Probe-sample Interaction Research Articles

In Situ Formation of Ripplocations in Hybrid Organic-Inorganic MXenes.

Inorganic-organic hybrid MXenes (h-MXenes) are a family of 2D transition metal carbides and nitrides functionalized with alkylimido and alkylamido surface groups. Using cryogenic and room temperature scanning transmission electron microscopy (STEM) and electron energy-loss spectroscopy (EELS), it is shown that ripplocations, a form of a fundamental defect in 2D and layered structures, are abundant in this family of materials. Furthermore, detailed studies of electron probe sample interactions, focusing on structural deformations caused by the electron beam are presented. The findings indicate that at cryogenic temperatures (≈100K) and below a specific dose threshold, the structure of h-MXenes remains largely intact. However, exceeding this threshold leads to electron beam-induced deformation through ripplocations. Interestingly, the deformation behavior, required dose, and resultant structure are highly dependent on temperature. At 100K, it is demonstrated that the electron beam can induce ripplocations in situ with a high degree of precision.

Scanning microwave impedance microscopy and its applications: A review

Scanning microwave impedance microscopy (sMIM) has become a powerful tool for nanoscale characterization, utilizing microwave frequencies to probe the material properties of diverse systems with remarkable spatial resolution. This review offers an in-depth analysis of the foundational principles, technological advancements, and broad applications of sMIM. By harnessing near-field microwave interactions between a sharp metallic probe and the sample, sMIM enables simultaneous acquisition of both real (resistive) and imaginary (capacitive) components of the reflected signal, providing detailed insights into the local permittivity and conductivity of materials at the nanoscale. We address critical challenges, including impedance matching, probe–sample interactions, and the influence of environmental factors such as surface water layers and meniscus formation on resolution and contrast. Recent advancements in finite element modeling and the application of lumped-element circuit models have further enhanced the precision of signal interpretation, enabling more accurate analysis of complex systems. This review highlights sMIM’s wide-ranging applications, from material science and semiconductor diagnostics to biological systems, showcasing its ability to perform non-destructive, high-resolution imaging down to the single-digit nanometer scale. These capabilities position sMIM as an indispensable tool for advancing future innovations in nanotechnology and related fields.

Microscopic examination of rf-cavity-quality niobium films through local nonlinear microwave response

The performance of superconducting radio-frequency (SRF) cavities is sometimes limited by local defects. To investigate the rf properties of these local defects, especially those that nucleate rf magnetic vortices, a near-field magnetic microwave microscope is employed. Local third-harmonic response (P3f) and its temperature dependence and rf power dependence are measured for one Nb/Cu film grown by direct current magnetron sputtering (DCMS) and six Nb/Cu films grown by high-power impulse magnetron sputtering (HiPIMS) with systematic variation of deposition conditions. Five out of the six HiPIMS Nb/Cu films show a strong third-harmonic response that is likely coming from rf vortex nucleation due to a low-Tc surface defect with a transition temperature between 6.3 and 6.8 K, suggesting that this defect is a generic feature of air-exposed HiPIMS Nb/Cu films. A phenomenological model of surface-defect grain boundaries hosting a low-Tc impurity phase is introduced and studied with time-dependent Ginzburg-Landau (TDGL) simulations of probe-sample interaction to better understand the measured third-harmonic response. The simulation results show that the third-harmonic response of rf vortex nucleation caused by surface defects exhibits the same general features as the data, including peaks in third-harmonic response with temperature, and their shift and broadening with higher microwave amplitude. We find that the parameters of the phenomenological model (the density of surface defects that nucleate rf vortices and the depth an rf vortex travels through these surface defects) vary systematically with film deposition conditions. From the point of view of these two properties, the Nb/Cu film that is most effective at reducing the nucleation of rf vortices associated with surface defects can be identified. Published by the American Physical Society 2024

Calibration method for complex permittivity measurements using s-SNOM combining multiple probe tapping harmonics.

Scattering-type scanning near-field optical microscopy (s-SNOM) enables sub-diffraction spectroscopy, featuring high sensitivity to small spatial permittivity variations of the sample surface. However, due to the complexity of the near-field probe-sample interaction, the quantitative extraction of the complex permittivity leads to a computationally demanding inverse problem, requiring further approximation of the system to an invertible model. Black-box calibration methods, similar to those applied to microwave vector network analyzers, allow the extraction of the permittivity without detailed electromagnetic modeling of the probe-sample interaction. These methods, however, are typically designed for stationary setups. In contrast, the distance between the sample and the probe tip of the s-SNOM is periodically modulated to differentiate the near-field interaction from the far-field background via lock-in detection of the harmonics of the periodic motion. This paper proposes an improved black-box calibration method that takes account of the effects of the probe tapping, including its multiple harmonics, and far-field background. The method is validated for an s-SNOM operating in the mid-infrared spectral range by applying it to spectroscopic measurements of silicon microstructures of different but well characterized doping.

Control of the Probe-Sample Interaction Force at the Piconewton Scale by a Magnetic Microprobe in Aqueous Solutions

This article describes the design and implementation of a control system that controls the probe-sample interaction force at the piconewton scale by manipulating a magnetic microprobe in aqueous solutions under a microscope. The control system has two functions, namely accurate force generation by magnetic flux control and precise control of the probe-sample interaction force. Magnetic flux control uses an improved six-input-six-output digital control law along with a disturbance estimator to achieve two control objectives. First, the magnetic flux at each pole tip of a previously developed hexapole electromagnetic actuator can be individually and precisely controlled at frequencies over 4 kHz, and the experimental results precisely followed the theoretical predictions based on the design. Second, together with the optimized flux allocation, the flux control system generates precise magnetic forces, making the six-input hexapole actuator behave like a decoupled three-axis force generator with a bandwidth of more than 4 kHz. Interaction force control compares the measured deformation of the sample with the expected deformation, updated in real time by a deformation predictor, to generate the magnetic force to control the interaction between the probe and the sample. Digital control laws, the estimator, and the predictor are all implemented using a high-speed Field Programmable Gate Array (FPGA) system. Experiments confirm that through mathematical modeling, digital control technology, high-speed electronics, and real-time computation, accurate three-dimensional force generation at the piconewton scale with high bandwidth and precise interaction force control with zero-mean random error, attributed to random thermal force and measurement noise, are achieved.

Energy measurements remain thermometrically optimal beyond weak coupling

We develop a general perturbative theory of finite-coupling quantum thermometry up to second order in probe-sample interaction. By assumption, the probe and sample are in thermal equilibrium, so the probe is described by the mean-force Gibbs state. We prove that the ultimate thermometric precision can be achieved – to second order in the coupling – solely by means of local energy measurements on the probe. Hence, seeking to extract temperature information from coherences or devising adaptive schemes confers no practical advantage in this regime. Additionally, we provide a closed-form expression for the quantum Fisher information, which captures the probe's sensitivity to temperature variations. Finally, we benchmark and illustrate the ease of use of our formulas with two simple examples. Our formalism makes no assumptions about separation of dynamical timescales or the nature of either the probe or the sample. Therefore, by providing analytical insight into both the thermal sensitivity and the optimal measurement for achieving it, our results pave the way for quantum thermometry in setups where finite-coupling effects cannot be ignored.

Large-range high-speed dynamic-mode atomic force microscope imaging: adaptive tapping towards minimal force

In this paper, a software-hardware integrated approach is proposed for high-speed, large-range tapping mode imaging of atomic force microscope (AFM). High speed AFM imaging is needed in various applications, particularly in interrogating dynamic processes at nanoscale such as polymer crystallization process. Achieving high speed in tapping-mode AFM imaging is challenging as the probe-sample interaction during the imaging process is highly nonlinear, making the tapping motion highly sensitive to the probe sample spacing, and thereby, difficult to maintain at high speed. Increasing the speed via hardware bandwidth enlargement, however, leads to a substantially reduction of the imaging area. Contrarily, the imaging speed can be increased without loss of the scan size through control (algorithm)-based approach. For example, the recently-developed adaptive multiloop mode (AMLM) technique has demonstrated its efficacy in increasing the tapping-mode imaging speed without loss of scan size. Further improvement, however, has been limited by the hardware bandwidth and the online signal processing speed and computation complexity involved. Thus, in this paper, the AMLM technique is further enhanced to optimize the probe tapping regulation, and integrated with a field programmable gate array platform to further increase the imaging speed without loss of quality and scan range. Experimental implementation of the proposed approach demonstrates that high-quality imaging can be achieved at a high-speed scanning rate of 100 Hz and higher, and over a large imaging area of over 20 μm.

AFM SMILER: A Scale Model Interactive Learning Extended Reality Toolkit for Atomic Force Microscopy Created With Digital Twin Technology

The Atomic Force Microscope (AFM) is a precision mechatronic system for nanoscale imaging of surfaces. Due to limited instrument access and lack of visualization techniques, understanding its principles can be challenging. Digital twin technology allows the creation of virtual representations of physical systems, which can be particularly useful to address challenges in AFM education. To realistically simulate nanoscale physics, we first developed new efficient algorithms for four virtual scale models, including cantilever mechanics, probe transducers, controller tuning, and contact mechanics. Second, three simulated experiment interactive learning modules are developed for instrument operation, including virtual imaging, system overview, and imaging modalities. In the end, three hardware systems are integrated for an extended reality experience, including a macroscopic AFM scale model, a haptic device for probe-sample interaction force feedback, and an upgraded low-cost educational AFM for nanoscale imaging and instrumentation. This completes the eight total modules for the AFM SMILER: A scale model interactive learning extended reality toolkit. Preliminary studies show the toolkit being helpful for AFM education. In addition to mechatronics and nanotechnology education, techniques developed in this work can be generally applied to computationally efficient realistic digital twin creation.

Optimal nonequilibrium thermometry in Markovian environments

What is the minimum time required to take a temperature? In this paper, we solve this question for a large class of processes where temperature is inferred by measuring a probe (the thermometer) weakly coupled to the sample of interest, so that the probe's evolution is well described by a quantum Markovian master equation. Considering the most general control strategy on the probe (adaptive measurements, arbitrary control on the probe's state and Hamiltonian), we provide bounds on the achievable measurement precision in a finite amount of time, and show that in many scenarios these fundamental limits can be saturated with a relatively simple experiment. We find that for a general class of sample-probe interactions the scaling of the measurement uncertainty is inversely proportional to the time of the process, a shot-noise like behaviour that arises due to the dissipative nature of thermometry. As a side result, we show that the Lamb shift induced by the probe-sample interaction can play a relevant role in thermometry, allowing for finite measurement resolution in the low-temperature regime. More precisely, the measurement uncertainty decays polynomially with the temperature as T→0, in contrast to the usual exponential decay with T−1. We illustrate these general results for (i) a qubit probe interacting with a bosonic sample, where the role of the Lamb shift is highlighted, and (ii) a collective superradiant coupling between a N-qubit probe and a sample, which enables a quadratic decay with N of the measurement uncertainty.

Data-driven dynamics-based optimal filtering of acoustic noise at arbitrary location in atomic force microscope imaging

This paper presents a post-filtering approach to eliminate distortions in atomic force microscope (AFM) images caused by acoustic noise from an unknown location. AFM operations are sensitive to external disturbances including acoustic noise, as disturbances to the probe-sample interaction directly results in distortions in the sample images obtained. Although conventional passive noise cancellation has been employed, limitation exists and residual noise still persists. Advanced online control techniques face difficulty in capturing the complex noise dynamic and limited system bandwidth imposed by robustness requirement. In this work, we propose a dynamics-based optimal filtering technique to remove the acoustic-caused distortions in AFM images. A dictionary-approach is integrated with time-delay measurement to localize the noise source and estimate the corresponding acoustic dynamics. Then a noise-to-image coherence minimization approach is proposed to minimize the acoustic-caused image distortion via a gradient-based optimization to seek an optimal modulator to the acoustic dynamics. Finally, the filter is obtained as the finite-impulse response of the optimized acoustic dynamics. Experimental implementation is presented and discussed to illustrate the proposed technique.

Large Area, High Resolution Mapping of Approximate Rotational Symmetries in a Pd77.5Cu6Si16.5 Metallic Glass Thin Film

Densely spaced four-dimensional scanning transmission electron microscopy (4D STEM) analyzed using correlation symmetry coefficients enables large area mapping of approximate rotational symmetries in amorphous materials. Here, we report the effects of Poisson noise, limited electron counts, probe coherence, reciprocal space sampling, and the probe-sample interaction volume on 4D STEM symmetry mapping experiments. These results lead to an experiment parameter envelope for high quality, high confidence 4D STEM symmetry mapping. We also establish a direct link between the symmetry coefficients and approximate rotational symmetries of nearest-neighbor atomic clusters using electron diffraction simulations from atomic models of a metallic glass. Experiments on a Pd77.5Cu6Si16.5 metallic glass thin film demonstrate the ability to image the types, sizes, volume fractions, and spatial correlations amongst local rotationally symmetry regions in the glass.

Bending the rules of low-temperature thermometry with periodic driving

There exist severe limitations on the accuracy of low-temperature thermometry, which poses a major challenge for future quantum-technological applications. Low-temperature sensitivity might be manipulated by tailoring the interactions between probe and sample. Unfortunately, the tunability of these interactions is usually very restricted. Here, we focus on a more practical solution to boost thermometric precision – driving the probe. Specifically, we solve for the limit cycle of a periodically modulated linear probe in an equilibrium sample. We treat the probe-sample interactions exactly and hence, our results are valid for arbitrarily low temperatures T and any spectral density. We find that weak near-resonant modulation strongly enhances the signal-to-noise ratio of low-temperature measurements, while causing minimal back action on the sample. Furthermore, we show that near-resonant driving changes the power law that governs thermal sensitivity over a broad range of temperatures, thus `bending' the fundamental precision limits and enabling more sensitive low-temperature thermometry. We then focus on a concrete example – impurity thermometry in an atomic condensate. We demonstrate that periodic driving allows for a sensitivity improvement of several orders of magnitude in sub-nanokelvin temperature estimates drawn from the density profile of the impurity atoms. We thus provide a feasible upgrade that can be easily integrated into low-T thermometry experiments.

Electric-Field-Assisted Contact Mode AFM-Based Nanolithography with Low Stiffness Conductive Probes

Abstract Electric-field-assisted atomic force microscope (E-AFM) nanolithography is a novel polymer-patterning technique that has diverse applications. E-AFM uses a biased AFM tip with conductive coatings to make patterns with little probe-sample interaction, which thereby avoids the tip wear that is a major issue for contact-mode AFM-based lithography, which usually requires a high probe-sample contact force to fabricate nanopatterns; however, the relatively large tip radius and large tip-sample separation limit its capacity to fabricate high-resolution nanopatterns. In this paper, we developed a contact mode E-AFM nanolithography approach to achieve high-resolution nanolithography of poly (methyl methacrylate) (PMMA) using a conductive AFM probe with a low stiffness (~0.16 N/m). The nanolithography process generates features by biasing the AFM probe across a thin polymer film on a metal substrate. A small constant force (0.5-1 nN) applied on the AFM tip helps engage the tip-film contact, which enhances nanomachining resolution. This E-AFM nanolithography approach enables high-resolution nanopatterning with feature width down to ~16 nm, which is less than one half of the nominal tip radius of the employed conductive AFM probes.

Noise Rejection Mode Imaging of Atomic Force Microscope

This paper presents an imaging mode of atomic force microscope (AFM) that is robust to the environmental acoustic noise. AFM operations are sensitive to external disturbances including acoustic noise, as disturbances to the probe-sample interaction directly results in distortions in the sample images obtained. Although conventionally passive noise cancellation has been employed, the passive-noise apparatus limits the function of AFM and its use in emerging applications. Moreover, residual noise still persists. In this work, we propose a noise rejection mode (NRM) of AFM imaging to avoid and eliminate the acoustic-caused disturbance to the imaging process. Contrary to other existing AFM imaging modes, in the proposed NRM approach, the set-point of the feedback loop for tracking the sample topography is adjusted online such that the AFM system is insensitive and thereby, robust to the environmental noise. Then, a feedforward controller is augmented to counter act the noise-caused vibration in the feedback loop. Both the set-point adjustment and the feedforward noise cancellation are implemented through finite-impulse-response (FIR) filters. Experimental examples are presented and discussed to illustrate the proposed technique.

Compensating for artifacts in scanning near-field optical microscopy due to electrostatics

Nanotechnology and modern materials science demand reliable local probing techniques on the nanoscopic length scale. Most commonly, scanning probe microscopy methods are applied in numerous variants and shades, for probing the different sample properties. Scattering scanning near-field optical microscopy (s-SNOM), in particular, is sensitive to the local optical response of a sample, by scattering light off an atomic force microscopy (AFM) tip, yielding a wavelength-independent lateral resolution in the order of ∼10 nm. However, local electric potential variations on the sample surface may severely affect the probe–sample interaction, thereby introducing artifacts into both the optical near-field signal and the AFM topography. On the other hand, Kelvin-probe force microscopy (KPFM) is capable of both probing and compensating such local electric potentials by applying a combination of ac and dc-voltages to the AFM tip. Here, we propose to combine s-SNOM with KPFM in order to compensate for undesirable electrostatic interaction, enabling the in situ probing of local electric potentials along with pristine optical responses and topography of sample surfaces. We demonstrate the suitability of this method for different types of materials, namely, metals (Au), semiconductors (Si), dielectrics (SiO2), and ferroelectrics (BaTiO3), by exploring the influence of charges in the systems as well as the capability of KPFM to compensate for the resulting electric force interactions.

Optical constants from scattering-type scanning near-field optical microscope

Scattering-type scanning near-field optical microscopy (s-SNOM) allows for the characterization of optical properties of samples at the nanoscale, well below the diffraction limit of the interrogating wavelength. Typically, it relies on a model for the probe-sample interaction to extract complex optical constants of the sample. Here, we propose an s-SNOM calibration method that allows for the extraction of these constants without prior knowledge of the probe geometry nor the details of the probe-sample interactions. We illustrate the technique using terahertz time-domain spectroscopy-based s-SNOM to extract the optical properties of several organic and inorganic materials and differently doped regions of a standard silicon random access memory sample. The accuracy of the technique is comparable to that of conventional far-field techniques while additionally providing spatial distribution of optical constants at the nanoscale. The source-independent nature of the proposed technique makes it directly applicable for s-SNOM measurements in other spectral ranges.

Оптимизация измерений вектора силы взаимодействия в атомно-силовой микроскопии

The issue of optimization of measurements of three spatial components of the probe-sample interaction force and the corresponding displacement vector of the "ideal cantilever" is considered. To determine these components in an atomic force microscope with an optical beam deflection scheme, it is necessary to register the bending angles at least at two points on the rectangular cantilever and the torsion angle at any of them. It has been proven analytically that one optimal point is the intersection of the probe axis with the console plane. A method to calculate the position of another optimal point has been developed. An experiment was carried out to map the force and displacement vector, and satisfactory agreement with the theory was obtained.

Multiple-fibre interferometry setup for probe sample interaction measurements in atomic force microscopy

Atomic force microscopy (AFM) often relies on the assumption that cantilever bending can be described by simple beam theory and that the displacement of the tip can be evaluated from the cantilever angle. Some more advanced metrological instruments use free-space or fibre interferometers for measuring the position of the cantilever apex directly, thereby simplifying the metrology traceability chain. The next logical development, covering measurements of both the cantilever apex position and its deformation due to lateral forces acting during different AFM measurement regimes, is presented in this paper. It is based on using a set of closely packed fibre interferometers that can be used to determine localised bending of the cantilever at different positions along the cantilever. This can be used for detection of cantilever deformation beyond classical beam theory, and can yield both better understanding of sources of uncertainty in individual AFM force–distance measurements and more accurate scanning in constant height mode in high-speed AFM applications.

Rapid Probe Engagement and Withdrawal With Force Minimization in Atomic Force Microscopy: A Learning-Based Online-Searching Approach

In this article, the problem of rapid probe engagement and withdrawal in atomic force microscopy (AFM) is addressed. Probe engagement and withdrawal is needed in almost all AFM operations, ranging from imaging to nanomanipulation. However, due to the highly nonlinear force-distance relation, large probe-sample interaction force can be induced during the probe engagement and withdrawal process, resulting in sample deformation and damage and measurement errors. Rapid probe engagement and withdrawal is needed to achieve high-speed AFM operations, particularly, to capture and interrogate dynamic evolutions of the sample. We propose an online-searching-based optimization approach to minimize both the engagement (and withdrawal) time and the interaction force. The force-displacement profile of the probe is partitioned and then optimized sequentially, by immersing optimal trajectory design and iterative learning control into the Fibonacci search process. The proposed approach is illustrated through experimental implementations on two different types of polymer species, a polydimethylsiloxane sample, and a dental silicone sample, respectively.

Quantitative Scanning Microwave Microscopy of the Evolution of a Live Biological Cell in a Physiological Buffer

This article reports the first quantitative characterization by scanning microwave microscopy (SMM) of a live cell in its physiological buffer. The challenges for quantitative SMM of soft matter in liquid were overcome mainly by characterizing the probe–sample interaction through multiscale finite-element full-wave electromagnetic simulation of not only the probe tip but also the probe body and holder. Using quantitative SMM, the relative permittivity of the center of a live L6 cell on the top of its nucleus was determined to be ( $32\pm 6)-j(20 \pm 4)$ , which was in general agreement with the literature and simple estimation. Moreover, taking advantage of the noninvasiveness and subsurface sensitivity of SMM, it was used to monitor the physiological condition of the cell for hours. The results showed that the gradual shrinking of the cell footprint did not impact cell vitality significantly. These results implied that SMM could be a valuable technique for label-free noninvasive characterization of subcellular structures in a live cell, as well as its physio-pathological conditions.