Quantification of van der Waals forces in bimodal and trimodal AFM.

The multifrequency formalism is generalized and exploited to quantify attractive forces, i.e., van der Waals interactions, with small amplitudes or gentle forces in bimodal and trimodal atomic force microscopy (AFM). The multifrequency force spectroscopy formalism with higher modes, including trimodal AFM, can outperform bimodal AFM for material property quantification. Bimodal AFM with the second mode is valid when the drive amplitude of the first mode is approximately an order of magnitude larger than that of the second mode. The error increases in the second mode but decreases in the third mode with a decreasing drive amplitude ratio. Externally driving with higher modes provides a means to extract information from higher force derivatives while enhancing the range of parameter space where the multifrequency formalism holds. Thus, the present approach is compatible with robustly quantifying weak long range forces while extending the number of channels available for high resolution.

The Mendeleev-Meyer force project.

Here we present the Mendeleev-Meyer Force Project which aims at tabulating all materials and substances in a fashion similar to the periodic table. The goal is to group and tabulate substances using nanoscale force footprints rather than atomic number or electronic configuration as in the periodic table. The process is divided into: (1) acquiring nanoscale force data from materials, (2) parameterizing the raw data into standardized input features to generate a library, (3) feeding the standardized library into an algorithm to generate, enhance or exploit a model to identify a material or property. We propose producing databases mimicking the Materials Genome Initiative, the Medical Literature Analysis and Retrieval System Online (MEDLARS) or the PRoteomics IDEntifications database (PRIDE) and making these searchable online via search engines mimicking Pubmed or the PRIDE web interface. A prototype exploiting deep learning algorithms, i.e. multilayer neural networks, is presented.

Unlocking higher harmonics in atomic force microscopy with gentle interactions.

In dynamic atomic force microscopy, nanoscale properties are encoded in the higher harmonics. Nevertheless, when gentle interactions and minimal invasiveness are required, these harmonics are typically undetectable. Here, we propose to externally drive an arbitrary number of exact higher harmonics above the noise level. In this way, multiple contrast channels that are sensitive to compositional variations are made accessible. Numerical integration of the equation of motion shows that the external introduction of exact harmonic frequencies does not compromise the fundamental frequency. Thermal fluctuations are also considered within the detection bandwidth of interest and discussed in terms of higher-harmonic phase contrast in the presence and absence of an external excitation of higher harmonics. Higher harmonic phase shifts further provide the means to directly decouple the true topography from that induced by compositional heterogeneity.

Spatial horizons in amplitude and frequency modulation atomic force microscopy.

In dynamic atomic force microscopy (AFM) the cantilever is vibrated and its dynamics are monitored to probe the sample with nanoscale and atomic resolution. Amplitude and frequency modulation atomic force microscopy (AM-AFM and FM-AFM) have established themselves as the most powerful methods in the field. Nevertheless, it is still debatable whether one or the other technique is preferred in a given medium or experiment. Here, we quantitatively establish and compare the limitations in resolution of both techniques by introducing the concept of spatial horizon (SH) and quantifying it. The SH is the limiting spatial boundary beyond which collective atomic interactions do not affect the detection parameters of a given feedback system. We show that while an FM-AFM feedback can resolve a single atom or atomic defect where an AM feedback might fail, relative contrast is in fact equivalent for both feedback systems. That is, if the AM feedback could detect sufficiently small amplitude shifts and there was no noise, the detection of single atoms or atomic defects would be equivalent in AM-AFM and FM-AFM.

Investigation of Nanoscale Interactions by Means of Subharmonic Excitation.

Multifrequency atomic force microscopy holds promise as a method to provide qualitative and quantitative information about samples with high spatial resolution. Here, we provide experimental evidence of the excitation of subharmonics in ambient conditions in the regions where capillary interactions are predicted to be the mechanism of excitation. We also experimentally decouple a second mechanism for subharmonic excitation that is highly independent of environmental conditions such as relative humidity. This implies that material properties could be mapped. Subharmonic excitation could lead to experimental determination of surface water affinity in the nanoscale whenever water interactions are the mechanism of excitation.

The intrinsic resolution limit in the atomic force microscope: implications for heights of nano-scale features.

BACKGROUND: Accurate mechanical characterization by the atomic force microscope at the highest spatial resolution requires that topography is deconvoluted from indentation. The measured height of nanoscale features in the atomic force microscope (AFM) is almost always smaller than the true value, which is often explained away as sample deformation, the formation of salt deposits and/or dehydration. We show that the real height of nano-objects cannot be obtained directly: a result arising as a consequence of the local probe-sample geometry. METHODS AND FINDINGS: We have modeled the tip-surface-sample interaction as the sum of the interaction between the tip and the surface and the tip and the sample. We find that the dynamics of the AFM cannot differentiate between differences in force resulting from 1) the chemical and/or mechanical characteristics of the surface or 2) a step in topography due to the size of the sample; once the size of a feature becomes smaller than the effective area of interaction between the AFM tip and sample, the measured height is compromised. This general result is a major contributor to loss of height and can amount to up to ∼90% for nanoscale features. In particular, these very large values in height loss may occur even when there is no sample deformation, and, more generally, height loss does not correlate with sample deformation. DNA and IgG antibodies have been used as model samples where experimental height measurements are shown to closely match the predicted phenomena. CONCLUSIONS: Being able to measure the true height of single nanoscale features is paramount in many nanotechnology applications since phenomena and properties in the nanoscale critically depend on dimensions. Our approach allows accurate predictions for the true height of nanoscale objects and will lead to reliable mechanical characterization at the highest spatial resolution.

How localized are energy dissipation processes in nanoscale interactions?

We describe fundamental energy dissipation in dynamic nanoscale processes in terms of the localization of the interactions. In this respect, the areal density of the energy dissipated per cycle and the effective area of interaction in which each process occurs are calculated for four elementary dissipative processes. It is the ratio between these two, which we term M, that provides information about how localized the interactions are. While our results are general, we use concepts from dynamic atomic force microscopy to describe the physical phenomenon. We show that neither the phase lag, nor the magnitude of the energy dissipated alone provide information about how dissipative processes are localized. Instead, M has to be considered.

Bi-stability of amplitude modulation AFM in air: deterministic and stochastic outcomes for imaging biomolecular systems.

The dynamics of the oscillating microcantilever for amplitude modulation atomic force microscopy (AM AFM) operating in air is well understood theoretically but the experimental outcomes are still emerging. We use double-stranded DNA on mica as a model biomolecular system for investigating the connection between theory and experiment. A demonstration that the switching between the two cantilever oscillation states is stochastic in nature is achieved, and it can be induced by means of topographical anomalies on the surface. Whether one or the other attractor basin is accessed depends on the tip-sample separation history used to achieve the imaging conditions, and we show that the behaviour is reproducible when the tip is stable and well characterized. Emergence of background noise occurs in certain regions of parameter space regardless of whether two cantilever oscillation states coexist. The low state has been explored in detail and we note that at low to intermediate values of the free amplitude, noise-free imaging is achieved. The outcomes shown here are general and demonstrate that a thorough and systematic experimental approach in conjunction with standard modelling gives insight into the mechanisms behind image contrast formation in AM AFM in air.