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Ultrathin ferroelectric materials could potentially enable low-power logic and nonvolatile memories 1 , 2 . As ferroelectric materials are made thinner, however, the ferroelectricity is usually suppressed. Size effects in ferroelectrics have been thoroughly investigated in perovskite oxides—the archetypal ferroelectric system 3 . Perovskites, however, have so far proved unsuitable for thickness scaling and integration with modern semiconductor processes 4 . Here we report ferroelectricity in ultrathin doped hafnium oxide (HfO 2 ), a fluorite-structure oxide grown by atomic layer deposition on silicon. We demonstrate the persistence of inversion symmetry breaking and spontaneous, switchable polarization down to a thickness of one nanometre. Our results indicate not only the absence of a ferroelectric critical thickness but also enhanced polar distortions as film thickness is reduced, unlike in perovskite ferroelectrics. This approach to enhancing ferroelectricity in ultrathin layers could provide a route towards polarization-driven memories and ferroelectric-based advanced transistors. This work shifts the search for the fundamental limits of ferroelectricity to simpler transition-metal oxide systems—that is, from perovskite-derived complex oxides to fluorite-structure binary oxides—in which ‘reverse’ size effects counterintuitively stabilize polar symmetry in the ultrathin regime. Enhanced switchable ferroelectric polarization is achieved in doped hafnium oxide films grown directly onto silicon using low-temperature atomic layer deposition, even at thicknesses of just one nanometre.

The extraordinary optoelectronic performance of hybrid organic–inorganic perovskites has resulted in extensive efforts to unravel their properties. Recently, observations of ferroic twin domains in methylammonium lead triiodide drew significant attention as a possible explanation for the current–voltage hysteretic behaviour in these materials. However, the properties of the twin domains, their local chemistry and the chemical impact on optoelectronic performance remain unclear. Here, using multimodal chemical and functional imaging methods, we unveil the mechanical origin of the twin domain contrast observed with piezoresponse force microscopy in methylammonium lead triiodide. By combining experimental results with first principles simulations we reveal an inherent coupling between ferroelastic twin domains and chemical segregation. These results reveal an interplay of ferroic properties and chemical segregation on the optoelectronic performance of hybrid organic–inorganic perovskites, and offer an exploratory path to improving functional devices.

Piezoresponse force microscopy (PFM) has emerged as a tool of choice to probe ferroelectric materials through electrochemomechanical coupling at the nanoscale. However, this technique is not without its challenges, with artefacts related to electrostatic and topographical features presenting a significant obstacle to the accurate interpretation of PFM data. Here, we investigate the bias-dependent off-surface electrostatic response of soda lime glass, a material not traditionally associated with electromechanical activity. Unexpectedly, we observe a distinctive ferroelectric-like hysteresis behavior that is highly dependent on both the tip-sample separation and relative humidity. We also show the dynamic nature of these interactions, through a temporal analysis of the relaxation of this electrochemomechanical response. While the presence of an electrostatic force is expected, we can infer that this hysteretic effect is not inherent to the pure electrostatics of the voltage application and residual surface charges in an air-water capacitor, but is probably due to the incomplete charge and discharge dynamics of the soda lime glass. The choice of tip and the control of environmental conditions are thus essential for the measurement of true electromechanical responses of ferroelectrics.

Recent theoretical predictions of ferroelectricity in two-dimensional (2D) van der Waals materials reveal exciting possibilities for their use in scalable low-power electronic devices with polarization-dependent functionalities. These prospects have been further invigorated by the experimental evidence of the polarization response in some transition metal chalcogenides (TMCs)—a group of narrow-band semiconductors and semimetals with a wealth of application potential. Among the TMCs, molybdenum disulfide (MoS2) is known as one of the most promising and robust 2D electronic materials. However, in spite of theoretical predictions, no ferroelectricity has been experimentally detected in MoS2, while the emergence of this property could enhance its potential for electronics applications. Here, we report the experimental observation of a stable room-temperature out-of-plane polarization ordering in 2D MoS2 layers, where polarization switching is realized by mechanical pressure induced by a tip of a scanning probe microscope. Using this approach, we create the bi-domain polarization states, which exhibit different piezoelectric activity, second harmonic generation, surface potential, and conductivity. Ferroelectric MoS2 belongs to the distorted trigonal structural 1T” phase, where a spontaneous polarization is inferred by its P3m1 space-group symmetry and corroborated by theoretical modeling. Experiments on the flipped flakes reveal that the 1T”-MoS2 samples consist of the monolayers with randomly alternating polarization orientation, which form stable but switchable “antipolar” head-to-head or tail-to-tail dipole configurations. Mechanically written domains are remarkably stable facilitating the application of 1T”-MoS2 in flexible memory and electromechanical devices.

Bimodal atomic force microscopy uses a cantilever that is simultaneously driven at two of its eigenmodes (resonant modes). Parameters associated with both resonances can be measured and used to extract quantitative nanomechanical information about the sample surface. Driving the first eigenmode at a large amplitude and a higher eigenmode at a small amplitude simultaneously provides four independent observables that are sensitive to the tip–sample nanomechanical interaction parameters. To demonstrate this, a generalized theoretical framework for extracting nanomechanical sample properties from bimodal experiments is presented based on Hertzian contact mechanics. Three modes of operation for measuring cantilever parameters are considered: amplitude, phase, and frequency modulation. The experimental equivalence of all three modes is demonstrated on measurements of the second eigenmode parameters. The contact mechanics theory is then extended to power-law tip shape geometries, which is applied to analyze the experimental data and extract a shape and size of the tip interacting with a polystyrene surface.

The atomic force microscope is a high-resolution scanning-probe instrument which has become an important tool for cellular and molecular biophysics in recent years but lacks the time resolution and functional specificities offered by fluorescence microscopic techniques. To exploit the advantages of both methods, here we developed a spatially and temporally synchronized total internal reflection fluorescence and atomic force microscope system. The instrument, which we hereby call STIRF-AFM, is a stage-scanning device in which the mechanical and optical axes are coaligned to achieve spatial synchrony. At each point of the scan the sample topography (atomic force microscope) and fluorescence (photon count or intensity) information are simultaneously recorded. The tool was tested and validated on various cellular (monolayer cells in which actin filaments and intermediate filaments were fluorescently labeled) and biomolecular (actin filaments and titin molecules) systems. We demonstrate that with the technique, correlated sample topography and fluorescence images can be recorded, soft biomolecular systems can be mechanically manipulated in a targeted fashion, and the fluorescence of mechanically stretched titin can be followed with high temporal resolution.

Ferroic-order parameters 1 are useful as state variables in non-volatile information storage media because they show a hysteretic dependence on their electric or magnetic field. Coupling ferroics with quantum-mechanical tunnelling allows a simple and fast readout of the stored information through the influence of ferroic orders on the tunnel current. For example, data in magnetic random-access memories 2 are stored in the relative alignment of two ferromagnetic electrodes separated by a non-magnetic tunnel barrier, and data readout is accomplished by a tunnel current measurement. However, such devices based on tunnel magnetoresistance 3 typically exhibit OFF/ON ratios of less than 4, and require high powers for write operations (>1 × 10 6  A cm −2 ). Here, we report non-volatile memories with OFF/ON ratios as high as 100 and write powers as low as ∼1 × 10 4  A cm −2 at room temperature by storing data in the electric polarization direction of a ferroelectric tunnel barrier. The junctions show large, stable, reproducible and reliable tunnel electroresistance, with resistance switching occurring at the coercive voltage of ferroelectric switching. These ferroelectric devices emerge as an alternative to other resistive memories 4 , and have the advantage of not being based on voltage-induced migration of matter at the nanoscale 5 , 6 , but on a purely electronic mechanism 7 . A tunnel junction that consists of a ferroelectric barrier layer sandwiched between two electrodes can operate as a fast, low-power and non-volatile nanoscale solid-state memory.

The ability to spatially resolve the chemical distribution of compounds on a surface is important in many applications ranging from biological to material science. To this extent, we have recently introduced a hybrid atomic force microscopy (AFM)-mass spectrometry (MS) system for direct thermal desorption and pyrolysis of material with nanoscale chemical resolution. However, spatially resolved direct surface heating using local thermal desorption becomes challenging on material surfaces with low melting points, because the material will undergo a melting phase transition due to heat dissipation prior to onset of thermal desorption. Therefore, we developed an approach using mechanical sampling and collection of surface materials on an AFM cantilever probe tip for real-time analysis directly from the AFM tip. This approach allows for material to be concentrated directly onto the probe for subsequent MS analysis. We evaluate the performance metrics of the technique and demonstrate localized MS sampling from a candelilla wax matrix containing UV stabilizers avobenzone and oxinoxate from areas down to 250 nm × 250 nm. Overall, this approach removes heat dissipation into the bulk material allowing for a faster desorption and concentration of the gas phase analyte from a single heating pulse enabling higher signal levels from a given amount of material in a single sampling spot.Graphical abstract