arXiv subjects

Ramamoorthy Ramesh

Publications and source records attributed to Ramamoorthy Ramesh.

At least 55 records · Page 3Linked to original sources

arXiv2023

Persistent anisotropy of the spin cycloid in BiFeO3 through ferroelectric switching

A key challenge in antiferromagnetic spintronics is the control of spin configuration on nanometer scales applicable to solid-state technologies. Bismuth ferrite (BiFeO3) is a multiferroic material that exhibits both ferroelectricity and canted antiferromagnetism at room temperature, making it a unique candidate in the development of electric-field controllable magnetic devices. The magnetic moments in BiFeO3 are arranged into a spin cycloid, resulting in unique magnetic properties which are tied to the ferroelectric order. Previous understanding of this coupling has relied on average, mesoscale measurements to infer behavior. Using nitrogen vacancy-based diamond magnetometry, we show that the spin cycloid can be deterministically controlled with an electric field. The energy landscape of the cycloid is shaped by both the ferroelectric degree of freedom and strain-induced anisotropy, restricting the magnetization changes to specific ferroelectric switching events. This study provides understanding of the antiferromagnetic texture in BiFeO3 and paves new avenues for designing magnetic textures and spintronic devices.

cond-mat.mtrl-sci↗

arXiv2023

Universal spin wavepacket transport in van der Waals antiferromagnets

Antiferromagnets (AFMs) are promising platforms for the transmission of quantum information via magnons (the quanta of spin waves), offering advantages over ferromagnets with regard to dissipation, speed of response, and immunity to external fields. Recently, it was shown that in the insulating van der Waals (vdW) semiconductor, CrSBr, strong spin-exciton coupling enables readout of magnon density and propagation using photons of visible light. This exciting observation came with a puzzle: photogenerated magnons were observed to propagate 10$^3$ times faster than the velocity inferred from neutron scattering, leading to a conjecture that spin wavepackets are carried along by coupling to much faster elastic modes. Here we show, through a combination of theory and experiment, that the propagation mechanism is, instead, coupling within the magnetic degrees of freedom through long range dipole-dipole coupling. This mechanism is an inevitable consequence of Maxwell's equations, and as such, will dominate the propagation of spin at long wavelengths in the entire class of vdW magnets currently under intense investigation. Moreover, identifying the mechanism of spin propagation provides a set of optimization rules, as well as caveats, that are essential for any future applications of these promising systems.

cond-mat.str-el↗

arXiv2023

Imaging the electron charge density in monolayer MoS2 at the Ångstrom scale

Four-dimensional scanning transmission electron microscopy (4D-STEM) has recently gained widespread attention for its ability to image atomic electric fields with sub-Ångstrom spatial resolution. These electric field maps represent the integrated effect of the nucleus, core electrons and valence electrons, and separating their contributions is non-trivial. In this paper, we utilized simultaneously acquired 4D-STEM center of mass (CoM) images and annular dark field (ADF) images to determine the electron charge density in monolayer MoS2. We find that both the core electrons and the valence electrons contribute to the derived electron charge density. However, due to blurring by the probe shape, the valence electron contribution forms a nearly featureless background while most of the spatial modulation comes from the core electrons. Our findings highlight the importance of probe shape in interpreting charge densities derived from 4D STEM.

cond-mat.mtrl-sci↗

arXiv2023

Manipulating chiral-spin transport with ferroelectric polarization

A collective excitation of the spin structure in a magnetic insulator can transmit spin-angular momentum with negligible dissipation. This quantum of a spin wave, introduced more than nine decades ago, has always been manipulated through magnetic dipoles, (i.e., timereversal symmetry). Here, we report the experimental observation of chiral-spin transport in multiferroic BiFeO3, where the spin transport is controlled by reversing the ferroelectric polarization (i.e., spatial inversion symmetry). The ferroelectrically controlled magnons produce an unprecedented ratio of up to 18% rectification at room temperature. The spin torque that the magnons in BiFeO3 carry can be used to efficiently switch the magnetization of adja-cent magnets, with a spin-torque efficiency being comparable to the spin Hall effect in heavy metals. Utilizing such a controllable magnon generation and transmission in BiFeO3, an alloxide, energy-scalable logic is demonstrated composed of spin-orbit injection, detection, and magnetoelectric control. This observation opens a new chapter of multiferroic magnons and paves an alternative pathway towards low-dissipation nanoelectronics.

physics.app-ph↗

arXiv2023

The 4D Camera: an 87 kHz direct electron detector for scanning/transmission electron microscopy

We describe the development, operation, and application of the 4D Camera -- a 576 by 576 pixel active pixel sensor for scanning/transmission electron microscopy which operates at 87,000 Hz. The detector generates data at approximately 480 Gbit/s which is captured by dedicated receiver computers with a parallelized software infrastructure that has been implemented to process the resulting 10 - 700 Gigabyte-sized raw datasets. The back illuminated detector provides the ability to detect single electron events at accelerating voltages from 30 - 300 keV. Through electron counting, the resulting sparse data sets are reduced in size by 10 - 300x compared to the raw data, and open-source sparsity-based processing algorithms offer rapid data analysis. The high frame rate allows for large and complex 4D-STEM experiments to be accomplished with typical STEM scanning parameters.

physics.ins-det↗

arXiv2023

Uncovering polar vortex structures by inversion of multiple scattering with a stacked Bloch wave model

Nanobeam electron diffraction can probe local structural properties of complex crystalline materials including phase, orientation, tilt, strain, and polarization. Ideally, each diffraction pattern from a projected area of a few unit cells would produce clear a Bragg diffraction pattern, where the reciprocal lattice vectors can be measured from the spacing of the diffracted spots, and the spot intensities are equal to the square of the structure factor amplitudes. However, many samples are too thick for this simple interpretation of their diffraction patterns, as multiple scattering of the electron beam can produce a highly nonlinear relationship between the spot intensities and the underlying structure. Here, we develop a stacked Bloch wave method to model the diffracted intensities from thick samples with structure that varies along the electron beam. Our method reduces the large parameter space of electron scattering to just a few structural variables per probe position, making it fast enough to apply to very large fields of view. We apply our method to SrTiO$_3$/PbTiO$_3$/SrTiO$_3$ multilayer samples, and successfully disentangle specimen tilt from the mean polarization of the PbTiO$_3$ layers. We elucidate the structure of complex vortex topologies in the PbTiO$_3$ layers, demonstrating the promise of our method to extract material properties from thick samples.

cond-mat.mtrl-sci↗

arXiv2023

Emergent chirality in a polar meron to skyrmion phase transition

Polar skyrmions are predicted to emerge from the interplay of elastic, electrostatic and gradient energies, in contrast to the key role of the anti-symmetric Dzyalozhinskii-Moriya interaction in magnetic skyrmions. With the discovery of topologically-stable polar skyrmions, it is of both fundamental and practical interest to understand the microscopic nature and the possibility of temperature- and strain-driven phase transitions in ensembles of such polar skyrmions. Here, we explore the reversible transition from a skyrmion state (topological charge of -1) to a two-dimensional, tetratic lattice of merons (with topological charge of -1/2) upon varying the temperature and elastic boundary conditions in [(PbTiO3)16/(SrTiO3)16]8 lifted-off membranes. This topological phase transition is accompanied by a change in chirality, from zero-net chirality (in meronic phase) to net-handedness (in skyrmionic phase). To map these changes microscopically required developing new imaging methods. We show how scanning convergent beam electron diffraction provides a robust measure of the local polarization simultaneously with the strain state at sub-nm resolution, while also directly mapping the chirality of each skyrmion. Using this, we demonstrate strain as a crucial order parameter to drive isotropic-to-anisotropic structural transitions of chiral polar skyrmions to non-chiral merons, validated with X-ray reciprocal space mapping and theoretical phase-field simulations. These results revealed by our new measurement methods provide the first illustration of systematic control of rich variety of topological dipole textures by altering the mechanical boundary conditions, which may offer a promising way to control their functionalities in ferroelectric nanodevices using the local and spatial distribution of chirality and order.

cond-mat.mes-hall↗

arXiv2022

Controlled Ordering of Room-Temperature Magnetic Skyrmions in a Polar Van der Waals Magnet

Control and understanding of ensembles of skyrmions is important for realization of future technologies. In particular, the order-disorder transition associated with the 2D lattice of magnetic skyrmions can have significant implications for transport and other dynamic functionalities. To date, skyrmion ensembles have been primarily studied in bulk crystals, or as isolated skyrmions in thin film devices. Here, we investigate the condensation of the skyrmion phase at room temperature and zero field in a polar, Van der Waals magnet. We demonstrate that we can engineer an ordered skyrmion crystal through structural confinement on the $μ$m scale, showing control over this order-disorder transition on scales relevant for device applications.

cond-mat.mtrl-sci↗

arXiv2022

Thermal cycling induced alteration of the stacking order and spin-flip in the room temperature van der Waals magnet Fe$_5$GeTe$_2$

The magnetic properties of the quasi-two-dimensional van der Waals magnet Fe$_{5-δ}$GeTe$_2$ (F5GT), which has a high ferromagnetic ordering temperature $T_{\text{C}}$ $\sim$ 315 K, remains to be better understood. It has been demonstrated that the magnetization of F5GT is sensitive to both the Fe deficiency $δ$ and the thermal cycling history. Here, we investigate the structural and magnetic properties of F5GT with a minimal Fe deficiency ($|δ|$ $\le$ 0.1), utilizing combined x-ray and neutron scattering techniques. Our study reveals that the quenched F5GT single crystals experience an irreversible, first-order transition at $T_{\text{S}}$ $\sim$ 110 K upon first cooling, where the stacking order partly or entirely converts from ABC-stacking to AA-stacking order. Importantly, the magnetic properties, including the magnetic moment direction and the enhanced $T_{\text{C}}$ after the thermal cycling, are intimately related to the alteration of the stacking order. Our work highlights the significant influence of the lattice symmetry to the magnetism in F5GT.

cond-mat.str-el↗

arXiv2022

Nonvolatile Electric Field Control of Thermal Magnons in the Absence of an Applied Magnetic Field

Spin transport through magnetic insulators has been demonstrated in a variety of materials and is an emerging pathway for next-generation spin-based computing. To modulate spin transport in these systems, one typically applies a sufficiently strong magnetic field to allow for deterministic control of magnetic order. Here, we make use of the well-known multiferroic magnetoelectric, BiFeO3, to demonstrate non-volatile, hysteretic, electric-field control of thermally excited magnon current in the absence of an applied magnetic field. These findings are an important step toward magnon-based devices, where electric-field-only control is highly desirable.

cond-mat.mtrl-sci↗

arXiv2022

Antiferromagnetic order in Co-doped Fe$_5$GeTe$_2$ probed by resonant magnetic x-ray scattering

The quasi-two-dimensional van der Waals magnet Fe$_{5-δ}$GeTe$_2$ has emerged as a promising platform for electronic and spintronic functionalities at room temperature, owing to its large ferromagnetic ordering temperature $T_{\text{C}}$ $\sim$ 315 K. Interestingly, by cobalt (Co) substitution of iron in F5GT, $i.e.$ $({\text{Fe}}_{1-x}{\text{Co}}_x)_{5-δ}{\text{GeTe}}_2$ (Co-F5GT), not only can its magnetic transition temperature be further enhanced, but the magnetic and structural ground states can also be tuned. Specifically, an antiferromagnetic (AFM) order is induced beyond the Co doping level $x \ge 0.4$. Here, we investigate the magnetic properties of a Co-F5GT single crystal at $x = 0.45(1)$, by utilizing the element specific, resonant magnetic x-ray scattering technique. Our study reveals an A-type, Ising-like AFM ground state, with a transition temperature $T_{\text{N}}$ $\sim$ 340 K. In addition, our work unveils an important contribution from Co magnetic moments to the magnetic order. The application of the in-plane magnetic fields gradually polarize the spin moments along the field direction, but without inducing incommensurate spin texture(s).

cond-mat.mtrl-sci↗

arXiv2022

Hyperspectral imaging of excitons within a moiré unit-cell with a sub-nanometer electron probe

Electronic and optical excitations in two-dimensional moiré systems are uniquely sensitive to local atomic registries, leading to materials- and twist-angle specific correlated electronic ground states with varied degree of localization. However, there has been no direct experimental correlation between the sub-nanometer structure and emergent excitonic transitions, comprising tightly-bound pairs of photoexcited electrons and holes. Here, we use cryogenic transmission electron microscopy and spectroscopy to simultaneously image the structural reconstruction and associated localization of the lowest-energy intralayer exciton in a rotationally aligned heterostructure of WS2 and WSe2 monolayers. In conjunction with optical spectroscopy and ab initio calculations, we determine that the exciton center-of-mass wavefunction is strongly modulated in space, confined to a radius of ~ 2 nm around the highest-energy stacking site in the moiré unit-cell, forming a triangular lattice. Our results provide direct evidence that atomic reconstructions lead to the strongly confining moiré potentials and that engineering strain at the nanoscale will enable new types of excitonic lattices.

cond-mat.mtrl-sci↗

arXiv2022

Pervasive beyond room-temperature ferromagnetism in a doped van der Waals magnet: Ni doped Fe$_5$GeTe$_2$ with $T_{\text{C}}$ up to 478 K

The existence of long range magnetic order in low dimensional magnetic systems, such as the quasi-two-dimensional (2D) van der Waals (vdW) magnets, has attracted intensive studies of new physical phenomena. The vdW Fe$_N$GeTe$_2$ ($N$ = 3, 4, 5; FGT) family is exceptional owing to its vast tunability of magnetic properties. Particularly, a ferromagnetic ordering temperature ($T_{\text{C}}$) above room temperature at $N$ = 5 (F5GT) is observed. Here, our study shows that, by nickel (Ni) substitution of iron (Fe) in F5GT, a record high $T_{\text{C}}$ = 478(6) K is achieved. Importantly, pervasive, beyond-room-temperature ferromagnetism exists in almost the entire doping range of the phase diagram of Ni-F5GT. We argue that this striking observation in Ni-F5GT can be possibly due to several contributing factors, in which the structural alteration enhanced 3D magnetic couplings might be critical for enhancing the ferromagnetic order.

cond-mat.mtrl-sci↗

arXiv2022

A single-projection three-dimensional reconstruction algorithm for scanning transmission electron microscopy data

Increasing interest in three-dimensional nanostructures adds impetus to electron microscopy techniques capable of imaging at or below the nanoscale in three dimensions. We present a reconstruction algorithm that takes as input a focal series of four-dimensional scanning transmission electron microscopy (4D-STEM) data. We apply the approach to a lead iridate, Pb$_2$Ir$_2$O$_7$, and yttrium-stabilized zirconia,Y$_{0.095}$Zr$_{0.905}$O$_2$ , heterostructure from data acquired with the specimen in a single plan-view orientation, with the epitaxial layers stacked along the beam direction. We demonstrate that Pb-Ir atomic columns are visible in the uppermost layers of the reconstructed volume. We compare this approach to the alternative techniques of depth sectioning using differential phase contrast scanning transmission electron microscopy (DPC-STEM) and multislice ptychographic reconstruction.

cond-mat.mtrl-sci↗

arXiv2022

Nonvolatile Electric-Field Control of Inversion Symmetry

In condensed-matter systems, competition between ground states at phase boundaries can lead to significant changes in material properties under external stimuli, particularly when these ground states have different crystal symmetries. A key scientific and technological challenge is to stabilize and control coexistence of symmetry-distinct phases with external stimuli. Using BiFeO3 (BFO) layers confined between layers of the dielectric TbScO3 as a model system, we stabilize the mixed-phase coexistence of centrosymmetric and non-centrosymmetric BFO phases with antipolar, insulating and polar, semiconducting behavior, respectively at room temperature. Application of in-plane electric (polar) fields can both remove and introduce centrosymmetry from the system resulting in reversible, nonvolatile interconversion between the two phases. This interconversion between the centrosymmetric insulating and non-centrosymmetric semiconducting phases coincides with simultaneous changes in the non-linear optical response of over three orders of magnitude, a change in resistivity of over five orders of magnitude, and a change in the polar order. Our work establishes a materials platform allowing for novel cross-functional devices which take advantage of changes in optical, electrical, and ferroic responses.

cond-mat.mtrl-sci↗

arXiv2021

Order-disorder transitions in a polar vortex lattice

Order-disorder transitions are widely explored in various vortex structures in condensed matter physics, i.e., in the type-II superconductors and Bose-Einstein condensates. In this study, we have investigated the ordering of the polar vortex phase in the (PZT)n/(STO)n superlattice systems through phase-field simulations. An antiorder state is discovered for short periodicity superlattice on an SSO substrate, owing to the huge interfacial coupling between PZT and STO as well as the giant in-plane polarization in STO layers due to the large tensile strain. Increasing the periodicity leads to the anti-order to disorder transition, resulting from the loss of interfacial coupling and disappearance of the polarization in STO layers. On the other hand, for short periodicity superlattices, order-disorder-antiorder transition can be engineered by mediating the substrate strain, due to the delicate competition between the depoling effect, interfacial coupling, and strain effect. We envision this study to spur further interest towards the understanding of order-disorder transition in ferroelectric topological structures.

cond-mat.mtrl-sci↗

arXiv2021

Erbium-Implanted Materials for Quantum Communication Applications

Erbium-doped materials can serve as spin-photon interfaces with optical transitions in the telecom C-band, making them an exciting class of materials for long-distance quantum communication. However, the spin and optical coherence times of Er3+ ions are limited by currently available host materials, motivating the development of new Er3+-containing materials. Here, we demonstrate the use of ion implantation to efficiently screen prospective host candidates, and show that disorder introduced by ion implantation can be mitigated through post-implantation thermal processing to achieve inhomogeneous linewidths comparable to bulk linewidths in as-grown samples. We present optical spectroscopy data for each host material, which allows us to determine the level structure of each site, allowing us to compare the environments of Er3+ introduced via implantation and via doping during growth. We demonstrate that implantation can generate a range of local environments for Er3+, including those observed in bulk-doped materials, and that the populations of these sites can be controlled with thermal processing.

cond-mat.mtrl-sci↗

arXiv2021

Nanoscale Phonon Spectroscopy Reveals Emergent Interface Vibrational Structure of Superlattices

As the length-scales of materials decrease, heterogeneities associated with interfaces approach the importance of the surrounding materials. Emergent electronic and magnetic interface properties in superlattices have been studied extensively by both experiments and theory. $^{1-6}$ However, the presence of interfacial vibrations that impact phonon-mediated responses, like thermal conductivity $^{7,8}$, has only been inferred in experiments indirectly. While it is accepted that intrinsic phonons change near boundaries $^{9,10}$, the physical mechanisms and length-scales through which interfacial effects influence materials remain unclear. Herein, we demonstrate the localized vibrational response associated with the interfaces in SrTiO$_3$-CaTiO$_3$ superlattices by combining advanced scanning transmission electron microscopy imaging and spectroscopy and density-functional-theory calculations. Symmetries atypical of either constituent material are observed within a few atomic planes near the interface. The local symmetries create local phonon modes that determine the global response of the superlattice once the spacing of the interfaces approaches the phonon spatial extent. The results provide direct visualization and quantification, illustrating the progression of the local symmetries and interface vibrations as they come to determine the vibrational response of an entire superlattice; stated differently, the progression from a material with interfaces, to a material dominated by interfaces, to a material of interfaces as the period decreases. Direct observation of such local atomic and vibrational phenomena demonstrates that their spatial extent needs to be quantified to understand macroscopic behavior. Tailoring interfaces, and knowing their local vibrational response, provides a means of pursuing designer solids having emergent infrared and thermal responses.

cond-mat.mtrl-sci↗