David J. Rowe

Phosphorus-Doped Silicon Nanocrystals Exhibiting Mid-Infrared Localized Surface Plasmon Resonance

Localized surface plasmon resonances (LSPRs) enable tailoring of the optical response of nanomaterials through their free carrier concentration, morphology, and dielectric environment. Recent efforts to expand the spectral range of usable LSPR frequencies into the infrared successfully demonstrated LSPRs in doped semiconductor nanocrystals. Despite silicons importance for electronic and photonic applications, no LSPRs have been reported for doped silicon nanocrystals. Here we demonstrate doped silicon nanocrystals synthesized via a nonthermal plasma technique that exhibits tunable LSPRs in the energy range of 0.07-0.3 eV or mid-infrared wavenumbers of 600-2500 cm(-1).

Boron- and phosphorus-doped silicon germanium alloy nanocrystals—Nonthermal plasma synthesis and gas-phase thin film deposition

Alloyed silicon-germanium (SiGe) nanostructures are the topic of renewed research due to applications in modern optoelectronics and high-temperature thermoelectric materials. However, common techniques for producing nanostructured SiGe focus on bulk processing; therefore little is known of the physical properties of SiGe nanocrystals (NCs) synthesized from molecular precursors. In this letter, we synthesize and deposit thin films of doped SiGe NCs using a single, flow-through nonthermal plasma reactor and inertial impaction. Using x-ray and vibrational analysis, we show that the SiGe NC structure appears truly alloyed for Si1−xGex for 0.16 < x < 0.24, and quantify the atomic dopant incorporation within the SiGe NC films.

Influence of the surface termination on the light emission of crystalline silicon nanoparticles.

The light emission properties of silicon crystalline nanoparticles (SiNPs) have been investigated using steady-state and time-resolved photoluminescence measurements carried out at 12 K and at room temperature. To enable a comparative study of the role of surface terminal groups on the optical properties, we investigated SiNPs-H ensembles with the same mean NP diameter but differing on the surface termination, namely organic-functionalized with 1-dodecene (SiNPs-C12) and H-terminated (SiNPs-H). We show that although the spectral dependence of the light emission is rather unaffected by surface termination, characterized by a single broad band peaking at ∼1.64 eV, both the exciton recombination lifetimes and quantum yields display a pronounced dependence on the surface termination. Exciton lifetimes and quantum yields are found to be significantly lower in SiNPs-H compared SiNPs-C12. This difference is due to distinct non-radiative recombination probabilities resulting from inter-NP exciton migration, which in SiNPs-C12 is inhibited by the energy barriers imposed by the bulky surface groups. The surface groups of organic-terminated SiPs are responsible for the inhibition of inter-NP exciton transfer, yielding a higher quantum yield compared to SiNPs-H. The surface oxidation of SiNPs-C12 leads to the appearance of a phenomenon of an exciton transference from to the Si core to oxide-related states that contribute to light emission. These excitons recombine radiatively, explaining why the emission quantum of the organic-terminated SiNPs is the same after surface oxidation of SiNPs-C12.