Philippe Caroff

Australian National University, Canberra, Australian Capital Territory, Australia

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Publications (124)443.11 Total impact

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    ABSTRACT: Obtaining compositional homogeneity without compromising morphological or structural quality is one of the biggest challenges in growing ternary alloy compound semiconductor nanowires. Here we report growth of Au-seeded InxGa1-xAs nanowires via metal-organic vapour phase epitaxy with uniform composition, morphology and pure wurtzite (WZ) crystal phase by carefully optimizing growth temperature and V/III ratio. We find that high growth temperatures allow the InxGa1-xAs composition to be more uniform by suppressing the formation of typically observed spontaneous In-rich shells. A low V/III ratio results in the growth of pure WZ phase InxGa1-xAs nanowires with uniform composition and morphology while a high V/III ratio allows pure zinc-blende (ZB) phase to form. Ga incorporation is found to be dependent on the crystal phase favouring higher Ga concentration in ZB phase compared to the WZ phase. Tapering is also found to be more prominent in defective nanowires hence it is critical to maintain the highest crystal structure purity in order to minimize tapering and inhomogeneity. The InP capped pure WZ In0.65Ga0.35As core-shell nanowire heterostructures show 1.54 μm photoluminescence, close to the technologically important optical fibre telecommunication wavelength, which is promising for application in photodetectors and nanoscale lasers.
    Nanotechnology 05/2015; 26(20):205604. DOI:10.1088/0957-4484/26/20/205604 · 3.67 Impact Factor
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    ABSTRACT: We demonstrate a simple way of fabricating high performance tunnel devices from p-doped InAs nanowires by tailoring the n-doped surface accumulation layer inherent to InAs surfaces. By using appropriate ammonium sulfide based surface passivation before metallization without any further thermal treatment, we demonstrate characteristics of tunnel p-n junctions, namely Esaki and backward diodes, with figures of merit better than previously published for InAs homojunctions. The further optimization of both the surface doping, in a quantitative way, and the device geometry allows us to demonstrate that these nanowire-based technologically-simple diodes have promising direct current characteristics for integrated high frequency detection or generation.
    Nano Research 03/2015; 8(3):980-989. DOI:10.1007/s12274-014-0579-8 · 6.96 Impact Factor
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    ABSTRACT: While III-V binary nanowires are now well controlled and their growth mechanisms reasonably well understood, growing ternary nanowires, including controlling their morphology, composition and crystal structure remains a challenge. However, understanding and control of ternary alloys is of fundamental interest and critical to enable a new class of nanowire devices. Here, we report on the progress in understanding the complex growth behaviour of gold-seeded GaAs1-xSbx nanowires grown by metalorganic vapour phase epitaxy. The competition between As and Sb atoms for incorporation into the growing crystal leads to a tunability of the Sb over a broad range (x varies from 0.09 to 0.6), solely by changing the AsH3 flow. In contrast, changing TMSb flow is more effective in affecting the morphology and crystal structure of the nanowires. Inclined faults are found in some of these nanowires, directly related to the kinking of the nanowires and controlled by TMSb flow. Combined with the observed sharp increase of wetting angle between the Au seed and nanowire, the formation of inclined faults are attributed to the Au seed being dislodged from the growth front to wet the sidewalls of the nanowires, and are ascribed to the surfactant role of Sb. The insights provided by this study should benefit future device applications relying on taper- and twin-free ternary antimonides III-V nanowire alloys and their heterostructures.
    Nanoscale 02/2015; DOI:10.1039/C4NR06307D · 6.74 Impact Factor
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    ABSTRACT: The development of earth abundant materials for optoelectronics and photovoltaics promises improvements in sustainability and scalability. Recent studies have further demonstrated enhanced material efficiency through the superior light management of novel nanoscale geometries such as the nanowire. Here we show that an industry standard epitaxy technique can be used to fabricate high quality II-V nanowires (1D) and nanoplatelets (2D) of the earth abundant semiconductor Zn3As2. We go on to establish the optoelectronic potential of this material by demonstrating efficient photoemission and detection at 1.0 eV, an energy significant to both photovoltaics and optical telecommunications. Dynamical spectroscopy reveals this superior performance as resulting from a low rate of surface recombination combined with a high rate of radiative recombination. These results introduce nanostructured Zn3As2 as a high quality optoelectronic material ready for device exploration.
    Nano Letters 11/2014; 15(1). DOI:10.1021/nl5036918 · 12.94 Impact Factor
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    ABSTRACT: Combination of mismatched materials in semiconductor nanowire heterostructures offers a freedom of bandstructure engineering that is impossible in standard planar epitaxy. Nevertheless, the presence of strain and/or structural defects directly control the optoelectronic properties of these nanomaterials. Understanding with atomic accuracy how mismatched heterostructures release or accommodate strain is therefore highly desirable. By using atomic resolution high angle annular dark field scanning transmission electron microscopy combined with geometrical phase analyses and computer simulations we are able to establish the relaxation mechanism (including both elastic and plastic deformations) involved in order to release the mismatch strain in axial nanowire heterostructures. Formation of misfit dislocations, diffusion of atomic species, polarity transfer and induced structural transformations are studied at atomic resolution at the intermediate ternary interfaces. Two nanowire heterostructure systems with promising applications (InAs/InSb and GaAs/GaSb) have been selected as key examples.
    Nano Letters 10/2014; 14(11). DOI:10.1021/nl503273j · 12.94 Impact Factor
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    ABSTRACT: We report the growth of stacking-fault-free and taper-free wurtzite InP nanowires with diameters ranging from 80 to 600 nm using selective-area metalorganic vapor-phase epitaxy and experimentally determine a quantum efficiency of similar to 50%, which is on par with InP epilayers. We also demonstrate room-temperature, photonic mode lasing from these nanowires. Their excellent structural and optical quality opens up new possibilities for both fundamental quantum optics and optoelectronic devices.
    Nano Letters 08/2014; 14(9). DOI:10.1021/nl5021409 · 12.94 Impact Factor
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    ABSTRACT: Growth of III-V nanowires on the [100]-oriented industry standard substrates is critical for future integrated nanowire device development. Here we present an in-depth analysis of the seemingly complex ensembles of epitaxial nanowires grown on InP (100) substrates. The nanowires are categorized into 3 types as vertical, non-vertical and planar, and the growth directions, facets and crystal structure of each type are investigated. The non-vertical growth directions are mathematically modelled using a 3-dimensional multiple order twinning concept. The non-vertical nanowires can be further classified into two different types, with one type growing in the <111> directions and the other in the <100> directions after initial multiple three dimensional twinning. We find that 99% of the total nanowires are grown either along <100>, <111> or <110> growth directions by {100} or {111} growth facets. We also demonstrate relative control of yield of these different types of nanowires, by tuning pre-growth annealing conditions and growth parameters. Together, the knowledge and controllability of the types of nanowires provide an ideal foundation to explore novel geometries that combine different crystal structures, with potential for both fundamental science research as well as device applications.
    ACS Nano 06/2014; 8(7). DOI:10.1021/nn5017428 · 12.03 Impact Factor
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    ABSTRACT: We report on magneto-transport measurements in InAs nanowires under large magnetic field (up to 55T), providing a direct spectroscopy of the 1D electronic band structure. Large modulations of the magneto-conductance mediated by an accurate control of the Fermi energy reveal the Landau fragmentation, carrying the fingerprints of the confined InAs material. Our numerical simulations of the magnetic band structure consistently support the experimental results and reveal key parameters of the electronic confinement.
    Physical Review Letters 02/2014; 112:076801. DOI:10.1103/PhysRevLett.112.076801 · 7.73 Impact Factor
  • Kimberly A Dick, Philippe Caroff
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    ABSTRACT: Semiconductor nanowires composed of III-V materials have enormous potential to add new functionality to electronics and optical applications. However, integration of these promising structures into applications is severely limited by the current near-universal reliance on gold nanoparticles as seeds for nanowire fabrication. Although highly controlled fabrication is achieved, this metal is entirely incompatible with the Si-based electronics industry. In this Feature we review the progress towards developing gold-free bottom-up synthesis techniques for III-V semiconductor nanowires. Three main categories of nanowire synthesis are discussed: selective-area epitaxy, self-seeding and foreign metal seeding, with main focus on the metal-seeded techniques. For comparison, we also review the development of foreign metal seeded synthesis of silicon and germanium nanowires. Finally, directions for future development and anticipated important trends are discussed. We anticipate significant development in the use of foreign metal seeding in particular. In addition, we speculate that multiple different techniques must be developed in order to replace gold and to provide a variety of nanowire structures and properties suited to a diverse range of applications.
    Nanoscale 02/2014; DOI:10.1039/c3nr06692d · 6.74 Impact Factor
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    ABSTRACT: We explore the signatures of Majorana fermions in a nanowire based topological superconductor-quantum dot-topological superconductor hybrid device by charge transport measurements. The device is made from an epitaxially grown InSb nanowire with two superconductor Nb contacts on a Si/SiO$_2$ substrate. At low temperatures, a quantum dot is formed in the segment of the InSb nanowire between the two Nb contacts and the two Nb contacted segments of the InSb nanowire show superconductivity due to the proximity effect. At zero magnetic field, well defined Coulomb diamonds and the Kondo effect are observed in the charge stability diagram measurements in the Coulomb blockade regime of the quantum dot. Under the application of a finite, sufficiently strong magnetic field, a zero-bias conductance peak structure is observed in the same Coulomb blockade regime. It is found that the zero-bias conductance peak is present in many consecutive Coulomb diamonds, irrespective of the even-odd parity of the quasi-particle occupation number in the quantum dot. In addition, we find that the zero-bias conductance peak is in most cases accompanied by two differential conductance peaks, forming a triple-peak structure, and the separation between the two side peaks in bias voltage shows oscillations closely correlated to the background Coulomb conductance oscillations of the device. The observed zero-bias conductance peak and the associated triple-peak structure are in line with the signatures of Majorana fermion physics in a nanowire based topological superconductor-quantum dot-topological superconductor system, in which the two Majorana bound states adjacent to the quantum dot are hybridized into a pair of quasi-particle states with finite energies and the other two Majorana bound states remain as the zero-energy modes located at the two ends of the entire InSb nanowire.
    Scientific Reports 01/2014; 4(7621). DOI:10.1038/srep07261 · 5.58 Impact Factor
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    ABSTRACT: The modified phonon dispersion is of importance for understanding the origin of the reduced heat conductivity in nanowires. We have measured the phonon dispersion for 50 nm diameter InSb (111) nanowires using time-resolved X-ray diffraction. By comparing the sound speed of the bulk (3880 m/s) and that of a classical thin rod (3600 m/s) to our measurement (2880 m/s), we conclude that the origin of the reduced sound speed and thereby to the reduced heat conductivity is that the C44 elastic constant is reduced by 35% compared to the bulk material.
    Nano Letters 01/2014; 14(2). DOI:10.1021/nl403596b · 12.94 Impact Factor
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    ABSTRACT: Understanding surface structure and surface composition is of particular importance for semiconductor nanowire applications, since they might strongly contribute to the electrical, optical and thermal properties of the Nanowires. A prototypical material is GaAs, where polytype inclusions consisting of zinc-blende (ZB) and wurtzite (WZ) segments form during the growth of nanowires, in particular when Sb atoms are incorporated. Here, we will investigate the structural and electronic properties of GaAs and GaAsSb nanowires with scanning tunneling microscopy and spectroscopy. These techniques gives access to the nanofaceting morphology of a single semiconductor nanowire with a detailed picture of the sidewall structural and compositional properties at the atomic scale. It will also be used to measure the band gap and the position of the Fermi level at the surface. In particular, we will show that the ZB_WZ structures on the surface of GaAs nanowires naturally introduce p-i juntions solely due to the Fermi level pinning at different energies on the non-polar WZ and ZB sidewall facets.
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    ABSTRACT: With the continued maturation of III-V nanowire research, expectations of material quality should be concomitantly raised. Ideally, III-V nanowires integrated on silicon should be entirely free of extended planar defects such as twins, stacking faults or polytypism, position-controlled for convenient device processing, and gold-free for compatibility with standard CMOS processing tools. Here we demonstrate large area vertical GaAsxSb1-x nanowire arrays grown on silicon (111) by molecular beam epitaxy. The nanowires' complex faceting, pure zinc blende crystal structure and composition are mapped using characterization techniques both at the nanoscale and in large-area ensembles. We prove unambiguously that these gold-free nanowires are entirely twin-free down to the first bilayer and reveal their three-dimensional composition evolution, paving the way for novel infra-red devices integrated directly on the cost-effective Si platform.
    Nano Letters 12/2013; 14(1). DOI:10.1021/nl404085a · 12.94 Impact Factor
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    ABSTRACT: With the continued maturation of III−V nanowire research, expectations of material quality should be concomitantly raised. Ideally, III−V nanowires integrated on silicon should be entirely free of extended planar defects such as twins, stacking faults, or polytypism, position-controlled for convenient device processing, and gold-free for compatibility with standard complementary metal−oxide−semiconductor (CMOS) processing tools. Here we demonstrate large area vertical GaAsxSb1−x nanowire arrays grown on silicon (111) by molecular beam epitaxy. The nanowires’ complex faceting, pure zinc blende crystal structure, and composition are mapped using characterization techniques both at the nanoscale and in large-area ensembles. We prove unambiguously that these gold-free nanowires are entirely twin-free down to the first bilayer and reveal their three-dimensional composition evolution, paving the way for novel infrared devices integrated directly on the costeffective Si platform.
    Nano Letters 12/2013; 14:326. · 12.94 Impact Factor
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    ABSTRACT: Antimonide-based nanowires represent an important new class of material with great promise for both fundamental physics studies and various device applications. We report a comprehensive study on understanding the growth behaviour of GaxIn1-xSb nanowires on GaAs substrates using Au nanoparticles. First, the effect of growth parameters on the morphology and composition of GaxIn1-xSb nanowires is extensively studied over the entire compositional range (from 3 to ∼100% of In). Second, the obtained compositional results are explained by a kinetic model, suggesting an Arrhenius-type behavior for the trimethylindium (TMIn) precursor. Third, the particle composition is fully investigated and the implications for growth are discussed with reference to our calculated Au-Ga-In phase diagram. Fourth, a mechanism is presented to explain the temperature-dependent morphology and radial growth of the GaxIn1-xSb nanowires. Finally, we demonstrate homogeneous compositions in both axial and radial directions and the nanowires remain entirely twin-free zinc blende. The understanding gained from this study together with the potential to precisely tailor the band gap, wavelength and carrier mobilities allows fabrication of various GaxIn1-xSb-based nanowire devices.
    Nanoscale 12/2013; 6(2). DOI:10.1039/c3nr05079c · 6.74 Impact Factor
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    ABSTRACT: Organized growth of high aspect-ratio nanostructures such as membranes is interesting for opto-electronic and energy harvesting applications. Recently, we reported a new form of InAs nano-membranes grown on Si substrates with enhanced light scattering properties. In this paper we study how to tune the morphology of the membranes by changing the growth conditions. We examine the role of the V/III ratio, substrate temperature, mask opening size and inter-hole distances in determining the size and shape of the structures. Our results show that the nano-membranes form by a combination of the growth mechanisms of nanowires and the Stranski-Krastanov type of quantum dots: in analogy with nanowires, the length of the membranes strongly depends on the growth temperature and the V/III ratio; the inter-hole distance of the sample determines two different growth regimes: competitive growth for small distances and an independent regime for larger distances. Conversely, and similarly to quantum dots, the width of the nano-membranes increases with the growth temperature and does not exhibit dependence on the V/III ratio. These results constitute an important step towards achieving rational design of high aspect-ratio nanostructures.
    Nanotechnology 11/2013; 24(43):435603. DOI:10.1088/0957-4484/24/43/435603 · 3.67 Impact Factor
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    ABSTRACT: The band structure and the Fermi level pinning at clean and well-ordered sidewall surfaces of zincblende (ZB)-wurtzite (WZ) GaAs nanowires are investigated by scanning tunneling spectroscopy and density functional theory calculations. The WZ-ZB phase transition in GaAs nanowires introduces p-i junctions at the sidewall surfaces. This is caused by the presence of numerous steps, which induce a Fermi level pinning at different energies on the non-polar WZ and ZB sidewall facets. (C) 2013 AIP Publishing LLC.
    Applied Physics Letters 09/2013; 103(12):122104-122104-4. DOI:10.1063/1.4821293 · 3.52 Impact Factor
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    ABSTRACT: Thanks to their wide band structure tunability, GaAs1-xSbx nanowires provide exciting perspectives in optoelectronic and energy harvesting applications. The control of composition and strain of these ternary alloys is crucial in the determination of their optical and electronic properties. Raman scattering provides information on the vibrational properties of materials, which can be related to the composition and strain. We present a systematic study of the vibrational properties of GaAs1-xSbx nanowires for Sb contents from 0 to 44%, as determined by energy-dispersive x-ray analyses. We find that optical phonons red-shift with increasing Sb content. We explain the shift by alloying effects, including mass disorder, dielectric changes and ionic plasmon coupling. The influence of Sb on the surface optical modes is addressed. Finally, we compare the luminescence yield between GaAs and GaAs1-xSbx, which can be related to a lower surface recombination rate. This work provides a reference for the study of ternary alloys in the form of nanowires, and demonstrates the tunability and high material quality of gold-free ternary antimonide nanowires directly grown on silicon.
    Nanotechnology 09/2013; 24(40):405707. DOI:10.1088/0957-4484/24/40/405707 · 3.67 Impact Factor
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    ABSTRACT: Semiconductor nanowires have proven a versatile platform for the realization of novel structures unachievable by traditional planar epitaxy techniques. Amongst these, the periodic arrangement of twin planes to form twinning superlattice structures has generated particular interest. Here we demonstrate twinning superlattice formation in GaAs nanowires and investigate the diameter dependence of both morphology and twin plane spacing. An approximately linear relationship is found between plane spacing and nanowire diameter which contrasts with previous results reported for both InP and GaP. Through modeling we relate this to both the higher twin plane surface energy of GaAs coupled with the lower supersaturation relevant to Au seeded GaAs nanowire growth. Understanding and modeling the mechanism of twinning superlattice formation in III-V nanowires not only provides fundamental insight into the growth process but also opens the door to the possibility of tailoring twin spacing for various electronic and mechanical applications.
    ACS Nano 08/2013; 7(9). DOI:10.1021/nn403390t · 12.03 Impact Factor
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    ABSTRACT: We have investigated in-situ Si doping of InAs nanowires grown by molecular beam epitaxy from gold seeds. The effectiveness of n-type doping is confirmed by electrical measurements showing an increase of the electron density with the Si flux. We also observe an increase of the electron density along the nanowires from the tip to the base, attributed to the dopant incorporation on the nanowire facets whereas no detectable incorporation occurs through the seed. Furthermore the Si incorporation strongly influences the lateral growth of the nanowires without giving rise to significant tapering, revealing the complex interplay between axial and lateral growth.
    Applied Physics Letters 07/2013; 102(22). DOI:10.1063/1.4809576 · 3.52 Impact Factor

Publication Stats

2k Citations
443.11 Total Impact Points

Institutions

  • 2013–2014
    • Australian National University
      • Department of Electronic Materials Engineering (EME)
      Canberra, Australian Capital Territory, Australia
  • 2010–2014
    • Lund University
      • Division of Solid State Physics
      Lund, Skåne, Sweden
  • 2007–2014
    • French National Centre for Scientific Research
      Lutetia Parisorum, Île-de-France, France
  • 2006–2009
    • Institut National des Sciences Appliquées de Rennes
      Roazhon, Brittany, France
  • 2005
    • INSA
      Альтамира, Tamaulipas, Mexico