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Jiangyu Li

Publications and source records attributed to Jiangyu Li.

31 records · Page 2Linked to original sources

Mapping Intrinsic Electromechanical Responses at the Nanoscale via Sequential Excitation Scanning Probe Microscopy Empowered by Deep Data

Ever increasing hardware capabilities and computation powers have made acquisition and analysis of big scientific data at the nanoscale routine, though much of the data acquired often turns out to be redundant, noisy, and/or irrelevant to the problems of interests, and it remains nontrivial to draw clear mechanistic insights from pure data analytics. In this work, we use scanning probe microscopy (SPM) as an example to demonstrate deep data methodology, transitioning from brute force analytics such as data mining, correlation analysis, and unsupervised classification to informed and/or targeted causative data analytics built on sound physical understanding. Three key ingredients of such deep data analytics are presented. A sequential excitation scanning probe microscopy (SE-SPM) technique is first adopted to acquire high quality, efficient, and physically relevant data, which can be easily implemented on any standard atomic force microscope (AFM). Brute force physical analysis is then carried out using simple harmonic oscillator (SHO) model, enabling us to derive intrinsic electromechanical coupling of interests. Finally, principal component analysis (PCA) is carried out, which not only speeds up the analysis by four orders of magnitude, but also allows a clear physical interpretation of its modes in combination with SHO analysis. A rough piezoelectric material has been probed using such strategy, enabling us to map its intrinsic electromechanical properties at the nanoscale with high fidelity, where conventional methods fail. The SE in combination with deep data methodology can be easily adapted for other SPM techniques to probe a wide range of functional phenomena at the nanoscale.

cond-mat.mtrl-sci↗

Artificial Intelligent Atomic Force Microscope Enabled by Machine Learning

Artificial intelligence (AI) and machine learning have promised to revolutionize the way we live and work, and one of particularly promising areas for AI is image analysis. Nevertheless, many current AI applications focus on post-processing of data, while in both materials sciences and medicines, it is often critical to respond to the data acquired on the fly. Here we demonstrate an artificial intelligent atomic force microscope (AI-AFM) that is capable of not only pattern recognition and feature identification in ferroelectric materials and electrochemical systems, but can also respond to classification via adaptive experimentation with additional probing at critical domain walls and grain boundaries, all in real time on the fly without human interference. We believe such a strategy empowered by machine learning is applicable to a wide range of instrumentations and broader physical machineries.

cond-mat.mtrl-sci↗

Piezoelectricity of Atomically Thin WSe2 via Laterally Excited Scanning Probe Microscopy

Lattices of odd-layered two-dimensional (2D) transition metal dichalcogenides (TMDs) such as WSe2 are non-centrosymmetric, and thus could possess linear piezoelectricity that is attractive for applications such as nanoelectromechanical systems (NEMS) and nanogenerators. Measuring the electromechanical coupling of 2D TMDs, however, is rather challenging, since its D3h point group symmetry makes conventional piezoresponse force microscopy (PFM) inapplicable. Here we develop a lateral excitation scanning probe microscopy (SPM) technique that enables mapping of the piezoelectric response of atomically thin WSe2 directly on a substrate with high spatial resolution. Planar electrodes are used to excite piezoelectric vibrations while imposing anisotropic in-plane mechanical constraint to the WSe2, resulting in an out-of-plane deformation due to Poisson's effect that can be measured by an SPM probe. Using this technique, we show that WSe2 monolayer and trilayers exhibit strong electromechanical response linear to the applied excitation biases that is distinct from the substrate, while WSe2 bilayer show negligible electromechanical response as expected. The effective piezoelectric coefficient is estimated to be 5.2 pm/V from the measurement, consistent with theoretical predictions. This method can be conveniently applied to a wide range of 2D materials with similar symmetry.

cond-mat.mtrl-sci↗

Quardratic Electromechanical Strain in Silicon Investigated by Scanning Probe Microscopy

Piezoresponse force microscopy (PFM) is a powerful tool widely used to characterize piezoelectricity and ferroelectricity at the nanoscale. However, it is necessary to distinguish microscopic mechanisms between piezoelectricity and non-piezoelectric contributions measured by PFM. In this work, we systematically investigate the first and second harmonic apparent piezoresponses of silicon wafer in both vertical and lateral modes, and we show that it exhibits apparent electromechanical response that is quadratic to the applied electric field, possibly arising from ionic electrochemical dipoles induced by the charged probe. As a result, the electromechanical response measured is dominated by the second harmonic response in vertical mode, and its polarity can be switched by the DC voltage with evolving coercive field and maximum amplitude, in sharp contrast with typical ferroelectric materials we used as control. The ionic activity in silicon is also confirmed by scanning thermo-ionic microscopy (STIM) measurement, and this work points toward a set of methods to distinguish true piezoelectricity from the apparent ones.

cond-mat.mtrl-sci↗

Resolving Local Electrochemistry at the Nanoscale via Electrochemical Strain Microscopy: Modeling and Experiments

Electrochemistry is the underlying mechanism in a variety of energy conversion and storage systems, and it is well known that the composition, structure, and properties of electrochemical materials near active interfaces often deviates substantially and inhomogeneously from the bulk properties. A universal challenge facing the development of electrochemical systems is our lack of understanding of physical and chemical rates at local length scales, and the recently developed electrochemical strain microscopy (ESM) provides a promising method to probe crucial local information regarding the underlying electrochemical mechanisms. Here we develop a computational model that couples mechanics and electrochemistry relevant for ESM experiments, with the goal to enable quantitative analysis of electrochemical processes underneath a charged scanning probe. We show that the model captures the essence of a number of different ESM experiments, making it possible to de-convolute local ionic concentration and diffusivity via combined ESM mapping, spectroscopy, and relaxation studies. Through the combination of ESM experiments and computations, it is thus possible to obtain deep insight into the local electrochemistry at the nanoscale.

cond-mat.mtrl-sci↗

Ferroic Domains of Alternating Polar and Nonpolar Orders Regulate Photocurrent in Single Crystalline CH3NH3PbI3 Films Self-grown on FTO/TiO2 Substrate

Photovoltaic conversion efficiency (PCE) of halide perovskite solar cells has risen spectacularly, yet the very crystalline structure of CH3NH3PbI3 remains ambiguous after extensive researches, and its polar nature remains hotly debated. Here we present compelling evidences that CH3NH3PbI3 crystals self-grown on FTO/TiO2 substrate consist of ferroic domains with alternating polar and nonpolar orders, in contrast to previous experimental and theoretical expectations, and polar domains possess reduced photocurrent. It is found that polar and nonpolar orders of CH3NH3PbI3 can be distinguished from their distinct lateral piezoresponse, energy dissipation, first and second harmonic electromechanical couplings, and temperature variation, even though their difference in crystalline lattice is very subtle, and they possess two-way memory effect through cubic-tetragonal phase transition. These findings resolve key questions regarding polar nature of CH3NH3PbI3 and its implication on photovoltaics, reconcile contradictory data widely reported, and point a direction toward engineering ferroic domains for enhanced PCE.

cond-mat.mtrl-sci↗

Phase-field modeling and electronic structural analysis of flexoelectric effect at 180° domain walls in ferroelectric PbTiO3

Flexoelectric effect is the coupling between strain, polarization and their gradients, which are prominent at the nanoscale. Although this effect is important to understand nanostructures, such as domain walls in ferroelectrics, its electronic mechanism is not clear. In this work, we combined phase-field simulations and first-principles calculations to study the 180° domain walls in tetragonal ferroelectric PbTiO3, and found that the ultimate source of Néel components is the gradient of the square of spontaneous polarizations. Electronic structural analysis reveals that there is a redistribution of electronic charge density and potential around domain walls, which produces the electric field and Néel components. This work thus sheds light on the electronic mechanism of the flexoelectric effect around 180° domain walls in tetragonal ferroelectrics.

cond-mat.mtrl-sci↗

Scanning Thermo-ionic Microscopy: Probing Nanoscale Electrochemistry via Thermal Stress-induced Oscillation

A universal challenge facing the development of electrochemical materials is our lack of understanding of physical and chemical processes at local length scales in 10-100 nm regime, and acquiring this understanding requires a new generation of imaging techniques. In this article, we introduce the scanning thermo-ionic microscopy (STIM) for probing local electrochemistry at the nanoscale, using for imaging the Vegard strain induced via thermal stress excitations. Since ionic oscillation is driven by the stress instead of voltage, the responses are insensitive to the electromechanical, electrostatic, and capacitive effects, and they are immune to global current perturbation, making in-operando testing possible.

cond-mat.mes-hall↗

Touching is believing: interrogating organometal halide perovskite solar cells at the nanoscale via scanning probe microscopy

Halide perovskite solar cells based on CH3NH3PbI3 and related materials have emerged as the most exciting development in the next generation photovoltaic technologies, yet the microscopic phenomena involving photo-carriers, ionic defects, spontaneous polarization, and molecular vibration and rotation interacting with numerous grains, grain boundaries, and interfaces are still inadequately understood. In fact, there is still need for an effective method to interrogate the local photovoltaic properties of halide perovskite solar cells that can be directly traced to their microstructures on one hand and linked to their device performance on the other hand. In this perspective, we propose that scanning probe microscopy techniques have great potential to realize such promises at the nanoscale, and highlight some of the recent progresses and challenges along this line of investigation toward local probing of photocurrent, work function, ionic activities, polarization switching, and chemical degradation. We also emphasize the importance of multi-modality imaging, in-operando scanning, big data analysis, and multidisciplinary collaboration for further studies toward fully understanding of these complex systems.

cond-mat.mtrl-sci↗

Imaging Ferroelectric Domains via Charge Gradient Microscopy Enhanced by Principal Component Analysis

Local domain structures of ferroelectrics have been studied extensively using various modes of scanning probes at the nanoscale, including piezoresponse force microscopy (PFM) and Kelvin probe force microscopy (KPFM), though none of these techniques measure the polarization directly, and the fast formation kinetics of domains and screening charges cannot be captured by these quasi-static measurements. In this study, we used charge gradient microscopy (CGM) to image ferroelectric domains of lithium niobate based on current measured during fast scanning, and applied principal component analysis (PCA) to enhance the signal-to-noise ratio of noisy raw data. We found that the CGM signal increases linearly with the scan speed while decreases with the temperature under power-law, consistent with proposed imaging mechanisms of scraping and refilling of surface charges within domains, and polarization change across domain wall. We then, based on CGM mappings, estimated the spontaneous polarization and the density of surface charges with order of magnitude agreement with literature data. The study demonstrates that PCA is a powerful method in imaging analysis of scanning probe microscopy (SPM), with which quantitative analysis of noisy raw data becomes possible.

cond-mat.mtrl-sci↗

Quantitative Nanoscale Mapping of Three-Phase Thermal Conductivities in Filled Skutterudites via Scanning Thermal Microscopy

In the last two decades, a nanostructuring paradigm has been successfully applied in a wide range of thermoelectric materials, resulting in significant reduction in thermal conductivity and superior thermoelectric performance. These advances, however, have been accomplished without directly investigating the local thermoelectric properties, even though local electric current can be mapped with high spatial resolution. In fact, there still lacks an effective method that links the macroscopic thermoelectric performance to the local microstructures and properties. Here, we show that local thermal conductivity can be mapped quantitatively with good accuracy, nanometer resolution, and one-to-one correspondence to the microstructure using a three-phase skutterudite as a model system. Scanning thermal microscopy combined with finite element simulations demonstrate close correlation between sample conductivity and probe resistance, enabling us to distinguish thermal conductivities spanning orders of magnitude, yet resolving thermal variation across a phase interface with small contrast. The technique thus provides a powerful tool to correlate local thermal conductivities, microstructures, and macroscopic properties for nanostructured materials in general, and nanostructured thermoelectrics in particular.

cond-mat.mtrl-sci↗

High density array of epitaxial BiFeO3 nanodots with robust and reversibly switchable topological domain states

The exotic topological domains in ferroelectrics and multiferroics have attracted extensive interest in recent years due to their novel functionalities and potential applications in nanoelectronic devices. One of the key challenges for such applications is a realization of robust yet reversibly switchable nanoscale topological domain states with high density, wherein spontaneous topological structures can be individually addressed and controlled. This has been accomplished in our work using high density arrays of epitaxial BiFeO3 (BFO) nanodots with lateral size as small as ~60 nm. We demonstrate various types of spontaneous topological domain structures, including center-convergent domains, center-divergent domains, and double-center domains, which are stable over sufficiently long time yet can be manipulated and reversibly switched by electric field. The formation mechanisms of these topological domain states, assisted by the accumulation of compensating charges on the surface, have also been revealed. These result demonstrated that these reversibly switchable topological domain arrays are promising for applications in high density nanoferroelectric devices such as nonvolatile memories

cond-mat.mtrl-sci↗

Mechanisms of Electromechanical Coupling in Strain Based Scanning Probe Microscopy

Electromechanical coupling is ubiquitous in nature and underpins the functionality of materials and systems as diverse as ferroelectric and multiferroic materials, electrochemical devices, and biological systems, and strain-based scanning probe microscopy (s-SPM) techniques have emerged as a powerful tool in characterizing and manipulating electromechanical coupling at the nanoscale. Uncovering underlying mechanisms of electromechanical coupling in these diverse materials and systems, however, is a difficult outstanding problem, and questions and confusions arise from recent experiment observations of electromechanical coupling and its apparent polarity switching in some unexpected materials. We propose a series of s-SPM experiments to identify different microscopic mechanisms underpinning electromechanical coupling, and demonstrate their feasibility using three representative materials. By employing a combination of spectroscopic studies and different modes of s-SPM, we show that it is possible to distinguish electromechanical coupling arising from spontaneous polarization, induced dipole moment, and ionic Vegard strain, and this offer a clear guidance on using s-SPM to study a wide variety of functional materials and systems.

cond-mat.mtrl-sci↗