No Arabic abstract
DNA origami is a modular platform for the combination of molecular and colloidal components to create optical, electronic, and biological devices. Integration of such nanoscale devices with microfabricated connectors and circuits is challenging: large numbers of freely diffusing devices must be fixed at desired locations with desired alignment. We present a DNA origami molecule whose energy landscape on lithographic binding sites has a unique maximum. This property enables device alignment within 3.2$^{circ}$ on SiO$_2$. Orientation is absolute (all degrees of freedom are specified) and arbitrary (every molecules orientation is independently specified). The use of orientation to optimize device performance is shown by aligning fluorescent emission dipoles within microfabricated optical cavities. Large-scale integration is demonstrated via an array of 3,456 DNA origami with 12 distinct orientations, which indicates the polarization of excitation light.
Surface enhanced Raman scattering (SERS) is optically sensitive and chemically specific to detect single molecule spectroscopic signatures. Facilitating this capability in optically-trapped nanoparticles at low laser power remains a significant challenge. In this letter, we show single molecule SERS signatures in reversible assemblies of trapped plasmonic nanoparticles using a single laser excitation (633 nm). Importantly, this trap is facilitated by the thermoplasmonic field of a single gold nanoparticle dropcasted on a glass surface. We employ bi-analyte SERS technique to ascertain the single molecule statistical signatures, and identify the critical parameters of the thermoplasmonic tweezer that provide this sensitivity. Furthermore, we show the utility of this low power ($approx$0.1 mW/$mu$m^2) tweezer platform to trap single gold nanoparticle and transport assembly of nanoparticles. Given that our configuration is based on a dropcasted gold nanoparticle, we envisage its utility to create reconfigurable plasmonic metafluids in physiological and catalytic environments, and can be potentially adapted as an in-vivo plasmonic tweezer.
This mini review focuses on conductance measurements through molecular junctions containing few tens of molecules, which are fabricated along two approaches: (i) conducting atomic force microscope contacting a self-assembled monolayers on metal surface, and (ii) tiny molecular junctions made of metal nanodot (diameter < 10 nm), covered by fewer than 100 molecules and contacted by a conducting atomic force microscope. In particular, this latter approach has allowed to obtain new results or to revisit previous ones, which are reviewed here: (i) how the electron transport properties of molecular junctions are modified by mechanical constraint, (ii) the role of intermolecular interactions on the shape of conductance histograms of molecular junctions, and (iii) the demonstration that a molecular diode can operate in the microwave regime up to 18 GHz.
We report a comparison of two photonic techniques for single-molecule sensing: fluorescence nanoscopy and optoplasmonic sensing. As the test system, oligonucleotides with and without fluorescent labels are transiently hybridized to complementary docking strands attached to gold nanorods. Comparing the measured single-molecule kinetics helps to examine the influence of fluorescent labels as well as factors arising from different sensing geometries. Our results demonstrate that DNA dissociation is not significantly altered by the fluorescent label, while DNA association is affected by geometric factors in the two techniques. These findings open the door to exploiting plasmonic sensing and fluorescence nanoscopy in a complementary fashion, which will aid in building more powerful sensors and uncovering the intricate effects that influence the behavior of single molecules.
Nanomagnetometry using the nitrogen-vacancy (NV) centre in diamond has attracted a great deal of interest because of the combined features of room temperature operation, nanoscale resolution and high sensitivity. One of the important goals for nano-magnetometry is to be able to detect nanoscale nuclear magnetic resonance (NMR) in individual molecules. Our theoretical analysis shows how a single molecule at the surface of diamond, with characteristic NMR frequencies, can be detected using a proximate NV centre on a time scale of order seconds with nanometer precision. We perform spatio-temporal resolution optimisation and also outline paths to greater sensitivity. In addition, the method is suitable for application in low and relatively inhomogeneous background magnetic fields in contrast to both conventional liquid and solid state NMR spectroscopy.
Nanopore desalination technology hinges on high water-permeable membranes which, at the same time, block ions efficiently. In this study, we consider a recently synthesized [Science 363, 151-155 (2019)] phenine nanotube (PNT) for water desalination applications. Using both equilibrium and non-equilibrium molecular dynamics simulations, we show that the PNT membrane completely rejects salts, but permeates water at a rate which is an order-of-magnitude higher than that of all the membranes used for water filtration. We provide the microscopic mechanisms of salt rejection and fast water-transport by calculating the free-energy landscapes and electrostatic potential profiles. A collective diffusion model accurately predicts the water permeability obtained from the simulations over a wide range of pressure gradients. We propose a method to calculate the osmotic pressure ($Pi$) from the simulation data and find that $Pi$ across the membrane is very low (~1-2 MPa), which thus makes it a suitable nanomaterial for energy-efficient reverse osmosis. These remarkable properties of PNT can be applied in various nanofluidic applications, such as ion-selective channels, ionic transistors, sensing, molecular sieving, and blue energy harvesting.