Search

This comment on the paper "A comprehensive modeling and vibration analysis of AFM microcantilevers subjected to nonlinear tip-sample interaction forces" by Sohrab Eslami and Jalili (2012) [1] aims to: (1) discuss and elucidate the concept of "virtual resonance" and thus (2) avert a misinterpretation of the experimental results and findings reported in the Tetard et al. Physical Review Letters 106, 180801 (2011) [2]., (Copyright © 2013 Elsevier B.V. All rights reserved.)

Scanning probe microscopy has emerged as a powerful approach to a broader understanding of the molecular architecture of cell walls, which may shed light on the challenge of efficient cellulosic ethanol production. We have obtained preliminary images of both Populus and switchgrass samples using atomic force microscopy (AFM). The results show distinctive features that are shared by switchgrass and Populus. These features may be attributable to the lignocellulosic cell wall composition, as the collected images exhibit the characteristic macromolecular globule structures attributable to the lignocellulosic systems. Using both AFM and a single case of mode synthesizing atomic force microscopy (MSAFM) to characterize Populus, we obtained images that clearly show the cell wall structure. The results are of importance in providing a better understanding of the characteristic features of both mature cells as well as developing plant cells. In addition, we present spectroscopic investigation of the same samples.

The emerging interest in understanding the interactions of nanomaterial with biological systems necessitates imaging tools that capture the spatial and temporal distributions and attributes of the resulting nano-bio amalgam. Studies targeting organ specific response and/or nanoparticle-specific system toxicity would be profoundly benefited from tools that would allow imaging and tracking of in-vivo or in-vitro processes and particle-fate studies. Recently we demonstrated that mode synthesizing atomic force microscopy (MSAFM) can provide subsurface nanoscale information on the mechanical properties of materials at the nanoscale. However, the underlying mechanism of this imaging methodology is currently subject to theoretical and experimental investigation. In this paper we present further analysis by investigating tip-sample excitation forces associated with nanomechanical image formation. Images and force curves acquired under various operational frequencies and amplitudes are presented. We examine samples of mouse cells, where buried distributions of single-walled carbon nanohorns and silica nanoparticles are visualized.

This work demonstrated the feasibility of detecting divalent Cd(II) ions using antibody-modified microcantilever (MCL) sensors. Different surface modification methods were compared and multilayer approach was found superior than others for MCL surface modifications for antibody-based Cd(II) sensor development. When the Cd(II)-EDTA complex sample is injected into the fluid cell where the MCL is held, the MCL bends upon the recognition of the Cd(II) complex by the antibody on the surface of the MCL. Control experiments showed that complex that does not contain Cd(II) did not cause any bending of the MCL. The detection limit of the sensor was approximately 10(-9) M. The reaction rate analysis indicated that Langmuir adsorption model is appropriate to describe the absorption of Cd(II)-EDTA-BSA on the antibody-covered MCL surface.

We present an implementation of pure-time-delay generation in analog signals located in the kilo-Hertz frequency band. The controlled constant delays that are produced engage in a feedback system to investigate the dynamic response of microcantilevers. Delayed systems offer a vast richness of eigenvalues resulting in the possibility of excitations at frequencies other than that of the fundamental mode. Different cantilever actuation and delay generation approaches are investigated and compared, and detailed experimental observation of the dynamic response of the system is presented. Based on our results, an acoustic excitation is devised that may be used as an efficient sensor.

Hydrodynamic predictions of fluid velocity and pressure distribution are made for fluid in a confined space bounded by a vibrating microcantilever and a fixed surface. The results are used to quantify damping factors and predict frequency response amplitudes of a microcantilever vibrating near a fixed surface. The theoretical predictions of vibration response compare favorably with experimental data.

An analytical approach to determine the streamlines of fluid flow adjacent to the surfaces of vibrating cantilevers is presented. Fluid flow over the top and bottom surfaces of a microcantilever is established by solving two-dimensional Navier-Stokes equations for viscous flow. The x and y velocity components are used to establish streamlines for absolute fluid motion. These streamlines show a central stagnation core perpendicular and central to the cantilever surface extending along the full length of cantilevers, which most likely accounts for the added mass effect (induced mass) of fluid media around vibrating microcantilevers.

Microcantilevers undergo quasi-static bending due to adsorption-induced stress when adsorption is confined to a single surface. Understanding the origin of surface stress is crucial for optimizing sensor performance. We have investigated the effect of surface morphology of gold-coated cantilevers on the adsorption characteristics of self-assembled monolayers of alkanethiols. Self-assembly of alkanethiols from liquid phase closely follows Langmuir-type kinetics up to a single monolayer assembly. Our results indicate that alkanethiol adsorption-induced surface stress is largely unaffected by surface roughness of the cantilever. Unlike prior reports that suggest surface roughness enhances adsorption-induced stress, we observe that nanometer-size roughness slightly decreases surface stress and adsorption kinetics.

We present experimental results from an all-optical microfluidic platform that may be complimented by a thin film all-electrical network. Using these configurations we have studied the microfluidic convective flow systems of silicone oil, glycerol, and 1,3,5-trinitrotoluene on open surfaces through the production of surface tension gradients derived from thermal gradients. We show that sufficient localized thermal variation can be created utilizing surface plasmons and/or engaging individually addressable resistive thermal elements. Both studies manipulate fluids via Marangoni forces, each having their unique exploitable advantages. Surface plasmon excitation in metal foils are the driving engine of many physical-, chemical-, and bio-sensing applications. Incorporating, for the first time, the plasmon concept in microfluidics, our results thus demonstrate great potential for simultaneous fluid actuation and sensing.

Since the discovery in the late 18th century of electrically induced mechanical response in muscle tissue, coupling between electrical and mechanical phenomena has been shown to be a near-universal feature of biological systems. Here, we employ scanning probe microscopy (SPM) to measure the sub-Angstrom mechanical response of a biological system induced by an electric bias applied to a conductive SPM tip. Visualization of the spiral shape and orientation of protein fibrils with 5 nm spatial resolution in a human tooth and chitin molecular bundle orientation in a butterfly wing is demonstrated. In particular, the applicability of SPM-based techniques for the determination of molecular orientation is discussed.

Nanotechnology-based platforms for the high-throughput, multiplexed detection of proteins and nucleic acids in heretofore unattainable abundance ranges promise to bring substantial advances in molecular medicine. The emerging approaches reviewed in this article, with reference to their diagnostic potential, include nanotextured surfaces for proteomics, a two-particle sandwich assay for the biological amplification of low-concentration biomolecular signals, and silicon-based nanostructures for the transduction of molecular binding into electrical and mechanical signals, respectively.

We measured the desorption of explosive trinitrotoluene (TNT), pentaerythritol tetranitrate (PETN), and hexahydro-1,3,5-triazine (RDX) vapors from piezoresistive silicon microcantilevers under ambient air. Depending on the amount of vapor loaded on the cantilever, TNT desorption took a few minutes to tens of minutes (for nanogram quantities). On the other hand, no significant loss of PETN or RDX was observed after many hours. We also measured desorption of common "nonexplosive" compounds (water, acetone, and ethyl alcohol) and observed that desorption was too fast to be measured. There is a good correlation between the desorption time and the melting point (or the vapor pressure) of a particular substance. In principle, this method can be used to measure desorption rates of various substances from cantilever surfaces.

The potential-induced surface stress of a solid electrode was investigated in an electrochemical cell. Gold-coated atomic force microscopy microcantilevers were used as working electrodes to measure the current-potential response (by cyclic voltammetry) and simultaneous bending characteristics in solutions of NaNO3 and K3Fe(CN)6/NaNO3. The observed changes of differential surface stress at a microcantilever electrode were attributed to electrochemical-potential-induced changes in surface charge density, ion adsorption/desorption, and electron transfer across the electrode surface. The potential dependent change in stress shows promise for the study of microscopic properties at the solid-electrolyte interface.

The interference of surface plasmons can provide important information regarding the surface features of the hosting thin metal film. We present an investigation of the interference of optically excited surface plasmons in the Kretschmann configuration in the visible spectrum. Large area surface plasmon interference regions are generated at several wavelengths and imaged with the photon scanning tunneling microscope. Furthermore, we discuss the non-retarded dispersion relations for the surface plasmons in the probe-metal system modeled as confocal hyperboloids of revolution in the spheroidal coordinate systems.

Experimental observation of self-sustaining oscillations via a delayed feedback system is presented for a rectangular silicon microcantilever. The system is modeled as one and two-dimensional damped oscillator and the resulting delay differential equations are studied in frequency and time domain. The shortcomings of each model are outlined, and an improved formulation of the dynamics of the cantilever is presented.

Understanding the kinetics of adsorption and desorption of explosive vapors such as TNT from surfaces is important in the design of sensors. We report for the first time, the adsorption-desorption characteristics of TNT from a Si-microcantilever exposed to vapors of TNT. It was observed that TNT readily sticks to the exposed Si surface with the adsorption kinetics showing an initial exponential behavior followed by roughly linear kinetics. It was also observed that for cantilever temperatures close to room temperature, TNT desorbs spontaneously from the surface with decaying exponential kinetics. Based on the known equilibrium partial vapor pressures of TNT, the "effective" sticking coefficient for the silicon oxide surface at room temperature under the experimental conditions was calculated to be about 0.02. This information can be very useful in the design of sensors and that of vapor-delivery systems.

The variation in resonance response of microcantilevers was investigated as a function of pressure (10(-2)-10(6)Pa) and temperature (290-390K) in atmospheres of helium (He) and dry nitrogen (N(2)). Our results for a silicon cantilever under vacuum show that the frequency varies in direct proportion to the temperature. The linear response is explained by the decrease in Young's modulus with increasing the temperature. However, when the cantilever is bimaterial, the response is nonlinear due to differential thermal expansion. Resonance response as a function of pressure shows three different regions, which correspond to molecular flow regime, transition regime, and viscous regime. The deflection in flow transition regime resulting from thermal variation has minimal effect on frequency. The frequency variation of the cantilever is caused mainly by changes in the mean free path of gas molecules.

The Knudsen effect is estimated theoretically and observed experimentally using a U-shaped silicon microcantilever. Though Knudsen forces are extremely small in most cases involving microcantilevers, there exist situations where these forces can be significant and may be important in atomic force microscopy and in microelectromechanical systems (MEMS). The criteria for the presence of Knudsen forces are outlined and an analytical expression in the form of a linear function of the pressure is given for the force in the free molecular regime. The experimental results display peaks in the transitional regime while varying linearly in the molecular regime.

We have investigated chemical reactions between adsorbed water and active sites on a silicon nitride surface as a function of temperature and relative humidity using microcantilevers. Effects that might produce a change in the response of the microcantilever, such as a mass adsorption, surface tension of the adsorbed water, and changes in thermal conductivity, were systematically investigated. It is shown that the judicious choice of experimental conditions could make these effects essentially inconsequential in comparison with the instrument response produced by the change in free surface energy of the microcantilever due to the chemical reactions. Using this method, the variation in free surface energy when changing from dry to high humidity conditions was found and the number of active sites that reacted was estimated. This method may be extended to other problems for use in determining surface free energy change and thus the density of reactant sites under different conditions of interest.

Study of vertical transport through heterostructures consisting of single, double, or multiple quantum barriers is of both fundamental and technological interest. While extensive data regarding electron transport is available for single- and double-barrier structures, relatively less information is available for transport through step-barrier structures. In this paper, we present results from a study of room temperature vertical transport through a GaAs/GaAlAs/InAlAs/GaAs multistep-barrier heterostructure. A typical atomic force microscope has been adapted to perform transport measurements, thus allowing precise control of the physical location of the region of measurement. I-V measurements reveal negative differential resistance (NDR) peaks, thus confirming the formation of resonant states in a triangular well created when a voltage bias is applied across the step barrier. I-V curves have also been calculated by numerically solving the Schrödinger wave equation for this step-barrier structure. Comparison between the measured and calculated I-V curves shows reasonable agreement in the number of NDR peaks. However, discrepancies exist between the measured and calculated values for the voltages at which these NDR peaks occur. Some possible reasons for these discrepancies are discussed in this work.

We describe a novel technique for measuring magnetic susceptibilities of nanogram quantities of magnetic materials that utilizes the extreme force sensitivity of microcantilevers. The magnetic force acting on samples attached to the free end of a cantilever can be measured as changes in the resonance response of the cantilever. The shift in resonance frequency of the cantilever is proportional to the field gradient, whereas the deflection of a cantilever is proportional to the magnetic force. The magnetic susceptibility measurement is based on comparison of the forces acting on the sample and a reference material in the same magnetic field and field gradient. We have determined the magnetic susceptibilities of nanogram quantities of many paramagnetic materials. The measured magnetic susceptibilities show excellent agreement with values found in the literature.

We have investigated electrostatic spraying of DNA onto gold surfaces as an alternative sample-preparation technique for STM studies. Preliminary results show that a higher distribution of isolated strands as well as well ordered aggregates can be obtained with this technique when compared with electrodeposition or drop evaporation. In many places, the well ordered aggregates were found to cleave in a direction perpendicular to their length after repeated scanning in the same direction.

We have employed an atomic force microscope (AFM) to image in air isolated strands of pBS+ plasmid DNA adsorbed onto freshly cleaved mica. At a DNA concentration below 0.3 micrograms/ml isolated strands of the plasmid DNA are usually seen, while for concentrations higher than 3 micrograms/ml a uniform coverage of interconnected DNA strands was observed. We found that the contrast and the width of DNA were dependent upon humidity. When the relative humidity exceeds 60%, negative contrast images with strand widths 20 times the width of DNA are found, while positive contrast images with 7 to 10 times the width of DNA are found when the humidity is below 30%. By placing the AFM in an environment where the humidity could be controlled, we were able to switch between positive and negative contrasts.

pBS+ plasmid deoxyribonucleic acid (DNA) was imaged by scanning tunneling microscopy (STM) after mounting microdroplets by aerosol deposition onto heated epitaxial gold surfaces. However, the instability of the adsorbate to forces exerted by the tunneling tip points out the need for more aggressive bonding of molecules to surfaces. We describe a sensitive assay for the qualitative and quantitative evaluation of chemical agents to influence binding of DNA to surfaces using 32P-labeled pBS+ plasmid DNA. We propose that such an assay can make an important contribution to immobilization techniques prior to STM imaging.

We have studied gold and graphite electrodes in an electrochemistry cell under various solutions using the scanning tunneling microscope (STM). The gold (111) surface yields quite reproducible images and cyclic voltammograms. In situ voltammograms show that, under certain conditions, nanomolar quantities of DNA fragments can suppress the adsorption of a buffer salt of millimolar concentration. When the DNA concentration is reduced below that required for a monolayer coverage, the salt adsorption is restored. We show images of bare gold, gold covered with an adsorbate produced by the buffer salt, and gold prepared with a concentration of DNA fragments close to that required for monolayer coverage added to the buffer. Under these conditions, the surface is found to be uniformly covered with a characteristic structure.