[Show abstract][Hide abstract] 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.
[Show abstract][Hide abstract] 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.
[Show abstract][Hide abstract] 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.
[Show abstract][Hide abstract] 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 nonlinear 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.
[Show abstract][Hide abstract] 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.
[Show abstract][Hide abstract] 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.
[Show abstract][Hide abstract] ABSTRACT: We have measured the intrinsic exciton dephasing in high-quality zinc blende CdSe/CdS colloidal quantum dots in the temperature range from 5 to 170 K using a sensitive three-beam photon echo technique in heterodyne detection, which is not affected by spectral diffusion. Pure dephasing via acoustic phonons dominates the initial dynamics, followed by an exponential zero-phonon line dephasing. From the temperature dependence of the zero-phonon line dephasing, the exciton lifetime, and the exciton thermalization within its fine structure, we show that the zero-phonon line dephasing of the lowest bright state originates from the phonon-assisted spin-flip to dark exciton states. Importantly, we can control the dephasing by tailoring the exciton fine structure through its dependence on the dot core size and shell thickness, as expected from the spin-flip mechanism. By reducing the electron-hole exchange interaction with increasing core size and delocalization of the electron wave function in the quasi-type-II core/shell band alignment, we find the longest zero-phonon line dephasing time of ∼110 ps at 5 K in dots with the largest core diameter (5.7 nm) and the thickest CdSe shell (9 monolayers) in the series studied.
[Show abstract][Hide abstract] 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 05/2012; 8(15):2341-4.
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