The motion of electrons through quantum dots is strongly modified by single-electron charging and the quantization of energy levels1,2. Much effort has been directed towards extending studies of electron transport to chemical nanostructures, including molecules3,4,5,6,7,8, nanocrystals9,10,11,12,13 and nanotubes14,15,16,17. Here we report the fabrication of single-molecule transistors based on individual C60 molecules connected to gold electrodes. We perform transport measurements that provide evidence for a coupling between the centre-of-mass motion of the C60 molecules and single-electron hopping18—a conduction mechanism that has not been observed previously in quantum dot studies. The coupling is manifest as quantized nano-mechanical oscillations of the C60 molecule against the gold surface, with a frequency of about 1.2 THz. This value is in good agreement with a simple theoretical estimate based on van der Waals and electrostatic interactions between C60 molecules and gold electrodes.

Nanomechanical oscillations in a single-C60 transistor

We have derived the general solution of a wave equation describing the dynamics of two-layer viscoelastic polymer materials of arbitrary thickness deposited on solid (quartz) surfaces in a fluid environment. Within the Voight model of viscoelastic element, we calculate the acoustic response of the system to an applied shear stress, i.e. we find the shift of the quartz generator resonance frequency and of the dissipation factor, and show that it strongly depends on the viscous loading of the adsorbed layers and on the shear storage and loss moduli of the overlayers. These results can readily be applied to quartz crystal acoustical measurements of the viscoelasticity of polymers which conserve their shape under the shear deformations and do not flow, and layered structures such as protein films adsorbed from solution onto the surface of self-assembled monolayers.

https://iopscience.iop.org/article/10.1238/Physica.Regular.059a00391/pdf

Viscoelastic Acoustic Response of Layered Polymer Films at Fluid-Solid Interfaces: Continuum Mechanics Approach

Protein adhesion plays a major role in determining the biocompatibility of materials. The first stage of implant integration is the adhesion of protein followed by cell attachment. Surface modification of implants (surface chemistry and topography) to induce and control protein and cell adhesion is currently of great interest. This communication presents data on protein adsorption (bovine serum albumin and fibrinogen) onto model hydrophobic (CH3) and hydrophilic (OH) surfaces, investigated using a quartz crystal microbalance (QCM) and grazing angle infrared spectroscopy. Our data suggest that albumin undergoes adsorption via a single step whereas fibrinogen adsorption is a more complex, multistage process. Albumin has a stronger affinity toward the CH3 compared to OH terminated surface. In contrast, fibrinogen adheres more rapidly to both surfaces, having a slightly higher affinity toward the hydrophobic surface. Conformational assessment of the adsorbed proteins by grazing angle infrared spectroscopy (GA...

Interpretation of Protein Adsorption: Surface-Induced Conformational Changes

Supramolecular nanotube architectures based on amphiphilic molecules.

We have measured the time-resolved adsorption kinetics of the mussel adhesive protein (Mefp-1) on a nonpolar, methyl-terminated (thiolated) gold surface, using three independent techniques:  quartz crystal microbalance with dissipation monitoring (QCM-D), surface plasmon resonance, and ellipsometry. The QCM-D and ellipsometry data shows that, after adsorption to saturation of Mefp-1, cross-linking of the protein layer using NaIO4 transforms it from an extended (∼20 nm), water-rich, and hydrogel-like state to a much thinner (∼5 nm), compact, and less water-rich state. Furthermore, we show how quantitative data about the thickness, shear elastic modulus, and shear viscosity of the protein film can be obtained with the QCM-D technique, even beyond the Sauerbrey regime, if frequency (f) and energy dissipation (D) measurements measured at multiple harmonics are combined with theoretical simulations using a Voight-based viscoelastic model. The modeling result was confirmed by substituting H2O for D2O. As expect...

Variations in Coupled Water, Viscoelastic Properties, and Film Thickness of a Mefp-1 Protein Film during Adsorption and Cross-Linking: A Quartz Crystal Microbalance with Dissipation Monitoring, Ellipsometry, and Surface Plasmon Resonance Study

We have measured the energy dissipation of the quartz crystal microbalance(QCM), operating in the liquid phase, when mono- or multi-layers of bio-molecules and biofilms form on the QCM electrode (with a time resolution of ca. 1 s). Examples are taken from protein adsorption, lipid vesicle adsorption and cell adhesion studies. Our results show that even very thin (a few nm) biofilms dissipate a significant amount of energy owing to the QCM oscillation. Various mechanisms for this energy dissipation are discussed. Three main contributions to the measured increase in energy dissipation are considered. (i) A viscoelastic porous structure (the biofilm) that is strained during oscillation, (ii) trapped liquid that moves between or in and out of the pores due to the deformation of the film and (iii) the load from the bulk liquid which increases the strain of the film. These mechanisms are, in reality, not entirely separable, rather, they constitute an effective viscoelastic load. The biofilms can therefore not be considered rigidly coupled to the QCM oscillation. It is further shown theoretically that viscoelastic layers with thicknesses comparable to the biofilms studied in this work can induce energy dissipation of the same magnitude as the measured ones.

Simultaneous frequency and dissipation factor QCM measurements of biomolecular adsorption and cell adhesion

Missing mass effect in biosensor's QCM applications.

Room-temperature Coulomb blockade of charge transport through composite nanostructures containing organic interlinks has recently been observed. A pronounced charging effect in combination with the softness of the molecular links implies that charge transfer gives rise to a significant deformation of these structures. For a simple model system, we show that self-excitation of periodic cluster oscillations in conjunction with sequential processes of cluster charging and decharging appears for a sufficiently large bias voltage. This new ``electron shuttle'' mechanism of discrete charge transfer gives rise to a current through the nanostructure which is proportional to the cluster vibration frequency.

https://arxiv.org/pdf/cond-mat/9711196.pdf

Shuttle Mechanism for Charge Transfer in Coulomb Blockade Nanostructures

Methods based on self-assembly, self-organization, and forced shape transformations to form synthetic or semisynthetic enclosed lipid bilayer structures with several properties similar to biological nanocompartments are reviewed. The procedures offer unconventional micro- and nanofabrication routes to yield complex soft-matter devices for a variety of applications for example, in physical chemistry and nanotechnology. In particular, we describe novel micromanipulation methods for producing fluid-state lipid bilayer networks of nanotubes and surface-immobilized vesicles with controlled geometry, topology, membrane composition, and interior contents. Mass transport in nanotubes and materials exchange, for example, between conjugated containers, can be controlled by creating a surface tension gradient that gives rise to a moving boundary or by induced shape transformations. The network devices can operate with extremely small volume elements and low mass, to the limit of single molecules and particles at a length scale where a continuum mechanics approximation may break down. Thus, we also describe some concepts of anomalous fluctuation-dominated kinetics and anomalous diffusive behaviours, including hindered transport, as they might become important in studying chemistry and transport phenomena in these confined systems. The networks are suitable for initiating and controlling chemical reactions in confined biomimetic compartments for rationalizing, for example, enzyme behaviors, as well as for applications in nanofluidics, bioanalytical devices, and to construct computational and complex sensor systems with operations building on chemical kinetics, coupled reactions and controlled mass transport.

M. V. Voinova

Papers

Viscoelastic Acoustic Response of Layered Polymer Films at Fluid-Solid Interfaces: Continuum Mechanics Approach

Simultaneous frequency and dissipation factor QCM measurements of biomolecular adsorption and cell adhesion

Missing mass effect in biosensor's QCM applications.

Shuttle Mechanism for Charge Transfer in Coulomb Blockade Nanostructures

Biomimetic nanoscale reactors and networks.