PubMed Health⌕ Search

Biomedical subjects

Hongjie Dai

Publications and source records attributed to Hongjie Dai.

At least 19 recordsLinked to original sources
PubMed2006

FeCo/graphitic-shell nanocrystals as advanced magnetic-resonance-imaging and near-infrared agents.

Nanocrystals with advanced magnetic or optical properties have been actively pursued for potential biological applications, including integrated imaging, diagnosis and therapy. Among various magnetic nanocrystals, FeCo has superior magnetic properties, but it has yet to be explored owing to the problems of easy oxidation and potential toxicity. Previously, FeCo nanocrystals with multilayered graphitic carbon, pyrolytic carbon or inert metals have been obtained, but not in the single-shelled, discrete, chemically functionalized and water-soluble forms desired for biological applications. Here, we present a scalable chemical vapour deposition method to synthesize FeCo/single-graphitic-shell nanocrystals that are soluble and stable in water solutions. We explore the multiple functionalities of these core-shell materials by characterizing the magnetic properties of the FeCo core and near-infrared optical absorbance of the single-layered graphitic shell. The nanocrystals exhibit ultra-high saturation magnetization, r1 and r2 relaxivities and high optical absorbance in the near-infrared region. Mesenchymal stem cells are able to internalize these nanoparticles, showing high negative-contrast enhancement in magnetic-resonance imaging (MRI). Preliminary in vivo experiments achieve long-lasting positive-contrast enhancement for vascular MRI in rabbits. These results point to the potential of using these nanocrystals for integrated diagnosis and therapeutic (photothermal-ablation) applications.

Animals↗
PubMed2006

Selective etching of metallic carbon nanotubes by gas-phase reaction.

Metallic and semiconducting carbon nanotubes generally coexist in as-grown materials. We present a gas-phase plasma hydrocarbonation reaction to selectively etch and gasify metallic nanotubes, retaining the semiconducting nanotubes in near-pristine form. With this process, 100% of purely semiconducting nanotubes were obtained and connected in parallel for high-current transistors. The diameter- and metallicity-dependent "dry" chemical etching approach is scalable and compatible with existing semiconductor processing for future integrated circuits.

Journal Article↗
PubMed2006

Hydrogenation and hydrocarbonation and etching of single-walled carbon nanotubes.

We present a systematic experimental investigation of the reactions between hydrogen plasma and single-walled carbon nanotubes (SWNTs) at various temperatures. Microscopy, infrared (IR) and Raman spectroscopy, and electrical transport measurements are carried out to investigate the properties of SWNTs after hydrogenation. Structural deformations, drastically reduced electrical conductance, and an increased semiconducting nature of SWNTs upon sidewall hydrogenation are observed. These changes are reversible upon thermal annealing at 500 degrees C via dehydrogenation. Harsh plasma or high temperature reactions lead to etching of nanotubes likely via hydrocarbonation. Smaller SWNTs are markedly less stable against hydrocarbonation than larger tubes. The results are fundamental and may have implications to basic and practical applications including hydrogen storage, sensing, band gap engineering for novel electronics, and new methods of manipulation, functionalization, and etching of nanotubes.

Journal Article↗
PubMed2006

DNA functionalization of carbon nanotubes for ultrathin atomic layer deposition of high kappa dielectrics for nanotube transistors with 60 mV/decade switching.

For single-walled carbon nanotube (SWNT) field effect transistors, vertical scaling of high kappa dielectrics by atomic layer deposition (ALD) currently stands at approximately 8 nm with a subthreshold swing S approximately 70-90 mV/decade at room temperature. ALD on as-grown pristine SWNTs is incapable of producing a uniform and conformal dielectric layer due to the lack of functional groups on nanotubes and because nucleation of an oxide dielectric layer in the ALD process hinges upon covalent chemisorption on reactive groups on surfaces. Here, we show that by noncovalent functionalization of SWNTs with poly-T DNA molecules (dT40-DNA), one can impart functional groups of sufficient density and stability for uniform and conformal ALD of high kappa dielectrics on SWNTs with thickness down to 2-3 nm. This enables approaching the ultimate vertical scaling limit of nanotube FETs and reliably achieving S approximately 60 mV/decade at room temperature, and S approximately 50 mV/decade in the band-to-band tunneling regime of ambipolar transport. We have also carried out microscopy investigations to understand ALD processes on SWNTs with and without DNA functionalization.

DNA↗
PubMed2006

Thermally and molecularly stimulated relaxation of hot phonons in suspended carbon nanotubes.

The high-bias electrical transport properties of suspended metallic single-walled carbon nanotubes (SWNTs) are investigated at various temperatures in vacuum, in various gases, and when coated with molecular solids. It is revealed that nonequilibrium optical phonon effects in suspended nanotubes decrease as the ambient temperature increases. Gas molecules surrounding suspended SWNTs assist the relaxation of hot phonons and afford enhanced current flow along nanotubes. Molecular solids of carbon dioxide frozen onto suspended SWNTs quench the nonequilibrium phonon effect. The discovery of strong environmental effects on high current transport in nanotubes is important to high performance nanoelectronics applications of 1D nanowires in general.

Journal Article↗
PubMed2006

Thermal conductance of an individual single-wall carbon nanotube above room temperature.

The thermal properties of a suspended metallic single-wall carbon nanotube (SWNT) are extracted from its high-bias (I-V) electrical characteristics over the 300-800 K temperature range, achieved by Joule self-heating. The thermal conductance is approximately 2.4 nW/K, and the thermal conductivity is nearly 3500 Wm(-1)K(-1) at room temperature for a SWNT of length 2.6 mum and diameter 1.7 nm. A subtle decrease in thermal conductivity steeper than 1/T is observed at the upper end of the temperature range, which is attributed to second-order three-phonon scattering between two acoustic modes and one optical mode. We discuss sources of uncertainty and propose a simple analytical model for the SWNT thermal conductivity including length and temperature dependence.

Journal Article↗
PubMed2006

Neural stimulation with a carbon nanotube microelectrode array.

We present a novel prototype neural interface using vertically aligned multiwalled carbon nanotube (CNT) pillars as microelectrodes. Functionalized hydrophilic CNT microelectrodes offer a high charge injection limit (1-1.6 mC/cm2) without faradic reactions. The first repeated in vitro stimulation of hippocampal neurons with CNT electrodes is demonstrated. These results suggest that CNTs are capable of providing far safer and more efficacious solutions for neural prostheses than previous metal electrode approaches.

Action Potentials↗
PubMed2006

Parallel core-shell metal-dielectric-semiconductor germanium nanowires for high-current surround-gate field-effect transistors.

Core-shell germanium nanowires (GeNW) are formed with a single-crystalline Ge core and concentric shells of nitride and silicon passivation layer by chemical vapor deposition (CVD), an Al2O3 gate dielectric layer by atomic layer deposition (ALD), and an Al metal surround-gate (SG) shell by isotropic magnetron sputter deposition. Surround-gate nanowire field-effect transistors (FETs) are then constructed using a novel self-aligned fabrication approach. Individual SG GeNW FETs show improved switching over GeNW FETs with planar gate stacks owing to improved electrostatics. FET devices comprised of multiple quasi-aligned SG GeNWs in parallel are also constructed. Collectively, tens of SG GeNWs afford on-currents exceeding 0.1 mA at low source-drain bias voltages. The self-aligned surround-gate scheme can be generalized to various semiconductor nanowire materials.

Journal Article↗
PubMed2005

Ultra-high-yield growth of vertical single-walled carbon nanotubes: Hidden roles of hydrogen and oxygen.

An oxygen-assisted hydrocarbon chemical vapor deposition method is developed to afford large-scale, highly reproducible, ultra-high-yield growth of vertical single-walled carbon nanotubes (V-SWNTs). It is revealed that reactive hydrogen species, inevitable in hydrocarbon-based growth, are damaging to the formation of sp(2)-like SWNTs in a diameter-dependent manner. The addition of oxygen scavenges H species and provides a powerful control over the C/H ratio to favor SWNT growth. The revelation of the roles played by hydrogen and oxygen leads to a unified and universal optimum-growth condition for SWNTs. Further, a versatile method is developed to form V-SWNT films on any substrate, lifting a major substrate-type limitation for aligned SWNTs.

Journal Article↗
PubMed2005

Negative differential conductance and hot phonons in suspended nanotube molecular wires.

Freely suspended metallic single-walled carbon nanotubes (SWNTs) exhibit reduced current carrying ability compared to those lying on substrates, and striking negative differential conductance at low electric fields. Theoretical analysis reveals significant self-heating effects including electron scattering by hot nonequilibrium optical phonons. Electron transport characteristics under strong self-heating are exploited for the first time to probe the thermal conductivity of individual SWNTs (approximately 3600 W m-1 K-1 at T=300 K) up to approximately 700 K, and reveal a 1/T dependence expected for umklapp phonon scattering at high temperatures.

Journal Article↗
PubMed2005

Functionalization of carbon nanotubes via cleavable disulfide bonds for efficient intracellular delivery of siRNA and potent gene silencing.

We present a novel functionalization scheme for single-walled carbon nanotubes (SWNTs) to afford nanotube-biomolecule conjugates with the incorporation of cleavable bonds to enable controlled molecular releasing from nanotube surfaces, thus creating "smart" nanomaterials with high potential for chemical and biological applications. With this versatile functionalization, we demonstrate transporting, enzymatic cleaving and releasing of DNA from SWNT transporters, and subsequent nuclear translocation of DNA oligonucleotides in mammalian cells. We further show highly efficient delivery of siRNA by SWNTs and achieving more potent RNAi functionality than a widely used conventional transfection agent. Thus, the novel functionalization of SWNTs with cleavable bonds is highly promising for a wide range of applications including gene and protein therapy.

DNA↗
PubMed2005

Electron transport in very clean, as-grown suspended carbon nanotubes.

Single-walled carbon nanotubes have shown a wealth of quantum transport phenomena thus far. Defect-free, unperturbed single-walled carbon nanotubes with well behaved or tunable metal contacts are important for probing the intrinsic electrical properties of nanotubes. Meeting these conditions experimentally is non-trivial owing to numerous disorder and randomizing factors. Here we show that approximately 1-microm-long fully suspended single-walled carbon nanotubes grown in place between metal contacts afford devices with well defined characteristics over much wider energy ranges than nanotubes pinned on substrates. Various low-temperature transport regimes in true-metallic, small- and large-bandgap semiconducting nanotubes are observed, including quantum states shell-filling, -splitting and -crossing in magnetic fields owing to the Aharonov-Bohm effect. The clean transport data show a correlation between the contact junction resistance and the various transport regimes in single-walled-carbon-nanotube devices. Furthermore, we show that electrical transport data can be used to probe the band structures of nanotubes, including nonlinear band dispersion.

Crystallization↗
PubMed2005

Regular arrays of 2 nm metal nanoparticles for deterministic synthesis of nanomaterials.

A novel method is developed to enable the formation, positioning, and patterning of individual metal nanoclusters with controllable and monodispersed sizes down to 1-2 nm scale. The method is generic for fabricating designed arrays of virtually any type of metal nanoparticles well below 10 nm. Among the wide range of potential applications in surface and materials science, the nanoparticle arrays are used for deterministic synthesis of monodispersed single-walled carbon nanotubes at individually controlled locations with near 1:1 yield, reaching one of the ultimate goals of nanotube synthesis.

Journal Article↗
PubMed2005

Oxidation resistant germanium nanowires: bulk synthesis, long chain alkanethiol functionalization, and Langmuir-Blodgett assembly.

A simple method is developed to synthesize gram quantities of uniform Ge nanowires (GeNWs) by chemical vapor deposition on preformed, monodispersed seed particles loaded onto a high surface area silica support. Various chemical functionalization schemes are investigated to passivate the GeNW surfaces using alkanethiols and alkyl Grignard reactions. The stability of functionalization against oxidation of germanium for various alkyl chain lengths is elucidated by X-ray photoelectron spectroscopy. Among all schemes tested, long chain alkanethiols (> or = C12) are found to impart the most stable GeNW passivation against oxidation upon extended exposure to ambient air. Further, the chemically functionalized oxidation-resistant nanowires are soluble in organic solvents and can be readily assembled into close-packed Langmuir-Blodgett films potentially useful for future high performance electronic devices.

Germanium↗
PubMed2005

Carbon nanotubes as multifunctional biological transporters and near-infrared agents for selective cancer cell destruction.

Biological systems are known to be highly transparent to 700- to 1,100-nm near-infrared (NIR) light. It is shown here that the strong optical absorbance of single-walled carbon nanotubes (SWNTs) in this special spectral window, an intrinsic property of SWNTs, can be used for optical stimulation of nanotubes inside living cells to afford multifunctional nanotube biological transporters. For oligonucleotides transported inside living cells by nanotubes, the oligos can translocate into cell nucleus upon endosomal rupture triggered by NIR laser pulses. Continuous NIR radiation can cause cell death because of excessive local heating of SWNT in vitro. Selective cancer cell destruction can be achieved by functionalization of SWNT with a folate moiety, selective internalization of SWNTs inside cells labeled with folate receptor tumor markers, and NIR-triggered cell death, without harming receptor-free normal cells. Thus, the transporting capabilities of carbon nanotubes combined with suitable functionalization chemistry and their intrinsic optical properties can lead to new classes of novel nanomaterials for drug delivery and cancer therapy.

Cell Death↗
PubMed2005

Carbon nanotubes as intracellular protein transporters: generality and biological functionality.

Various proteins adsorb spontaneously on the sidewalls of acid-oxidized single-walled carbon nanotubes. This simple nonspecific binding scheme can be used to afford noncovalent protein-nanotube conjugates. The proteins are found to be readily transported inside various mammalian cells with nanotubes acting as the transporter via the endocytosis pathway. Once released from the endosomes, the internalized protein-nanotube conjugates can enter into the cytoplasm of cells and perform biological functions, evidenced by apoptosis induction by transported cytochrome c. Carbon nanotubes represent a new class of molecular transporters potentially useful for future in vitro and in vivo protein delivery applications.

Animals↗
PubMed2005

On the origin of preferential growth of semiconducting single-walled carbon nanotubes.

A correlation is observed between the diameters (d) of single-walled carbon nanotubes and the percentages of metallic and semiconducting tubes synthesized at 600 degrees C by plasma-assisted chemical vapor deposition. Small tubes (d approximately 1.1 nm) show semiconductor percentages that are much higher than expected for a random chirality distribution. Density functional theory calculations reveal differences in the heat of formation energies for similar-diameter metallic, quasi-metallic, and semiconducting nanotubes. Semiconducting tubes exhibit the lowest energies and the stabilization scales with approximately 1/d(2). This could be a thermodynamic factor in the preferential growth of small semiconducting nanotubes.

Journal Article↗