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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 demonstrate calibration and operation of a Mueller matrix imaging microscope using dual continuously rotating anisotropic mirrors for polarization state generation and analysis. The mirrors contain highly spatially coherent nanostructure slanted columnar titanium thin films deposited onto optically thick titanium layers on quartz substrates. The first mirror acts as polarization state image generator and the second mirror acts as polarization state image detector. The instrument is calibrated using samples consisting of laterally homogeneous properties such as straight-through-air, a clear aperture linear polarizer, and a clear aperture linear retarder waveplate. Mueller matrix images are determined for spatially varying anisotropic samples consisting of a commercially available (Thorlabs) birefringent resolution target and a spatially patterned titanium slanted columnar thin film deposited onto a glass substrate. Calibration and operation are demonstrated at a single wavelength (530 nm) only, while, in principle, the instrument can operate regardless of wavelength. We refer to this imaging ellipsometry configuration as rotating-anisotropic-mirror-sample-rotating-anisotropic-mirror ellipsometry (RAM-S-RAM-E). 

We demonstrate calibration and operation of a single wavelength (660 nm) Mueller matrix ellipsometer in normal transmission configuration using dual continuously rotating anisotropic mirrors. The mirrors contain highly spatially coherent nanostructure slanted columnar titanium thin films deposited onto optically thick gold layers on glass substrates. Upon rotation around the mirror normal axis, sufficient modulation of the Stokes parameters of light reflected at oblique angle of incidence is achieved. Thereby, the mirrors can be used as a polarization state generator and polarization state analyzer in a generalized ellipsometry instrument. A Fourier expansion approach is found sufficient to render and calibrate the effects of the mirror rotations onto the polarized light train within the ellipsometer. The Mueller matrix elements of a set of anisotropic samples consisting of a linear polarizer and a linear retarder are measured and compared with model data, and very good agreement is observed. 

Abstract Designing broadband enhanced chirality is of strong interest to the emerging fields of chiral chemistry and sensing, or to control the spin orbital momentum of photons in recently introduced nanophotonic chiral quantum and classical optical applications. However, chiral light‐matter interactions have an extremely weak nature, are difficult to control and enhance, and cannot be made tunable or broadband. In addition, planar ultrathin nanophotonic structures to achieve strong, broadband, and tunable chirality at the technologically important visible to ultraviolet spectrum still remain elusive. Here, these important problems are tackled by experimentally demonstrating and theoretically verifying spectrally tunable, extremely large, and broadband chiroptical response by nanohelical metamaterials. The reported new designs of all‐dielectric and dielectric‐metallic (hybrid) plasmonic metamaterials permit the largest and broadest ever measured chiral Kuhn's dissymmetry factor achieved by a large‐scale nanophotonic structure. In addition, the strong circular dichroism of the presented bottom‐up fabricated optical metamaterials can be tuned by varying their dimensions and proportions between their dielectric and plasmonic helical subsections. The currently demonstrated ultrathin optical metamaterials are expected to provide a substantial boost to the developing field of chiroptics leading to significantly enhanced and broadband chiral light‐matter interactions at the nanoscale.