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Aubrey Penn

Publications and source records attributed to Aubrey Penn.

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Laterally Differentiated Polymorphs: a route to multifunctional nanostructures

Multifunctional materials can exhibit emergent behavior from the coupling of two or more different properties. For example, coupling between magnetic and ferroelectric order enables electrical control of the magnetic state, enabling for example magnetoelectric memory or logic devices that combine the nonvolatility of magnetic order with the energy efficiency of voltage control. Magnetic iron garnets have outstanding magnonic and magnetooptical properties making them valuable in a range of technologies, but they have not been successfully incorporated into thin film two-phase magnetoelectric nanocomposites. Taking advantage of heterogeneously patterned substrates, this work demonstrates the engineering of garnet-perovskite composites in which both phases are polymorphs with the same composition but dramatically different structures and properties. Applying an electric field to the perovskite phase modulates the magnon dispersion and magnetooptical response of the garnet, opening a path to voltage-controlled garnet devices.

cond-mat.mtrl-sci

Defect complexes in CrSBr revealed through electron microscopy and deep learning

Atomic defects underpin the properties of van der Waals materials, and their understanding is essential for advancing quantum and energy technologies. Scanning transmission electron microscopy is a powerful tool for defect identification in atomically thin materials, and extending it to multilayer and beam-sensitive materials would accelerate their exploration. Here we establish a comprehensive defect library in a bilayer of the magnetic quasi-1D semiconductor CrSBr by combining atomic-resolution imaging, deep learning, and ab-initio calculations. We apply a custom-developed machine learning work flow to detect, classify and average point vacancy defects. This classification enables us to uncover several distinct Cr interstitial defect complexes, combined Cr and Br vacancy defect complexes and lines of vacancy defects that extend over many unit cells. We show that their occurrence is in agreement with our computed structures and binding energy densities, reflecting the intriguing layer interlocked crystal structure of CrSBr. Our ab-initio calculations show that the interstitial defect complexes give rise to highly localized electronic states. These states are of particular interest due to the reduced electronic dimensionality and magnetic properties of CrSBr and are furthermore predicted to be optically active. Our results broaden the scope of defect studies in challenging materials and reveal new defect types in bilayer CrSBr that can be extrapolated to the bulk and to over 20 materials belonging to the same FeOCl structural family.

cond-mat.mtrl-sci

The effect of surface oxidation and crystal thickness on magnetic properties and magnetic domain structures of Cr2Ge2Te6

Van der Waals (vdW) magnetic materials such as Cr2Ge2Te6 (CGT) show promise for novel memory and logic applications. This is due to their broadly tunable magnetic properties and the presence of topological magnetic features such as skyrmionic bubbles. A systematic study of thickness and oxidation effects on magnetic domain structures is important for designing devices and vdW heterostructures for practical applications. Here, we investigate thickness effects on magnetic properties, magnetic domains, and bubbles in oxidation-controlled CGT crystals. We find that CGT exposed to ambient conditions for 5 days forms an oxide layer approximately 5 nm thick. This oxidation leads to a significant increase in the oxidation state of the Cr ions, indicating a change in local magnetic properties. This is supported by real space magnetic texture imaging through Lorentz transmission electron microscopy. By comparing the thickness dependent saturation field of oxidized and pristine crystals, we find that oxidation leads to a non-magnetic surface layer which is thicker than the oxide layer alone. We also find that the stripe domain width and skyrmionic bubble size are strongly affected by the crystal thickness in pristine crystals. These findings underscore the impact of thickness and surface oxidation on the properties of CGT such as saturation field and domain/skyrmionic bubble size and suggest a pathway for manipulating magnetic properties through a controlled oxidation process.

cond-mat.mtrl-sci

The bulk van der Waals layered magnet CrSBr is a quasi-1D material

Correlated quantum phenomena in one-dimensional (1D) systems that exhibit competing electronic and magnetic order are of strong interest for studying fundamental interactions and excitations, such as Tomonaga-Luttinger liquids and topological orders and defects with properties completely different from the quasiparticles expected in their higher-dimensional counterparts. However, clean 1D electronic systems are difficult to realize experimentally, particularly magnetically ordered systems. Here, we show that the van der Waals layered magnetic semiconductor CrSBr behaves like a quasi-1D material embedded in a magnetically ordered environment. The strong 1D electronic character originates from the Cr-S chains and the combination of weak interlayer hybridization and anisotropy in effective mass and dielectric screening with an effective electron mass ratio of $m^e_X/m^e_Y \sim 50$. This extreme anisotropy experimentally manifests in strong electron-phonon and exciton-phonon interactions, a Peierls-like structural instability and a Fano resonance from a van Hove singularity of similar strength of metallic carbon nanotubes. Moreover, due to the reduced dimensionality and interlayer coupling, CrSBr hosts spectrally narrow (1 meV) excitons of high binding energy and oscillator strength that inherit the 1D character. Overall, CrSBr is best understood as a stack of weakly hybridized monolayers and appears to be an experimentally attractive candidate for the study of exotic exciton and 1D correlated many-body physics in the presence of magnetic order.

cond-mat.mes-hall

Kinetic control for planar oxidation of MoS$_2$

Layered transition metal dichalcogenide (TMD) semiconductors oxidize readily in a variety of conditions, and a thorough understanding of this oxide formation is required for the advancement of TMD-based microelectronics. Here, we combine scanning transmission electron microscopy (STEM) with spectroscopic ellipsometry (SE) to investigate oxide formation at the atomic scale of the most widely-studied TMD, MoS$_2$. We find that aggressive thermal oxidation results in $α$-phase plate-like crystalline MoO$_3$ with sharp interfaces, voids, and a textured alignment with the underlying MoS$_2$. Experiments with remote substrates and patterned MoS$_2$ prove that thermal oxidation proceeds via vapor-phase mass transport and redeposition - a challenge to forming thin, conformal planar oxide films. We accelerate the kinetics of oxidation relative to the kinetics of mass transport using a non-thermal oxygen plasma process, to form a smooth and conformal amorphous oxide. The resulting amorphous MoO$_3$ films can be grown several nanometers thick, and we calibrate the oxidation rate for varying plasma processing conditions. Our results illustrate how TMD semiconductor oxidation differs significantly from oxidation of legacy semiconductors, most notably silicon, and provide quantitative guidance for managing both the atomic scale structure and thin film morphology of oxides in the design and processing of MoS$_2$ semiconductor devices.

physics.app-ph

Confinement of magnetism in atomically-thin $La_{0.7}Sr_{0.3}CrO_3$/$La_{0.7}Sr_{0.3}MnO_3$ heterostructures

At crystalline interfaces where a valence mismatch exists, electronic and structural interactions may occur to relieve the polar mismatch leading to the stabilization of non-bulklike phases. We show that spontaneous reconstructions at polar $La_{0.7}Sr_{0.3}MnO_3$ interfaces are correlated with suppressed ferromagnetism for film thicknesses on the order of a unit cell. We investigate the structural and magnetic properties of valence-matched $La_{0.7}Sr_{0.3}CrO_3$ - $La_{0.7}Sr_{0.3}MnO_3$ interfaces using a combination of high-resolution electron microscopy, first principles theory, synchrotron X-ray scattering and magnetic spectroscopy and temperature-dependent magnetometry. A combination of an antiferromagnetic coupling between the $La_{0.7}Sr_{0.3}CrO_3$ and $La_{0.7}Sr_{0.3}MnO_3$ layers and a suppression of interfacial polar distortions are found to result in robust long range ferromagnetic ordering for ultra-thin $La_{0.7}Sr_{0.3}MnO_3$. These results underscore the critical importance of interfacial structural and magnetic interactions in the design of devices based on two-dimensional oxide magnetic systems.

cond-mat.str-el

Charge transfer and tunable built-in electric fields across semiconductor-crystalline oxide interfaces

Built-in electric fields across heterojunctions between semiconducting materials underpin the functionality of modern device technologies. Heterojunctions between semiconductors and epitaxially grown crystalline oxides provide a rich setting in which built-in fields can be explored. Here, we present an electrical transport and hard X-ray photoelectron spectroscopy study of epitaxial SrNbxTi1-xO3-δ / Si heterojunctions. A non-monotonic anomaly in the sheet resistance is observed near room temperature, which is accompanied by a crossover in sign of the Hall resistance. The crossover is consistent with the formation of a hole gas in the Si and the presence of a built-in field. Hard X-ray photoelectron spectroscopy measurements reveal pronounced asymmetric features in both the SrNbxTi1-xO3-δ and Si core-level spectra that we show arise from built-in fields. The extended probe depth of hard X-ray photoelectron spectroscopy enables band bending across the SrNbxTi1-xO3-δ / Si heterojunction to be spatially mapped. Band alignment at the interface and surface depletion in SrNbxTi1-xO3-δ are implicated in the formation of the hole gas and built-in fields. Control of charge transfer and built-in electric fields across semiconductor-crystalline oxide interfaces opens a pathway to novel functional heterojunctions.

cond-mat.mtrl-sci