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    ABSTRACT: We have investigated the ability of dual-frequency Coherent Antistokes Raman Scattering (D-CARS) micro-spectroscopy, based on femtosecond pulses (100 fs or 5 fs) spectrally focussed by glass dispersion, to distinguish the chemical composition of micron-sized lipid droplets consisting of different triglycerides types (poly-unsaturated glyceryl trilinolenate, mono-unsaturated glyceryl trioleate and saturated glyceryl tricaprylate and glyceryl tristearate) in a rapid and label-free way. A systematic comparison of Raman spectra with CARS and D-CARS spectra was used to identify D-CARS spectral signatures which distinguish the disordered poly-unsaturated lipids from the more ordered saturated ones both in the CH-stretch vibration region and in the fingerprint region, without the need for lengthy CARS multiplex acquisition and analysis. D-CARS images of the lipid droplets at few selected wavenumbers clearly resolved the lipid composition differences, and exemplify the potential of this technique for label-free chemically selective rapid imaging of cytosolic lipid droplets in living cells. (© 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim).
    Journal of Biophotonics 01/2014; 7(1-2). DOI:10.1002/jbio.201200197
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    ABSTRACT: We report a simple technique for mapping Electrostatic Force Microscopy (EFM) bias sweep data into 2D images. The method allows simultaneous probing, in the same scanning area, of the contact potential difference and the second derivative of the capacitance between tip and sample, along with the height information. The only required equipment consists of a microscope with lift-mode EFM capable of phase shift detection. We designate this approach as Scanning Probe Potential Electrostatic Force Microscopy (SPP-EFM). An open-source MATLAB Graphical User Interface (GUI) for images acquisition, processing and analysis has been developed. The technique is tested with Indium Tin Oxide (ITO) and with poly(3-hexylthiophene) (P3HT) nanowires for organic transistor applications.
    Scientific Reports 11/2013; 3:3352. DOI:10.1038/srep03352
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    ABSTRACT: We report scanning tunnelling microscope (STM) measurements of the single molecule conductance of α,ω-alkanedithiols for a large range of molecular chain lengths (N = 3-10) and temperatures (180-390 K) under ultra high vacuum. Two STM-based measurement techniques were employed on molecules trapped between tip and substrate: (i) the well established current-distance or I(z) technique and (ii) a new I(V,z) technique in which the current-voltage characteristics are determined as the tip-substrate distance z is varied. Low, medium, and high conductance groups were observed for each molecular length, which were temperature independent over the range examined, consistent with off-resonance tunnelling. For N > 4 the current-voltage characteristics and conductance trend with chain length is well described using a simple rectangular tunnel barrier model with parameters in excellent agreement with previously reported values. However, both 1,3-propanedithiol (N = 3) and 1,4-butanedithiol (N = 4) show an anomalous behaviour which is qualitatively similar to, but much less pronounced than, that reported by Haiss et al. (Phys. Chem. Chem. Phys., 2009, 11, 10831) for measurements performed under air and nitrogen gas.
    Nanoscale 08/2013; 5(19). DOI:10.1039/c3nr03682k
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    ABSTRACT: In the era of high precision CMB measurements, systematic effects are beginning to limit the ability to extract subtler cosmological information. The non-circularity of the experimental beam has become progressively important as CMB experiments strive to attain higher angular resolution and sensitivity. The effect of non-circular beam on the power spectrum is important at multipoles larger than the beam-width. For recent experiments with high angular resolution, optimal methods of power spectrum estimation are computationally prohibitive and sub-optimal approaches, such as the Pseudo-Cl method are used. We provide an analytic framework for correcting the power spectrum for the effect of beam non-circularity and non-uniform sky coverage (including incomplete/masked sky maps). The approach is perturbative in the distortion of the beam from non-circularity allowing for rapid computations when the beam is mildly non-circular. We advocate that when the non-circular beams are important, it is computationally advantageous to employ ‘soft’ azimuthally apodized masks whose spherical harmonic transforms die down fast with m.
    New Astronomy Reviews 07/2013; DOI:10.1016/j.newar.2006.09.011
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    ABSTRACT: In the last decade, coherent anti-Stokes Raman scattering (CARS) microscopy has emerged as a powerful multiphoton imaging technique offering label-free chemical sensitivity and high three-dimensional resolution. However, its widespread application in the life sciences has been hampered by the use of costly pulsed lasers, the existence of a nonresonant background requiring involved technical solutions for its efficient suppression, and the limited acquisition speed of multiplex techniques addressing several vibrational resonances, if improved chemical specificity is needed. We have recently reported a differential CARS technique (D-CARS), which simultaneously measures two vibrational frequencies, enhancing the chemical selectivity and sensitivity without introducing costly hardware, while maintaining fast acquisition. In this study, we demonstrate a compact, fully automated, cost-effective module, which integrates on hardware and software level with a commercial multiphoton microscope based on a single 100 fs Ti:Sapphire oscillator and enables D-CARS microscopy in a user-friendly format for applications in the life sciences.
    Journal of Biomedical Optics 06/2013; 18(6):66004. DOI:10.1117/1.JBO.18.6.066004
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    ABSTRACT: A Reply to the Comment by M. J. Fernée, et al..
    Physical Review Letters 11/2012; 109(22):229702. DOI:10.1103/PhysRevLett.109.229702
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    ABSTRACT: Under optical excitation, coupled quantum wells are known to reveal fascinating features in the photoluminescence pattern originating from dipole orientated indirect excitons. The appearance of an external ring has been attributed to macroscopic charge separation in the quantum well plane. We present a classical model of non-linear diffusion to account for the observed fragmentation of the external ring into a periodic array of islands. The model incorporates the Coulomb interactions between electrons, holes and indirect excitons. At low temperatures, these interactions lead to pattern formation similar to the experimentally observed ring fragmentation. The fragmentation is found to persist to temperatures above the quantum degeneracy temperature of indirect excitons.
    Physical Review Letters 11/2012; 109(18):187402. DOI:10.1103/PhysRevLett.109.187402
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    ABSTRACT: The electron transfer properties of proteins are normally measured as molecularly averaged ensembles. Through these and related measurements, proteins are widely regarded as macroscopically insulating materials. Using scanning tunnelling microscopy (STM), we present new measurements of the conductance through single-molecules of the electron transfer protein cytochrome b(562) in its native conformation, under pseudo-physiological conditions. This is achieved by thiol (SH) linker pairs at opposite ends of the molecule through protein engineering, resulting in defined covalent contact between a gold surface and a platinum-iridium STM tip. Two different orientations of the linkers were examined: a long-axis configuration (SH-LA) and a short-axis configuration (SH-SA). In each case, the molecular conductance could be 'gated' through electrochemical control of the heme redox state. Reproducible and remarkably high conductance was observed in this relatively complex electron transfer system, with single-molecule conductance values peaking around 18 nS and 12 nS for the SH-SA and SH-LA cytochrome b(562) molecules near zero electrochemical overpotential. This strongly points to the important role of the heme co-factor bound to the natively structured protein. We suggest that the two-step model of protein electron transfer in the STM geometry requires a multi-electron transfer to explain such a high conductance. The model also yields a low value for the reorganisation energy, implying that solvent reorganisation is largely absent.
    Nanoscale 10/2012; 4:7106-7113. DOI:10.1039/c2nr32131a
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    ABSTRACT: We perform an extensive numerical study of coalescing black-hole binaries to understand the gravitational-wave spectrum of quasinormal modes excited in the merged black hole. Remarkably, we find that the masses and spins of the progenitor are clearly encoded in the mode spectrum of the ringdown signal. Some of the mode amplitudes carry the signature of the binary's mass ratio, while others depend critically on the spins. Simulations of precessing binaries suggest that our results carry over to generic systems. Using Bayesian inference, we demonstrate that it is possible to accurately measure the mass ratio and a proper combination of spins even when the binary is itself invisible to a detector. Using a mapping of the binary masses and spins to the final black-hole spin allows us to further extract the spin components of the progenitor. Our results could have tremendous implications for gravitational astronomy by facilitating novel tests of general relativity using merging black holes.
    Physical Review Letters 10/2012; 109(14):141102. DOI:10.1103/PhysRevLett.109.141102
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    ABSTRACT: An electron transfer protein is engineered with two thiol groups introduced at different positions in the molecular structure to allow robust binding to two gold electrodes. Atomic force microscopy and scanning tunneling microscopy single-molecule studies show that the engineered proteins: (1) bind to a gold electrode in defined orientation dictated by the thiol-pair utilised, and (2) have a higher conductance than the wild-type proteins indicating a more efficient electron transmission due to the strong gold-thiol contacts.
    Small 08/2012; 8(15):2341-4. DOI:10.1002/smll.201102416
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