We study the effect of the zero- to one-dimensional (1D) transformation on multiparticle Auger recombination using a series of elongated semiconductor nanocrystals (quantum rods). We observe a transition from the three- to two-particle recombination process as the nanocrystal aspect ratio is increased. This transition indicates that in the 1D confinement limit, Auger decay is dominated by Coulomb interactions between 1D excitons that recombine in a bimolecular fashion. One consequence of this effect is strongly reduced decay rates of higher multiparticle states that lead to increased optical-gain lifetimes and efficient light amplification due to involvement of excited electronic states.
We perform side-by-side comparison of optical gain properties of spherical and elongated nanocrystals (quantum dots and quantum rods, respectively). This comparison indicates that elongated nanoparticles provide several features beneficial for lasing applications, such as enhanced absorption cross sections (and hence reduced lasing threshold and improved photostability), increased optical gain lifetime, and extended optical gain spectral range through the use of transitions that involve both ground and excited electronic states.
For advanced device applications, increasing the compositional abruptness of axial heterostructured and modulation doped nanowires is critical for optimizing performance. For nanowires grown from metal catalysts, the transition region width is dictated by the solute solubility within the catalyst. For example, as a result of the relatively high solubility of Si and Ge in liquid Au for vapor-liquid-solid (VLS) grown nanowires, the transition region width between an axial Si-Ge heterojunction is typically on the order of the nanowire diameter. When the solute solubility in the catalyst is lowered, the heterojunction width can be made sharper. Here we show for the first time the systematic increase in interface sharpness between axial Ge-Si heterojunction nanowires grown by the VLS growth method using a Au-Ga alloy catalyst. Through in situ tailoring of the catalyst composition using trimethylgallium, the Ge-Si heterojunction width is systematically controlled by tuning the semiconductor solubility within a metal Au-Ga alloy catalyst. The present approach of alloying to control solute solubilities in the liquid catalyst may be extended to increasing the sharpness of axial dopant profiles, for example, in Si-Ge pn-heterojunction nanowires which is important for such applications as nanowire tunnel field effect transistors or in Si pn-junction nanowires.
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