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Abstract The inherently weak chiroptical responses of natural materials limit their usage for controlling and enhancing chiral light-matter interactions. Recently, several nanostructures with subwavelength scale dimensions were demonstrated, mainly due to the advent of nanofabrication technologies, as a potential alternative to efficiently enhance chirality. However, the intrinsic lossy nature of metals and the inherent narrowband response of dielectric planar thin films or metasurface structures pose severe limitations toward the practical realization of broadband and tailorable chiral systems. Here, we tackle these problems by designing all-dielectric silicon-based L-shaped optical metamaterials based on tilted nanopillars that exhibit broadband and enhanced chiroptical response in transmission operation. We use an emerging bottom-up fabrication approach, named glancing angle deposition, to assemble these dielectric metamaterials on a wafer scale. The reported strong chirality and optical anisotropic properties are controllable in terms of both amplitude and operating frequency by simply varying the shape and dimensions of the nanopillars. The presented nanostructures can be used in a plethora of emerging nanophotonic applications, such as chiral sensors, polarization filters, and spin-locked nanowaveguides. 

Abstract Nanostructures represent a frontier where meticulous attention to the control and assessment of structural dimensions becomes a linchpin for their seamless integration into diverse technological applications. However, determining the critical dimensions and optical properties of nanostructures with precision still remains a challenging task. In this study, by using an integrative and comprehensive methodical series of studies, the evolution of the depolarization factors in the anisotropic Bruggeman effective medium approximation (AB‐EMA) is investigated. It is found that these anisotropic factors are extremely sensitive to the changes in critical dimensions of the nanostructure platforms. In order to perform a systematic characterization of these parameters, spatially coherent, highly‐ordered slanted nanocolumns are fabricated from zirconia, silicon, titanium, and permalloy on silicon substrates with varying column lengths using glancing angle deposition (GLAD). In tandem, broad‐spectral range Mueller matrix spectroscopic ellipsometry data, spanning from the near‐infrared to the vacuum UV (0.72–6.5 eV), is analyzed with a best‐match model approach based on the anisotropic Bruggeman effective medium theory. The anisotropic optical properties, including complex dielectric function, birefringence, and dichroism, are thereby extracted. Most notably, the research unveils a generalized, material‐independent inverse relationship between depolarization factors and column length. It is envisioned that the presented scaling rules will permit accurate prediction of optical properties of nanocolumnar thin films improving their integration and optimization for optoelectronic and photonic device applications. As an outlook, the highly porous nature and extreme birefringence properties of the fabricated columnar metamaterial platforms are further explored in the detection of nanoparticles from the cross‐polarized integrated spectral color variations. 

We investigate the time evolution of ZnO thin film growth in oxygen plasma-enhanced atomic layer deposition using in situ spectroscopic ellipsometry. The recently proposed dynamic-dual-box-model approach [Kilic et al., Sci. Rep. 10, 10392 (2020)] is used to analyze the spectroscopic data post-growth. With the help of this model, we explore the in-cycle surface modifications and reveal the repetitive layer-by-layer growth and surface roughness modification mechanisms during the ZnO ultrathin film deposition. The in situ complex-valued dielectric function of the amorphous ZnO thin film is also determined from the model analysis for photon energies of 1.7–4 eV. The dielectric function is analyzed using a critical point model approach providing parameters for bandgap energy, amplitude, and broadening in addition to the index of refraction and extinction coefficient. The dynamic-dual-box-model analysis reveals the initial nucleation phase where the surface roughness changes due to nucleation and island growth prior to film coalescence, which then lead to the surface conformal layer-by-layer growth with constant surface roughness. The thickness evolution is resolved with Angstrom-scale resolution vs time. We propose this method for fast development of growth recipes from real-time in situ data analysis. We also present and discuss results from x-ray diffraction, x-ray photoelectron spectroscopy, and atomic force microscopy to examine crystallographic, chemical, and morphological characteristics of the ZnO film.