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Autonomous systems that combine synthesis, characterization, and artificial intelligence can greatly accelerate the discovery and optimization of materials, however platforms for growth of macroscale thin films by physical vapor deposition techniques have lagged far behind others. Here this study demonstrates autonomous synthesis by pulsed laser deposition (PLD), a highly versatile synthesis technique, in the growth of ultrathin WSe2 films. By combing the automation of PLD synthesis and in situ diagnostic feedback with a high‐throughput methodology, this study demonstrates a workflow and platform which uses Gaussian process regression and Bayesian optimization to autonomously identify growth regimes for WSe2 films based on Raman spectral criteria by efficiently sampling 0.25% of the chosen 4D parameter space. With throughputs at least 10x faster than traditional PLD workflows, this platform and workflow enables the accelerated discovery and autonomous optimization of the vast number of materials that can be synthesized by PLD. [ABSTRACT FROM AUTHOR]

Materials synthesis platforms that are designed for autonomous experimentation are capable of collecting multimodal diagnostic data that can be utilized for feedback to optimize material properties. Pulsed laser deposition (PLD) is emerging as a viable autonomous synthesis tool, and so the need arises to develop machine learning (ML) techniques that are capable of extracting information from in situ diagnostics. Here, we demonstrate that intensified-CCD image sequences of the plasma plume generated during PLD can be used for anomaly detection and the prediction of thin film growth kinetics. We develop multi-output (2 + 1)D convolutional neural network regression models that extract deep features from plume dynamics that not only correlate with the measured chamber pressure and incident laser energy, but more importantly, predict parameters of an auto-catalytic film growth model derived from in situ laser reflectivity experiments. Our results demonstrate how ML with in situ plume diagnostics data in PLD can be utilized to maintain deposition conditions in an optimal regime. Further, the predictive capabilities of plume dynamics on the kinetics of film growth or other film properties prior to deposition provides a means for rapid pre-screening of growth conditions for the non-expert, which promises to accelerate materials optimization with PLD. [ABSTRACT FROM AUTHOR]

Magnetoelectric (ME) composite thin films are promising candidates for novel applications in future nanoelectronics, spintronics, memory, and other multifunctional devices as they exhibit much higher ME coupling and transition temperatures (Tc) than well-known single phase multiferroics discovered to date. Among the three types of multiferroic composite nanostructures, (2–2) layered and (1–3) vertically aligned composite nanostructures exhibit comparatively smaller ME coupling due to different shortcomings that restrict their use in many applications. Here, we study the morphological, piezoresponse force microscopic (PFM), ferroelectric, magnetic, and magnetodielectric properties of 0–3 [magnetic nanoparticles (0) homogeneously distributed in ferroelectric matrices (3)] multiferroic composite thin films. The Pb(Fe0.5Nb0.5)O3 (PFN)–Ni0.65Zn0.35Fe2O4 (NZFO) particulate composite films were synthesized by pulsed laser deposition. These particulate composite thin films are completely c-axis oriented with very low surface roughness. We observed magnetic and ferroelectric Tc above room temperature (RT) for all composite thin films. The PFN–NZFO 0–3 composites exhibit large polarization, high saturated magnetization with low coercive field, and low dielectric loss along with magnetodielectric coupling at RT. These nanocomposites might be utilized in next generation nano/microelectronics and spintronic devices. [ABSTRACT FROM AUTHOR]

Ferroelectrics are being increasingly called upon for electronic devices in extreme environments. Device performance and energy efficiency is highly correlated to clock frequency, operational voltage, and resistive loss. To increase performance it is common to engineer ferroelectric domain structure with highly‐correlated electrical and elastic coupling that elicit fast and efficient collective switching. Designing domain structures with advantageous properties is difficult because the mechanisms involved in collective switching are poorly understood and difficult to investigate. Collective switching is a hierarchical process where the nano‐ and mesoscale responses control the macroscopic properties. Using chemical solution synthesis, epitaxially nearly‐relaxed (100) BaTiO3 films are synthesized. Thermal strain induces a strongly‐correlated domain structure with alternating domains of polarization along the [010] and [001] in‐plane axes and 90° domain walls along the [011] or [011¯$\bar{1}$] directions. Simultaneous capacitance–voltage measurements and band‐excitation piezoresponse force microscopy revealed strong collective switching behavior. Using a deep convolutional autoencoder, hierarchical switching is automatically tracked and the switching pathway is identified. The collective switching velocities are calculated to be ≈500 cm s−1 at 5 V (7 kV cm−1), orders‐of‐magnitude faster than expected. These combinations of properties are promising for high‐speed tunable dielectrics and low‐voltage ferroelectric memories and logic. [ABSTRACT FROM AUTHOR]

With the rapid development of new device miniaturization technology, there is invigorated interest in magnetic nanostructures for potential application in novel multifunctional devices. In continuation to our search for a suitable magnetic material having Curie temperature (Tc) well above room temperature for multifunctional applications, we have studied the dielectric, optical, magnetic, and resistance switching characteristics of Ni0.65Zn0.35Fe2O4 (NZFO) thin films. The observation of only (004) reflection in the X-ray diffraction patterns confirms the c-axis orientation and high quality growth of NZFO thin films. The presence of mixed valences of Fe2+/Fe3+ cations is probed by X-ray photon spectroscopy, which supports the cationic ordering-mediated large dielectric response. Our investigations reveal NZFO to be an indirect band gap material (~1.8eV) with a direct gap at ~2.55eV. These nanostructures exhibit high saturation magnetization and a low coercive field with a ferrimagnetic-paramagnetic phase transition of ~713K. Magnetic force microscopy studies revealed the stripe-like domain structure of the investigated thin films. In addition, these thin films exhibit reliable and repeatable unipolar resistive switching characteristics. The observed high dielectric permittivity with low loss tangent, large magnetization with soft magnetic behavior, striped magnetic domain structure and reliable resistance switching in NZFO thin films above room temperature suggest potential application in memory, spintronics, and multifunctional devices. [ABSTRACT FROM AUTHOR]

Topological defects in ferroelectric materials have attracted much attention due to the emergence of conductive, ferroic, and magnetic functionalities. However, many topological configurations dynamically evolve during the switching processes, making them a challenge to characterize via traditional techniques. Here, we implement an automated experimentation approach for the exploration of functional properties in BiFeO3 thin films. Specifically, we visualize the ferroelectric domain structures via single frequency piezoresponse force microscopy and implement a computer vision-based algorithm to discover features of interest at which spectroscopic measurements are taken. Subsequently, we employ dimensionality reduction techniques to reveal characteristic polarization behaviors at these features. This approach can be extended to other spectroscopies and modalities to probe only specific features of interest, ultimately enabling dynamical processes in ferroelectrics to be studied. [ABSTRACT FROM AUTHOR]

Ferroelectric domain walls have continued to attract widespread attention due to both the novelty of the phenomena observed and the ability to reliably pattern them in nanoscale dimensions. However, the conductivity mechanisms remain in debate, particularly around nominally uncharged walls. Here, we posit a conduction mechanism relying on field-modification effect from polarization re-orientation and the structure of the reverse-domain nucleus. Through conductive atomic force microscopy measurements on an ultra-thin (001) BiFeO3 thin film, in combination with phase-field simulations, we show that the field-induced twisted domain nucleus formed at domain walls results in local-field enhancement around the region of the atomic force microscope tip. In conjunction with slight barrier lowering, these two effects are sufficient to explain the observed emission current distribution. These results suggest that different electronic properties at domain walls are not necessary to observe localized enhancement in domain wall currents. [ABSTRACT FROM AUTHOR]

Understanding the dynamic behavior of interfaces in ferroic materials is an important field of research with widespread practical implications, as the motion of domain walls and phase boundaries are associated with substantial increases in dielectric and piezoelectric effects. Although commonly studied in the macroscopic regime, the local dynamics of interfaces have received less attention, with most studies limited to domain growth and/or reversal by piezoresponse force microscopy (PFM). Here, spatial mapping of local domain wall‐related relaxation in a tensile‐strained PbTiO3 thin film using time‐resolved band‐excitation PFM is demonstrated, which allows exploring of the field‐induced strain (piezoresponse) as a function of applied voltage and time. Through multivariate statistical analysis on the resultant 4‐dimensional dataset (x,y,V,t) with functional fitting, it is determined that the relaxation is strongly correleated with the distance to the domain walls, and varies based on the type of domain wall present in the probed volume. Phase‐field modeling shows the relaxation behavior near and away from the interfaces, and confirms the modulation of the z‐component of polarization by wall motion, yielding the observed piezoresponse relaxation. These studies shed light on the local dynamics of interfaces in ferroelectric thin films, and are therefore important for the design of ferroelectric‐based components in microelectromechanical systems. [ABSTRACT FROM AUTHOR]

The influence of surface morphology on the local piezoelectric response of highly (100)-textured 0.70PbMg2/3Nb1/3O3-0.30PbTiO3 thin films is studied using piezoresponse force microscopy in band-excitation mode. The local electromechanical response is mostly suppressed in direct proximity of the grain boundaries. However, within 100-200 nm of the grain boundary, the piezoresponse is substantially enhanced, before decaying again within a region at the center of the grain itself. Nested piezoresponse hysteresis curves confirm the influence of topography descriptors on parameters affecting the hysteresis loop shape. The enhancement of the electromechanical response is rationalized through reduced lateral clamping in the grains with deep trenched boundaries, as well as an expected lower energy for complex domain wall structures, due to curved ferroelectric surfaces. The lower piezoresponse at the center of the grain is assigned to the lateral clamping by the surrounding piezoelectric material. [ABSTRACT FROM AUTHOR]

Functional properties of ferroelectric materials depend both on the residual domain states and on the mobility of domain walls in response to the applied electric and stress fields. This paper reviews the use of multidimensional scanning probe microscopy to assess these factors in the time- and voltage domains, with an emphasis on the manner in which domain walls respond collectively to stimuli. It is found that in many PbZr1-xTixO3-based capacitors, domain wall motion is correlated over length scales that exceed the domain and grain sizes by orders of magnitude, suggesting emergent collective electromechanical behavior. The role of mechanical boundary conditions and field history on the domain wall contributions and the stability of the ferroelectric domain state are discussed. [ABSTRACT FROM AUTHOR]

The nonlinear response of a ferroic to an applied field has been studied through the phenomenological Rayleigh Law for over a hundred years. Yet, despite this, the fundamental physical mechanisms at the nanoscale that lead to macroscopic Rayleigh behavior have remained largely elusive, and experimental evidence at small length scales is limited. Here, it is shown using a combination of scanning probe techniques and phase field modeling, that nanoscale piezoelectric response in prototypical Pb(Zr,Ti)O3 films appears to follow a distinctly non-Rayleigh regime. Through statistical analysis, it is found that an averaging of local responses can lead directly to Rayleigh-like behavior of the strain on a macroscale. Phase-field modeling confirms the twist of the ferroelastic interface is key in enhancing piezoelectric response. The studies shed light on the nanoscale origins of nonlinear behavior in disordered ferroics. [ABSTRACT FROM AUTHOR]

The ability to manipulate domains underpins function in applications of ferroelectrics. While there have been demonstrations of controlled nanoscale manipulation of domain structures to drive emergent properties, such approaches lack an internal feedback loop required for automatic manipulation. Here, using a deep sequence-to-sequence autoencoder we automate the extraction of latent features of nanoscale ferroelectric switching from piezoresponse force spectroscopy of tensile-strained PbZr0.2Ti0.8O3 with a hierarchical domain structure. We identify characteristic behavior in the piezoresponse and cantilever resonance hysteresis loops, which allows for the classification and quantification of nanoscale-switching mechanisms. Specifically, we identify elastic hardening events which are associated with the nucleation and growth of charged domain walls. This work demonstrates the efficacy of unsupervised neural networks in learning features of a material's physical response from nanoscale multichannel hyperspectral imagery and provides new capabilities in leveraging in operando spectroscopies that could enable the automated manipulation of nanoscale structures in materials. The scale and dimensionality of imaging data means information is commonly overlooked. Here, using recurrent neural networks we understand temporal dependencies in hyperspectral imagery, enabling the observation of differences in ferroelectric switching mechanisms in PbZr0.2Ti0.8O3 thin films due to formation of charged domain walls. [ABSTRACT FROM AUTHOR]