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A. S. Disa

Publications and source records attributed to A. S. Disa.

6 recordsLinked to original sources

Quenched lattice fluctuations in optically driven SrTiO3

Many functionally relevant ferroic phenomena in quantum materials can be manipulated by driving the lattice coherently with optical and terahertz pulses. New physical phenomena and non-equilibrium phases that have no equilibrium counterpart have been discovered following these protocols. The underlying structural dynamics has been mostly studied by recording the average atomic position along dynamical structural coordinates with elastic scattering methods. However, crystal lattice fluctuations, which are known to influence phase transitions in equilibrium, are also expected to determine these dynamics but have rarely been explored. Here, we study the driven dynamics of the quantum paraelectric SrTiO3, in which mid-infrared drives have been shown to induce a metastable ferroelectric state. Crucial in these physics is the competition between the polar instability and antiferrodistortive rotations, which in equilibrium frustrate the formation of long-range ferroelectricity. We make use of high intensity mid-infrared optical pulses to resonantly drive a Ti-O stretching mode at 17 THz, and we measure the resulting change in lattice fluctuations using time-resolved x-ray diffuse scattering at a free electron laser. After a prompt increase, we observe a long-lived quench in R-point antiferrodistortive lattice fluctuations. The enhancement and reduction in lattice fluctuations are explained theoretically by considering fourth-order nonlinear phononic interactions and third-order coupling to the driven optical phonon and to lattice strain, respectively. These observations provide a number of new and testable hypotheses for the physics of light-induced ferroelectricity.

cond-mat.mtrl-sci

Optical Stabilization of Fluctuating High Temperature Ferromagnetism in YTiO$_3$

In quantum materials, degeneracies and frustrated interactions can have a profound impact on the emergence of long-range order, often driving strong fluctuations that suppress functionally relevant electronic or magnetic phases. Engineering the atomic structure in the bulk or at heterointerfaces has been an important research strategy to lift these degeneracies, but these equilibrium methods are limited by thermodynamic, elastic, and chemical constraints. Here, we show that all-optical, mode-selective manipulation of the crystal lattice can be used to enhance and stabilize high-temperature ferromagnetism in YTiO$_3$, a material that exhibits only partial orbital polarization, an unsaturated low-temperature magnetic moment, and a suppressed Curie temperature, $T_c$ = 27 K. The enhancement is largest when exciting a 9 THz oxygen rotation mode, for which complete magnetic saturation is achieved at low temperatures and transient ferromagnetism is realized up to $T_{neq} >$ 80 K, nearly three times the thermodynamic transition temperature. First-principles and model calculations of the nonlinear phonon-orbital-spin coupling reveal that these effects originate from dynamical changes to the orbital polarization and the makeup of the lowest quasi-degenerate Ti $t_{2g}$ levels. Notably, light-induced high temperature ferromagnetism in YTiO$_3$ is found to be metastable over many nanoseconds, underscoring the ability to dynamically engineer practically useful non-equilibrium functionalities.

cond-mat.str-el

Probing photo-induced rearrangements in the NdNiO$_{3}$ magnetic spiral with polarization-sensitive ultrafast resonant soft x-ray scattering

We use resonant soft X-ray diffraction to track the photo-induced dynamics of the antiferromagnetic structure in a NdNiO$_{3}$ thin film. Femtosecond laser pulses with a photon energy of 0.61 eV, resonant with electron transfer between long-bond and short-bond nickel sites, are used to excite the material and drive an ultrafast insulator-metal transition. Polarization sensitive soft X-ray diffraction, resonant to the nickel L$_{3}$-edge, then probes the evolution of the underlying magnetic spiral as a function of time delay with 80 picosecond time resolution. By modelling the azimuthal dependence of the scattered intensity for different linear X-ray polarizations, we benchmark the changes of the local magnetic moments and the spin alignment. The measured changes are consistent with a reduction of the long-bond site magnetic moments and an alignment of the spins towards a more collinear structure at early time delays.

cond-mat.str-el

Magnetic-Field Tuning of Light-Induced Superconductivity in Striped La$_{2-x}$Ba$_x$CuO$_4$

Optical excitation of stripe-ordered La$_{2-x}$Ba$_x$CuO$_4$ has been shown to transiently enhance superconducting tunneling between the CuO$_2$ planes. This effect was revealed by a blue-shift, or by the appearance of a Josephson Plasma Resonance in the terahertz-frequency optical properties. Here, we show that this photo-induced state can be strengthened by the application of high external magnetic fields oriented along the c-axis. For a 7-Tesla field, we observe up to a ten-fold enhancement in the transient interlayer phase correlation length, accompanied by a two-fold increase in the relaxation time of the photo-induced state. These observations are highly surprising, since static magnetic fields suppress interlayer Josephson tunneling and stabilize stripe order at equilibrium. We interpret our data as an indication that optically-enhanced interlayer coupling in La$_{2-x}$Ba$_x$CuO$_4$ does not originate from a simple optical melting of stripes, as previously hypothesized. Rather, we speculate that the photo-induced state may emerge from activated tunneling between optically-excited stripes in adjacent planes.

cond-mat.supr-con

Structural Distortions At Polar Manganite Interfaces

Electronic, lattice, and spin interactions at the interfaces between crystalline complex transition metal oxides can give rise to a wide range of functional electronic and magnetic phenomena not found in bulk. At hetero-interfaces, these interactions may be enhanced by combining oxides where the polarity changes at the interface. The physical structure between non-polar SrTiO$_3$ and polar La$_{1-x}$Sr$_x$MnO$_3$(x=0.2) is investigated using high resolution synchrotron x-ray diffraction to directly determine the role of structure in compensating the polar discontinuity. At both the oxide-oxide interface and vacuum-oxide interfaces, the lattice is found to expand and rumple along the growth direction. The SrTiO$_3$/La$_{1-x}$Sr$_x$MnO$_3$ interface also exhibits intermixing of La and Sr over a few unit cells. The results, hence, demonstrate that polar distortions and ionic intermixing coexist and both pathways play a significant role at interfaces with polar discontinuities.

cond-mat.str-el

Orbital engineering in nickelate heterostructures driven by anisotropic oxygen hybridization rather than orbital energy levels

Resonant inelastic x-ray scattering is used to investigate the electronic origin of orbital polarization in nickelate heterostructures taking $\mathrm{LaTiO_3-LaNiO_3-3x(LaAlO_3)}$, a system with exceptionally large polarization, as a model system. We find that heterostructuring generates only minor changes in the Ni $3d$ orbital energy levels, contradicting the often-invoked picture in which changes in orbital energy levels generate orbital polarization. Instead, O $K$-edge x-ray absorption spectroscopy demonstrates that orbital polarization is caused by an anisotropic reconstruction of the oxygen ligand hole states. This provides an explanation for the limited success of theoretical predictions based on tuning orbital energy levels and implies that future theories should focus on anisotropic hybridization as the most effective means to drive large changes in electronic structure and realize novel emergent phenomena.

cond-mat.str-el