School of Chemistry - Research Publications
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ItemElectronic Structure Engineering in ZnSe/CdS Type-II Nanoparticles by Interface Alloying(American Chemical Society, 2014-06-19)We report the synthesis and characterization of type-II ZnSe/CdS semiconductor nanocrystals that exhibit strong charge separation, high photoluminescence quantum yields, low optical gain thresholds, and alloyed core–shell interfaces. Shell growth rates and the degree of alloying both depend strongly on the shelling temperature. The core–shell NCs exhibit band edge PL with emission wavelengths spanning the blue to orange region of the electromagnetic spectrum (380–562 nm). Fluorescence quantum yields up to 75% can be obtained by deposition of an additional ZnS layer. Transient absorption spectroscopy reveals that the population of the first two exciton states (1Se–1Sh, 1Se–2Sh) in the type-II structures can be controlled by alloying. Increased alloying leads to a greater population of the 2S hole state exciton.
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ItemNo Preview AvailableCharacterization of Size, Anisotropy, and Density Heterogeneity of Nanoparticles by Sedimentation Velocity(AMER CHEMICAL SOC, 2014-08-05)A critical problem in materials science is the accurate characterization of the size dependent properties of colloidal inorganic nanocrystals. Due to the intrinsic polydispersity present during synthesis, dispersions of such materials exhibit simultaneous heterogeneity in density ρ, molar mass M, and particle diameter d. The density increments ∂ρ/∂d and ∂ρ/∂M of these nanoparticles, if known, can then provide important information about crystal growth and particle size distributions. For most classes of nanocrystals, a mixture of surfactants is added during synthesis to control their shape, size, and optical properties. However, it remains a challenge to accurately determine the amount of passivating ligand bound to the particle surface post synthesis. The presence of the ligand shell hampers an accurate determination of the nanocrystal diameter. Using CdSe and PbS semiconductor nanocrystals, and the ultrastable silver nanoparticle (M4Ag44(p-MBA)30), as model systems, we describe a Custom Grid method implemented in UltraScan-III for the characterization of nanoparticles and macromolecules using sedimentation velocity analytical ultracentrifugation. We show that multiple parametrizations are possible, and that the Custom Grid method can be generalized to provide high resolution composition information for mixtures of solutes that are heterogeneous in two out of three parameters. For such cases, our method can simultaneously resolve arbitrary two-dimensional distributions of hydrodynamic parameters when a third property can be held constant. For example, this method extracts partial specific volume and molar mass from sedimentation velocity data for cases where the anisotropy can be held constant, or provides anisotropy and partial specific volume if the molar mass is known.
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ItemNo Preview AvailableMonitoring ion-channel function in real time through quantum decoherence(NATL ACAD SCIENCES, 2010-11-02)In drug discovery, there is a clear and urgent need for detection of cell-membrane ion-channel operation with wide-field capability. Existing techniques are generally invasive or require specialized nanostructures. We show that quantum nanotechnology could provide a solution. The nitrogen-vacancy (NV) center in nanodiamond is of great interest as a single-atom quantum probe for nanoscale processes. However, until now nothing was known about the quantum behavior of a NV probe in a complex biological environment. We explore the quantum dynamics of a NV probe in proximity to the ion channel, lipid bilayer, and surrounding aqueous environment. Our theoretical results indicate that real-time detection of ion-channel operation at millisecond resolution is possible by directly monitoring the quantum decoherence of the NV probe. With the potential to scan and scale up to an array-based system, this conclusion may have wide-ranging implications for nanoscale biology and drug discovery.
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ItemFilling schemes at submicron scale: Development of submicron sized plasmonic colour filters(NATURE PORTFOLIO, 2014-09-22)The pixel size imposes a fundamental limit on the amount of information that can be displayed or recorded on a sensor. Thus, there is strong motivation to reduce the pixel size down to the nanometre scale. Nanometre colour pixels cannot be fabricated by simply downscaling current pixels due to colour cross talk and diffraction caused by dyes or pigments used as colour filters. Colour filters based on plasmonic effects can overcome these difficulties. Although different plasmonic colour filters have been demonstrated at the micron scale, there have been no attempts so far to reduce the filter size to the submicron scale. Here, we present for the first time a submicron plasmonic colour filter design together with a new challenge - pixel boundary errors at the submicron scale. We present simple but powerful filling schemes to produce submicron colour filters, which are free from pixel boundary errors and colour cross- talk, are polarization independent and angle insensitive, and based on LCD compatible aluminium technology. These results lay the basis for the development of submicron pixels in displays, RGB-spatial light modulators, liquid crystal over silicon, Google glasses and pico-projectors.
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ItemDetection of atomic spin labels in a lipid bilayer using a single-spin nanodiamond probe(NATL ACAD SCIENCES, 2013-07-02)Magnetic field fluctuations arising from fundamental spins are ubiquitous in nanoscale biology, and are a rich source of information about the processes that generate them. However, the ability to detect the few spins involved without averaging over large ensembles has remained elusive. Here, we demonstrate the detection of gadolinium spin labels in an artificial cell membrane under ambient conditions using a single-spin nanodiamond sensor. Changes in the spin relaxation time of the sensor located in the lipid bilayer were optically detected and found to be sensitive to near-individual (4 ± 2) proximal gadolinium atomic labels. The detection of such small numbers of spins in a model biological setting, with projected detection times of 1 s [corresponding to a sensitivity of ∼5 Gd spins per Hz(1/2)], opens a pathway for in situ nanoscale detection of dynamical processes in biology.
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ItemSurface plasmon coupling in end-to-end linked gold nanorod dimers and trimers(ROYAL SOC CHEMISTRY, 2013)Colloidal gold nanorods were aligned end-to-end via dithiol coupling. The scattering properties of the resultant nanostructures were investigated at the single particle level by combining dark-field microscopy and high resolution scanning electron microscopy. The longitudinal surface plasmon resonance of end-to-end coupled Au nanorods exhibited a red-shift as the number of rods in the chain increased. The nanostructures exhibited polarization-dependent optical properties, due to selective excitation of collective bonding and anti-bonding modes. The surface plasmon peak energy was not strongly dependent on the angle of rod-sphere-rod trimers. The experimental scattering spectra were compared with the results obtained from theoretical calculations using the Finite Element Method (FEM) and found to be in good agreement.