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1.
J Phys Condens Matter ; 36(31)2024 May 09.
Artículo en Inglés | MEDLINE | ID: mdl-38657622

RESUMEN

It has been suggested that Ba3In2O6might be a high-Tcsuperconductor. Experimental investigation of the properties of Ba3In2O6was long inhibited by its instability in air. Recently epitaxial Ba3In2O6with a protective capping layer was demonstrated, which finally allows its electronic characterization. The optical bandgap of Ba3In2O6is determined to be 2.99 eV in-the (001) plane and 2.83 eV along thec-axis direction by spectroscopic ellipsometry. First-principles calculations were carried out, yielding a result in good agreement with the experimental value. Various dopants were explored to induce (super-)conductivity in this otherwise insulating material. NeitherA- norB-site doping proved successful. The underlying reason is predominately the formation of oxygen interstitials as revealed by scanning transmission electron microscopy and first-principles calculations. Additional efforts to induce superconductivity were investigated, including surface alkali doping, optical pumping, and hydrogen reduction. To probe liquid-ion gating, Ba3In2O6was successfully grown epitaxially on an epitaxial SrRuO3bottom electrode. So far none of these efforts induced superconductivity in Ba3In2O6,leaving the answer to the initial question of whether Ba3In2O6is a high-Tcsuperconductor to be 'no' thus far.

2.
Nat Mater ; 23(3): 363-368, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38302742

RESUMEN

Crystal lattice fluctuations, which are known to influence phase transitions of quantum materials in equilibrium, are also expected to determine the dynamics of light-induced phase changes. However, they have only rarely been explored in these dynamical settings. Here we study the time evolution of lattice fluctuations in 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 polar instabilities 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 the 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. Their enhancement and reduction are theoretically explained by considering the fourth-order nonlinear phononic interactions to the driven optical phonon and third-order coupling to lattice strain, respectively. These observations provide a number of testable hypotheses for the physics of light-induced ferroelectricity.

3.
Nature ; 617(7959): 73-78, 2023 05.
Artículo en Inglés | MEDLINE | ID: mdl-37138109

RESUMEN

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 phases1-7. 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 constraints8. Here we show that all-optical, mode-selective manipulation of the crystal lattice can be used to enhance and stabilize high-temperature ferromagnetism in YTiO3, a material that shows only partial orbital polarization, an unsaturated low-temperature magnetic moment and a suppressed Curie temperature, Tc = 27 K (refs. 9-13). 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 Tneq > 80 K, nearly three times the thermodynamic transition temperature. We interpret these effects as a consequence of the light-induced dynamical changes to the quasi-degenerate Ti t2g orbitals, which affect the magnetic phase competition and fluctuations found in the equilibrium state14-20. Notably, the light-induced high-temperature ferromagnetism discovered in our work is metastable over many nanoseconds, underscoring the ability to dynamically engineer practically useful non-equilibrium functionalities.

4.
Science ; 364(6445): 1075-1079, 2019 06 14.
Artículo en Inglés | MEDLINE | ID: mdl-31197010

RESUMEN

Fluctuating orders in solids are generally considered high-temperature precursors of broken symmetry phases. However, in some cases, these fluctuations persist to zero temperature and prevent the emergence of long-range order. Strontium titanate (SrTiO3) is a quantum paraelectric in which dipolar fluctuations grow upon cooling, although a long-range ferroelectric order never sets in. Here, we show that optical excitation of lattice vibrations can induce polar order. This metastable polar phase, observed up to temperatures exceeding 290 kelvin, persists for hours after the optical pump is interrupted. Furthermore, hardening of a low-frequency vibration points to a photoinduced ferroelectric phase transition, with a spatial domain distribution suggestive of a photoflexoelectric coupling.

5.
Phys Rev Lett ; 121(26): 267003, 2018 Dec 28.
Artículo en Inglés | MEDLINE | ID: mdl-30636150

RESUMEN

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 blueshift, or by the appearance of a Josephson plasma resonance in the terahertz-frequency optical properties. Here, we show that this photoinduced state can be strengthened by the application of high external magnetic fields oriented along the c axis. For a 7 T field, we observe up to a tenfold enhancement in the transient interlayer phase correlation length, accompanied by a twofold increase in the relaxation time of the photoinduced 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 photoinduced state may emerge from activated tunneling between optically excited stripes in adjacent planes.

6.
Phys Rev Lett ; 117(14): 147401, 2016 Sep 30.
Artículo en Inglés | MEDLINE | ID: mdl-27740843

RESUMEN

Resonant inelastic x-ray scattering is used to investigate the electronic origin of orbital polarization in nickelate heterostructures taking LaTiO_{3}-LaNiO_{3}-3×(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.

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