and valence state stability,
that critically govern thermomechanical properties. This study elucidates the fundamental mechanisms
dictating the trade-offs between low thermal conductivity and high K in these oxide families, thereby
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providing an essential data-driven foundation to guide the rational selection and design of next-generation
TBC materials. Moreover, the methodological framework demonstrated herein exemplifies how data-driven
approaches can significantly advance the fundamental understanding of structure–property relationships in
complex multicomponent ceramic systems, aligning closely with current objectives in high-impact materials
science research.