Liquid Ga droplets play a double role in the self-catalyzed growth of GaAs nanowires on Si(111) substrates covered with a native SiO x layer: they induce the formation of nanosized holes in SiO x and then drive the uniaxial nanowire growth directly onto the underlying Si. The independent control of the two mechanisms is a prerequisite for mastering the growth of nanowires, but it is challenging in a conventional growth procedure where they both take place under the same droplets. To that end, we have developed an in situ procedure where the Ga droplets used for the formation of SiO x holes are removed before new Ga droplets drive the growth of GaAs nanowires. In that way, it was possible to study the interaction between Ga droplets and SiO x , to create holes in SiO x with controlled number density and size, and, finally, to grow GaAs nanowires only within those holes. Our results show unprecedented control of the nanowire nucleation with unique possibilities: (1) deliberate control of the number density of nanowires within 3 orders of magnitude (106–109 cm–2) without patterning the substrate and without changing the growth conditions, (2) highly synchronous nucleation events and, thus, exceptionally narrow nanowire length distributions (standard deviation <1% for 3 μm long nanowires), (3) high yield of vertical nanowires up to 80% (against GaAs islands), (4) highly reproducible results, and (5) independent control of the nanowire diameter from the number density. We anticipate that our methodology could be also exploited for different materials or other types of nanostructures.
We demonstrate a simple route to grow ensembles of self-catalyzed GaAs nanowires with a remarkably narrow statistical distribution of lengths on natively oxidized Si(111) substrates. The fitting of the nanowire length distribution (LD) with a theoretical model reveals that the key requirements for narrow LDs are the synchronized nucleation of all nanowires on the substrate and the absence of beam shadowing from adjacent nanowires. Both requirements are fulfilled by controlling the size and number density of the openings in SiO x , where the nanowires nucleate. This is achieved by using a pre-growth treatment of the substrate with Ga droplets and two annealing cycles. The narrowest nanowire LDs are markedly sub-Poissonian, which validates the theoretical predictions about temporally anti-correlated nucleation events in individual nanowires, the so-called nucleation antibunching. Finally, the reproducibility of sub-Poissonian LDs attests the reliability of our growth method.
We introduce droplet-confined alternate pulsed epitaxy for the self-catalyzed growth of GaAs nanowires on Si(111) substrates in the temperature range from 550 °C down to 450 °C. This unconventional growth mode is a modification of the migration-enhanced epitaxy, where alternating pulses of Ga and As4 are employed instead of a continuous supply. The enhancement of the diffusion length of Ga adatoms on the {11̅0} nanowire sidewalls allows for their targeted delivery to the Ga droplets at the top of the nanowires and, thus, for a highly directional growth along the nanowire axis even at temperatures as low as 450 °C. We demonstrate that the axial growth can be simply and abruptly interrupted at any time without the formation of any defects, whereas the growth rate can be controlled with high accuracy down to the monolayer scale, being limited only by the stochastic nature of nucleation. Taking advantage of these unique possibilities, we were able to probe and describe quantitatively the population dynamics of As inside the Ga droplets in specially designed experiments. After all, our growth method combines all necessary elements for precise growth control, in-depth investigation of the growth mechanisms and compatibility with fully processed Si-CMOS substrates.
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