arXiv subjects

Brian J. Rodriguez

Publications and source records attributed to Brian J. Rodriguez.

11 recordsLinked to original sources

arXiv2026

Low-Field Ferroelectric Switching realised by Forced Harmonic Oscillation of Domain Walls

Conventionally, dc fields are used for switching dipole orientations in ferroelectrics. Such fields tilt the potential surface experienced by domain walls and thereby lower activation energies for their movement: escape from tilted potential wells is then realised by thermal excitation, allowing a "creep" process of pinning and depinning to develop. Borrowing ideas of domain wall resonance from the magnetic racetrack community, we show that ac fields, applied at the right frequency, can cause switching at much lower field magnitudes than dc ones (by factors of 4-5). Ferroelectric wall motion appears to be overdamped in the system studied (relaxor strontium barium niobate) and so the maximum in switching efficacy observed, at ~100 kHz, cannot be associated with resonant amplification, which needs an underdamped environment. Instead, in this high viscosity system, the frequency at which the maximum switching efficacy occurs seems to represent a compromise between the attempt frequency for wall depinning (which increases with frequency) and the extent to which energy is transferred to the wall within each field cycle (which decreases with frequency). Notwithstanding the absence of true resonance, the observation that ac excitation can dramatically reduce the bias levels needed for ferroelectric switching could still have significant ramifications for low energy memory technology.

cond-mat.mtrl-sci↗

arXiv2024

AFM-based Functional Tomography-To Mill or not to Mill, that is the Question!

The electrical response of ferroelectric domain walls is often influenced by their geometry underneath the sample surface. Tomographic imaging in these material systems has therefore become increasingly important for its ability to correlate the surface-level functional response with subsurface domain microstructure. In this context, AFM-based tomography emerges as a compelling choice because of its simplicity, high resolution and robust contrast mechanism. However, to date, the technique has been implemented in a limited number of ferroelectric materials, typically to depths of a few hundred nanometers or on relatively soft materials, resulting in an unclear understanding of its capabilities and limitations. In this work, AFM tomography is carried out in YbMnO3, mapping its complex domain microstructure up to a depth of around 1.8 um along with its current pathways. A model is presented, describing the impact of interconnected domain walls within the network, which act as current dividers and codetermine how currents distribute. Finally, challenges such as tip-blunting and subsurface amorphisation are identified through TEM studies, and strategies to address them are also put forward. This study highlights the potential of AFM tomography and could spur interest within the ferroics community for its use in the investigation of similar material systems.

cond-mat.mtrl-sci↗

arXiv2024

Evidence of the Monopolar-Dipolar Crossover Regime: A Multiscale Study of Ferroelastic Domains by In-Situ Microscopy Techniques

The elastic interaction between kinks (and antikinks) within domain walls plays a pivotal role in shaping the domain structure, and their dynamics. In bulk materials, kinks interact as elastic monopoles, dependent on the distance between walls, and typically characterised by a rigid and straight domain configuration. In this work we investigate the evolution of the domain structure as the sample size decreases, by means of in-situ heating techniques on free-standing samples. A significant transformation is observed: domain walls exhibit pronounced curvature, accompanied by an increase in both domain wall and junction density. This transformation is attributed to the pronounced influence of kinks, inducing sample warping, where 'dipole dipole' interactions are dominant. Moreover, we experimentally identify a critical thickness range that delineates a cross-over between the monopolar and dipolar regimens and corroborated this by detailed atomic simulations. These findings are relevant for in-situ TEM studies and for the development of novel devices based on free-standing ferroic thin films and nanomaterials.

cond-mat.mes-hall↗

arXiv2024

Spatially Resolved High Voltage Kelvin Probe Force Microcopy: A Novel Avenue for Examining Electrical Phenomena at Nanoscale

Kelvin probe microscopy (KPFM) is a well-established scanning probe technique, used to measure surface potential accurately; it has found extensive use in the study of a range of materials phenomena. In its conventional form, KPFM frustratingly precludes imaging samples or scenarios where large surface potential exists or large surface potential gradients are created outside the typical +/-10V window. If the potential regime measurable via KPFM could be expanded, to enable precise and reliable metrology, through a high voltage KPFM (HV-KPFM) adaptation, it could open up pathways towards a range of novel experiments, where the detection limit of regular KPFM has so far prevented the use of the technique. In this work, HV-KPFM has been realised and shown to be capable of measuring large surface potential and potential gradients with accuracy and precision. The technique has been employed to study a range of materials (positive temperature coefficient of resistivity ceramics, charge storage fluoropolymers and pyroelectrics) where accurate spatially resolved mapping of surface potential within high voltage regime facilitates novel physical insight. The results demonstrate that HV-KPFM can be used as an effective tool to fill in existing gaps in surface potential measurements while also opening routes for novel studies in materials physics.

cond-mat.mtrl-sci↗

arXiv2019

Giant negative electrostriction and dielectric tunability in a van der Waals layered ferroelectric

The interest in ferroelectric van der Waals crystals arises from the potential to realize ultrathin ferroic systems owing to the reduced surface energy of these materials and the layered structure that allows for exfoliation. Here, we quantitatively unravel giant negative electrostriction of van der Waals layered copper indium thiophosphate (CIPS), which exhibits an electrostrictive coefficient Q33 as high as -3.2 m4/C2 and a resulting bulk piezoelectric coefficient d33 up to -85 pm/V. As a result, the electromechanical response of CIPS is comparable in magnitude to established perovskite ferroelectrics despite possessing a much smaller spontaneous polarization of only a few uC/cm2. In the paraelectric state, readily accessible owing to low transition temperatures, CIPS exhibits large dielectric tunability, similar to widely-used barium strontium titanate, and as a result both giant and continuously tunable electromechanical response. The persistence of electrostrictive and tunable responses in the paraelectric state indicates that even few layer films or nanoparticles will sustain significant electromechanical functionality, offsetting the inevitable suppression of ferroelectric properties in the nanoscale limit. These findings can likely be extended to other ferroelectric transition metal thiophosphates and (quasi-) two-dimensional materials and might facilitate the quest towards novel ultrathin functional devices incorporating electromechanical response.

cond-mat.mtrl-sci↗

arXiv2017

Nanoscale electrical measurements in liquids using AFM - progress and outlook

Fundamental mechanisms of energy storage, corrosion, sensing, and multiple biological functionalities are directly coupled to electrical processes and ionic dynamics at solid-liquid interfaces. In many cases, these processes are spatially inhomogeneous taking place at grain boundaries, step edges, point defects, ion channels, etc. and possess complex time and voltage dependent dynamics. This necessitates time-resolved and real-space probing of these phenomena. In this review, we discuss the applications of force-sensitive voltage modulated scanning probe microscopy (SPM) for probing electrical phenomena at solid-liquid interfaces. We first describe the working principles behind electrostatic and Kelvin Probe Force microscopies (EFM & KPFM) at the gas-solid interface, review the state of the art in advanced KPFM methods and developments to (i) overcome limitations of classical KPFM, (i) expand the information accessible from KPFM, and (iii) extend KPFM operation to liquid environments. We briefly discuss the theoretical framework of the electrical double layer (EDL) forces and dynamics, the implications and breakdown of classical EDL models for highly charged interfaces, or under high ion concentrations, and briefly describe recent modifications of the classical EDL theory relevant for understanding nanoscale electrical measurements at the solid-liquid interface. We further review the latest achievements in mapping surface charge, dielectric constants, and electrodynamic and electrochemical processes in liquids. Finally, we outline the key challenges and opportunities that exist in the field of nanoscale electrical measurements in liquid as well as provide a roadmap for the future development of liquid KPFM.

cond-mat.mtrl-sci↗

arXiv2008

Imaging Mechanism of Piezoresponse Force Microscopy in Capacitor Structures

The image formation mechanism in Piezoresponse Force Microscopy (PFM) of capacitor structures is analyzed. We demonstrate that the spatial resolution is a bilinear function of film and top electrode thicknesses, and derive the corresponding analytical expressions. For many perovskites, the opposite contributions of d31 and d33 components can result in anomalous domain wall profiles. This analysis establishes the applicability limits of PFM for polarization dynamics studies in capacitors, and applies to other structural probes, including focused X-ray studies of capacitor structures.

cond-mat.mtrl-sci↗

arXiv2007

Local Polarization Switching in the Presence of Surface Charged Defects: Microscopic Mechanisms and Piezoresponse Force Spectroscopy Observations

The thermodynamics and kinetics of tip-induced polarization switching in Piezoresponse Force Microscopy in the presence of surface charge defects is studied using the combination of analytical and numerical techniques. The signature of the defects in hysteresis loop fine structure and Switching Spectroscopy PFM images is identified and compared to experimental observations. An approach for the deconvolution of PFM spectroscopy measurements to extract relevant defect parameters is derived. This methodology is universal and can be extended to switching in other ferroics and in reversible electrochemical processes, establishing a pathway for the understanding of the thermodynamics and kinetics of phase transitions at a single defect level.

cond-mat.mtrl-sci↗

arXiv2007

Towards local electromechanical probing of cellular and biomolecular systems in a liquid environment

Electromechanical coupling is ubiquitous in biological systems with examples ranging from simple piezoelectricity in calcified and connective tissues to voltage-gated ion channels, energy storage in mitochondria, and electromechanical activity in cardiac myocytes and outer hair cell stereocilia. Piezoresponse force microscopy (PFM) has originally emerged as a technique to study electromechanical phenomena in ferroelectric materials, and in recent years, has been employed to study a broad range of non-ferroelectric polar materials, including piezoelectric biomaterials. At the same time, the technique has been extended from ambient to liquid imaging on model ferroelectric systems. Here, we present results on local electromechanical probing of several model cellular and biomolecular systems, including insulin and lysozyme amyloid fibrils, breast adenocarcinoma cells, and bacteriorhodopsin in a liquid environment. The specific features of SPM operation in liquid are delineated and bottlenecks on the route towards nanometer-resolution electromechanical imaging of biological systems are identified.

cond-mat.other↗

arXiv2006

Nanoscale polarization manipulation and imaging in ferroelectric Langmuir-Blodgett polymer films

The behavior of ferroelectricity at the nanoscale is the focus of increasing research activity because of intense interest in the fundamental nature of spontaneous order in condensed-matter systems and because of the many practical applications of ferroelectric thin films to, for example, electromechanical transducers, infrared imaging sensors, and nonvolatile random-access memories. Ferroelectricity, in analogy with its namesake ferromagnetism, is the property of some crystalline systems to maintain a permanent, but reversible, electrical polarization in the absence of an external electric field. The imaging and dynamics of the piezoelectric response at the nanoscale is perhaps the most direct means of probing polarization, as has been demonstrated in a number of thin films and nanostructures . Here we report the use of piezoresponse force microscopy (PFM) and switching spectroscopy PFM (SSPFM) to image the ferroelectric properties, domain structure, and polarization switching of ultrathin ferroelectric Langmuir-Blodgett films of poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE)) copolymers. PFM imaging of P(VDF-TrFE) thin films reveals ferroelectric domain sizes on the order of 25-50 nm and an imaging resolution below 5 nm. The feature sizes in topography and PFM images are comparable and the boundaries of uniformly polarized regions coincide with topographic features. Arbitrary polarization patterns could be repeatedly written and erased, with writing resolution limited by the grain size. Hysteresis loops from individual domains show clear coercive voltage, but are not well saturated at +/-10 V amplitude.

cond-mat.mtrl-sci↗

arXiv2006

Piezoresponse Force Spectroscopy of Ferroelectric Materials

Piezoresponse Force Spectroscopy (PFS) has emerged as a powerful technique for probing highly localized switching behavior and the role of microstructure and defects on switching. The application of a dc bias to a scanning probe microscope tip in contact with a ferroelectric surface results in the nucleation and growth of a ferroelectric domain below the tip, resulting in changes in local electromechanical response. Resulting hysteresis loops contains information on local ferroelectric switching behavior. The signal in PFS is the convolution of the volume of the nascent domain and the probing volume of the tip. Here, we analyze the signal formation mechanism in PFS by deriving the main parameters of domain nucleation in a semi-infinite material and establishing the relationships between domain parameters and PFM signal using a linear Greens function theory. The effect of surface screening and finite Debye length on the switching behavior is established. In particular, we predict that the critical nucleus size in PFM is controlled by the surface screening mechanism and in the absence of screening, tip-induced switching is impossible. Future prospects of PFS to study domain nucleation in the vicinity of defects, local switching centers in ferroelectrics, and unusual polarization states in low-dimensional ferroelectrics are discussed.

cond-mat.mtrl-sci↗