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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.
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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.
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The interplay between charge order and superconductivity remains one of the central themes of research in quantum materials. In the case of cuprates, the coupling between striped charge fluctuations and local electromagnetic fields is especially important, as it affects transport properties, coherence, and dimensionality of superconducting correlations. Here, we study the emission of coherent terahertz radiation in single-layer cuprates of the La2-xBaxCuO4 family, for which this effect is expected to be forbidden by symmetry. We find that emission vanishes for compounds in which the stripes are quasi-static but is activated when c-axis inversion symmetry is broken by incommensurate or fluctuating charge stripes, such as in La1.905Ba0.095CuO4 and in La1.845Ba0.155CuO4. In this case, terahertz radiation is emitted by surface Josephson plasmons, which are generally dark modes, but couple to free space electromagnetic radiation because of the stripe modulation.
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Nonlinear optical techniques at visible frequencies have long been applied to condensed matter spectroscopy. However, because many important excitations of solids are found at low energies, much can be gained from the extension of nonlinear optics to mid-infrared and terahertz frequencies. For example, the nonlinear excitation of lattice vibrations has enabled the dynamic control of material functions. So far it has only been possible to exploit second-order phonon nonlinearities at terahertz field strengths near one million volts per centimetre. Here we achieve an order-of-magnitude increase in field strength and explore higher-order phonon nonlinearities. We excite up to five harmonics of the A1 (transverse optical) phonon mode in the ferroelectric material lithium niobate. By using ultrashort mid-infrared laser pulses to drive the atoms far from their equilibrium positions, and measuring the large-amplitude atomic trajectories, we can sample the interatomic potential of lithium niobate, providing a benchmark for ab initio calculations for the material. Tomography of the energy surface by high-order nonlinear phononics could benefit many aspects of materials research, including the study of classical and quantum phase transitions.
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We use coherent midinfrared optical pulses to resonantly excite large-amplitude oscillations of the Si-C stretching mode in silicon carbide. When probing the sample with a second pulse, we observe parametric optical gain at all wavelengths throughout the reststrahlen band. This effect reflects the amplification of light by phonon-mediated four-wave mixing and, by extension, of optical-phonon fluctuations. Density functional theory calculations clarify aspects of the microscopic mechanism for this phenomenon. The high-frequency dielectric permittivity and the phonon oscillator strength depend quadratically on the lattice coordinate; they oscillate at twice the frequency of the optical field and provide a parametric drive for the lattice mode. Parametric gain in phononic four-wave mixing is a generic mechanism that can be extended to all polar modes of solids, as a means to control the kinetics of phase transitions, to amplify many-body interactions or to control phonon-polariton waves.
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Terahertz-frequency optical pulses can resonantly drive selected vibrational modes in solids and deform their crystal structures. In complex oxides, this method has been used to melt electronic order, drive insulator-to-metal transitions and induce superconductivity. Strikingly, coherent interlayer transport strongly reminiscent of superconductivity can be transiently induced up to room temperature (300 kelvin) in YBa2Cu3O6+x (refs 9, 10). Here we report the crystal structure of this exotic non-equilibrium state, determined by femtosecond X-ray diffraction and ab initio density functional theory calculations. We find that nonlinear lattice excitation in normal-state YBa2Cu3O6+x at above the transition temperature of 52 kelvin causes a simultaneous increase and decrease in the Cu-O2 intra-bilayer and, respectively, inter-bilayer distances, accompanied by anisotropic changes in the in-plane O-Cu-O bond buckling. Density functional theory calculations indicate that these motions cause drastic changes in the electronic structure. Among these, the enhancement in the character of the in-plane electronic structure is likely to favour superconductivity.
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The ultrafast dynamics of the octahedral rotation in Ca:SrTiO_{3} is studied by time-resolved x-ray diffraction after photoexcitation over the band gap. By monitoring the diffraction intensity of a superlattice reflection that is directly related to the structural order parameter of the soft-mode driven antiferrodistortive phase in Ca:SrTiO_{3}, we observe an ultrafast relaxation on a 0.2 ps timescale of the rotation of the oxygen octahedron, which is found to be independent of the initial temperature despite large changes in the corresponding soft-mode frequency. A further, much smaller reduction on a slower picosecond timescale is attributed to thermal effects. Time-dependent density-functional-theory calculations show that the fast response can be ascribed to an ultrafast displacive modification of the soft-mode potential towards the normal state induced by holes created in the oxygen 2p states.
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We describe a mechanism by which nonlinear phononics allows ultrafast coherent and directional control of transient structural distortions. With ErFeO_{3} as a model system, we use density functional theory to calculate the structural properties as input into an anharmonic phonon model that describes the response of the system to a pulsed optical excitation. We find that the trilinear coupling of two orthogonal infrared-active phonons to a Raman-active phonon causes a transient distortion of the lattice. In contrast to the quadratic-linear coupling that has been previously explored, the direction of the distortion is determined by the polarization of the exciting light, introducing a novel mechanism for nonlinear phononic switching. Since the occurrence of the coupling is determined by the symmetry of the system we propose that it is a universal feature of orthorhombic and tetragonal perovskites.
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We employ time-resolved resonant x-ray diffraction to study the melting of charge order and the associated insulator-to-metal transition in the doped manganite Pr_{0.5}Ca_{0.5}MnO_{3} after resonant excitation of a high-frequency infrared-active lattice mode. We find that the charge order reduces promptly and highly nonlinearly as function of excitation fluence. Density-functional theory calculations suggest that direct anharmonic coupling between the excited lattice mode and the electronic structure drives these dynamics, highlighting a new avenue of nonlinear phonon control.
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Optically driven quantum materials exhibit a variety of non-equilibrium functional phenomena, which to date have been primarily studied with ultrafast optical, X-Ray and photo-emission spectroscopy. However, little has been done to characterize their transient electrical responses, which are directly associated with the functionality of these materials. Especially interesting are linear and nonlinear current-voltage characteristics at frequencies below 1 THz, which are not easily measured at picosecond temporal resolution. Here, we report on ultrafast transport measurements in photo-excited K3C60. Thin films of this compound were connected to photo-conductive switches with co-planar waveguides. We observe characteristic nonlinear current-voltage responses, which in these films point to photo-induced granular superconductivity. Although these dynamics are not necessarily identical to those reported for the powder samples studied so far, they provide valuable new information on the nature of the light-induced superconducting-like state above equilibrium Tc. Furthermore, integration of non-equilibrium superconductivity into optoelectronic platforms may lead to integration in high-speed devices based on this effect.
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We report on the first results of diode pumped laser operation of Pr3+:LaF3 in a quasi continuous wave (qcw) mode with average output powers of up to 80.0 mW (≈ 161.3 mW qcw) and a maximum slope efficiency of 37% at 719.8 nm. Furthermore it was possible to operate the laser at 537.1 nm and 635.4 nm and to tune the emission wavelength from 609 nm to 623 nm. The pump source was an InGaN laser diode with a maximum output power of 1 W at a central emission wavelength of 442 nm.
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Láseres de Estado Sólido , Análisis Espectral/instrumentación , Diseño de Equipo , Análisis de Falla de EquipoRESUMEN
In this Letter, we report on laser operation of Pr3+,Mg2+:SrAl12O19 pumped by a frequency-doubled optically pumped semiconductor laser. By employing a V-type cavity, we demonstrate cw laser operation at room temperature in the green spectral range in a doped oxide host for the first time to the best of our knowledge. Furthermore, efficient laser operation was realized in the orange, red, and deep red spectral range with output powers exceeding 1.1 W at emission wavelengths of 643.6 and 724.4 nm.
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Magnetoelectric coupling allows for manipulating the magnetization by an external electric field or the electrical polarization by an external magnetic field. Here, we propose a mechanism to electrically induce 180° magnetization switching combining two effects: the magnetoelectric coupling at a multiferroic interface and magnetic interlayer exchange coupling. By means of first-principles methods, we investigate a ferroelectric layer in contact with a Fe/Au/Fe trilayer. The calculations show that the interface magnetism is strongly coupled to the ferroelectric layer. Furthermore, under certain conditions a reversal of polarization causes a sign reversal of the interlayer exchange coupling which is results in a 180° switching of the free layer magnetization. We argue that this magnetoelectric coupling mechanism is very robust and can find applications in magnetic data storage.
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We use symmetry analysis and first-principles calculations to show that the linear magnetoelectric effect can originate from the response of orbital magnetic moments to the polar distortions induced by an applied electric field. Using LiFePO(4) as a model compound we show that spin-orbit coupling partially lifts the quenching of the 3d orbitals and causes small orbital magnetic moments (µ((L)) ≈ 0.3 µ(B)) parallel to the spins of the Fe(2+) ions. An applied electric field E modifies the size of these orbital magnetic moments inducing a net magnetization linear in E.
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Photoemission electron microscopy performed on a well-prepared surface of BaTiO3 reveals the persistence of surface domains at temperatures well above the bulk Curie temperature. Their patterns follow the ferroelectric domain structure observed at 300 K. The contrast between formerly outward polarized domains and in-plane polarized domains is preserved across the transition, while the contrast of inward polarized domains changes sign. The work functions of different possible structures are compared by first-principles calculations. The domain contrast in photoemission above the bulk Curie temperature is associated with a remaining tetragonal distortion of the topmost unit cells which is stabilized by an ionic surface relaxation.
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The Double Chooz experiment presents an indication of reactor electron antineutrino disappearance consistent with neutrino oscillations. An observed-to-predicted ratio of events of 0.944±0.016(stat)±0.040(syst) was obtained in 101 days of running at the Chooz nuclear power plant in France, with two 4.25 GW(th) reactors. The results were obtained from a single 10 m(3) fiducial volume detector located 1050 m from the two reactor cores. The reactor antineutrino flux prediction used the Bugey4 flux measurement after correction for differences in core composition. The deficit can be interpreted as an indication of a nonzero value of the still unmeasured neutrino mixing parameter sin(2)2θ(13). Analyzing both the rate of the prompt positrons and their energy spectrum, we find sin(2)2θ(13)=0.086±0.041(stat)±0.030(syst), or, at 90% C.L., 0.017
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We present an experimental and theoretical study of the geometric structure of ultrathin BaTiO(3) films grown on Fe(001). Surface x-ray diffraction reveals that the films are terminated by a BaO layer, while the TiO(2) layer is next to the top Fe layer. Cations in termination layers have incomplete oxygen shells inducing strong vertical relaxations. Onset of polarization is observed at a minimum thickness of two unit cells. Our findings are supported by first-principles calculations providing a quantitative insight into the multiferroic properties on the atomic scale.
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BACKGROUND AND STUDY AIM: The aim of this study was to develop an algorithm to detect small-bowel metastasis (SBM) of melanoma by sequential laboratory parameters and pan-intestinal endoscopy (PIE) including video capsule endoscopy (VCE). PATIENTS AND METHODS: A total of 390 melanoma patients (AJCC stage I/II/III/IV, 140/80/121/49) were screened for signs of intestinal blood loss (fecal occult blood test [FOBT] or overt bleeding) in an open, multicenter, prospective study, and those who were positive underwent PIE. Independent of the presence of intestinal bleeding, all stage IV patients were offered PIE. Follow-up was obtained in 357 patients (91.5 %) for a median of 16 months. We undertook to identify possible associations between SBM and clinical and laboratory data. Survival data were analyzed with regard to clinical and laboratory data and small-bowel findings. RESULTS: Intestinal blood loss was suspected in 49 of 390 patients (12.6 %), 38 of whom (77.6 %) agreed to undergo endoscopy. In 10 patients, SBM was detected by VCE (intention-to-diagnose, 20.4 %; AJCC III, n = 2; AJCC IV, n = 8). The SBM was resected in five patients. Total detection rates of SBM were 14 of 49 patients in stage IV (28.6 %, intention-to-diagnose), 2 of 121 in stage III (1.7 %), and 0 in stage I/II. In FOBT-positive patients, SBM detection rates were 72.7 %, 14.3 %, and 0 % in tumor stages IV, III, and I/II, respectively. Positive FOBT proved to be an independent negative prognostic factor for total survival in stage III and IV melanoma. CONCLUSIONS: SBMs are frequent in advanced melanoma. In stage III patients, screening for intestinal blood loss by PIE may help to identify SBMs. In stage IV, indication for PIE should depend on the individual consequences of detecting SBM, but not on bleeding symptoms alone.
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Algoritmos , Endoscopía Gastrointestinal , Hemorragia Gastrointestinal/etiología , Neoplasias Intestinales/secundario , Melanoma/secundario , Sangre Oculta , Neoplasias Cutáneas/patología , Adulto , Anciano , Anciano de 80 o más Años , Femenino , Humanos , Neoplasias Intestinales/complicaciones , Neoplasias Intestinales/diagnóstico , Neoplasias Intestinales/cirugía , Masculino , Melanoma/patología , Persona de Mediana Edad , Estudios Prospectivos , Tasa de Supervivencia , Adulto JovenRESUMEN
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.
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Unconventional superconductivity in the cuprates coexists with other types of electronic order. However, some of these orders are invisible to most experimental probes because of their symmetry. For example, the possible existence of superfluid stripes is not easily validated with linear optics, because the stripe alignment causes interlayer superconducting tunneling to vanish on average. Here we show that this frustration is removed in the nonlinear optical response. A giant terahertz third harmonic, characteristic of nonlinear Josephson tunneling, is observed in La1.885Ba0.115CuO4 above the transition temperature Tc = 13 kelvin and up to the charge-ordering temperature Tco = 55 kelvin. We model these results by hypothesizing the presence of a pair density wave condensate, in which nonlinear mixing of optically silent tunneling modes drives large dipole-carrying supercurrents.