Physical investigations of small particles : (I) aerosol particle charging and flux enhancement and (II) whispering gallery mode sensing

Part I

Particles are a key feature of planetary atmospheres. On Earth they represent the greatest source of uncertainty in the global energy budget. This uncertainty can be addressed by making more measurement, by improving the theoretical analysis of measurements, and by better modeling basic particle nucleation and initial particle growth within an atmosphere. This work will focus on the latter two methods of improvement.

Uncertainty in measurements is largely due to particle charging. Accurate descriptions of particle charging are challenging because one deals with particles in a gas as opposed to a vacuum, so different length scales come into play. Previous studies have considered the effects of transition between the continuum and kinetic regime and the effects of two and three body interactions within the kinetic regime. These studies, however, use questionable assumptions about the charging process which resulted in skewed observations, and bias in the proposed dynamics of aerosol particles. These assumptions affect both the ions and particles in the system. Ions are assumed to be point monopoles that have a single characteristic speed rather than follow a distribution. Particles are assumed to be perfect conductors that have up to five elementary charges on them. The effects of three body interaction, ion-molecule-particle, are also overestimated. By revising this theory so that the basic physical attributes of both ions and particles and their interactions are better represented, we are able to make more accurate predictions of particle charging in both the kinetic and continuum regimes.

The same revised theory that was used above to model ion charging can also be applied to the flux of neutral vapor phase molecules to a particle or initial cluster. Using these results we can model the vapor flux to a neutral or charged particle due to diffusion and electromagnetic interactions. In many classical theories currently applied to these models, the finite size of the molecule and the electromagnetic interaction between the molecule and particle, especially for the neutral particle case, are completely ignored, or, as is often the case for a permanent dipole vapor species, strongly underestimated. Comparing our model to these classical models we determine an “enhancement factor” to characterize how important the addition of these physical parameters and processes is to the understanding of particle nucleation and growth.

Part II

Whispering gallery mode (WGM) optical biosensors are capable of extraordinarily sensitive specific and non-specific detection of species suspended in a gas or fluid. Recent experimental results suggest that these devices may attain single-molecule sensitivity to protein solutions in the form of stepwise shifts in their resonance wavelength, \lambda_{R}, but present sensor models predict much smaller steps than were reported. This study examines the physical interaction between a WGM sensor and a molecule adsorbed to its surface, exploring assumptions made in previous efforts to model WGM sensor behavior, and describing computational schemes that model the experiments for which single protein sensitivity was reported. The resulting model is used to simulate sensor performance, within constraints imposed by the limited material property data. On this basis, we conclude that nonlinear optical effects would be needed to attain the reported sensitivity, and that, in the experiments for which extreme sensitivity was reported, a bound protein experiences optical energy fluxes too high for such effects to be ignored.

The significance of sedimentation and sediments to phytoplankton growth in drinking-water reservoirs

In the mesotrophic-eutrophic Saidenbach Reservoir in Saxony, the nanoplankton and cyanobacteria have increased at the expense of diatom dominance, due to a doubling of the external phosphorus load in the last 15 years. However, the phosphorus sedimentation flux is still very high (up to 80% of the input), corresponding to more than 2 g m2 d-1 in terms of dry weight. There is a strong correlation between the abundance of diatoms in the euphotic zone and their sedimentation flux (with a delay of about 2 weeks). Only about 25% of the deposited material could be clearly attributed to plankton biomass; the remainder resulted from flocculation and precipitation processes or directly from the inflow of clay minerals. The ash content of the deposited material was high (73%). Thus the sedimentation flux can be considered to operate as an internal water-treatment/oligotrophication process within the lake. The neighbouring Neunzehnhain Reservoir still has a very clear water with a transparency up to 18 m depth. Though the sediment was not much lower than Saidenbach sediment in total phosphorus and total numbers of bacteria, sulphide was always absent and the ratio of Fe 2+ to Fe 3+ was very low in the upper (0- 5 cm) layer. Thus the external and internal phosphorus loads do not attain the critical level necessary to induce a ”phosphorus - phytoplankton” feedback loop.

Ni-silicide growth kinetics in Si and Si/SiO2 core/shell nanowires.

A systematic study of the kinetics of axial Ni silicidation of as-grown and oxidized Si nanowires (SiNWs) with different crystallographic orientations and core diameters ranging from ∼ 10 to 100 nm is presented. For temperatures between 300 and 440 °C the length of the total axial silicide intrusion varies with the square root of time, which provides clear evidence that the rate limiting step is diffusion of Ni through the growing silicide phase(s). A retardation of Ni-silicide formation for oxidized SiNWs is found, indicative of a stress induced lowering of the diffusion coefficients. Extrapolated growth constants indicate that the Ni flux through the silicided NW is dominated by surface diffusion, which is consistent with an inverse square root dependence of the silicide length on the NW diameter as observed for (111) orientated SiNWs. In situ TEM silicidation experiments show that NiSi(2) is the first forming phase for as-grown and oxidized SiNWs. The silicide-SiNW interface is thereby atomically abrupt and typically planar. Ni-rich silicide phases subsequently nucleate close to the Ni reservoir, which for as-grown SiNWs can lead to a complete channel break-off for prolonged silicidation due to significant volume expansion and morphological changes.

Seeded infiltration and growth of bulk YBCO nano-composites

The seeded infiltration and growth (SIG) technique offers near-net shape processing of bulk superconductors with significant improvement in reduced Y2BaCuO5 (Y-211) inclusion size, reduced shrinkage, reduced porosity and improved current density compared to samples fabricated by top seeded melt growth (TSMG). Y2Ba4CuMOy phases where M=Nb, Mo, W, Ta, etc., have been shown to form nano-scale inclusions in the YBa2Cu3Oy (Y-123) phase matrix and to contribute to enhanced magnetic flux pinning in these materials. In this paper, we describe the introduction of Y2Ba 4CuWOy nano-scale inclusions into bulk superconductors processed by the seeded infiltration growth process. Critical current density, Jc, in excess of 105 A/cm2 at 77 K in self-field is observed for samples containing Y2Ba 4CuWOy. © 2011 IEEE.

Flux line lattice structure and behavior in antiphase boundary free vicinal YBa2Cu3O7-delta thin films

Field angle dependent critical current, magneto-optical microscopy and high resolution electron microscopy studies have been performed on YBa2Cu3O7-delta thin films grown on miscut substrates. High resolution electron microscopy images show that the films studied exhibited clean epitaxial growth with a low density of antiphase boundaries and stacking faults. Any antiphase boundaries (APBs) formed near the film substrate interface rapidly healed rather than extending through the thickness of the film. Unlike vicinal films grown on annealed substrates, which contain a high density of antiphase boundaries, magneto-optical imaging showed no filamentary flux penetration in the films studied. The flux penetration is, however, asymmetric. This is associated with intrinsic pinning of flux strings by the tilted a-b planes and the dependence of the pinning force on the angle between the local field and the a-b planes. Field angle dependent critical current measurements exhibited the striking vortex channeling effect previously reported in vicinal films. By combining the results of three complementary characterization techniques it is shown that extended APB free films exhibit markedly different critical current behavior compared to APB rich films. This is attributed to the role of APB sites as strong pinning centers for Josephson string vortices between the a-b planes. (C) 2003 American Institute of Physics.

Growth of large sized y Ba 2Cu 3O 7 single crystals using the top seeded melt growth process

Neutron scattering experiments are fundamental to the study of magnetic order and related phenomena in a range of superconducting and magnetic materials. Traditional methods of crystal growth, however, do not yield single crystals of sufficient size for practical neutron scattering measurements. In this paper, we demonstrate the growth of relatively pure, large Y Ba 2Cu 3O 7 single crystals up to 30mm in diameter using a top seeded melt growth process. The characterization of the microstructural and magnetic properties of these crystals indicates that they contain <2% of impurity phases and, hence, exhibit only weak flux pinning behaviour. © 2012 IOP Publishing Ltd.

Identification of a gene, ccr-1 (sll1242), required for chill-light tolerance and growth at 15 degrees C in Synechocystis sp PCC 6803

Synechocystis sp. PCC 6803 exposed to chill (5 degrees C)-light (100 mu mol photons m(-2) s(-1)) stress loses its ability to reinitiate growth. From a random insertion mutant library of Synechocystis sp. PCC 6803, a sll1242 mutant showing increased sensitivity to chill plus light was isolated. Mutant reconstruction and complementation with the wild-type gene confirmed the role of sll1242 in maintaining chill-light tolerance. At 15 degrees C, the autotrophic and mixotrophic growth of the mutant were both inhibited, paralleled by decreased photosynthetic activity. The expression of sll1242 was upregulated in Synechocystis sp. PCC 6803 after transfer from 30 to 15 degrees C at a photosynthetic photon flux density of 30 mu mol photons m(-2) S-1. sll1242, named ccr (cyanobacterial cold resistance gene)- 1, may be required for cold acclimation of cyanobacteria in light.

Systematic investigation on the influence of the As-4 flux on the magnetic property of (In,Cr)As quantum dots

We study the structure, optical and magnetic characteristics of self-assembled (In,Cr) As diluted magnetic semiconductor quantum dots as a function of the As-4 flux. Increasing the surface energy by increasing the As4 pressure leads to a smaller number of larger dots for a higher As-4 flux. The remanent magnetization measured at 5K also increases with increasing As-4 flux, which is attributed to the enhancement of the effective Cr content due to the As-4-rich condition. We explore the possibility of tailoring magnetism by controlling the As-4/In flux ratio without changing the Cr concentration. Furthermore, extremely low-density QDs have also been successfully grown. Copyright (C) EPLA, 2008

Growth of GaSb layers on GaAs (001) substrate by molecular beam epitaxy

GaSb 1 mu m-thick layers were grown by molecular beam epitaxy on GaAs (001). The effects of the growth conditions on the crystalline quality, surface morphology, electrical properties and optical properties were studied by double crystalline x-ray diffraction, atomic force microscopy, Hall measurement and photoluminescence spectroscopy, respectively. It was found that the surface roughness and hole mobility are highly dependent on the antimony-to-gallium flux ratios and growth temperatures. The crystalline quality, electrical properties and optical properties of GaSb layers were also studied as functions of growth rate, and it was found that a suitably low growth rate is beneficial for the crystalline quality and electrical and optical properties. Better crystal quality GaSb layers with a minimum root mean square surface roughness of 0.1 nm and good optical properties were obtained at a growth rate of 0.25 mu m h(-1).

Effect of Al incorporation on the AlGaN growth by metalorganic chemical vapor deposition

The effect of Al incorporation on the AlGaN growth by metalorganic chemical vapor deposition is investigated. With the increase of trimethylalluminum (TMAl) flux, the crystal quality becomes worse, and the epilayer surface becomes rougher. An interesting phenomenon is that the growth rate of AlGaN decrease with increasing TMAl flux, which is opposite to the AlN growth rate dependence on the TMAl flux. All these effects are attributed to the different properties of At atoms due to the higher bond strength of Al-N compared with Ga-N, which lead to lower surface mobility and stronger competitive ability of Al atoms during the growth. The enhancement of the surface mobility of Al is especially important for improving the quality of AlGaN. (c) 2006 Elsevier B.V. All rights reserved.

Parasitic reaction and its effect on the growth rate of AlN by metalorganic chemical vapor deposition

The Al composition of metalorganic chemical vapor deposition (MOCVD)-grown AlGaN alloy layers is found to be greatly influenced by the parasitic reaction between ammonia (NH3) and trimethylaluminum (TMAI). The growth process of AlN is carefully investigated by monitoring the in situ optical reflection. The abnormal dependencies of growth rate on growth temperature, reactor pressure, and flux of NH3 are observed and can be well explained by the effect of parasitic reaction. The increase of growth rate with increasing flux of TMAI is found to depend on the growth temperature and reactor pressure due to the presence of parasitic effect. A relatively low growth temperature and a reduced reactor pressure are suggested for the effective decrease of parasitic reaction during the MOCVD growth of AlN and probably lead to a more effective incorporation of Al into the AlGaN layers. (c) 2005 Elsevier B.V. All rights reserved.

Growth mode and strain evolution during InN growth on GaN(0001) by molecular-beam epitaxy

Epitaxial growth of InN on GaN(0001) by plasma-assisted molecular-beam epitaxy is investigated over a range of growth parameters including source flux and substrate temperature. Combining reflection high-energy electron diffraction (RHEED) and scanning tunneling microscopy (STM), we establish a relationship between film growth mode and the deposition condition. Both two-dimensional (2D) and three-dimensional (3D) growth modes of the film are observed. For 2D growth, sustained RHEED intensity oscillations are recorded while STM reveals 2D nucleation islands. For 3D growth, less than three oscillation periods are observed indicating the Stranski-Krastanov (SK) growth mode of the film. Simultaneous measurements of (reciprocal) lattice constant by RHEED suggest a gradual relaxation of the strain in film, which commences during the first bilayer (BL) deposition and almost completes after 2-4 BLs. For SK growth, 3D islanding initiates after the strain has mostly been relieved, presumably by dislocations, so the islands are likely strain free. (C) 2002 American Institute of Physics.

Improvement of the photoluminescence from gallium nitride layers grown by MBE with an additional incident indium flux

The effect of using an indium flux during the MBE growth of GaN layers was investigated. The properties of these layers were studied using electron probe microanalysis, secondary ion mass spectroscopy, photoluminescence and cathodoluminescence. The optical properties of the GaN layers are shown to improve as compared with undoped GaN layers grown under nominally the same conditions but without an additional indium flux.

Low-temperature growth properties of Si1-xGex by disilane and solid-Ge molecular beam epitaxy

Low temperature (similar to 500 degrees C) growth properties of Si1-xGex by disilane and solid-Ge molecular beam epitaxy have been studied with an emphasis on surface morphology and growth kinetics. It is found that low-temperature growth(<500 degrees C) is in layer-by-layer mode and atomically-smooth surfaces have been obtained in as-grown samples with large Ge composition (>0.5). Ge composition dependence on substrate temperature, Ge cell temperature and disilane flow rate have been investigated. It is found that in low-temperature growth (less than or equal to 500 degrees C) and under large disilane flux, Ge composition increases with the increase of Ge flux and further increase of Ge flux leads to the saturation of Ge composition. Similar compositional dependence has been found at different growth temperatures. The saturated composition increases with the decrease of substrate temperature. The results can be explained if H desorption is assumed to occur from both Si and Ge monohydrides without diffusional exchange and the presence of Ge enhances H desorption on a Si site. (C) 1998 Elsevier Science B.V. All rights reserved.

Molecular beam epitaxy growth of Iny2Al1-y2As/In0.73Ga0.27As/Iny1Al1-y1As/InP P-HEMTs with enhancement conductivity using an intentional nonlattice-matched buffer layer

Pseudomorphic Iny2Al1-y2As/In0.73Ga0.27As/Iny1Al1-y1As (y1 greater than or equal to 0.52) modulation-doped heterostructures with an intentional nonlattice-matched buffer layer were successfully grown by molecular beam epitaxy on (100)InP substrates. Fourier transform photoluminescence and double crystal x-ray diffraction measurements show a superior crystalline quality in the high In content channel, when In mole fraction increases from y1=0.52 to 0.55 in the Iny1Al1-y1As buffer layer. In this case, an increasing of 16.3% and 23.5% for conductivity (mu xn(s)) and mobility, related to the strain compensation in the In0.73Ga0.27As channel, was achieved, respectively, comparing to the structure containing a well-lattice matched buffer layer. With increasing the mismatch further (y1=0.58), a morphology with cross-hatched pattern was observed due to the onset of a large amount of misfit dislocations, and the electronic characterization is not able to be improved continuously. Because we can realize high quality strained P-HEMTs in a relative wide range of equivalent beam flux (EBF) ratios, the stringent control over the constant EBF is not indispensable on this In-based material system. (C) 1997 American Vacuum Society.