Nanophotonic materials offer spectral and directional control over thermal emission, but in high-temperature oxidizing environments, their stability remains low. This limits their applications in technologies such as solid-state energy conversion and thermal barrier coatings. Here we show an epitaxial heterostructure of perovskite BaZr0.5Hf0.5O3 (BZHO) and rocksalt MgO that is stable up to 1,100 °C in air. The heterostructure exhibits coherent atomic registry and clearly separated refractive-index-mismatched layers after prolonged exposure to this extreme environment. The immiscibility of the two materials is corroborated by the high formation energy of substitutional defects from density functional theory calculations. The epitaxy of immiscible refractory oxides is, therefore, an effective method to avoid prevalent thermal instabilities in nanophotonic materials, such as grain-growth degradation, interlayer mixing and oxidation. As a functional example, a BZHO/MgO photonic crystal is implemented as a filter to suppress long-wavelength thermal emission from the leading bulk selective emitter and effectively raise its cutoff energy by 20%, which can produce a corresponding gain in the efficiency of mobile thermophotovoltaic systems. Beyond BZHO/MgO, computational screening shows that hundreds of potential cubic oxide pairs fit the design principles of immiscible refractory photonics. Extending the concept to other material systems could enable further breakthroughs in a wide range of photonic and energy conversion applications.
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Analysis code for raw data is available via Deep Blue Data at https://doi.org/10.7302/bvre-r767. Our open-source code to find lattice-matched immiscible oxides is available via GitHub at https://github.com/sean-mcsherry/lattice_matching_oxides.
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We acknowledge financial support from the Department of Defense, Defense Advanced Research Projects Agency, under grant no. HR00112190005. The views, opinions and/or findings expressed are those of the authors and should not be interpreted as representing the official views or policies of the Department of Defense or the US Government. S.M. acknowledges support by the National Science Foundation (NSF) Graduate Research Fellowship under grant no. NSF DGE 1256260 and the Rackham Predoctoral Fellowship. M.W. and J.T.H. acknowledge financial support from the University of Michigan College of Engineering and technical support from the Michigan Center for Materials Characterization. The defect calculations used resources of the National Energy Research Scientific Computing (NERSC) Center, a Department of Energy Office of Science User Facility, supported under contract no. DEAC0205CH11231. The optical and electrical calculations were performed on Rivanna, the high-performance computing system at the University of Virginia. We offer special thanks to B. Lezzi and M. Shtein for access to the ellipsometry equipment. We also thank W. Carter, R. Hovden and A. Hunter for helpful discussions and feedback.
The authors declare no competing interests.
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McSherry, S., Webb, M., Kaufman, J. et al. Nanophotonic control of thermal emission under extreme temperatures in air. Nat. Nanotechnol. 17, 1104–1110 (2022). https://doi.org/10.1038/s41565-022-01205-1