Nanoscale-Thick Thin Films of High-Density HfO 2 for Bulk-like Optical Responses
Abstract
The high refractive index, broadband transparency, and low spectral absorption of HfO 2 (hafnia) make it a suitable choice for thermally stable nanoscale optical filters, UV mirrors, and antireflection coatings. However, achieving dense thin films of HfO 2 with bulk-like optical properties has been a challenge due to differences in film stoichiometric and spatial uniformity at nanoscale thicknesses. Here, we assess HfO 2 thin films (i.e., <200 nm thicknesses) prepared using pulsed laser deposition (PLD) at different substrate temperatures (20–675 °C) and the associated chemical, structural, and optical properties are reported. X-ray diffraction analysis reveals that nanoscale-thick thin films of HfO 2 deposited at an ambient substrate temperature (20 °C) using PLD are amorphous with embedded nanocrystallites, whereas films deposited on heated substrates are polycrystalline monoclinic HfO 2 . For the films deposited on heated substrates, further analysis shows that the nanocrystalline phase does not change with increasing substrate temperatures; however, the texture of the crystalline orientation changes to favor ( 1 11) at 300–675 °C from the initial (002) orientation at ambient substrate temperature. Such differences in nanoscale-thick thin-film HfO 2 PLD process-dependent amorphousness, crystallinity, and surface textures discussed here exhibit minimal influence on the resulting broadband optical properties (250 nm–30 μm). Furthermore, we show that the complex refractive index of high-density nanoscale-thick thin-film HfO 2 prepared at an ambient substrate temperature using PLD resembles that of bulk HfO 2 responses. The achievement of fully stoichiometric, high-density, thin-film HfO 2 from PLD is expected to further enable thermally robust nanoscale photonic device integration involving low-dimensional high-performance optical and optoelectronic applications.
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HfO2 has a high refractive index, wide transparency from the UV to mid-IR region (bandgap larger than 5.5 eV), and significant thermal and chemical stability.
“Its high refractive index, wide transparency from UV to mid-IR region (due to its bandgap, which is larger than 5.5 eV [64]) and significant thermal and chemical stability [65] propelled HfO2 for the manufacture of antireflective coatings [66] and highly reflective mirrors [67], but also in other applications, such as memory devices [68], among others [69,70].”
From Metal Oxide Thin Films for Advanced Photonic Applications (2026) · cites this paper as [65]
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Metal Oxide Thin Films for Advanced Photonic Applications
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“…wide transparency from UV to mid-IR region (due to its bandgap, which is larger than 5.5 eV [64]) and significant thermal and chemical stability [65] propelled HfO 2 for the manufacture of antireflective coatings [66] and highly reflective mirrors [67], but also in other applications, such as…”
Influential
- Authors
- Sun, L., Jones, J. G., Grant, J. T., Murphy, N. R., Ramana, C. V., Eyink, K. G., Vernon, J. P., & Stevenson, P. R.
- Affiliations
- United States Air Force Research Laboratory (US)
- The University of Texas at El Paso (US)
- Corresponding author
- Stevenson, Peter R.
- ORCID
- Venue
- ACS Applied Nano Materials
- Publisher
- American Chemical Society (ACS)
- Published
- 2021-09-30
- Volume
- 4
- Issue
- 10
- Pages
- 10836-10844
- ISSN
- 2574-0970 (ISSN-L)
- OpenAlex
- W3203088458
- Cited by
- 13
- References
- 54
- Citations by year
- 2026: 2 · 2025: 1 · 2024: 2 · 2023: 3 · 2022: 5
- FWCI
- 0.72
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- Locations
- ACS Applied Nano Materials (publishedVersion)
- Funders
- Air Force Research Laboratory (FA8650-16-D-5404-0013)
- Air Force Office of Scientific Research (FA9550-18-1-0387)
- NSF-PREM (DMR-1827745)
- Topics
- Physical Sciences › Materials Science › Surfaces, Coatings and Films › Optical Coatings and Gratings
- Physical Sciences › Materials Science › Polymers and Plastics › Transition Metal Oxide Nanomaterials
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Semiconductor materials and devices
- Keywords
- hafnium oxide, HfO2 thin films, pulsed laser deposition, substrate temperature, monoclinic HfO2, complex refractive index, stoichiometric films, optical filters, antireflection coatings
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