Toward a New Primary Standardization of Radionuclide Massic Activity Using Microcalorimetry and Quantitative Milligram-Scale Samples.

We present a new paradigm for the primary standardization of radionuclide activity per mass of solution (Bq/g). Two key enabling capabilities are 4π decay-energy spectrometry using chip-scale sub-Kelvin microcalorimeters and direct realization of mass by gravimetric inkjet dispensing using an electrostatic force balance. In contrast to traditional traceability, which typically relies on chemical separation of single-radionuclide samples, 4π integral counting, and additional spectrometry methods to verify purity, the system described here has both 4π counting efficiency and spectroscopic resolution sufficient to identify multiple radionuclides in the same sample at once. This enables primary standardization of activity concentrations of mixed-radionuclide samples. A major benefit of this capability, beyond metrology, is in assay of environmental and forensics samples, for which the quantification of multiplenuclide samples can be achieved where presently inhibited by interferences. This can be achieved without the need for chemical separations or efficiency tracers, thereby vastly reducing time, radioactive waste, and resulting measurement uncertainty.

Simplified kilogram traceability for high-power laser measurement using photon momentum radiometers.

Photon momentum radiometers measure the force imparted by a reflected laser beam to determine the laser's optical power. This requires high-accuracy calibration of the force sensors using milligram and microgram mass artifacts. Calibrated test masses can therefore be used to provide traceability of these radiometers to the International System of Units, but low-noise calibration at these mass levels is difficult. Here, we present the improvement in calibration capability that we have gained from implementing a robotic mass delivery system. We quantify this in terms of the specific nuances of force measurements as implemented for laser power metrology.

Accurate flexural spring constant calibration of colloid probe cantilevers using scanning laser Doppler vibrometry.

Calibration of the flexural spring constant for atomic force microscope (AFM) colloid probe cantilevers provides significant challenges. The presence of a large attached spherical added mass complicates many of the more common calibration techniques such as reference cantilever, Sader, and added mass. Even the most promising option, AFM thermal calibration, can encounter difficulties during the optical lever sensitivity measurement due to strong adhesion and friction between the sphere and a surface. This may cause buckling of the end of the cantilever and hysteresis in the approach-retract curves resulting in increased uncertainty in the calibration. Most recently, a laser Doppler vibrometry thermal method has been used to accurately calibrate the normal spring constant of a wide variety of tipped and tipless commercial cantilevers. This paper describes a variant of the technique, scanning laser Doppler vibrometry, optimized for colloid probe cantilevers and capable of spring constant calibration uncertainties near ±1%.

Gravimetric deposition of microliter drops with radiometric confirmation.

A manual microliter gravimetric dispensing technique is demonstrated using a micropipettor modified for use with removeable microcapillaries. Liquid scintillation sources were prepared from a well-characterized 241Am reference solution, providing a radiometric check of dispensed masses. Further experiments confirmed controlled dispensing of drops onto gold foils with losses ≤0.34(4) % of the total drop activity. A detailed measurement equation for the weighing technique, including the corrections for evaporation, is presented with a full accounting of associated uncertainties.

Toggling bistable atoms via mechanical switching of bond angle.

We reversibly switch the state of a bistable atom by direct mechanical manipulation of bond angle using a dynamic force microscope. Individual buckled dimers at the Si(100) surface are flipped via the formation of a single covalent bond, actuating the smallest conceivable in-plane toggle switch (two atoms) via chemical force alone. The response of a given dimer to a flip event depends critically on both the local and nonlocal environment of the target atom-an important consideration for future atomic scale fabrication strategies.

The stiffness of collagen fibrils influences vascular smooth muscle cell phenotype.

Cells receive signals from the extracellular matrix through receptor-dependent interactions, but they are also influenced by the mechanical properties of the matrix. Although bulk properties of substrates have been shown to affect cell behavior, we show here that nanoscale properties of collagen fibrils also play a significant role in determining cell phenotype. Type I collagen fibrils assembled into thin films provide excellent viewing of cells interacting with individual fibrils. Cells can be observed to extensively manipulate the fibrils, and this behavior seems to result in an incompletely spread stellate morphology and a nonproliferative phenotype that is typical of these cells in collagen gels. We show here that thin films of collagen fibrils can be dehydrated, and when seeded on these dehydrated fibrils, smooth muscle cells spread and proliferate extensively. The dehydrated collagen fibrils appear to be similar to the fully hydrated collagen fibrils in topology and in presentation of beta(1) integrin ligation sites, but they are mechanically stiffer. This decrease in compliance of dehydrated fibrils is seen by a failure of cell movement of dehydrated fibrils compared to their ability to rearrange fully hydrated fibrils and from direct measurements by nanoindentation and quantitative atomic force measurements. We suggest that increase in the nanoscale rigidity of collagen fibrils can cause these cells to assume a proliferative phenotype.

A simple method for the determination of qPlus sensor spring constants.

qPlus sensors are widely used to measure forces at the atomic scale, however, confidence in these measurements is limited by inconsistent reports of the spring constant of the sensor and complications from finite tip heights. Here we combine a numerical investigation of the force reconstruction with an experimental characterization of the flexural mechanics of the qPlus sensor. Numerical studies reveal significant errors in reconstructed force for tip heights exceeding 400 µm or one sixth of the cantilever length. Experimental results with a calibrated nanoindenter reveal excellent agreement with an Euler-Bernoulli beam model for the sensor. Prior to the attachment of a tip, measured spring constants of 1902 ± 29 N/m are found to be in agreement with theoretical predictions for the geometry and material properties of the sensor once a peaked ridge in the beam cross section is included. We further develop a correction necessary to adjust the spring constant for the size and placement of the tip.

Calculation of the effect of tip geometry on noncontact atomic force microscopy using a qPlus sensor.

In qPlus atomic force microscopy the tip length can in principle approach the length of the cantilever. We present a detailed mathematical model of the effects this has on the dynamic properties of the qPlus sensor. The resulting, experimentally confirmed motion of the tip apex is shown to have a large lateral component, raising interesting questions for both calibration and force-spectroscopy measurements.

Accurate noncontact calibration of colloidal probe sensitivities in atomic force microscopy.

The absolute force sensitivities of colloidal probes comprised of atomic force microscope, or AFM, cantilevers with microspheres attached to their distal ends are measured. The force sensitivities are calibrated through reference to accurate electrostatic forces, the realizations of which are described in detail. Furthermore, the absolute accuracy of a common AFM force calibration scheme, known as the thermal noise method, is evaluated. It is demonstrated that the thermal noise method can be applied with great success to colloidal probe calibration in air and in liquid to yield force measurements with relative standard uncertainties below 5%. Techniques to combine the electrostatics-based determination of the AFM force sensitivity with measurements of the colloidal probe's thermal noise spectrum to compute noncontact estimates of the displacement sensitivity and spring constant are also developed.

SI traceable calibration of an instrumented indentation sensor spring constant using electrostatic force.

We present a measurement scheme for creating reference electrostatic forces that are traceable to the International System of Units. This scheme yields reference forces suitable for calibrating the force sensitivity of instrumented indentation machines and atomic force microscopes. Forces between 10 and 200 muN were created and expressed in terms of the voltage, length, and capacitance between a pair of interacting electrodes. The electrodes comprised an electrically conductive sphere mounted as a tip on an instrumented indentation sensor, and a planar counterelectrode fixed to a sample stage in close proximity to the sphere. For comparison, we applied mechanical forces of similar magnitudes, first using deadweights and then using a reference force sensor. The deflection of the sensor due to the various applied forces was measured using an interferometer. A spring constant for the sensor was computed from the observed records of force versus displacement. Each procedure yielded a relative standard uncertainty of approximately 1%; however, the electrostatic technique is scalable and could provide traceable reference forces as small as a few hundred piconewtons, a range far below anything yet achieved using deadweights.