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Juan Carlos Idrobo

Publications and source records attributed to Juan Carlos Idrobo.

At least 19 recordsLinked to original sources

Atomic-Scale Observation of Symmetry Breaking in Altermagnetic MnTe

The recent discovery of altermagnetism has sparked growing interest in compensated magnetic systems as promising platforms for highly scalable spintronics. Altermagnetism is a distinct magnetic order where opposite spin sublattices are connected by rotation, yielding zero net magnetization but momentum-dependent spin splitting. To date, experimental verification of altermagnetic order has been achieved predominantly through bulk-sensitive techniques, including spin-dependent electronic spectra and transport responses. However, direct atomic-scale evidence that explicitly correlates crystal symmetry, local structural distortions, and magnetic ordering has remained unexplored. Here, we report the direct atomic-scale observation of coexisting polar distortions and altermagnetic order in MnTe, combining atomic resolution scanning transmission electron microscopy (STEM) imaging with electron magnetic chiral dichroism (EMCD) measurements. We reveal that MnTe is not an ideal uniform P63/mmc g-wave altermagnet at the atomic scale. Instead, it hosts ubiquitous inversion-symmetry-breaking distortions that lower the spin-space-group (SSG) symmetry, admits d-wave altermagnetic components, and in lower-symmetry regimes, even allow s-wave spin splitting (net magnetization). The coexistence of ferroelectric signatures and altermagnetic order establishes local lattice symmetry in MnTe as a control knob for altermagnetic spin splitting, spin current generation, and multiferroic memory applications.

cond-mat.mtrl-sci↗

Temperature-dependent acoustic loss at microwave frequencies in thin-film lithium niobate

Thin-film lithium niobate (TFLN) has emerged as a versatile platform for phononic and photonic devices with applications ranging from classical signal processing to quantum technologies. However, acoustic loss fundamentally limits the performance of acoustic devices on TFLN platforms, yet its physical origin remains insufficiently understood. Here, we systematically investigate acoustic propagation loss in various TFLN platforms, including lithium niobate on insulator (LNOI), lithium niobate on sapphire (LNOS), suspended LN thin films, and bulk LN at gigahertz frequencies over temperatures ranging from 4 K to above room temperature. Using a delay-line method, we extract frequency- and temperature-dependent losses for Rayleigh, shear-horizontal, and Lamb modes. We observe an anomalous non-monotonic temperature dependence in LNOI that closely resembles acoustic loss in amorphous materials, indicating a dominant loss channel associated with the buried oxide layer at low temperatures. At elevated temperatures, the loss converges to the Akhiezer damping governed by phonon-phonon interactions. High-resolution electron microscopy further reveals nanoscale interfacial crystal impurities that may contribute to the increased acoustic loss in TFLN platforms relative to bulk LN. These results elucidate the acoustic loss mechanisms in TFLN and provide guidelines for designing low-loss acoustic devices.

physics.app-ph↗

Hydrogen bonding in water under extreme confinement

Fluids under extreme confinement exhibit unique structures and intermolecular bonding, distinct from their bulk analogs, driving innovative applications at the water-energy nexus. Probing confined water experimentally at the length scale of intermolecular and surface forces has, however, remained a challenge. Here, we report direct molecular-level observations of hydrogen bonding in water confined inside individual carbon nanotubes, enabled by in-situ vibrational electron energy-loss spectroscopy with nanoscale resolution. Hydrogen bonding is probed via the intramolecular O-H stretching frequency, which serves as a sensitive spectral signature of the local intermolecular bonding environment. Water in larger carbon nanotubes exhibit the bonded O-H vibrations of bulk water, but at smaller diameters, the frequency blueshifts to near the free O-H stretch found in water vapor and hydrophobic surfaces, indicating a highly dispersed, non-H-bonded environment. Theoretical analysis based on quantum vibrational oscillators indicates that enhanced damping rates, corresponding to rapid hydrogen-bond fluctuations, leads the bimodal spectral peaks to merge into a single broad feature, matching the experimental observation. Furthermore, cryogenic experiments provide insights into complex structural phase transitions of confined water. This research reveals the quantum and dynamic nature of hydrogen bonds under confinement and the potential impact of unveiling molecular-level structure and bonding in confined fluids.

physics.chem-ph↗

Detecting Linear Dichroism with Atomic Resolution

X-ray linear dichroism has been pivotal for probing electronic anisotropies, but its inherent limited spatial resolution precludes atomic-scale investigations of orbital polarization. Here we introduce a versatile electron linear dichroism methodology in scanning transmission electron microscopy that overcomes these constraints. By exploiting momentum-transfer-dependent electron energy-loss spectroscopy with an atomic-sized probe, we directly visualize orbital occupation at individual atomic columns in real space. Using strained La0.7Sr0.3MnO3 thin films as a model system, we resolve the Mn-3d eg orbital polarization with sub-angstrom precision. We show that compressive strain stabilizes 3z2-r2 occupation while tensile strain favors x2-y2. These results validate our approach against established X-ray measurements while achieving the ultimate single atomic-column sensitivity. We further demonstrate two optimized signal extraction protocols that adapt to experimental constraints without compromising sensitivity. This generalizable platform opens unprecedented opportunities to study symmetry-breaking phenomena at individual defects, interfaces, and in quantum materials where atomic-scale electronic anisotropy governs emergent functionality.

cond-mat.mtrl-sci↗

Antiferroelectric Hafnia Down to the 2D Limit

Antiferroelectricity is a material property characterized by alternating electric dipoles spontaneously ordered in antiparallel directions. Antiferroelectrics are promising for energy storage, solid-state cooling, and memory technologies; however, these materials are scarce, and their scalability remains largely unexplored. In this work, we demonstrate that single-crystalline hafnia, a lead-free CMOS-compatible material, exhibits antiferroelectricity under compressive-strain conditions. We observe antiparallel sublattice polarization and stable double-hysteresis in single-crystalline (111)-oriented epitaxial La-doped hafnia films grown on yttrium-stabilized zirconia and show that the antipolar orthorhombic phase of hafnia adheres to the Kittel model of antiferroelectricity. Notably, compressive strain strengthens the antiferroelectric order in thinner La-doped hafnia films, achieving an unprecedented 850 C ordering temperature in the two-dimensional limit, highlighting hafnia's potential for advanced antiferroelectric devices.

cond-mat.mtrl-sci↗

Magnon spectroscopy in the electron microscope

The miniaturisation of transistors is approaching its limits due to challenges in heat management and information transfer speed. To overcome these obstacles, emerging technologies such as spintronics are being developed, which leverage the electron's spin in addition to its charge. Local phenomena at interfaces or structural defects will greatly influence the efficiency of spin-based devices, making the ability to study and control spin wave propagation at the nano- and atomic scales a key challenge. The development of high-spatial-resolution tools to probe spin waves, also called magnons, at relevant lengthscales is thus essential to understand how their properties are affected by such local features. Here, we show the first experimental detection of bulk magnons at the nanoscale using scanning transmission electron microscopy. By employing high-resolution electron energy loss spectroscopy with hybrid-pixel direct electron detectors optimized for low acceleration voltages, we successfully overcome the challenges posed by weak signals and identify magnon excitations in a thin NiO nanocrystal. Advanced inelastic electron scattering simulations corroborate our findings. These results open new avenues for detecting magnons, exploring their dispersions and their modifications arising from nanoscale structural or chemical defects. This marks an important milestone in magnonics and presents exciting opportunities for the future development of spintronic devices.

cond-mat.mtrl-sci↗

Giant coercivity and enhanced intrinsic anomalous Hall effect at vanishing magnetization in a compensated kagome ferrimagnet

Ferrimagnets that can be driven to magnetic compensation show promise for use in spintronics as they exhibit a finite anomalous Hall effect at zero magnetic field without having a significant magnetic moment. Compensated ferrimagnet spintronic devices with both a large anomalous Hall effect and a high coercivity would be simultaneously easy to read and difficult to erase. The kagome ferrimagnet TbMn$_6$Sn$_6$ has been reported to host a large intrinsic anomalous Hall effect. Here, we demonstrate that doping the Mn sites with Cr drives the system towards magnetic compensation. For nearly compensated compositions at low temperatures, giant coercive fields exceeding 14 T are observed. Additionally, Cr doping significantly enhances the intrinsic anomalous Hall effect, which can be attributed to a shift in the Fermi level. Our results extend the range of unique magnetic states observed in kagome materials, demonstrating that chemical doping is an effective strategy to tune and realize these states.

cond-mat.str-el↗

Direct observation of nanometer-scale orbital angular momentum accumulation

Conversion of charge to orbital angular momentum through the orbital Hall effect (OHE) holds transformative potential for the development of orbital-based electronics, however, it is challenging to directly observe the electrically generated orbital accumulation. Here, we detect the OHE by directly quantifying the orbital accumulation along the edges of a titanium thin film using a scanning transmission electron microscope. We measure the Ti L-edge using electron energy-loss spectroscopy with nanometer resolution and find a sizable orbital accumulation at the sample's outer perimeters, consistent with all signatures expected for the OHE, and determine an orbital diffusion length $\ell_o \approx 7.3$ nm. Our data points to a surprising dependence of the orbital diffusion length on the nano-structural morphology.

cond-mat.mes-hall↗

Imaging of Antiferroelectric Dark Modes in an Inverted Plasmonic Lattice

Plasmonic lattice nanostructures are of technological interest because of their capacity to manipulate light below the diffraction limit. Here, we present a detailed study of dark and bright modes in the visible and near-infrared energy regime of an inverted plasmonic honeycomb lattice by a combination of Au+ focused ion beam lithography with nanometric resolution, optical and electron spectroscopy, and finite-difference time-domain simulations. The lattice consists of slits carved in a gold thin film, exhibiting hotspots and a set of bright and dark modes. We proposed that some of the dark modes detected by electron energy-loss spectroscopy are caused by antiferroelectric arrangements of the slit polarizations with two times the size of the hexagonal unit cell. The plasmonic resonances take place within the 0.5_2 eV energy range, indicating that they could be suitable for a synergistic coupling with excitons in two-dimensional transition metal dichalcogenides materials or for designing nanoscale sensing platforms based on near-field enhancement over a metallic surface.

physics.optics↗

High-temperature phonons in h-BN: momentum-resolved vibrational spectroscopy and theory

Vibrations in materials and nanostructures at sufficiently high temperatures result in anharmonic atomic displacements, which leads to new phenomena such as thermal expansion and multiphonon scattering processes, with a profound impact on temperature-dependent material properties including thermal conductivity, phonon lifetimes, nonradiative electronic transitions, and phase transitions. Nanoscale momentum-resolved vibrational spectroscopy, which has recently become possible on monochromated scanning-transmission-electron microscopes, is a unique method to probe the underpinnings of these phenomena. Here we report momentum-resolved vibrational spectroscopy in hexagonal boron nitride at temperatures of 300, 800, and 1300 K across three Brillouin zones (BZs) that reveals temperature-dependent phonon energy shifts and demonstrates the presence of strong Umklapp processes. Density-functional-theory calculations of temperature-dependent phonon self-energies reproduce the observed energy shifts and identify the contributing mechanisms.

cond-mat.mtrl-sci↗

Unveiling the impact of temperature on magnon diffuse scattering detection in the transmission electron microscope

Magnon diffuse scattering (MDS) signals could be studied with high spatial resolution in scanning transmission electron microscopy (STEM), thanks to recent technological progress in electron energy loss spectroscopy. However, detecting MDS signals in STEM is challenging due to their overlap with stronger thermal diffuse scattering (TDS) signals. In bcc Fe at 300 K, MDS signals greater than or comparable to TDS signals occur under the central Bragg disk, into a currently inaccesible energy-loss region. Therefore, to detect MDS in STEM, it is necessary to find conditions in which TDS and MDS signals can be separated. Temperature may be a key factor due to the distinct thermal signatures of magnon and phonon signals. In this work, we present a study on the effects of temperature on MDS and TDS in bcc Fe -- considering a detector outside the central Bragg disk and a fixed convergent electron probe -- using the frozen phonon and frozen magnon multislice methods. Our study reveals that neglecting the effects of atomic vibrations causes the MDS signal to grow approximately linearly up to the Curie temperature of Fe, after which it exhibits less variation. The MDS signal displays an alternating behavior due to dynamical diffraction, instead of increasing monotonically as a function of thickness. Including the effects of atomic vibrations through a complex atomic electrostatic potential causes the linear growth of the MDS signal to change to a non-linear behavior that exhibits a predominant peak for a sample of thickness 16.072 nm at 1100 K. In contrast, the TDS signal grows more linearly than the MDS signal but still exhibits appreciable dynamical diffraction effects. An analysis of the signal-to-noise ratio (SNR) shows that the MDS signal can be a statistically significant contribution to the total scattering intensity under realizable measurement conditions and acquisition times.

cond-mat.mtrl-sci↗

Experimental Observation of Localized Interfacial Phonon Modes

Interfaces impede heat flow in micro/nanostructured systems. Conventional theories for interfacial thermal transport were derived based on bulk phonon properties of the materials making up the interface without explicitly considering the atomistic interfacial details, which are found critical to correctly describing thermal boundary conductance (TBC). Recent theoretical studies predicted the existence of localized phonon modes at the interface which can play an important role in understanding interfacial thermal transport. However, experimental validation is still lacking. Through a combination of Raman spectroscopy and high-energy resolution electron energy-loss spectroscopy (EELS) in a scanning transmission electron microscope, we report the first experimental observation of localized interfacial phonon modes at ~12 THz at a high-quality epitaxial Si-Ge interface. These modes are further confirmed using molecular dynamics simulations with a high-fidelity neural network interatomic potential, which also yield TBC agreeing well with that measured from time-domain thermoreflectance (TDTR) experiments. Simulations find that the interfacial phonon modes have obvious contribution to the total TBC. Our findings may significantly contribute to the understanding of interfacial thermal transport physics and have impact on engineering TBC at interfaces in applications such as electronics thermal management and thermoelectric energy conversion.

cond-mat.mes-hall↗

Magnon diffuse scattering in scanning transmission electron microscopy

We present a theory and a simulation of thermal diffuse scattering due to the excitation of magnons in scanning transmission electron microscopy. The calculations indicate that magnons can present atomic contrast when detected by electron energy-loss spectroscopy using atomic-size electron beams. The results presented here indicate that the intensity of the magnon diffuse scattering in bcc iron at 300~K is 4 orders of magnitude weaker than the intensity of thermal diffuse scattering arising from atomic vibrations. In an energy range where the phonon and magnon dispersions do not overlap, a monochromated scanning transmission electron microscope equipped with direct electron detectors for spectroscopy is expected to resolve the magnon spectral signatures.

cond-mat.mtrl-sci↗

Direct Observation of Infrared Plasmonic Fano Antiresonances by a Nanoscale Electron Probe

In this Letter, we exploit recent breakthroughs in monochromated aberration-corrected scanning transmission electron microscopy (STEM) to resolve infrared plasmonic Fano antiresonances in individual nanofabricated disk-rod dimers. Using a combination of electron energy-loss spectroscopy (EELS) and theoretical modeling, we investigate and characterize a subspace of the weak coupling regime between quasi-discrete and quasi-continuum localized surface plasmon resonances where infrared plasmonic Fano antiresonances appear. This work illustrates the capability of STEM instrumentation to experimentally observe nanoscale plasmonic responses that were previously the domain only of higher resolution infrared spectroscopies.

cond-mat.mes-hall↗

Seeing Site-Specific Isotopic Labeling of Amino Acids with Vibrational Spectroscopy in the Electron Microscope

Isotope labeling is a fundamental staple for the study of cellular metabolism and protein function. The conventional techniques that allow resolution and identification of isotopically-labeled biomarkers, such as mass spectrometry and infrared spectroscopy, are macroscopic in nature and have the disadvantage of requiring relatively large quantities of material and lacking spatial resolution. Here, we record the vibrational spectra of an α-amino acid, L-alanine, using spatially-resolved monochromated electron energy loss spectroscopy (EELS) to directly resolve carbon-site-specific isotopic labels in a scanning transmission electron microscope. The EELS is acquired in aloof mode, meaning the probe is positioned away from the sample (~20 nm) sparing the sensitive biomolecule from the high-energy excitations, while the vibrational modes are investigated. An isotopic red-shift of 5.3 meV was obtained for the C=O stretching mode in the carboxylic acid group for 13C-enriched L-alanine when compared with naturally occurring 12C L-alanine, which is confirmed by macroscopic infrared spectroscopy measurements and theoretical calculations. The EELS experiments presented here are the first demonstration of non-destructive resolution and identification of isotopically-labeled amino acids in the electron microscope, opening a new door for the study of biological matter at the nanoscale.

cond-mat.soft↗

Controlling the Infrared Dielectric Function through Atomic-Scale Heterostructures

Surface phonon polaritons (SPhPs) - the surface-bound electromagnetic modes of a polar material resulting from the coupling of light with optic phonons - offer immense technological opportunities for nanophotonics in the infrared (IR) spectral region. Here, we present a novel approach to overcome the major limitation of SPhPs, namely the narrow, material-specific spectral range where SPhPs can be supported, called the Reststrahlen band. We use an atomic-scale superlattice (SL) of two polar semiconductors, GaN and AlN, to create a hybrid material featuring layer thickness-tunable optic phonon modes. As the IR dielectric function is governed by the optic phonon behavior, such control provides a means to create a new dielectric function distinct from either constituent material and to tune the range over which SPhPs can be supported. This work offers the first glimpse of the guiding principles governing the degree to which the dielectric function can be designed using this approach.

cond-mat.mtrl-sci↗

Spatially and spectrally resolved orbital angular momentum interactions in plasmonic vortex generators

Understanding the near-field electromagnetic interactions that produce optical orbital angular momentum (OAM) is central to the integration of twisted light into nanotechnology. Here, we examine the cathodoluminescence (CL) of plasmonic vortices carrying OAM generated in spiral nanostructures through scanning transmission electron microscopy (STEM). The nanospiral geometry defines the photonic local density of states (LDOS) sampled by STEM-CL, which provides access to the phase and amplitude of the plasmonic vortex with nanometer spatial and meV spectral resolution. We map the full spectral dispersion of the plasmonic vortex in the spiral structure and examine the effects of increasing topological charge on the plasmon phase and amplitude in the detected CL signal. The vortex is mapped in CL over a broad spectral range, and deviations between the predicted and detected positions of near-field optical signatures of as much as 5 per cent are observed. Finally, enhanced luminescence is observed from concentric spirals of like handedness compared to that from concentric spirals of opposite handedness, indicating the potential to couple plasmonic vortices to chiral nanostructures for sensitive detection and manipulation of optical OAM.

physics.optics↗