Monocrystalline materials are essential for optoelectronic devices such as solar cells, LEDs, lasers, and transistors to reach the highest performance. Advances in synthetic chemistry now allow for high quality monocrystalline nanomaterials to be grown at low temperature in solution for many materials; however, the realization of extended structures with control over the final 3D geometry still remains elusive. Here, a new paradigm is presented, which relies on epitaxy between monocrystalline nanocube building blocks. The nanocubes are assembled in a predefined pattern and then epitaxially connected at the atomic level by chemical growth in solution, to form monocrystalline nanopatterns on arbitrary substrates. As a first demonstration, it is shown that monocrystalline silver structures obtained with such a process have optical properties and conductivity comparable to single-crystalline silver. This flexible multiscale process may ultimately enable the implementation of monocrystalline materials in optoelectronic devices, raising performance to the ultimate limit.

Cathodoluminescence spectroscopy is a key analysis technique in nanophotonics research and technology, yet many aspects of its fundamental excitation mechanisms are not well understood on the single-electron and single-photon level. Here, we determine the cathodoluminescence emission statistics of InGaN quantum wells embedded in GaN under 6-30-keV electron excitation and find that the light emission rate varies strongly from electron to electron. Strong photon bunching is observed for the InGaN quantum well emission at 2.77 eV due to the generation of multiple quantum well excitations by a single primary electron. The bunching effect, measured by the g(2)(t) autocorrelation function, decreases with increasing beam current in the range 3-350 pA. Under pulsed excitation (p=2-100ns; 0.13-6 electrons per pulse), the bunching effect strongly increases. A model based on Monte Carlo simulations is developed that assumes a fraction γ of the primary electrons generates electron-hole pairs that create multiple photons in the quantum wells. At a fixed primary electron energy (10 keV) the model explains all g(2) measurements for different beam currents and pulse durations using a single value for γ=0.5. At lower energies, when electrons cause mostly near-surface excitations, γ is reduced (γ=0.01 at 6 keV), which is explained by the presence of a AlGaN barrier layer that inhibits carrier diffusion to the buried quantum wells. The combination of g(2) measurements in pulsed and continuous mode with spectral analysis provides a powerful tool to study optoelectronic properties and may find application in many other optically active systems and devices.