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Mariana Palos

Publications and source records attributed to Mariana Palos.

5 recordsLinked to original sources

Polar Topologies in a Ferroelastic Metal Membrane

Polar metals, materials in which electric polarisation and metallicity coexist, are exceptionally rare because itinerant electrons screen long-range dipoles and favour centrosymmetric structures. Engineering polar textures in a conducting magnet holds promise for reconfigurable spin orbit coupling and magnetoelectric functionality. Here we show that releasing epitaxial SrRuO3 films from their substrates drives a hierarchy of ferroelastic domain refinement from micrometre to nanometre length scales, and that this structural reorganisation spontaneously generates two distinct classes of emergent polar texture that are ubiquitous across the freestanding membrane. Using correlative microscopy from mesoscale electron channelling contrast imaging (ECCI) to atomic resolution scanning transmission electron microscopy (STEM), we demonstrate that electric polarisation emerges selectively at translation-inequivalent antiphase boundaries (APBs). At these boundaries multicomponent aac tilt field undergoes Neel-like interpolation that preserves the in-phase tilt component and amplifies roto flexoelectric coupling, while translation-equivalent boundaries remain nonpolar. The Neel like interpolation at hard APBs and Ising like collapse of all tilt components at easy APBs is corroborated with ab initio calculations. While embedded 90 ferroelastic walls provide an additional mechanistically distinct source of electric polarisation resulting in polar nanoclusters (4 nm). These distinct nanotextures at 90 walls from via elastic accommodation of strain mismatch between variants and rotostriction as the tilt field interpolates across the boundaries. These findings show that, in a membrane form, metal oxides provide a robust platform for hosting nanoscale ferroelastic domains that generate polar textures.

cond-mat.mtrl-sci

Helium-Cooled Cryogenic STEM Imaging and Ptychography for Atomic-Scale Study of Low-Temperature Phases

Much of the exotic functionality of prime interest in quantum materials emerges from structural and electronic ground states that can only be accessed at cryogenic temperatures. Understanding device operation therefore requires structural characterization under the same low-temperature conditions at which these functional phases exist, as room-temperature measurements often probe a different structural state. Achieving atomic-resolution in scanning transmission electron microscopy imaging and particularly 4D-STEM electron ptychography at liquid helium temperature has remained extremely challenging because even small amounts of drift, vibration, and thermal instability associated with the cryogen can disrupt the stringent stability requirements of atomic-resolution STEM. In this work we demonstrate atomic-resolution STEM and multislice electron ptychography at temperatures as low as 20 K using a commercial helium cooled holder. We find that rapid scans and a multi-stage registration workflow are critical to reducing artifacts associated with cryogenic instability for atomic-resolution imaging, while for ptychography scan position correction including compensation for coupling between probe aberrations and position refinement is necessary for successful reconstructions. Together these results establish a pathway for reliable atomic-resolution STEM and ptychography at low temperature, enabling direct visualization of structural ground states relevant to quantum technology.

cond-mat.mtrl-sci

Quantifying Phase Transformations in Alloying Anodes via In-Situ Liquid Cell Hard X-ray Spectroscopy and Cryogenic Microscopy

Understanding electrochemical phenomena at complex liquid solid interfaces requires linking real time structural dynamics with atomic scale interfacial chemistry. Here, we integrate operando synchrotron X-ray fluorescence and diffraction with high resolution cryogenic electron and ion multi model microscopy to provide a mechanistic understanding of Pt based alloying anodes across length scales. We directly observe the initial lithiation driven formation of Li2Pt and its evolution to a stable LiPt intermetallic phase during extended cycling via a solid solution type reaction mechanism. Simultaneously, the solid electrolyte interphase transitions from an unstable carbonate rich to a stable LiF dominated composition, confirmed by cryogenic scanning transmission electron microscopy and electron energy loss spectroscopy. Crucially, cryogenic atom probe tomography reveals spatially distinct compositional regimes within the alloy anode, including lithium flux limited, heterogeneous interfacial zone and a diffusion controlled, homogeneous LiPt alloy bulk. This nanoscale compositional gradient rationalises the emergent solid solution reaction mechanism and highlights how kinetic limitations and interface dynamics govern alloy formation and electrochemical stability. Our findings demonstrate a broadly applicable correlative framework bridging operando structural dynamics with near atomic resolution interfacial chemistry, advancing the rational design of durable alloy electrodes for next generation energy storage.

cond-mat.mtrl-sci

Polarization Domain Mapping From 4D-STEM Using Deep Learning

Polarization in ferroelectric domains arises from atomic-scale structural variations that govern macroscopic functionalities. The interfaces between these domains known as domain walls host distinct physical responses, making their identification and control critical. Four dimensional scanning transmission electron microscopy (4DSTEM) enables simultaneous acquisition of real and reciprocal-space information at the atomic scale, offering a powerful platform for domain mapping. However, conventional analyses rely on computationally intensive processing and manual interpretation, which are time consuming and prone to misalignment and diffraction artefacts. Here, we present a convolutional neural network that, with minimal training, classifies polarization directions from diffraction data and segments domains in real space. We further introduce an adaptive sampling strategy that prioritizes images from domain wall regions, reducing the number of training images required while improving accuracy and interpretability. We demonstrate this approach for domain mapping in ferroelectric boracite, Cu3B7O13Cl.

cond-mat.mtrl-sci

Programmable Beam Control for Electron Energy-Loss Spectroscopy and Ptychography

Programmable electron-beam scanning offers new opportunities to improve dose efficiency and suppress scan-induced artifacts in scanning transmission electron microscopy. Here, we systematically benchmark the impact of non-raster trajectories, including spiral and multi-pass sequential patterns, on two dose sensitive techniques: electron energy-loss spectroscopy (EELS) and ptychography. Using DyScO3 as a model perovskite, we compare spatial resolution, spectral fidelity, and artifact suppression across scan modes. Ptychographic phase reconstructions consistently achieve atomic resolution and remain robust to large jumps in probe position. In contrast, atomic-resolution EELS maps show pronounced sensitivity to probe motion, with sequential and spiral scans introducing non-uniform elemental contrast. Finally, spiral scanning applied under cryogenic conditions in BaTiO3 thin films improves dose uniformity and mitigates drift related distortions. These results establish practical guidelines for the implementation of programmable scan strategies in low-dose 4D-STEM and highlight the inherent resilience of ptychography to trajectory-induced artifacts.

cond-mat.mtrl-sci