In recent years, imprint lithography has emerged as a promising patterning technique capable of high-speed and volume production. In this work, we report highly reproducible one-step printing of metal nanocubes. A dried film of monocrystalline silver cubes serves as the resist, and a soft polydimethylsiloxane stamp directly imprints the final pattern. The use of atomically smooth and sharp faceted nanocubes facilitates the printing of high-resolution and well-defined patterns with face-to-face alignment between adjacent cubes. It also permits digital control over the line width of patterns such as straight lines, curves, and complex junctions over an area of several square millimeters. Single-particle lattices as well as three-dimensional nanopatterns are also demonstrated with an aspect ratio up to 5 in the vertical direction. The high-fidelity nanocube patterning combined with the previously demonstrated epitaxial overgrowth can enable curved (single) crystals from solution at room temperature or highly efficient transparent conductors.

The use of colloidal self-assembly to form the complex multiscale patterns in many optoelectronic devices has been a long-standing dream of the nanoscience community. While great progress has been made using charged colloids in polar solvents, controlled assembly from nonpolar solvents is much more challenging. The major challenge is colloidal clustering caused by strong van der Waals (vdW) attraction between long-chain surface capping ligands passivating the surface of nanocrystals. Such clustering degrades ordering in packing during the self-assembly process. While ligand exchange to provide colloidal stability in polar phases is often an option, this is not the case for the exciting new class of halide perovskites due to the material’s solubility in essentially all polar solvents. Here, we report surface-functionalized self-assembly of luminescent CsPbBr 3 perovskite nanocubes by partially replacing long-chain oleyl groups (18 carbon chain) with short-chain thiocyanate (SCN – ). This enables the fabrication of ultrasmooth monolayer thin films of nanocubes with a root-mean-square (RMS) roughness of around 4 Å. This ultrasmooth large area self-assembled layer could act as high-efficiency optoelectronic devices like solar cells, light-emitting diodes (LEDs), transistors, etc. We correlate our experimental results with simulations, providing detailed predictions for lattice constants with chain conformations showing reduced free energy for cubes grafted with short-chain thiocyanate compared to long-chain oleyl groups, thus facilitating better self-assembly.

High-energy (1-100 keV) electrons can coherently couple to plasmonic and dielectric nanostructures creating cathodoluminescence (CL) of which the spectral features reveal details of the material's resonant modes at deepsubwavelength spatial resolution. While CL provides fundamental insight in optical modes, detecting its phase has remained elusive. Here, we introduce Fourier-transform CL holography as a method to determine the far-field phase distribution of scattered plasmonic fields. We record far-field interferences between a transition radiation reference field and surface plasmons scattered from plasmonic nanoholes, nanocubes and helical nano-apertures and reconstruct the angle-resolved phase distributions. From the derived fields we derive the relative strength and phase of induced scattering dipoles. The data show that each electron wavepacket collapses at the sample surface and coherently excites transition radiation and surface plasmon quanta. Fourier-transform CL holography opens up a new world of coherent light scattering and surface wave studies with nanoscale spatial resolution.

We investigate the nanoscale excitation of Ag nanocubes with coherent cathodoluminescence imaging spectroscopy (CL) to resolve the factors that determine the spatial resolution of CL as a deep-subwavelength imaging technique. The 10–30 keV electron beam coherently excites localized plasmons in 70 nm Ag cubes at 2.4 and 3.1 eV. The radiation from these plasmon modes is collected in the far-field together with the secondary electron intensity. CL line scans across the nanocubes show exponentially decaying tails away from the cube that reveal the evanescent coupling of the electron field to the resonant plasmon modes. The measured CL decay lengths range from 8 nm (10 keV) to 12 nm (30 keV) and differ from the calculated ones by only 1–3 nm. A statistical model of electron scattering inside the Ag nanocubes is developed to analyze the secondary electron images and compare them with the CL data. The Ag nanocube edges are derived from the CL line scans with a systematic error less than 3 nm. The data demonstrate that CL probes the electron-induced plasmon fields with nanometer accuracy.