Spontaneous Relaxation of Heteroepitaxial Thin Films by van der Waals-Like Bonding on Te-Terminated Sapphire Substrates.

Here the novel direct heteroepitaxial growth method of a 3D heteroepitaxial system is demonstrated on a 3D substrate, CdTe (111)/Al2 O3 (0001), which forms a spontaneous vdW-like bond at the interface, instead of the two 3D crystals being strongly bound. Despite a large lattice mismatch, the thin films are single crystals and maintain high quality due the compliance of the interface which accommodates strain. This weak bonding interface is accomplished by the self-assembly of a pseudomorphic chalcogenide layer on the sapphire surface during growth. Since the vdW-like interface forms spontaneously in situ during growth, it is easily scalable to large wafer sizes, without the need to layer transfer 2D materials onto the growth substrate for remote epitaxy. Further, the weak adhesion of the films on the substrates allow for epitaxial film transfer to a variety of other substrates, leaving the original growth substrate for future reuse. This type of 3D/3D vdW-like interface is exploitable as a compliant interlayer for additional epitaxy, and may even be observable directly in other material systems grown on complex oxides, allowing for the production of large area high quality freestanding and layer transferred epitaxial devices for material systems not currently possible by conventional processing techniques.

The dependence of the plasmon field induced nonradiative electronic relaxation mechanisms on the gold shell thickness in vertically aligned CdTe-Au core-shell nanorods.

The dependence of the plasmon field enhancement of the nonradiative relaxation rate of the band gap electrons in vertically aligned CdTe-Au core-shell nanorods on the plasmonic gold nanoshell thickness is examined. Increasing the thickness of the gold nanoshell from 15 to 26 nm is found to change the decay curve from being nonexponential and anisotropic to one that is fully exponential and isotropic (i.e., independent of the nanorod orientation with respect to the exciting light polarization direction). Analysis of the kinetics of the possible electronic relaxation enhancement mechanisms is carried out, and DDA simulated properties of the induced plasmonic field of the thin and thick gold nanoshells are determined. On the basis of the conclusions of these treatments and the experimental results, it is concluded that by increasing the nanoshell thickness the relaxation processes evolve from multiple enhancement mechanisms, dominated by highly anisotropic Auger processes, to mechanism(s) involving first-order excited electron ejection process(es). The former is shown to give rise to nonexponential anisotropic decays in the dipolar plasmon field of the thin nanoshell, while the latter exhibits an exponential isotropic decay in the unpolarized plasmonic field of the thick nanoshell.

Epitaxially driven formation of intricate supported gold nanostructures on a lattice-matched oxide substrate.

A new class of gold nanostructures has been fabricated on the (100), (111), and (110) surfaces of lattice-matched MgAl(2)O(4) substrates. The nanostructures were fabricated through a synthesis route where a thin gold film dewets, liquefies, and then slowly self-assembles. The supported nanostructures are intricately shaped, crystalline, and epitaxially aligned. Simulations based on a continuum elastic theory indicate that the self-assembly is driven by strained epitaxy and minimization of the surface free energy.

Exciton lifetime tuning by changing the plasmon field orientation with respect to the exciton transition moment direction: CdTe-Au core-shell nanorods.

We studied the anisotropy of the influence of plasmonic fields, arising from the optical excitation of a gold nanoshell plasmon absorption at 770 nm, on the lifetime of the bandgap state of the CdTe core in vertically aligned CdTe-Au core-shell nanorods. The previously observed decrease in the lifetime was studied as a function of the tilt angle between the long axis of the nanorod and the electric field polarization direction of the plasmon inducing exciting light. It is observed that the strongest enhancement to the exciton relaxation rate occurs when the two axes are parallel to one another. These results are discussed in terms of the coupling between the exciton transition moment of the CdTe rod and the electric field polarization direction of the gold nanoshell plasmon at 770 nm, which was determined from theoretical modeling based on the discrete dipole approximation.

Plasmon field effects on the nonradiative relaxation of hot electrons in an electronically quantized system: CdTe-Au core-shell nanowires.

The intense electromagnetic fields of plasmonic nanoparticles, resulting from the excitation of their localized surface plasmon oscillations, are known to enhance radiative processes. Their effect on the nonradiative electronic processes, however, is not as well-documented. Here, we report on the enhancement of the nonradiative electronic relaxation rates in CdTe nanowires upon the addition of a thin gold nanoshell, especially at excitation energies overlapping with those of the surface plasmon oscillations. Some possible mechanisms by which localized surface plasmon fields can enhance nonradiative relaxation processes of any quantized electronic excitations are proposed.