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Elizabeth Skoropata

Publications and source records attributed to Elizabeth Skoropata.

At least 19 recordsLinked to original sources

THz-induced phonon mode mixing and collective dynamics in a polar nanolattice

Manipulating phonons through symmetry is a fundamental approach to alter the dynamic responses of materials. Most often new phases are sought through control of the unit-cell (e.g. via strain, doping, light, etc.). By comparison, there is vast potential to look beyond the unit-cell into higher-order architectures to control wave scattering and interference effects that remains less explored. We describe the THz-induced dynamics of an SrTiO$_{3}$ thin film with a nanoscale ordered interfacial dislocation network probed with 2- and 3-dimensional time-resolved x-ray diffraction and classical molecular dynamics simulations. We find that symmetry breaking at all scales is an effective approach to create a dynamical electric polarization and to control phonon mixing that generates previously unreported collective modes in the THz regime with circular vortex-like displacements. This work opens a new pathway to explore dynamical functional properties that can be extended to magnetic, electric, and ferroelectric systems by controlling the real-space topology via epitaxy.

cond-mat.str-el

Coherent spin waves in a maximal entropy phase

In solids, disorder is conventionally regarded as detrimental to coherence. It typically localizes and dampens collective excitations, as exemplified by Anderson localization or the broadening of magnetic modes in systems lacking long-range order. While high-entropy materials are specifically designed to harness disorder and stabilize homogeneous mixed-phase structures that can display unique properties, this same disorder is nonetheless expected to preclude the formation of coherent magnetic excitations. To test the limits of this picture, we selected the antiferromagnetic system YBaCuFeO5, as it features two distinct transition metal atoms with significantly different magnetic moments, rendering its spin dynamics exceptionally sensitive to local atomic ordering. Combining resonant inelastic x-ray scattering and linear spin wave theory, we reveal a surprising paradox: YBaCuFeO5 exhibits an unexpected, entropy-driven mixed phase, in which disorder, rather than reducing the lifetime of the collective excitations, favors coherence. In this mixed phase, the spin waves remain dispersive, markedly distinct from those expected for an ordered ground state, and exhibit well-defined acoustic and optical branches separated by a large optical gap. These results demonstrate that in entropy-stabilized magnets, disorder can favor coherent collective modes previously thought to be exclusive to low-entropy systems.

cond-mat.str-el

Hierarchical quasiparticle dynamics in antiferromagnets revealed by time- and momentum-resolved X-ray scattering

Energy flows among coupled subsystems are essential for ultrafast dynamics and high-speed technologies. In magnetic materials, spin fluctuations -- magnons -- mediate these flows in ultrafast magnetism. Yet momentum-resolved access to low-energy magnons governing the microscopic dynamics has been lacking. Using time-resolved resonant diffuse scattering alongside complementary time-resolved X-ray techniques and quantum-kinetic simulations, we unveil the hierarchical energy pathways among correlated systems in the photoexcited antiferromagnet CuO. Above-bandgap excitation triggers near-instantaneous spin disorder, generating non-thermal magnons throughout reciprocal space within femtoseconds. Real-time momentum-resolved tracking reveals picosecond magnon quasi-thermalization, followed by nanosecond recovery via momentum-selective magnon-phonon scattering. The quasiparticle dispersion mismatch creates recovery bottlenecks that control non-equilibrium lifetimes. This microscopic framework transcends phenomenological models and generalizes across materials, establishing design principles for ultrafast control of material properties.

cond-mat.str-el

A light-induced charge order mode in a metastable cuprate ladder

We report the observation of an emergent charge order mode in the optically-excited cuprate ladder Sr$_{14}$Cu$_{24}$O$_{41}$. Near-infrared light in the ladder plane drives a symmetry-protected electronic metastable state together with a partial melting of the equilibrium charge order. Our time-resolved resonant inelastic x-ray scattering measurements at the upper Hubbard band reveal a gapless collective excitation dispersing from the charge-order wavevector up to 0.8 eV with a slope on the order of the quasiparticle velocity. These findings reveal a regime where correlated carriers acquire itinerant character at finite momentum, and charge order becomes dynamically fluctuating, offering a platform to explore light-induced pairing instabilities.

cond-mat.str-el

Coexistence of insulator-like paramagnon and metallic spin-orbit exciton modes in SrIrO$_3$

We probe the spectrum of elementary excitations in SrIrO$_3$ by using heterostructured [(SrIrO$_3$)$_m$/(SrTiO$_3$)$_l$] samples to approach the bulk limit. Our resonant inelastic x-ray scattering (RIXS) measurements at the Ir $L_3$-edge reveal a robust low-lying collective magnetic mode with an antiferromagnetic (AF) dispersion similar to the insulators Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$, albeit with a large gap and much larger linewidth. At higher energies we find the spin-orbit exciton, also strongly broadened, but with an inverted dispersion and doubled periodicity that are controlled by the charge hopping. These results demonstrate that the AF paramagnon persists, somewhat counterintuitively, far into the metallic regime of the insulator-metal transition driven by the degree of confinement in the heterostructure. We conclude that these two excitations, which are contrasting but coexisting hallmarks of strong AF pseudospin and charge fluctuations in a spin-orbit-coupled Mott-Slater material, are properties intrinsic to the ground state of semimetallic perovskite SrIrO$_3$.

cond-mat.str-el

Symmetry-protected electronic metastability in an optically driven cuprate ladder

Optically excited quantum materials exhibit nonequilibrium states with remarkable emergent properties, but these phenomena are usually transient, decaying on picosecond timescales and limiting practical applications. Advancing the design and control of nonequilibrium phases requires the development of targeted strategies to achieve long-lived, metastable phases. Here, we report the discovery of symmetry-protected electronic metastability in the model cuprate ladder Sr$_{14}$Cu$_{24}$O$_{41}$. Using femtosecond resonant x-ray scattering and spectroscopy, we show that this metastability is driven by a transfer of holes from chain-like charge reservoirs into the ladders. This ultrafast charge redistribution arises from the optical dressing and activation of a hopping pathway that is forbidden by symmetry at equilibrium. Relaxation back to the ground state is hence suppressed after the pump coherence dissipates. Our findings highlight how dressing materials with electromagnetic fields can dynamically activate terms in the electronic Hamiltonian, and provide a rational design strategy for nonequilibrium phases of matter.

cond-mat.str-el

Tuning chirality amplitude at ultrafast timescales

Chirality is a fundamental symmetry concept describing discrete states, i.e., left-handed, right-handed, or achiral, and existing at disparate scales and in many categories of scientific fields. Even though symmetry breaking is indispensable for describing qualitatively distinct phenomena, symmetry cannot quantitatively predict measurable quantities. One can continuously distort an object, introducing the concept of chirality amplitude, similar to representing magnetization as the amplitude of time-reversal symmetry breaking. Considering the role of magnetization in emergent phenomena with time-reversal symmetry breaking, chirality amplitude is intuitively a key quantity for controlling chirality-related emergent phenomena. Here, we propose two types of chiral lattice distortions and demonstrate the tunability of their amplitude in ultrafast timescales. Resonant X-ray diffraction with circular polarization is an established technique to measure crystal chirality directly. We quantify the ultrafast change in chirality amplitude in real time after an optical excitation. Using instead a THz excitation, we observe oscillations in the resonant diffraction intensities corresponding to specific phonon frequencies. This indicates the creation of additional asymmetry, which could also be described as an enhancement in chirality amplitude. Our proposed concept of chirality amplitude and its ultrafast control may lead to a unique approach to control chirality-induced emergent phenomena in ultrafast timescales.

cond-mat.str-el

Element-specific, non-destructive profiling of layered heterostructures

Fabrication of semiconductor heterostructures is now so precise that metrology has become a key challenge for progress in science and applications. It is now relatively straightforward to characterize classic III-V and group IV heterostructures consisting of slabs of different semiconductor alloys with thicknesses of $\sim$5 nm and greater using sophisticated tools such as X-ray diffraction, high energy X-ray photoemission spectroscopy, and secondary ion mass spectrometry. However, profiling thin layers with nm or sub-nm thickness, e.g. atomically thin dopant layers ($δ$-layers), of impurities required for modulation doping and spin-based quantum and classical information technologies is more challenging. Here, we present theory and experiment showing how resonant-contrast X-ray reflectometry meets this challenge. The technique takes advantage of the change in the scattering factor of atoms as their core level resonances are scanned by varying the X-ray energy. We demonstrate the capability of the resulting element-selective, non-destructive profilometry for single arsenic $δ$-layers within silicon, and show that the sub-nm electronic thickness of the $δ$-layers corresponds to sub-nm chemical thickness. In combination with X-ray fluorescence imaging, this enables non-destructive three-dimensional characterization of nano-structured quantum devices. Due to the strong resonances at soft X-ray wavelengths, the technique is also ideally suited to characterize layered quantum materials, such as cuprates or the topical infinite-layer nickelates.

quant-ph

Provoking topology by octahedral tilting in strained SrNbO$_3$

Transition metal oxides with a wide variety of electronic and magnetic properties offer an extraordinary possibility to be a platform for developing future electronics based on unconventional quantum phenomena, for instance, the topology. The formation of topologically non-trivial states is related to crystalline symmetry, spin-orbit coupling, and magnetic ordering. Here, we demonstrate how lattice distortions and octahedral rotation in SrNbO$_3$ films induce the band topology. By employing angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) calculations, we verify the presence of in-phase $a^0a^0c^+$ octahedral rotation in ultra-thin SrNbO$_3$ films, which causes the formation of topologically-protected Dirac band crossings. Our study illustrates that octahedral engineering can be effectively exploited for implanting and controlling quantum topological phases in transition metal oxides.

cond-mat.mtrl-sci

Combined theoretical and experimental study of the Moiré dislocation network at the SrTiO$_3$-(La,Sr)(Al,Ta)O$_3$ interface

Recently a highly ordered Moiré dislocation lattice was identified at the interface between a \ce{SrTiO3} (STO) thin film and the (LaAlO$_3$)$_{0.3}$(Sr$_2$TaAlO$_6$)$_{0.7}$ (LSAT) substrate. A fundamental understanding of the local ionic and electronic structure around the dislocation cores is crucial to further engineer the properties of these complex multifunctional heterostructures. Here we combine experimental characterization via analytical scanning transmission electron microscopy with results of molecular dynamics and density functional theory calculations to gain insights into the structure and defect chemistry of these dislocation arrays. Our results show that these dislocations lead to undercoordinated Ta/Al cations at the dislocation core, where oxygen vacancies can easily be formed, further facilitated by the presence of cation vacancies. The reduced Ti$^{3+}$ observed experimentally at the dislocations by electron energy-loss spectroscopy are a consequence of both the structure of the dislocation itself, as well as of the electron-doping due to oxygen vacancy formation. Finally, the experimentally observed Ti diffusion into LSAT around the dislocation core occurs only together with cation-vacancy formation in LSAT or Ta diffusion into STO.

cond-mat.mtrl-sci

Non-equilibrium dynamics of spin-lattice coupling

Interactions between the different degrees of freedom form the basis of many manifestations of intriguing physics in condensed matter. In this respect, quantifying the dynamics of normal modes that themselves arise from these interactions and how they interact with other excitations is of central importance. Of the different types of coupling that are often important, spin-lattice coupling is relevant to several sub-fields of condensed matter physics; examples include spintronics, high-TC superconductivity, and topological materials. While theories of materials where spin-lattice coupling is relevant can sometimes be used to infer the magnitude and character of this interaction, experimental approaches that can directly measure it are rare and incomplete. Here we use time-resolved X-ray diffraction to directly access the spin-lattice coupling by measuring both ultrafast atomic motion and the associated spin dynamics following the excitation of a coherent electromagnon by an intense THz pulse in a multiferroic hexaferrite. Comparing the dynamics of the two different components, one striking outcome is the different phase shifts relative to the driving field. This phase shift provides insight into the excitation process of such a coupled mode. This direct observation of combined lattice and magnetization dynamics paves the way to access the mode-selective spin-lattice coupling strength, which remains a missing fundamental parameter for ultrafast control of magnetism and is relevant to a wide variety of correlated electron physics.

cond-mat.str-el

Hole doping in compositionally complex correlated oxide enables tunable exchange biasing

Magnetic interfaces and the phenomena arising from them drive both the design of modern spintronics and fundamental research. Recently, it was revealed that through designing magnetic frustration in configurationally complex entropy stabilized oxides, exchange bias can occur in structurally single crystal films. This eliminates the need for complex heterostructures and nanocomposites in the design and control of magnetic response phenomena. In this work, we demonstrate through hole doping of a high entropy perovskite oxide that tuning of magnetic responses can be achieved. With detailed magnetometry, we show magnetic coupling exhibiting a variety of magnetic responses including exchange bias and antiferromagnetic spin reversal in the entropy stabilized ABO3 perovskite oxide La1-xSrx(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 family. We find that manipulation of the A-site charge state can be used to balance magnetic phase compositions and coupling responses. This allows for the creation of highly tunable exchange bias responses. In the low Sr doping regime, a spin frustrated region arising at the antiferromagnetic phase boundary is shown to directly couple to the antiferromagnetic moments of the film and emerges as the dominant mechanism, leading to a vertical shift of magnetization loops in response to field biasing. At higher concentrations, direct coupling of antiferromagnetic and ferromagnetic regions is observed. This tunability of magnetic coupling is discussed within the context of these three competing magnetic phases, revealing critical features in designing exchange bias through exploiting spin frustration and disorder in high entropy oxides.

cond-mat.str-el

Unusual ferrimagnetism in CaFe2O4

Incomplete cancellation of collinear antiparallel spins gives rise to ferrimagnetism. Even if the oppositely polarized spins are owing to the equal number of a single magnetic element having the same valence state, in principle, a ferrimagnetic state can still arise from the crystallographic inequivalence of the host ions. However, experimental identification of such a state as ferrimagnetic is not straightforward because of the tiny magnitude expected for M and the requirement for a sophisticated technique to differentiate similar magnetic sites. We report a synchrotron-based resonant x-ray investigation at the Fe L2,3 edges on an epitaxial film of CaFe2O4, which exhibits two magnetic phases with similar energies. We find that while one phase of CaFe2O4 is antiferromagnetic, the other one is ferrimagnetic with an antiparallel arrangement of an equal number of spins between two distinct crystallographic sites with very similar local coordination environments. Our results further indicate two distinct origins of an overall minute M; one is intrinsic, from distinct Fe3+ sites, and the other one is extrinsic, arising from defective Fe2+ likely forming weakly-coupled ferrimagnetic clusters. These two origins are uncorrelated and have very different coercive fields. Hence, this work provides a direct experimental demonstration of ferrimagnetism solely due to crystallographic inequivalence of the Fe3+ as the origin of the weak M of CaFe2O4.

cond-mat.mtrl-sci

Conical spin order with chiral quadrupole helix in CsCuCl3

Here we report a resonant x-ray diffraction (RXD) study at the Cu L3 edge on the multi-chiral system CsCuCl3, exhibiting helical magnetic order in a chiral crystal structure. RXD is a powerful technique to disentangle electronic degrees of freedom due to its sensitivity to electric monopoles (charge), magnetic dipoles (spin), and electric quadrupoles (orbital). We characterize electric quadrupole moments around Cu ascribed to the unoccupied Cu 3d orbital, whose quantization axis is off the basal plane. Detailed investigation of magnetic reflections reveals additional sinusoidal modulations along the principal axis superimposed on the reported helical structure, i.e., a longitudinal conical (helical-butterfly) structure. The out-of-plane modulations imply significant spin-orbit interaction despite S = 1/2 of Cu2+.

cond-mat.str-el

Correlated Oxide Dirac Semimetal in the Extreme Quantum Limit

Quantum materials (QMs) with strong correlation and non-trivial topology are indispensable to next-generation information and computing technologies. Exploitation of topological band structure is an ideal starting point to realize correlated topological QMs. Herein, we report that strain-induced symmetry modification in correlated oxide SrNbO3 thin films creates an emerging topological band structure. Dirac electrons in strained SrNbO3 films reveal ultra-high mobility (100,000 cm2/Vs), exceptionally small effective mass (0.04me), and non-zero Berry phase. More importantly, strained SrNbO3 films reach the extreme quantum limit, exhibiting a sign of fractional occupation of Landau levels and giant mass enhancement. Our results suggest that symmetry-modified SrNbO3 is a rare example of a correlated topological QM, in which strong correlation of Dirac electrons leads to the realization of fractional occupation of Landau levels.

cond-mat.str-el

Designer Magnetism in High Entropy Oxides

Disorder can have a dominating influence on correlated and quantum materials leading to novel behaviors which have no clean limit counterparts. In magnetic systems, spin and exchange disorder can provide access to quantum criticality, frustration, and spin dynamics, but broad tunability of these responses and a deeper understanding of strong limit disorder is lacking. In this work, we demonstrate that high entropy oxides present an unexplored route to designing quantum materials in which the presence of strong local compositional disorder hosted on a positionally ordered lattice can be used to generate highly tunable emergent magnetic behavior--from macroscopically ordered states to frustration-driven dynamic spin interactions. Single crystal La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 films are used as a structurally uniform model system hosting a magnetic sublattice with massive microstate disorder in the form of site-to-site spin and exchange type inhomogeneity. A classical Heisenberg model is found to be sufficient to describe how compositionally disordered systems can paradoxically host long-range magnetic uniformity and demonstrates that balancing the populating elements based on their discrete quantum parameters can be used to give continuous control over ordering types and critical temperatures. Theory-guided experiments show that composite exchange values derived from the complex mix of microstate interactions can be used to design the required compositional parameters for a desired response. These predicted materials are synthesized and found to possess an incipient quantum critical point when magnetic ordering types are designed to be in direct competition; this leads to highly controllable exchange bias sensitivity in the monolithic single crystal films previously accessible only in intentionally designed bilayer heterojunctions.

cond-mat.str-el

Effective reduction of PdCoO2 thin films via hydrogenation and sign tunable anomalous Hall effect

PdCoO2 , belonging to a family of triangular oxides called delafossite, is one of the most conducting oxides. Its in-plane conductivity is comparable to those of the best metals, and exhibits hydrodynamic electronic transport with extremely long mean free path at cryogenic temperatures. Nonetheless, it is nonmagnetic despite the presence of the cobalt ion. Here, we show that a mild hydrogenation process reduces PdCoO2 thin films to an atomically-mixed alloy of PdCo with strong out-of-plane ferromagnetism and sign-tunable anomalous Hall effect. Considering that many other compounds remain little affected under a similar hydrogenation condition, this discovery may provide a route to creating novel spintronic heterostructures combining strong ferromagnetism, involving oxides and other functional materials.

cond-mat.mtrl-sci

Magnetic Texture in Insulating Single Crystal High Entropy Oxide Spinel Films

Magnetic insulators are important materials for a range of next generation memory and spintronic applications. Structural constraints in this class of devices generally require a clean heterointerface that allows effective magnetic coupling between the insulating layer and the conducting layer. However, there are relatively few examples of magnetic insulators which can be synthesized with surface qualities that would allow these smooth interfaces and precisely tuned interfacial magnetic exchange coupling which might be applicable at room temperature. In this work, we demonstrate an example of how the configurational complexity in the magnetic insulator layer can be used to realize these properties. The entropy-assisted synthesis is used to create single crystal (Mg0.2Ni0.2Fe0.2Co0.2Cu0.2)Fe2O4 films on substrates spanning a range of strain states. These films show smooth surfaces, high resistivity, and strong magnetic responses at room temperature. Local and global magnetic measurements further demonstrate how strain can be used to manipulate magnetic texture and anisotropy. These findings provide insight into how precise magnetic responses can be designed using compositionally complex materials that may find application in next generation magnetic devices.

cond-mat.mtrl-sci