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Freeland, J. W.

Publications and source records attributed to Freeland, J. W..

11 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Magnetic order driven ultrafast phase transition in NdNiO 3

Ultrashort x-ray pulses can be used to disentangle magnetic and structural dynamics and are accordingly utilized here to study the photoexcitation of NdNiO 3 (NNO), a model nickelate exhibiting structural and magnetic dynamics that conspire to induce an insulator-to-metal transition (IMT). Here, during the course of the photoinduced IMT with above-gap excitation, we observe an ultrafast (< 180 fs) quenching of magnetic order followed by a time delayed collapse of the insulating phase probed by x-ray absorption and THz transmission (450 fs) that correlates with the slowest optical phonon mode involved in the structural transition. A simultaneous order-disorder response at the Ni site and displacive response at the Nd site coexist in the ultrafast magnetic response. Crucially, we observe the optical phonon through its coherent coupling with Nd magnetic order, demonstrating that the magnetic and structural degrees of freedom both contribute in driving the IMT. Density functional theory calculations reveal a consistent scenario where optically driven intersite charge transfer drives a collapse of antiferromagnetic order that in turn destabilizes the charge-ordered phase resulting in an IMT. These experiments provide different modalities for the control of electronic phase transitions in quantum materials based on the ultrafast interplay between structural and magnetic orders created by femtosecond photoexcitation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Growth and characterization of large (Y,La)TiO 3 and (Y,Ca)TiO 3 single crystals

The Mott-insulating rare-earth titanates ( R TiO 3 , with R being a rare-earth ion) are an important class of materials that encompasses interesting spin-orbital phases as well as ferromagnet-antiferromagnet and insulator-metal transitions. The growth of these materials has been plagued by difficulties related to overoxidation, which arises from a strong tendency of Ti 3 + to oxidize to Ti 4 + . We describe our efforts to grow sizable single crystals of YTiO 3 , Y 1 - x La x TiO 3 ( x ≤ 0.25 ), and Y 1 - y Ca y TiO 3 ( y ≤ 0.35 ) with the optical traveling-solvent floating-zone technique. Finally, we present sample characterization via chemical composition analysis, magnetometry, charge transport, neutron scattering, x-ray absorption spectroscopy, and x-ray magnetic circular dichroism to understand macroscopic physical property variations associated with overoxidation. Furthermore, we demonstrate a good signal-to-noise ratio in inelastic magnetic neutron scattering measurements of spin-wave excitations. A superconducting impurity phase, found to appear in Ca-doped samples at high doping levels, is identified as TiO.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Nature of the ferromagnetic-antiferromagnetic transition in Y 1- x La x TiO 3

In this work, we explore the magnetically ordered ground state of the isovalently substituted Mott insulator Y 1- x La x TiO 3 for x≤ 0.3 via single-crystal growth, magnetometry, neutron diffraction, x-ray magnetic circular dichroism, muon spin rotation, and small-angle neutron scattering (SANS). We find that the decrease in the magnetic transition temperature on approaching the ferromagnetic-antiferromagnetic phase boundary at the La concentration xc ≈ 0.3 is accompanied by a strong suppression of both bulk and local ordered magnetic moments, along with a volume wise separation into magnetically ordered and paramagnetic regions. The thermal phase transition does not show conventional second-order behavior since neither a clear signature of dynamic critical behavior nor a power-law divergence of the magnetic correlation length is found for the studied substitution range; this finding becomes increasingly obvious with increasing La substitution. We find no evidence for a spin-glass phase. Finally, from SANS and magnetometry measurements, we discern a crossover from easy-axis to easy-plane magnetocrystalline anisotropy with increasing La substitution. These results indicate complex changes in magnetic structure upon approaching the phase boundary.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Two-component electronic phase separation in the doped Mott insulator Y 1-x Ca x TiO 3

One of the major puzzles in condensed matter physics has been the observation of a Mott-insulating state away from half-filling. Several theoretical proposals aimed to elucidate this phenomenon have been put forth, a notable one being phase separation and an associated percolation-induced Mott insulator-metal transition. In the present work we study the prototypical doped Mott-insulating rare-earth titanate YTiO 3 , in which the insulating state survives up to a large hole concentration of 35%. Single crystals of Y 1-x Ca x TiO 3 with 0 ≤ x ≤ 0.5, spanning the insulator-metal transition, are grown and investigated. Using x-ray absorption spectroscopy, a powerful technique capable of probing element-specific electronic states, we find that the primary effect of hole doping is to induce electronic phase separation into hole-rich and hole-poor regions. The data reveal the formation of electronic states within the Mott-Hubbard gap, near the Fermi level, which increase in spectral weight with increasing doping. From a comparison with DFT+U calculations, we infer that the hole-poor and hole-rich components have charge densities that correspond to the insulating x = 0 and metallic x ~ 0.5 states, respectively, and that the new electronic states arise from the metallic component. Our results indicate that the doping-induced insulator-metal transition in Y 1-x Ca x TiO 3 is indeed percolative in nature, and thus of inherent first-order character.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Large intrinsic anomalous Hall effect in SrIrO 3 induced by magnetic proximity effect

The anomalous Hall effect (AHE) is an intriguing transport phenomenon occurring typically in ferromagnets as a consequence of broken time reversal symmetry and spin-orbit interaction. It can be caused by two microscopically distinct mechanisms, namely, by skew or side-jump scattering due to chiral features of the disorder scattering, or by an intrinsic contribution directly linked to the topological properties of the Bloch states. Here we show that the AHE can be artificially engineered in materials in which it is originally absent by combining the effects of symmetry breaking, spin orbit interaction and proximity-induced magnetism. In particular, we find a strikingly large AHE that emerges at the interface between a ferromagnetic manganite (La 0.7 Sr 0.3 MnO 3 ) and a semimetallic iridate (SrIrO 3 ). It is intrinsic and originates in the proximity-induced magnetism present in the narrow bands of strong spin-orbit coupling material SrIrO 3 , which yields values of anomalous Hall conductivity and Hall angle as high as those observed in bulk transition-metal ferromagnets. These results demonstrate the interplay between correlated electron physics and topological phenomena at interfaces between 3d ferromagnets and strong spin-orbit coupling 5d oxides and trace an exciting path towards future topological spintronics at oxide interfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Spin-liquid behavior of the three-dimensional magnetic system Ba 3 NiIr 2 O 9 with S = 1

The quantum spin liquid (QSL) is an exotic phase of magnetic materials where the spins continue to fluctuate without any symmetry breaking down to zero temperature. Among the handful reports of QSL with spin S ≥ 1, examples with magnetic ions on a three-dimensional (3D) magnetic lattice are extremely rare since both larger spin and higher dimension tend to suppress quantum fluctuations. In this work, we offer a new strategy to achieve 3D QSL with high spin by utilizing two types of transition metal ions; both are magnetically active but located at crystallographically inequivalent positions. Furthermore, we design a 3D magnetic system Ba 3 NiIr 2 O 9 consisting of interconnected corner-shared NiO 6 octahedra and face-shared Ir 2 O 9 dimer, both having triangular arrangements in a-b plane. X-ray absorption spectroscopy measurements confirm the presence of Ni 2+ (S = 1). Furthermore, our detailed thermodynamic and magnetic measurements reveal that this compound is a realization of gapless QSL state down to at least 100 mK. Ab initio calculations find a strong magnetic exchange between Ir and Ni sublattices and in-plane antiferromagnetic coupling between the dimers, resulting in dynamically fluctuating magnetic moments.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Oxygen vacancy induced electronic structure modification of KTaO 3

The observation of a metallic interface between band insulators LaAlO 3 and SrTiO 3 has led to massive efforts to understand the origin of the phenomenon as well as to search for other systems hosting such two-dimensional electron gases (2-DEGs). However, the understanding of the origin of the 2-DEG is very often hindered as several possible mechanisms such as polar catastrophe, cationic intermixing, and oxygen vacancy (OV) can be operative simultaneously. The presence of a heavy element makes the KTaO 3 (KTO) based 2-DEG a potential platform to investigate spin-orbit coupling driven novel electronic and magnetic phenomena. In this work, we investigate the sole effect of OV in KTO, which makes KTO metallic. O K-edge x-ray absorption spectroscopy measurements find that OV dopes electrons in Ta t * 2g antibonding states. Photoluminescence measurements reveal the existence of a highly localized deep midgap state in oxygen-deficient KTO. Our detailed ab initio calculations demonstrate that such deep midgap state arises due to the linear clustering of OVs around Ta. Finally, our present work emphasizes that we must pay attention to the possible presence of OVs in interpreting emergent behavior of KTO-based heterostructures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Local negative permittivity and topological phase transition in polar skyrmions

Topological solitons such as magnetic skyrmions have drawn attention as stable quasi-particle-like objects. The recent discovery of polar vortices and skyrmions in ferroelectric oxide superlattices has opened up new vistas to explore topology, emergent phenomena and approaches for manipulating such features with electric fields. Using macroscopic dielectric measurements, coupled with direct scanning convergent beam electron diffraction imaging on the atomic scale, theoretical phase-field simulations and second-principles calculations, we demonstrate that polar skyrmions in (PbTiO 3 ) n /(SrTiO 3 ) n superlattices are distinguished by a sheath of negative permittivity at the periphery of each skyrmion. This enhances the effective dielectric permittivity compared with the individual SrTiO 3 and PbTiO 3 layers. Moreover, the response of these topologically protected structures to electric field and temperature shows a reversible phase transition from the skyrmion state to a trivial uniform ferroelectric state, accompanied by large tunability of the dielectric permittivity. Pulsed switching measurements show a time-dependent evolution and recovery of the skyrmion state (and macroscopic dielectric response). The interrelationship between topological and dielectric properties presents an opportunity to simultaneously manipulate both by a single, and easily controlled, stimulus, the applied electric field. Polar skyrmions are topologically protected structures that can exist in (PbTiO 3 ) n /(SrTiO 3 ) n superlattices. Here, it is shown that they have negative permittivity at the surface, and that they can undergo a reversible phase transition with large dielectric tunability under an electric field.

36 MATERIALS SCIENCE↗
DOE OSTI2020

In-situ fabrication and transport properties of (111) Y 2 Ir 2 O 7 epitaxial thin film

We report on the successful fabrication of (111) oriented thin films of pyrochlore iridate Y 2 Ir 2 O 7 by means of solid phase epitaxy. Essentially, we developed an entirely in situ annealing protocol, which is superior to the conventional ex-situ routine that requires multi-hour annealing to stabilize the proper pyrochlore structure. The morphological quality of the films has been confirmed by x-ray diffraction, reflectivity, and reciprocal space mapping, demonstrating their high crystallinity with a pure pyrochlore phase and an expected epitaxial relation to the substrate. Strikingly, below the magnetic phase transition, the temperature dependence of resistivity shows a power-law behavior with the power exponent of similar to 3/2, characteristic of a Weyl semimetal in the presence of impurities and electron-electron correlations. Finally, below 10K, the magneto-transport measurements reveal the emergence of a non-saturated negative magnetoresistance up to 9T with a small "valley" around zero field. These findings are further interpreted in relation to the weak anti-localization effect and the non-collinear antiferromagnetic ordering on the Ir sublattice.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Epitaxial stabilization of ultra thin films of high entropy perovskite

High entropy oxides (HEOs) are a class of materials, containing equimolar portions of five or more transition metal and/or rare-earth elements. We report here about the layer-by-layer growth of HEO [(La 0.2 Pr 0.2 Nd 0.2 Sm 0.2 Eu 0.2 )NiO 3 ] thin films on NdGaO 3 substrates by pulsed laser deposition. The combined characterizations with in situ reflection high energy electron diffraction, atomic force microscopy, and x-ray diffraction affirm the single crystalline nature of the film with smooth surface morphology. The desired +3 oxidation of Ni has been confirmed by an element sensitive x-ray absorption spectroscopy measurement. Temperature dependent electrical transport measurements revealed a first order metal-insulator transition with the transition temperature very similar to the undoped NdNiO 3 . Furthermore, since both these systems have a comparable tolerance factor, this work demonstrates that the electronic behaviors of A-site disordered perovskite-HEOs are primarily controlled by the average tolerance factor.

36 MATERIALS SCIENCE↗