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

摘要

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 >6mh ~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.