ORCID Profile
0000-0002-6521-868X
Current Organisation
University of California, Irvine
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Publisher: The Electrochemical Society
Date: 2012
DOI: 10.1149/2.051209JES
Publisher: American Chemical Society (ACS)
Date: 21-11-2019
Publisher: Oxford University Press (OUP)
Date: 22-01-2009
Abstract: The short depth of focus of aberration-corrected scanning transmission electron microscopes (STEMs) could potentially enable 3D reconstruction of nanomaterials through acquisition of a through-focal series. However, the contrast transfer function of annular dark-field (ADF)-STEM depth sectioning has a missing-cone problem similar to that of tilt-series tomography. The elongation as a function of the probe-forming angle is found to be (square root of 3/2) x 1/alphamax. For existing aberration-corrected STEMs operated at optimal imaging conditions, the elongation factor for depth sectioning is larger than 30. This large elongation factor results in highly distorted shapes of 3D objects and unexpected artifacts due to the loss of information. Depth-sectioning experiments using a 33-mrad 100 keV C(5)-corrected aberration-corrected STEM demonstrate the elongation effect and the missing-cone problem in real and reciprocal space. The performance limits of different S/TEM-based imaging modes are compared. There is a missing cone of information for bright-field S/TEM, ADF-STEM, hollow-cone ADF-STEM and coherent scanning confocal electron microscopy (SCEM). Only incoherent SCEM fills the missing cone.
Publisher: AIP Publishing
Date: 07-01-2008
DOI: 10.1063/1.2828990
Abstract: The ability to detect in idual impurity atoms has been greatly enhanced by the development of aberration-corrected electron microscopes. The reduced depth of focus potentially enables three-dimensional reconstructions of impurity atoms from through-focal series. We test the robustness of this depth-sectioning method for detecting impurity atoms in gate oxides using multislice simulations. For amorphous materials, dopants can be reliably imaged, and are accurately described by a simpler three-dimensional linear imaging model. For crystalline materials, however, channeling artifacts can render the signal uninterpretable. These artifacts can be eliminated by orienting the crystal slightly off the zone axis, which still preserves atomic resolution.
Publisher: American Physical Society (APS)
Date: 31-12-2014
Publisher: Springer Science and Business Media LLC
Date: 18-09-2014
DOI: 10.1038/NCOMMS5971
Abstract: Ferroelectrics have been used as memory storage devices, with an upper bound on the total possible memory levels generally dictated by the number of degenerate states allowed by the symmetry of the ferroelectric phase. Here, we introduce a new concept for storage wherein the polarization can be rotated arbitrarily, effectively decoupling it from the crystallographic symmetry of the ferroelectric phase on the mesoscale. By using a Bi5Ti3FeO15-CoFe2O4 film and via Band-Excitation Piezoresponse Force Microscopy, we show the ability to arbitrarily rotate polarization, create a spectrum of switched states, and suggest the reason for polarization rotation is an abundance of sub-50 nm nanodomains. Transmission electron microscopy-based strain mapping confirms significant local strain undulations imparted on the matrix by the CoFe2O4 inclusions, which causes significant local disorder. These experiments point to controlled tuning of polarization rotation in a standard ferroelectric, and hence the potential to greatly extend the attainable densities for ferroelectric memories.
Publisher: American Chemical Society (ACS)
Date: 12-11-2013
DOI: 10.1021/NN404779X
Abstract: Epitaxial self-assembled ferro(i)magnetic spinel (CoFe2O4 (CFO)) and ferroelectric bismuth layered perovskite (Bi5Ti3FeO15 (BTFO)) pillar-matrix nanostructures are demonstrated on (001) single-crystalline strontium titanate substrates. The CFO remains embedded in the BTFO matrix as vertical pillars (∼50 nm in diameter) up to a volume fraction of 50%. Piezoresponse force microscopy experiments evidence a weak out-of-plane and a strong in-plane ferroelectricity in the BTFO phase, despite previously reported paraelectricity along the c-axis in a pure BTFO film. Phenomenological Landau-Ginzburg-Devonshire-based thermodynamic computations show that the radial stress induced by the CFO nanopillars can influence these ferroelectric phases, thus signifying the importance of the nanopillars. The CFO pillars demonstrate robust ferromagnetic hysteresis loops with little degradation in the saturation magnetization (ca. 4 μB/f.u.). Thus BTFO-CFO nanocomposites show significant promise as a lead-free magnetoelectric materials system.
Publisher: Springer Science and Business Media LLC
Date: 23-06-2016
DOI: 10.1038/NCOMMS11941
Abstract: Replacing platinum by a less precious metal such as palladium, is highly desirable for lowering the cost of fuel-cell electrocatalysts. However, the instability of palladium in the harsh environment of fuel-cell cathodes renders its commercial future bleak. Here we show that by incorporating trace amounts of gold in palladium-based ternary (Pd 6 CoCu) nanocatalysts, the durability of the catalysts improves markedly. Using aberration-corrected analytical transmission electron microscopy in conjunction with synchrotron X-ray absorption spectroscopy, we show that gold not only galvanically replaces cobalt and copper on the surface, but also penetrates through the Pd–Co–Cu lattice and distributes uniformly within the particles. The uniform incorporation of Au provides a stability boost to the entire host particle, from the surface to the interior. The spontaneous replacement method we have developed is scalable and commercially viable. This work may provide new insight for the large-scale production of non-platinum electrocatalysts for fuel-cell applications.
Publisher: AIP Publishing
Date: 14-09-2009
DOI: 10.1063/1.3213346
Abstract: We have studied the effect of biaxial strain on thin films of (001) La0.7Sr0.3MnO3. We deposited films by reactive molecular-beam epitaxy on different single crystalline substrates, varying the substrate-induced biaxial strain from −2.3% to +3.2%. Magnetization and electrical transport measurements reveal that the dependence of the Curie temperature on biaxial strain is in very good agreement with the theoretical predictions of Millis et al. [J. Appl. Phys. 83, 1588 (1998)].
Publisher: American Chemical Society (ACS)
Date: 12-01-2012
DOI: 10.1021/NL203920S
Abstract: We present an electron tomography method that allows for the identification of hundreds of electrocatalyst nanoparticles with one-to-one correspondence before and after electrochemical aging. This method allows us to track, in three-dimensions, the trajectories and morphologies of each Pt-Co nanocatalyst on a fuel cell carbon support. In conjunction with the use of atomic-scale electron energy loss spectroscopic imaging, our experiment enables the correlation of performance degradation of the catalyst with changes in particle/interparticle morphologies, particle-support interactions, and the near-surface chemical composition. We found that aging of the catalysts under normal fuel cell operating conditions (potential scans from +0.6 to +1.0 V for 30,000 cycles) gives rise to coarsening of the nanoparticles, mainly through coalescence, which in turn leads to the loss of performance. The observed coalescence events were found to be the result of nanoparticle migration on the carbon support during potential cycling. This method provides detailed insights into how nanocatalyst degradation occurs in proton exchange membrane fuel cells (PEMFCs) and suggests that minimization of particle movement can potentially slow down the coarsening of the particles and the corresponding performance degradation.
Publisher: Elsevier BV
Date: 07-2018
Publisher: American Chemical Society (ACS)
Date: 10-09-2012
DOI: 10.1021/NL302404G
Abstract: A promising electrocatalyst prototype of low Pt mole fraction, intermetallic nanoparticles of Cu(3)Pt, has been prepared using a simple impregnation-reduction method, followed by a post heat-treatment. Two dealloying methods (electrochemical and chemical) were implemented to control the atomic-level morphology and improve performance for the oxygen reduction reaction (ORR). The morphology and elemental composition of the dealloyed nanoparticles were characterized at angstrom resolution using an aberration-corrected scanning transmission electron microscope equipped with an electron energy loss spectrometer. We found that the electrochemical dealloying method led to the formation of a thin Pt skin of ca. 1 nm in thickness with an ordered Cu(3)Pt core structure, while chemical leaching gave rise to a "spongy" structure with no ordered structure being preserved. A three-dimensional tomographic reconstruction indicated that numerous voids were formed in the chemically dealloyed nanoparticles. Both dealloying methods yielded enhanced specific and mass activities toward the ORR and higher stability relative to Pt/C. The spongy nanoparticles exhibited better mass activity with a slightly lower specific activity than the electrochemically dealloyed nanoparticles after 50 potential cycles. In both cases, the mass activity was still enhanced after 5000 potential cycles.
Publisher: American Chemical Society (ACS)
Date: 07-12-2011
DOI: 10.1021/NL203975U
Abstract: The thousand-fold increase in data-collection speed enabled by aberration-corrected optics allows us to overcome an electron microscopy paradox: how to obtain atomic-resolution chemical structure in in idual nanoparticles yet record a statistically significant s le from an inhomogeneous population. This allowed us to map hundreds of Pt-Co nanoparticles to show atomic-scale elemental distributions across different stages of the catalyst aging in a proton-exchange-membrane fuel cell, and relate Pt-shell thickness to treatment, particle size, surface orientation, and ordering.
Publisher: American Association for the Advancement of Science (AAAS)
Date: 22-08-2014
Abstract: Size and shape drive the properties of metal nanoparticles. Understanding the factors that affect their growth is central to making use of the particles in a range of applications. Liao et al. tracked the growth of platinum nanoparticle shapes at high resolution using state-of-the-art liquid cells for in situ monitoring inside an electron microscope. The authors tracked changes in the growth rates at different crystal facets caused by differences in the mobility of the capping ligand. Science , this issue p. 916
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8TA03250E
Abstract: Tuning the hydrogen adsorption energy on Pt surface is essential for enhancing the HOR performance in alkaline media.
Publisher: American Chemical Society (ACS)
Date: 04-06-2012
DOI: 10.1021/CM203863D
Publisher: American Chemical Society (ACS)
Date: 13-02-2013
DOI: 10.1021/CM303489Z
Publisher: Oxford University Press (OUP)
Date: 15-06-2012
DOI: 10.1017/S1431927612000244
Abstract: The high beam current and subangstrom resolution of aberration-corrected scanning transmission electron microscopes has enabled electron energy loss spectroscopy (EELS) mapping with atomic resolution. These spectral maps are often dose limited and spatially overs led, leading to low counts/channel and are thus highly sensitive to errors in background estimation. However, by taking advantage of redundancy in the dataset map, one can improve background estimation and increase chemical sensitivity. We consider two such approaches—linear combination of power laws and local background averaging—that reduce background error and improve signal extraction. Principal component analysis (PCA) can also be used to analyze spectrum images, but the poor peak-to-background ratio in EELS can lead to serious artifacts if raw EELS data are PCA filtered. We identify common artifacts and discuss alternative approaches. These algorithms are implemented within the Cornell Spectrum Imager, an open source software package for spectroscopic analysis.
Publisher: Oxford University Press (OUP)
Date: 04-05-2012
DOI: 10.1017/S1431927612000189
Abstract: An accurate determination of specimen thickness is essential for quantitative analytical electron microscopy. Here we demonstrate that a position-averaged incoherent bright-field signal recorded on an absolute scale can be used to determine the thickness of on-axis crystals with a precision of ±1.6 nm. This method measures both the crystalline and the noncrystalline parts (surface amorphous layers) of the s le. However, it avoids the systematic error resulting from surface plasmon contributions to the inelastic mean-free-path thickness estimated by electron energy loss spectroscopy.
Publisher: Wiley
Date: 18-01-2019
Publisher: American Chemical Society (ACS)
Date: 10-09-2018
Publisher: AIP Publishing
Date: 31-05-2010
DOI: 10.1063/1.3442496
Abstract: The three-dimensional reconstruction of a porous low-dielectric constant film (κ=2.5), resolving pores as small as 1 nm, was achieved using annular dark-field scanning transmission electron tomography, enabling quantitative measurements of the pore morphologies and size distribution. Most large pores were elliptical. Together with log-normal pore-size distribution, this suggests pore coalescence during the material’s growth. Ellipsometric porosimetry indicates a high degree of interconnectivity between pores. Tomography shows the material exhibits little large-scale pore connectivity, thus placing an upper limit on the size of the interconnections at below 1 nm. Systematic errors in the tomographic and ellipsometric size distributions appear to be largely complementary.
Publisher: American Physical Society (APS)
Date: 28-09-2012
Publisher: American Association for the Advancement of Science (AAAS)
Date: 27-11-2009
Abstract: For single crystals to remain intact, there is a limit to the size and number of defects that can be included before the underlying lattice is destroyed. Biological crystals, however, are known to include large macromolecules. H. Li et al. (p. 1244 see the Perspective by Hollingsworth ) used electron tomography to study the crystallization of calcium carbonate inside an agarose gel, observing that the crystals physically entrapped the agarose macromolecules. To accommodate the curvature induced by the polymer chains, both high- and low-energy facets formed at the fiber-crystal interfaces. Thus, physical interactions alone may be sufficient for the incorporation of macromolecules in biological crystals and it may be possible to grow unusually shaped single crystals.
Publisher: Springer Science and Business Media LLC
Date: 28-10-2012
DOI: 10.1038/NMAT3458
Abstract: To enhance and optimize nanocatalyst performance and durability for the oxygen reduction reaction in fuel-cell applications, we look beyond Pt-metal disordered alloys and describe a new class of Pt-Co nanocatalysts composed of ordered Pt(3)Co intermetallic cores with a 2-3 atomic-layer-thick platinum shell. These nanocatalysts exhibited over 200% increase in mass activity and over 300% increase in specific activity when compared with the disordered Pt(3)Co alloy nanoparticles as well as Pt/C. So far, this mass activity for the oxygen reduction reaction is the highest among the Pt-Co systems reported in the literature under similar testing conditions. Stability tests showed a minimal loss of activity after 5,000 potential cycles and the ordered core-shell structure was maintained virtually intact, as established by atomic-scale elemental mapping. The high activity and stability are attributed to the Pt-rich shell and the stable intermetallic Pt(3)Co core arrangement. These ordered nanoparticles provide a new direction for catalyst performance optimization for next-generation fuel cells.
Publisher: American Physical Society (APS)
Date: 12-11-2012
Publisher: American Chemical Society (ACS)
Date: 04-10-2016
Publisher: American Chemical Society (ACS)
Date: 24-11-2010
DOI: 10.1021/JA107874U
Abstract: A simple method for the preparation of PdCo@Pd core-shell nanoparticles supported on carbon based on an adsorbate-induced surface segregation effect has been developed. The stability of these PdCo@Pd nanoparticles and their electrocatalytic activity for the oxygen reduction reaction (ORR) were enhanced by decoration with a small amount of Pt deposited via a spontaneous displacement reaction. The facile method described herein is suitable for large-scale, lower-cost production and significantly lowers the Pt loading and thus the cost. The as-prepared PdCo@Pd and Pd-decorated PdCo@Pd nanocatalysts have a higher methanol tolerance than Pt/C in the ORR and are promising cathode catalysts for fuel cell applications.
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0TA04244G
Abstract: The compressive stress at the NiOOH/NiO interface, created through the battery conversion chemistry, is found to influence the OER performance.
Publisher: Oxford University Press (OUP)
Date: 22-05-2013
DOI: 10.1017/S1431927613001438
Abstract: Finding a faster alternative to tilt-series electron tomography is critical for rapidly evolving fields such as the semiconductor industry, where failure analysis could greatly benefit from higher throughput. We present a theoretical and experimental evaluation of scanning confocal electron energy-loss microscopy (SCEELM) using valence-loss signals, which is a promising technique for the reliable reconstruction of materials with sub-10-nm resolution. Such a confocal geometry transfers information from the focused portion of the electron beam and enables rapid three-dimensional (3D) reconstruction by depth sectioning. SCEELM can minimize or eliminate the missing-information cone and the elongation problem that are associated with other depth-sectioning image techniques in a transmission electron microscope. Valence-loss SCEELM data acquisition is an order of magnitude faster and requires little postprocessing compared with tilt-series electron tomography. With postspecimen chromatic aberration ( C c ) correction, SCEELM signals can be acquired in parallel in the direction of energy dispersion with the aid of a physical pinhole. This increases the efficiency by 10×–100×, and can provide 3D resolved chemical information for multiple core-loss signals simultaneously.
Publisher: Springer Science and Business Media LLC
Date: 24-02-2014
DOI: 10.1038/NCOMMS4358
Publisher: Oxford University Press (OUP)
Date: 22-06-2010
DOI: 10.1017/S1431927610093360
Abstract: This article focuses on the development of a transparent and uniform understanding of possibilities for three-dimensional (3D) imaging in scanning transmission and confocal electron microscopes (STEMs and SCEMs), with an emphasis on the annular dark-field STEM (ADF-STEM), bright-field SCEM (BF-SCEM), and ADF-SCEM configurations. The incoherent imaging approximation and a 3D linear imaging model for ADF-STEM are reviewed. A 3D phase contrast model for coherent-SCEM as well as a pictorial way to find boundaries of information transfer in reciprocal space are reviewed and applied to both BF- and ADF-SCEM to study their 3D point spread functions and contrast transfer functions (CTFs). ADF-STEM is capable of detecting the depths of dopant atoms in amorphous materials but can fail for crystalline materials when channeling substantially modifies the electron propagation. For the imaging of extended (i.e., nonpointlike) features, ADF-STEM and BF-SCEM exhibit strong elongation artifacts due to the missing cone of information. ADF-SCEM shows an improvement over ADF-STEM/BF-SCEM due to its differential phase contrast eliminating slowly varying backgrounds, an effect that partially suppresses the elongation artifacts. However, the 3D CTF still has a cone of missing information that will result in some residual feature elongation as has been observed in A. Hashimoto et al., J Appl Phys 160 (8), 086101 (2009).
Publisher: American Chemical Society (ACS)
Date: 05-09-2012
DOI: 10.1021/JP306107T
Publisher: American Association for the Advancement of Science (AAAS)
Date: 08-10-2010
Abstract: Polymer templating has been used to fabricate a wide range of ordered materials, both due to the ability to pattern the polymers easily over a large area and their facile removal. However, the process is somewhat limited to the incorporation of materials that will flow easily into the templated areas. Arora et al. (p. 214 ) show that current techniques can be extended to the patterning of metals, through guided epitaxial growth. An excimer laser was used to control the flow of material into patterned templates formed from block copolymers.
Publisher: Oxford University Press (OUP)
Date: 02-12-2010
DOI: 10.1017/S1431927610094171
Abstract: Aberration-corrected scanning transmission electron microscopes (STEMs) provide sub-Angstrom lateral resolution however, the large convergence angle greatly reduces the depth of field. For microscopes with a small depth of field, information outside of the focal plane quickly becomes blurred and less defined. It may not be possible to image some s les entirely in focus. Extended depth-of-field techniques, however, allow a single image, with all areas in focus, to be extracted from a series of images focused at a range of depths. In recent years, a variety of algorithmic approaches have been employed for bright-field optical microscopy. Here, we demonstrate that some established optical microscopy methods can also be applied to extend the ∼6 nm depth of focus of a 100 kV 5th-order aberration-corrected STEM (α max = 33 mrad) to image Pt-Co nanoparticles on a thick vulcanized carbon support. These techniques allow us to automatically obtain a single image with all the particles in focus as well as a complimentary topography map.
Publisher: Wiley
Date: 14-04-2011
Publisher: American Chemical Society (ACS)
Date: 02-11-2016
Abstract: The nanoscale origins of ferroelastic domain wall motion in ferroelectric multilayer thin films that lead to giant electromechanical responses are investigated. We present direct evidence for complex underpinning factors that result in ferroelastic domain wall mobility using a combination of atomic-level aberration corrected scanning transmission electron microscopy and phase-field simulations in model epitaxial (001) tetragonal (T) PbZr
Publisher: Wiley
Date: 26-09-2011
DOI: 10.1111/J.1365-2818.2011.03553.X
Abstract: Black carbon (BC) is one of the most stable forms of soil organic matter. Its surface functional groups and structure have been well characterized by a range of analytical methods. However, little is known about the mechanisms of interactions between the BC particles and the surrounding mineral matter. In this paper a range of microscopy techniques, such as transmission electron microscopy and scanning transmission electron microscopy, were used to investigate the possible reactions of BC particles within microaggregates (<2 mm) found in Amazonian dark Earth. Attention is given to the interactions that occur at the interfacial regions between the organic and inorganic phases. Examination of Amazonian dark Earth showed that the carbon-rich phase detected within the BC particles has a significant calcium concentration and a high density of micropores was found at the BC-mineral interface. These observations provide evidence to support suggested mechanisms of interaction between these phases.
Publisher: Informa UK Limited
Date: 14-12-2010
Publisher: Elsevier BV
Date: 04-2014
DOI: 10.1016/J.ULTRAMIC.2014.01.006
Abstract: Recent work has convincingly argued that the Stobbs factor-disagreement in contrast between simulated and experimental atomic-resolution images-in ADF-STEM imaging can be accounted for by including the incoherent source size in simulation. However, less progress has been made for atomic-resolution STEM-EELS mapping. Here we have performed carefully calibrated EELS mapping experiments of a [101] DyScO3 single-crystal specimen, allowing atomic-resolution EELS signals to be extracted on an absolute scale for a large range of thicknesses. By simultaneously recording the elastic signal, also on an absolute scale, and using it to characterize the source size, s le thickness and inelastic mean free path, we eliminate all free parameters in the simulation of the core-loss signals. Coupled with double channeling simulations that incorporate both core-loss inelastic scattering and dynamical elastic and thermal diffuse scattering, the present work enables a close scrutiny of the scattering physics in the inelastic channel. We found that by taking into account the effective source distribution determined from the ADF images, both the absolute signal and the contrast in atomic-resolution Dy-M5 maps can be closely reproduced by the double-channeling simulations. At lower energy losses, discrepancies are present in the Sc-L2,3 and Dy-N4,5 maps due to the energy-dependent spatial distribution of the background spectrum, core-hole effects, and omitted complexities in the final states. This work has demonstrated the possibility of using quantitative STEM-EELS for element-specific column-by-column atom counting at higher energy losses and for atomic-like final states, and has elucidated several possible improvements for future theoretical work.
Publisher: Springer Science and Business Media LLC
Date: 06-2015
DOI: 10.1557/MRC.2015.12
No related grants have been discovered for Huolin Xin.