arXiv subjects

Padraic Shafer

Publications and source records attributed to Padraic Shafer.

At least 19 recordsLinked to original sources

arXiv2023

Spectral Evidence for Local-Moment Ferromagnetism in van der Waals Metals Fe$_3$GaTe$_2$ and Fe$_3$GeTe$_2$

Magnetism in two-dimensional (2D) materials has attracted considerable attention recently for both fundamental understanding of magnetism and their tunability towards device applications. The isostructural Fe$_3$GeTe$_2$ and Fe$_3$GaTe$_2$ are two members of the Fe-based van der Waals (vdW) ferromagnet family, but exhibit very different Curie temperatures (T$_C$) of 210 K and 360 K, respectively. Here, by using angle-resolved photoemission spectroscopy and density functional theory, we systematically compare the electronic structures of the two compounds. Qualitative similarities in the Fermi surface can be found between the two compounds, with expanded hole pockets in Fe$_3$GaTe$_2$ suggesting additional hole carriers compared to Fe$_3$GeTe$_2$. Interestingly, we observe no band shift in Fe$_3$GaTe$_2$ across its T$_C$ of 360 K, compared to a small shift in Fe$_3$GeTe$_2$ across its T$_C$ of 210 K. The weak temperature-dependent evolution strongly deviates from the expectations of an itinerant Stoner mechanism. Our results suggest that itinerant electrons have minimal contributions to the enhancement of T$_C$ in Fe$_3$GaTe$_2$ compared to Fe$_3$GeTe$_2$, and that the nature of ferromagnetism in these Fe-based vdW ferromagnets must be understood with considerations of the electron correlations.

cond-mat.str-el↗

arXiv2023

Site-selective polar compensation of Mott electrons in a double perovskite heterointerface

Double perovskite oxides (DPOs) with two transition metal ions ($A_2$$BB^\prime$O$_6$) offer a fascinating platform for exploring exotic physics and practical applications. Studying these DPOs as ultrathin epitaxial thin films on single crystalline substrates can add another dimension to engineering electronic, magnetic, and topological phenomena. Understanding the consequence of polarity mismatch between the substrate and the DPO would be the first step towards this broad goal. We investigate this by studying the interface between a prototypical insulating DPO Nd$_2$NiMnO$_6$ and a wide-band gap insulator SrTiO$_3$. The interface is found to be insulating in nature. By combining several experimental techniques and density functional theory, we establish a site-selective charge compensation process that occurs explicitly at the Mn site of the film, leaving the Ni sites inert. We further demonstrate that such surprising selectivity, which cannot be explained by existing mechanisms of polarity compensation, is directly associated with their electronic correlation energy scales. This study establishes the crucial role of Mott physics in polar compensation process and paves the way for designer doping strategies in complex oxides.

cond-mat.mtrl-sci↗

arXiv2023

Suppression of Spin Pumping at Metal Interfaces

An electrically conductive metal typically transmits or absorbs a spin current. Here, we report on evidence that interfacing two metal thin films can suppress spin transmission and absorption. We examine spin pumping in ferromagnet/spacer/ferromagnet heterostructures, in which the spacer -- consisting of metallic Cu and Cr thin films -- separates the ferromagnetic spin-source and spin-sink layers. The Cu/Cr spacer largely suppresses spin pumping -- i.e., neither transmitting nor absorbing a significant amount of spin current -- even though Cu or Cr alone transmits a sizable spin current. The antiferromagnetism of Cr is not essential for the suppression of spin pumping, as we observe similar suppression with Cu/V spacers where V is a nonmagnetic analogue of Cr. We speculate that diverse combinations of spin-transparent metals may form interfaces that suppress spin pumping, although the underlying mechanism remains unclear. Our work may stimulate a new perspective on understanding and engineering spin transport in metallic multilayers.

cond-mat.mtrl-sci↗

arXiv2023

Orthorhombic distortion drives orbital ordering in an antiferromagnetic 3$d^1$ Mott insulator

The orbital, which represents the shape of the electron cloud, very often strongly influences the manifestation of various exotic phenomena, e.g., magnetism, metal-insulator transition, colossal magnetoresistance, unconventional superconductivity etc. in solid-state systems. The observation of the antiferromagnetism in $RE$TiO$_3$ ($RE$=rare earth) series has been puzzling since the celebrated Kugel-Khomskii model of spin-orbital super exchange predicts ferromagnetism in an orbitally degenerate $d^1$ systems. Further, the existence of the orbitally ordered vs. orbital liquid phase in both antiferromagnetic and paramagnetic phase have been unsettled issues thus far. To address these long-standing questions, we investigate single crystalline film of PrTiO$_3$. Our synchrotron X-ray diffraction measurements confirm the retention of bulk-like orthorhombic ($D_{2h}$) symmetry in the thin film geometry. We observe similar X-ray linear dichroism signal in both paramagnetic and antiferromagnetic phase, which can be accounted by ferro orbital ordering (FOO). While the presence of $D_{2h}$ crystal field does not guarantee lifting of orbital degeneracy always, we find it to be strong enough in these rare-earth titanates, leading to the FOO state. Thus, our work demonstrates the orthorhombic distortion is the driving force for the orbital ordering of antiferromagnetic $RE$TiO$_3$.

cond-mat.str-el↗

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↗

arXiv2022

Antiferromagnetic metal phase in an electron-doped rare-earth nickelate

Long viewed as passive elements, antiferromagnetic materials have emerged as promising candidates for spintronic devices due to their insensitivity to external fields and potential for high-speed switching. Recent work exploiting spin and orbital effects has identified ways to electrically control and probe the spins in metallic antiferromagnets, especially in noncollinear or noncentrosymmetric spin structures. The rare earth nickelate NdNiO3 is known to be a noncollinear antiferromagnet where the onset of antiferromagnetic ordering is concomitant with a transition to an insulating state. Here, we find that for low electron doping, the magnetic order on the nickel site is preserved while electronically a new metallic phase is induced. We show that this metallic phase has a Fermi surface that is mostly gapped by an electronic reconstruction driven by the bond disproportionation. Furthermore, we demonstrate the ability to write to and read from the spin structure via a large zero-field planar Hall effect. Our results expand the already rich phase diagram of the rare-earth nickelates and may enable spintronics applications in this family of correlated oxides.

cond-mat.str-el↗

arXiv2022

Absorption of Transverse Spin Current in Ferromagnetic NiCu: Dominance of Bulk Dephasing over Spin-Flip Scattering

In ferromagnetic metals, transverse spin currents are thought to be absorbed via dephasing -- i.e., destructive interference of spins precessing about the strong exchange field. Yet, due to the ultrashort coherence length of $\approx$1 nm in typical ferromagnetic thin films, it is difficult to distinguish dephasing in the bulk from spin-flip scattering at the interface. Here, to assess which mechanism dominates, we examine transverse spin-current absorption in ferromagnetic NiCu alloy films with reduced exchange fields. We observe that the coherence length increases with decreasing Curie temperature, as weaker dephasing in the film bulk slows down spin absorption. Moreover, nonmagnetic Cu impurities do not diminish the efficiency of spin-transfer torque from the absorbed spin current. Our findings affirm that transverse spin current is predominantly absorbed by dephasing inside the nanometer-thick ferromagnetic metals, even with high impurity contents.

cond-mat.mes-hall↗

arXiv2022

Synthesis and electronic properties of Nd$_{n+1}$Ni$_{n}$O$_{3n+1}$ Ruddlesden-Popper nickelate thin films

The rare-earth nickelates possess a diverse set of collective phenomena including metal-to-insulator transitions, magnetic phase transitions, and, upon chemical reduction, superconductivity. Here, we demonstrate epitaxial stabilization of layered nickelates in the Ruddlesden-Popper form, Nd$_{n+1}$Ni$_n$O$_{3n+1}$, using molecular beam epitaxy. By optimizing the stoichiometry of the parent perovskite NdNiO$_3$, we can reproducibly synthesize the $n = 1 - 5$ member compounds. X-ray absorption spectroscopy at the O $K$ and Ni $L$ edges indicate systematic changes in both the nickel-oxygen hybridization level and nominal nickel filling from 3$d^8$ to 3$d^7$ as we move across the series from $n = 1$ to $n = \infty$. The $n = 3 - 5$ compounds exhibit weakly hysteretic metal-to-insulator transitions with transition temperatures that depress with increasing order toward NdNiO$_3$ ($n = \infty)$.

cond-mat.mtrl-sci↗

arXiv2021

State-resolved ultrafast charge and spin dynamics in [Co/Pd] multilayers

We use transient absorption spectroscopy with circularly polarized x-rays to detect laser-excited hole states below the Fermi level and compare their dynamics with that of unoccupied states above the Fermi level in ferromagnetic [Co/Pd] multilayers. While below the Fermi level an instantaneous and significantly stronger demagnetization is observed, above the Fermi level the demagnetization is delayed by 35+/-10 fs. This provides a direct visualization of how ultrafast demagnetization proceeds via initial spin-flip scattering of laser-excited holes to the subsequent formation of spin waves.

cond-mat.mtrl-sci↗

arXiv2021

Superconductivity in a quintuple-layer square-planar nickelate

Since the discovery of high-temperature superconductivity in the copper oxide materials, there have been sustained efforts to both understand the origins of this phase and discover new cuprate-like superconducting materials. One prime materials platform has been the rare-earth nickelates and indeed superconductivity was recently discovered in the doped compound Nd$_{0.8}$Sr$_{0.2}$NiO$_2$. Undoped NdNiO$_2$ belongs to a series of layered square-planar nickelates with chemical formula Nd$_{n+1}$Ni$_n$O$_{2n+2}$ and is known as the 'infinite-layer' ($n = \infty$) nickelate. Here, we report the synthesis of the quintuple-layer ($n = 5$) member of this series, Nd$_6$Ni$_5$O$_{12}$, in which optimal cuprate-like electron filling ($d^{8.8}$) is achieved without chemical doping. We observe a superconducting transition beginning at $\sim$13 K. Electronic structure calculations, in tandem with magnetoresistive and spectroscopic measurements, suggest that Nd$_6$Ni$_5$O$_{12}$ interpolates between cuprate-like and infinite-layer nickelate-like behavior. In engineering a distinct superconducting nickelate, we identify the square-planar nickelates as a new family of superconductors which can be tuned via both doping and dimensionality.

cond-mat.supr-con↗

arXiv2021

Epitaxial stabilization of thin films of the frustrated Ge-based spinels

Frustrated magnets can host numerous exotic many-body quantum and topological phenomena. GeNi$_2$O$_4$ is a three dimensional $S=1$ frustrated magnet with an unusual two-stage transition to the two-dimensional antiferromagnetic ground state, while GeCu$_2$O$_4$ is a high-pressure phase with a strongly tetragonally elongated spinel structure and magnetic lattice formed by $S=1/2$ CuO$_2$ linear chains with frustrated exchange interactions and exotic magnetic behavior. Here we report on the first thin-film epitaxial stabilization of these two compounds. Developed growth mode, surface morphology, crystal structure and copper valence state were characterized by in-situ reflection high-energy electron diffraction, atomic force microscopy, X-ray reflectivity, X-ray diffraction, X-ray photoelectron spectroscopy and resonant X-ray absorption spectroscopy. Our results pave an alternative route to the comprehensive investigation of the puzzling magnetic properties of these compounds and exploration of novel emergent features driven by strain.

cond-mat.str-el↗

arXiv2021

Search for $Q \sim 0$ order near a forbidden Bragg position in Bi$_{2.1}$Sr$_{1.9}$CaCu$_2$O$_{8+x}$ with resonant soft x-ray scattering

Identifying what broken symmetries are present in the cuprates has become a major area of research. Many authors have reported evidence for so-called "$Q \sim 0$" order that involves broken inversion, mirror, chiral, or time-reversal symmetry that is uniform in space. Not all these observations are well understood and new experimental probes are needed. Here we use resonant soft x-ray scattering (RSXS) to search for $Q \sim 0$ order in Bi$_{2.1}$Sr$_{1.9}$CaCu$_2$O$_{8+x}$ (Bi-2212) by measuring the region of a forbidden Bragg peak, $(0,0,3)$, which is normally extinguished by symmetry but may become allowed on resonance if valence band order is present. Using circularly polarized light, we found that this reflection becomes allowed on the Cu $L_3$ resonance for temperatures $T_c < T < T^\ast$, though remains absent in linear polarization and at other temperatures. This observation suggests the existence of spatially uniform valence band order near the pseudogap temperature. In addition, we observed periodic oscillations in the specular reflectivity from the sample surface that resemble thin film interference fringes, though no known film is present. These fringes are highly resonant, appear in all polarizations, and exhibit a period that depends on the location where the beam strikes the sample surface. We speculate that these fringes arise from interaction between some intrinsic valence band instability and extrinsic structural surface morphologies of the material. Our study supports the existence of some kind of $Q \sim 0$ broken symmetry state in Bi-2212 at intermediate temperatures, and calls for further study using a microfocused beam that could disentangle microscopic effects from macroscopic heterogeneities.

cond-mat.str-el↗

arXiv2020

Strain-induced anion ordering in perovskite oxyfluoride films

Anionic ordering is a promising route to engineer physical properties in functional heteroanionic materials. A central challenge in the study of anion-ordered compounds lies in developing robust synthetic strategies to control anion occupation and in understanding the resultant implications for electronic structure. Here, we show that epitaxial strain induces preferential occupation of F and O on the anion sites in perovskite oxyfluoride SrMnO2.5-dFg films grown on different substrates. Under compressive strain, F tends to take the apical-like sites, which was revealed by F and O K-edge linearly polarized x-ray absorption spectroscopy and density functional theory calculations, resulting in an enhanced c-axis expansion. Under tensile strain, F tends to take the equatorial-like sites, enabling the longer Mn-F bonds to lie within the plane. The anion ordered oxyfluoride films exhibit a significant orbital polarization of the 3d electrons, distinct F-site dependence to their valence band density of states, and an enhanced resistivity when F occupies the apical-like anion site compared to the equatorial-like site. By demonstrating a general strategy for inducing anion-site order in oxyfluoride perovskites, this work lays the foundation for future materials design and synthesis efforts that leverage this greater degree of atomic control to realize new polar or quasi-two-dimensional materials.

cond-mat.mtrl-sci↗

arXiv2020

Orientation-dependent stabilization of MgCr$_2$O$_4$ spinel thin films

AB$_2$O$_4$ normal spinels with a magnetic B site can host a variety of magnetic and orbital frustrations leading to spin-liquid phases and field-induced phase transitions. Here we report the first epitaxial growth of (111)-oriented MgCr$_2$O$_4$ thin films. By characterizing the structural and electronic properties of films grown along (001) and (111) directions, the influence of growth orientation has been studied. Despite distinctly different growth modes observed during deposition, the comprehensive characterization reveals no measurable disorder in the cation distribution nor multivalency issue for Cr ions in either orientation. Contrary to a naive expectation, the (111) stabilized films exhibit a smoother surface and a higher degree of crystallinity than (001)-oriented films. The preference in growth orientation is explained within the framework of heteroepitaxial stabilization in connection to a significantly lower (111) surface energy. These findings open broad opportunities in the fabrication of 2D kagome-triangular heterostructures with emergent magnetic behavior inaccessible in bulk crystals.

cond-mat.mtrl-sci↗

arXiv2020

Sub-Nanosecond Spin-Transfer Torque in an Ensemble of Superparamagnetic-Like Nanomagnets

Spin currents can exert spin-transfer torques on magnetic systems even in the limit of vanishingly small net magnetization, as is the case for antiferromagnets. Here, we experimentally show that a spin-transfer torque is operative in a material with weak, short-range magnetic order -- namely, a macroscopic ensemble of superparamagnetic-like Co nanomagnets. We employ element- and time-resolved X-ray ferromagnetic resonance (XFMR) spectroscopy to directly detect sub-ns dynamics of the Co nanomagnets, excited into precession with cone angle $\geq$0.003$^{\circ}$ by an oscillating spin current. XFMR measurements reveal that as the net moment of the ensemble decreases, the strength of the spin-transfer torque increases relative to those of magnetic field torques. Our findings point to spin-transfer torque as an effective way to manipulate the state of nanomagnet ensembles at sub-ns timescales.

cond-mat.mes-hall↗

arXiv2020

Cation- and lattice-site-selective magnetic depth profiles of ultrathin $\mathrm{Fe_3O_4}$(001) films

A detailed understanding of ultrathin film surface properties is crucial for the proper interpretation of spectroscopic, catalytic and spin-transport data. We present x-ray magnetic circular dichroism (XMCD) and x-ray resonant magnetic reflectivity (XRMR) measurements on ultrathin $\mathrm{Fe_3O_4}$ films to obtain magnetic depth profiles for the three resonant energies corresponding to the different cation species $\mathrm{Fe^{2+}_{oct}}$, $\mathrm{Fe^{3+}_{tet}}$ and $\mathrm{Fe^{3+}_{oct}}$ located on octahedral and tetrahedral sites of the inverse spinel structure of $\mathrm{Fe_3O_4}$. By analyzing the XMCD spectrum of $\mathrm{Fe_3O_4}$ using multiplet calculations, the resonance energy of each cation species can be isolated. Performing XRMR on these three resonant energies yields magnetic depth profiles that correspond each to one specific cation species. The depth profiles of both kinds of $\mathrm{Fe^{3+}}$ cations reveal a $\mathrm{3.9 \pm 1~Å}$-thick surface layer of enhanced magnetization, which is likely due to an excess of these ions at the expense of the $\mathrm{Fe^{2+}_{oct}}$ species in the surface region. The magnetically enhanced $\mathrm{Fe^{3+}_{tet}}$ layer is additionally shifted about $\mathrm{3\pm 1.5~Å}$ farther from the surface than the $\mathrm{Fe^{3+}_{oct}}$ layer.

cond-mat.mes-hall↗

arXiv2020

Strain-modulated Slater-Mott crossover of pseudospin-half square-lattice in (SrIrO3)1/ (SrTiO3)1 superlattices

We report on the epitaxial strain-driven electronic and antiferromagnetic modulations of a pseudospin-half square lattice realized in superlattices of (SrIrO3)1/(SrTiO3)1. With increasing compressive strain, we find the low-temperature insulating behavior to be strongly suppressed with a corresponding systematic reduction of both the Neel temperature and the staggered moment. However, despite such a suppression, the system remains weakly insulating above the Neel transition. The emergence of metallicity is observed under large compressive strain but only at temperatures far above the Néel transition. These behaviors are characteristics of the Slater-Mott crossover regime, providing a unique experimental model system of the spin-half Hubbard Hamiltonian with a tunable intermediate coupling strength.

cond-mat.str-el↗

arXiv2020

Correlation-driven eightfold magnetic anisotropy in a two-dimensional oxide monolayer

Engineering magnetic anisotropy in two-dimensional systems has enormous scientific and technological implications. The uniaxial anisotropy universally exhibited by two-dimensional magnets has only two stable spin directions, demanding 180 degrees spin switching between states. We demonstrate a novel eightfold anisotropy in magnetic SrRuO3 monolayers by inducing a spin reorientation in (SrRuO3)1/(SrTiO3)N superlattices, in which the magnetic easy axis of Ru spins is transformed from uniaxial <001> direction (N = 1 and 2) to eightfold <111> directions (N = 3, 4 and 5). This eightfold anisotropy enables 71 and 109 degrees spin switching in SrRuO3 monolayers, analogous to 71 and 109 degrees polarization switching in ferroelectric BiFeO3. First-principle calculations reveal that increasing the SrTiO3 layer thickness induces an emergent correlation-driven orbital ordering, tuning spin-orbit interactions and reorienting the SrRuO3 monolayer easy axis. Our work demonstrates that correlation effects can be exploited to substantially change spin-orbit interactions, stabilizing unprecedented properties in two-dimensional magnets and opening rich opportunities for low-power, multi-state device applications.

cond-mat.mtrl-sci↗