Current nanostructure fabrication by etching is usually limited to planar structures as they are defined by a planar mask. The realization of three-dimensional (3D) nanostructures by etching requires technologies beyond planar masks. We present a method for fabricating a 3D mask that allows one to etch three-dimensional monolithic nanostructures using only CMOS-compatible processes. The mask is written in a hard-mask layer that is deposited on two adjacent inclined surfaces of a Si wafer. By projecting in a single step two different 2D patterns within one 3D mask on the two inclined surfaces, the mutual alignment between the patterns is ensured. Thereby after the mask pattern is defined, the etching of deep pores in two oblique directions yields a three-dimensional structure in Si. As a proof of concept we demonstrate 3D mask fabrication for three-dimensional diamond-like photonic band gap crystals in silicon. The fabricated crystals reveal a broad stop gap in optical reflectivity measurements. We propose how 3D nanostructures with five different Bravais lattices can be realized, namely cubic, tetragonal, orthorhombic, monoclinic and hexagonal, and demonstrate a mask for a 3D hexagonal crystal. We also demonstrate the mask for a diamond-structure crystal with a 3D array of cavities. In general, the 2D patterns on the different surfaces can be completely independently structured and still be in perfect mutual alignment. Indeed, we observe an alignment accuracy of better than 3.0 nm between the 2D mask patterns on the inclined surfaces, which permits one to etch well-defined monolithic 3D nanostructures.

The identification of a complete three-dimensional (3D) photonic band gap in real crystals always employs theoretical or numerical models that invoke idealized crystal structures. Thus, this approach is prone to false positives (gap wrongly assigned) or false negatives (gap missed). Therefore, we propose a purely experimental probe of the 3D photonic band gap that pertains to many different classes of photonic materials. We study position and polarization-resolved reflectivity spectra of 3D inverse woodpile structures that consist of two perpendicular nanopore arrays etched in silicon. We observe intense reflectivity peaks (R > 90%) typical of high-quality crystals with broad stopbands. We track the stopband width versus pore radius, which agrees much better with the predicted 3D photonic band gap than with a directional stop gap on account of the large numerical aperture used. A parametric plot of s-polarized versus p-polarized stopband width agrees very well with the 3D band gap and is model-free. This practical probe provides fast feedback on the advanced nanofabrication needed for 3D photonic crystals and stimulates practical applications of band gaps in 3D silicon nanophotonics and photonic integrated circuits, photovoltaics, cavity QED, and quantum information processing. arXiv:1909.01899v2 [physics.optics]

To investigate the performance of three-dimensional (3D) nanostructures, it is vital to study their internal structure with a methodology that keeps the device fully functional and ready for further integration. To this aim, we introduce here traceless X-ray tomography (TXT) that combines synchrotron X-ray holographic tomography with high X-ray photon energies (17 keV) in order to study nanostructures “as is” on massive silicon substrates. The combined strengths of TXT are a large total sample size to field-of-view ratio and a large penetration depth. We study exemplary 3D photonic band gap crystals made by CMOS-compatible means and obtain real space 3D density distributions with 55 nm spatial resolution. TXT identifies why nanostructures that look similar in electron microscopy have vastly different nanophotonic functionality: one “good” crystal with a broad photonic gap reveals 3D periodicity as designed; a second “bad” structure without a gap reveals a buried void, and a third “ugly” one without gap is shallow due to fabrication errors. Thus, TXT serves to nondestructively differentiate between the possible reasons of not finding the designed and expected performance and is therefore a powerful tool to critically assess 3D functional nanostructures.

It is a major outstanding goal in nanotechnology to precisely position functional nanoparticles, such as quantum dots, inside a three-dimensional (3D) nanostructure in order to realize innovative functions. Once the 3D positioning is performed, the challenge arises how to nondestructively verify where the nanoparticles reside in the 3D nanostructure. Here, we study 3D photonic band gap crystals made of Si that are infiltrated with PbS nanocrystal quantum dots. The nanocrystals are covalently bonded to polymer brush layers that are grafted to the Si–air interfaces inside the 3D nanostructure using surface-initiated atom transfer radical polymerization (SI-ATRP). The functionalized 3D nanostructures are probed by synchrotron X-ray fluorescence (SXRF) tomography that is performed at 17 keV photon energy to obtain large penetration depths and efficient excitation of the elements of interest. Spatial projection maps were obtained followed by tomographic reconstruction to obtain the 3D atom density distribution with 50 nm voxel size for all chemical elements probed: Cl, Cr, Cu, Ga, Br, and Pb. The quantum dots are found to be positioned inside the 3D nanostructure, and their positions correlate with the positions of elements characteristic of the polymer brush layer and the ATRP initiator. We conclude that X-ray fluorescence tomography is very well suited to nondestructively characterize 3D nanomaterials with photonic and other functionalities.

We study the optical reflectivity of real three-dimensional (3D) photonic band-gap crystals with increasing thickness. The crystals consist of GaAs plates with nanorod arrays that are assembled by an advanced stacking method into high-quality 3D woodpile structures. We observe intense and broad reflectivity peaks with stop bands that correspond to a broad gap in the photonic band structures. The maximum reflectivity quickly reaches high values, even for a few crystal layers. Remarkably, the bandwidth of the stop bands hardly decreases with increasing crystal thickness, in good agreement with finite-difference time domain (FDTD) simulations. This behavior differs remarkably from the large changes observed earlier in weakly interacting 3D photonic crystals. The nearly constant bandwidth and high reflectivity are rationalized by multiple Bragg interference that occurs in strongly interacting photonic band-gap crystals, whereby the incident light scatters from multiple reciprocal lattice vectors simultaneously, in particular, from oblique ones that are parallel to a longer crystal dimension and thus experience hardly any finite-size effects. Our insights have favorable consequences for the application of 3D photonic band-gap crystals, notably since even thin structures reveal the full band-gap functionality, including devices that shield quantum bits from vacuum fluctuations.