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GaAs/Al0.1Ga0.9As core-shell nanowires (CSNWs), with average lateral size of 125 nm, were grown on gold nanoparticle-activated Si (100) and Si (111) substrates via molecular beam epitaxy. Room temperature-photoluminescence (RT-PL) from the samples showed bulk-like GaAs and Al0.1Ga0.9As bandgap emission peaks at 1.43 and 1.56 eV, respectively. Higher PL emission intensity of the sample on Si (111) compared to that on Si (100) is attributed to uniform Al0.1Ga0.9As shell passivation of surface states on Si (111)-grown CSNWs. Carrier dynamics in two different temporal regimes were studied. In the sub-nanosecond time scale (300–500 ps), time-resolved radiative recombination efficiency of carriers was examined. In the 0–4 ps range, surface field-driven ballistic transport of carriers was probed in terms of the radiated terahertz (THz) waves. Time-resolved PL measurements at 300 K revealed that the carrier recombination lifetime of the GaAs core on Si (100)-grown CSNWs is 333 ps while that on Si (111)-grown sample is 500 ps. Ultrafast photoexcitation of GaAs core on the two samples generated a negligible difference in the intensity and bandwidth of emitted THz radiation. This result is ascribed to the fact that the deposited GaAs material on both substrates produced samples with comparable NW densities and similar GaAs core average diameter of about 75 nm. The samples’ difference in GaAs core’s carrier recombination lifetime did not influence THz emission since the two processes involve distinct mechanisms. The THz spectrum of CSNWs grown on Si (111) exhibited Fabry-Perot modes that originated from multiple reflections of THz waves within the Si substrate.