Rate-limiting mechanisms in high-temperature growth of catalyst-free InAs nanowires with large thermal stability.

We identify the entire growth parameter space and rate-limiting mechanisms in non-catalytic InAs nanowires (NWs) grown by molecular beam epitaxy. Surprisingly huge growth temperature ranges are found with maximum temperatures close to ~600°C upon dramatic increase of V/III ratio, exceeding by far the typical growth temperature range for catalyst-assisted InAs NWs. Based on quantitative in situ line-of-sight quadrupole mass spectrometry, we determine the rate-limiting factors in high-temperature InAs NW growth by directly monitoring the critical desorption and thermal decomposition processes of InAs NWs. Both under dynamic (growth) and static (no growth, ultra-high vacuum) conditions the (111)-oriented InAs NWs evidence excellent thermal stability at elevated temperatures even under negligible supersaturation. The rate-limiting factor for InAs NW growth is hence dominated by In desorption from the substrate surface. Closer investigation of the group-III and group-V flux dependences on growth rate reveals two apparent growth regimes, an As-rich and an In-rich regime defined by the effective As/In flux ratio, and maximum achievable growth rates of > 6 µm h(-1). The unique features of high-T growth and excellent thermal stability provide the opportunity for operation of InAs-based NW materials under caustic environment and further allow access to temperature regimes suitable for alloying non-catalytic InAs NWs with GaAs.

Self-induced growth of vertical free-standing InAs nanowires on Si(111) by molecular beam epitaxy.

We report self-induced growth of vertically aligned (i.e. along the [111] direction), free-standing InAs nanowires on Si(111) substrates by solid-source molecular beam epitaxy. Implementation of an ultrathin amorphous SiO(x) mask on Si(111) facilitated epitaxial InAs nanowire growth, as confirmed by high-resolution x-ray diffraction 2theta-omega scans and transmission electron microscopy. Depending on growth temperature (in the range of 400-520 degrees C) substantial size variation of both nanowire length and diameter was found under preservation of uniform, non-tapered hexagon-shaped geometries. The majority of InAs nanowires exhibited phase-pure zinc blende crystal structure with few defective regions consisting of stacking faults. Photoluminescence spectroscopy at 20 K revealed peak emission of the InAs nanowires at 0.445 eV, which is approximately 30 meV blueshifted with respect to the emission of the bulk InAs reference due to radial quantum confinement effects. These results show a promising route towards integration of well-aligned, high structural quality InAs-based nanowires with the desired aspect ratio and tailored emission wavelengths on an Si platform.