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Self-assembly of vertically aligned III–V semiconductor nanowires (NWs) on two-dimensional (2D) van der Waals (vdW) nanomaterials allows for integration of novel mixed-dimensional nanosystems with unique properties for optoelectronic and nanoelectronic device applications. Here, selective-area vdW epitaxy (SA-vdWE) of InAs NWs on isolated 2D molybdenum disulfide (MoS 2 ) domains is reported for the first time. The MOCVD growth parameter space ( i.e. , V/III ratio, growth temperature, and total molar flow rates of metalorganic and hydride precursors) is explored to achieve pattern-free positioning of single NWs on isolated multi-layer MoS 2 micro-plates with one-to-one NW-to-MoS 2 domain placement. The introduction of a pre-growth poly- l -lysine surface treatment is highlighted as a necessary step for mitigation of InAs nucleation along the edges of triangular MoS 2 domains and for NW growth along the interior region of 2D micro-plates. Analysis of NW crystal structures formed under the optimal SA-vdWE condition revealed a disordered combination of wurtzite and zinc-blend phases. A transformation of the NW sidewall faceting structure is observed, resulting from simultaneous radial overgrowth during axial NW synthesis. A common lattice arrangement between axially-grown InAs NW core segments and MoS 2 domains is described as the epitaxial basis for vertical NW growth. A model is proposed for a common InAs/MoS 2 sub-lattice structure, consisting of three multiples of the cubic InAs unit cell along the [21̄1̄] direction, commensurately aligned with a 14-fold multiple of the Mo–Mo (or S–S) spacing along the [101̄0] direction of MoS 2 hexagonal lattice. The SA-vdWE growth mode described here enables controlled hybrid integration of mixed-dimensional III–V-on-2D heterostructures as novel nanosystems for applications in optoelectronics, nanoelectronics, and quantum enabling technologies.
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Improving pseudo-van der Waals epitaxy of self-assembled InAs nanowires on graphene via MOCVD parameter space mapping
Heterogeneous self-assembly of III–V nanostructures on inert two-dimensional monolayer materials enables novel hybrid nanosystems with unique properties that can be exploited for low-cost and low-weight flexible optoelectronic and nanoelectronic device applications. Here, the pseudo-van der Waals epitaxy (vdWE) growth parameter space for heterogeneous integration of InAs nanowires (NWs) with continuous films of single layer graphene (SLG) via metalorganic chemical vapor deposition (MOCVD) is investigated. The length, diameter, and number density of NWs, as well as areal coverage of parasitic islands, are quantified as functions of key growth variables including growth temperature, V/III ratio, and total flow rate of metalorganic and hydride precursors. A compromise between self-assembly of high aspect ratio NWs comprising high number density arrays and simultaneous minimization of parasitic growth coverage is reached under a selected set of optimal growth conditions. Exploration of NW crystal structures formed under various growth conditions reveals that a characteristic polytypic and disordered lattice is invariant within the explored parameter space. A growth evolution study reveals a gradual reduction in both axial and radial growth rates within the explored timeframe for the optimal growth conditions, which is attributed to a supply-limited competitive growth regime. Two strategies are introduced for further growth optimization. Firstly, it is shown that the absence of a pre-growth in situ arsine surface treatment results in a reduction of parasitic island coverage by factor of ∼0.62, while NW aspect ratio and number densities are simultaneously enhanced. Secondly, the use of a two-step flow-modulated growth procedure allows for realization of dense fields of high aspect ratio InAs NWs. As a result of the applied studies and optimization of the growth parameter space, the highest reported axial growth rate of 840 nm min −1 and NW number density of ∼8.3 × 10 8 cm −2 for vdWE of high aspect ratio (>80) InAs NW arrays on graphitic surfaces are achieved. This work is intended to serve as a guide for vdWE of self-assembled III–V semiconductor NWs such as In-based ternary and quaternary alloys on functional two-dimensional monolayer materials, toward device applications in flexible optoelectronics and tandem-junction photovoltaics.
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- Award ID(s):
- 1665086
- PAR ID:
- 10092175
- Date Published:
- Journal Name:
- CrystEngComm
- Volume:
- 21
- Issue:
- 4
- ISSN:
- 1466-8033
- Page Range / eLocation ID:
- 602 to 615
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/c8ce01666f
