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We study THz-driven condensate dynamics in epitaxial thin films of MgB_{2}, a prototype two-band superconductor (SC) with weak interband coupling. The temperature and excitation density dependent dynamics follow the behavior predicted by the phenomenological bottleneck model for the single-gap SC, implying adiabatic coupling between the two condensates on the ps timescale. The amplitude of the THz-driven suppression of condensate density reveals an unexpected decrease in pair-breaking efficiency with increasing temperature-unlike in the case of optical excitation. The reduced pair-breaking efficiency of narrow-band THz pulses, displaying minimum near ≈0.7 T_{c}, is attributed to THz-driven, long-lived, nonthermal quasiparticle distribution, resulting in Eliashberg-type enhancement of superconductivity, competing with pair breaking.
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Metals cannot exhibit ferroelectricity because static internal electric fields are screened by conduction electrons, but in 1965, Anderson and Blount predicted the possibility of a ferroelectric metal, in which a ferroelectric-like structural transition occurs in the metallic state. Up to now, no clear example of such a material has been identified. Here we report on a centrosymmetric (R3c) to non-centrosymmetric (R3c) transition in metallic LiOsO3 that is structurally equivalent to the ferroelectric transition of LiNbO3 (ref. 3). The transition involves a continuous shift in the mean position of Li(+) ions on cooling below 140 K. Its discovery realizes the scenario described in ref. 2, and establishes a new class of materials whose properties may differ from those of normal metals.
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A new quinary oxysulfide LaPbBiS3O was designed and successfully synthesized via a solid-state reaction in a sealed evacuated quartz tube. This material, composed of stacked NaCl-like [M4S6] (where M = Pb, Bi) layers and fluorite-type [La2O2] layers, crystallizes in the tetragonal space group P4/nmm with a = 4.0982(1) Å, c = 19.7754(6) Å, and Z = 2. Electrical resistivity and Hall effect measurements demonstrate that it is a narrow gap semiconductor with an activation energy of â¼17 meV. The thermopower and the figure of merit at room temperature were measured to be -52 µV/K and 0.23, respectively, which makes LaPbBiS3O and its derivatives be promising for thermoelectric applications.
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Single crystals of YbOs2Al10 and LuOs2Al10 were grown for the first time using an aluminum self-flux method. The compounds crystallized into a cagelike structure in space group Cmcm, similar to the prototype compound YbFe2Al10. YbOs2Al10 exhibited a mixed-valent nature, as determined by magnetic susceptibility measurements over a wide temperature range from 2 to 900 K, in which the inter-configuration-fluctuation model revealed a broad peak around 400 K. In contrast, LuOs2Al10 displayed Pauli-like paramagnetic behavior over the same temperature range. Both compounds were metallic in nature between 2 and 300 K. The electronic specific heat coefficient of 21.3(2) mJ mol(-1) K(-2) for YbOs2Al10 was determined to be larger than that for LuOs2Al10 [8.9(1) mJ mol(-1) K(-2)], reflecting the mixed-valent nature of the former. First-principles calculations predicted the presence of a mixed-valent state in YbOs2Al10, in agreement with the experimental observations. The novel compound YbOs2Al10 elucidates the evolution of the mixed-valent nature of the Yb-based ternary transition metal aluminides from the 3d to 5d elements.
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Optical nonlinearities are one of the most fascinating properties of two-dimensional (2D) materials. While tremendous efforts have been made to find and optimize the second-order optical nonlinearity in enormous 2D materials, opportunities to explore higher-order ones are elusive because of the much lower efficiency. Here, we report the giant high odd-order optical nonlinearities in centrosymmetric correlated van der Waals insulator manganese phosphorus triselenide. When illuminated by two near-infrared femtosecond lasers, the sample generates a series of profound four- and six-wave mixing outputs. The near-infrared third-order nonlinear susceptibility reaches near the highest record values of 2D materials. Comparative measurements to other prototypical nonlinear optical materials [lithium niobate, gallium(II) selenide, and tungsten disulfide] reveal its extraordinary wave mixing efficiency. The wave mixing processes are further used for nonlinear optical waveguide with multicolor emission. Our work highlights the promising prospect for future research of the nonlinear light-matter interactions in the correlated 2D system and for potential nonlinear photonic applications.
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We report on nonlinear terahertz third-harmonic generation (THG) measurements on YBa2Cu3O6+x thin films. Different from conventional superconductors, the THG signal starts to appear in the normal state, which is consistent with the crossover temperature T* of pseudogap over broad doping levels. Upon lowering the temperature, the THG signal shows an anomaly just below Tc in the optimally doped sample. Notably, we observe a beat pattern directly in the measured real-time waveform of the THG signal. We elaborate that the Higgs mode, which develops below Tc, couples to the mode already developed below T*, resulting in an energy level splitting. However, this coupling effect is not evident in underdoped samples. We explore different potential explanations for the observed phenomena. Our research offers valuable insight into the interplay between superconductivity and pseudogap.
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Charge density wave (CDW) orders in vanadium-based kagome metals have recently received tremendous attention, yet their origin remains a topic of debate. The discovery of ScV6Sn6, a bilayer kagome metal featuring an intriguing [Formula: see text] CDW order, offers a novel platform to explore the underlying mechanism behind the unconventional CDW. Here, we combine high-resolution angle-resolved photoemission spectroscopy, Raman scattering and density functional theory to investigate the electronic structure and phonon modes of ScV6Sn6. We identify topologically nontrivial surface states and multiple van Hove singularities (VHSs) in the vicinity of the Fermi level, with one VHS aligning with the in-plane component of the CDW vector near the [Formula: see text] point. Additionally, Raman measurements indicate a strong electron-phonon coupling, as evidenced by a two-phonon mode and new emergent modes. Our findings highlight the fundamental role of lattice degrees of freedom in promoting the CDW in ScV6Sn6.
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In continuation of the series of perovskite oxides that includes 3d(4) cubic BaFeO3 and 4d(4) cubic BaRuO3, 5d(4) cubic BaOsO3 was synthesized by a solid-state reaction at a pressure of 17 GPa, and its crystal structure was investigated by synchrotron powder X-ray diffraction measurements. In addition, its magnetic susceptibility, electrical resistivity, and specific heat were measured over temperatures ranging from 2 to 400 K. The results establish a series of d(4) cubic perovskite oxides, which can help in the mapping of the itinerant ferromagnetism that is free from any complication from local lattice distortions for transitions from the 3d orbital to the 5d orbital. Such a perovskite series has never been synthesized at any d configuration to date. Although cubic BaOsO3 did not exhibit long-range ferromagnetic order unlike cubic BaFeO3 and BaRuO3, enhanced feature of paramagnetism was detected with weak temperature dependence. Orthorhombic CaOsO3 and SrOsO3 show similar magnetic behaviors. CaOsO3 is not as conducting as SrOsO3 and BaOsO3, presumably due to impact of tilting of octahedra on the width of the t2g band. These results elucidate the evolution of the magnetism of perovskite oxides not only in the 5d system but also in group 8 of the periodic table.
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High-pressure angle-dispersive X-ray diffraction experiments on iron-based superconductor Ce(O(0.84)F(0.16))FeAs were performed up to 54.9 GPa at room temperature. A tetragonal to tetragonal isostructural phase transition starts at about 13.9 GPa, and a new high-pressure phase has been found above 33.8 GPa. At pressures above 19.9 GPa, Ce(O(0.84)F(0.16))FeAs completely transforms to a high-pressure tetragonal phase, which remains in the same tetragonal structure with a larger a-axis and smaller c-axis than those of the low-pressure tetragonal phase. The structure analysis shows a discontinuity in the pressure dependences of the Fe-As and Ce-(O, F) bond distances, as well as the As-Fe-As and Ce-(O, F)-Ce bond angles in the transition region, which correlates with the change in T(c) of this compound upon compression. The isostructural phase transition in Ce(O(0.84)F(0.16))FeAs leads to a drastic drop in the superconducting transition temperature T(c) and restricts the superconductivity at low temperature. For the 1111-type iron-based superconductors, the structure evolution and following superconductivity changes under compression are related to the radius of lanthanide cations in the charge reservoir layer.
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The advent of intense ultrashort optical pulses spanning a frequency range from terahertz to the visible has opened a new era in the experimental investigation and manipulation of quantum materials. The generation of strong optical field in an ultrashort time scale enables the steering of quantum materials nonadiabatically, inducing novel phenomenon or creating new phases which may not have an equilibrium counterpart. Ultrafast time-resolved optical techniques have provided rich information and played an important role in characterization of the nonequilibrium and nonlinear properties of solid systems. Here, some of the recent progress of ultrafast optical techniques and their applications to the detection and manipulation of physical properties in selected quantum materials are reviewed. Specifically, the new development in the detection of the Higgs mode and photoinduced nonequilibrium response in the study of superconductors by time-resolved terahertz spectroscopy are discussed.
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Nonlinear responses of superconductors to intense terahertz radiation has been an active research frontier. Using terahertz pump-terahertz probe spectroscopy, we investigate the c-axis nonlinear optical response of a high-temperature superconducting cuprate. After excitation by a single-cycle terahertz pump pulse, the reflectivity of the probe pulse oscillates as the pump-probe delay is varied. Interestingly, the oscillatory central frequency scales linearly with the probe frequency, a fact widely overlooked in pump-probe experiments. By theoretically solving the nonlinear optical reflection problem on the interface, we show that our observation is well explained by the Josephson-type third-order nonlinear electrodynamics, together with the emission coefficient from inside the material into free space. The latter results in a strong enhancement of the emitted signal whose physical frequency is around the Josephson plasma edge. Our result offers a benchmark for and new insights into strong-field terahertz spectroscopy of related quantum materials.
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Cuprate high-Tc superconductors are known for their intertwined interactions and the coexistence of competing orders. Uncovering experimental signatures of these interactions is often the first step in understanding their complex relations. A typical spectroscopic signature of the interaction between a discrete mode and a continuum of excitations is the Fano resonance/interference, characterized by the asymmetric light-scattering amplitude of the discrete mode as a function of the electromagnetic driving frequency. In this study, we report a new type of Fano resonance manifested by the nonlinear terahertz response of cuprate high-Tc superconductors, where we resolve both the amplitude and phase signatures of the Fano resonance. Our extensive hole-doping and magnetic field dependent investigation suggests that the Fano resonance may arise from an interplay between the superconducting fluctuations and the charge density wave fluctuations, prompting future studies to look more closely into their dynamical interactions.
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The physical properties of copper oxide high-temperature superconductors have been studied extensively, such as the band structure and doping effects of Bi2Sr2CaCu2O8+δ (Bi-2212). However, some chemical-related properties of these superconductors are rarely reported, such as their stability in water-bearing environments. Herein, we report experiments combined with ab initio calculations that address the effects of water in contact with Bi-2212. The evolution of Bi-2212 flakes with exposure to water for different time intervals was tested and characterized by optical microscopy (OM), atomic force microscopy (AFM), Raman spectroscopy, transmission electron microscopy (TEM), and electrical measurements. The thickness of Bi-2212 flakes is gradually decreased in water, and some thin flakes can be completely etched away after a few days. The stability of Bi-2212 in other solvents is also evaluated, including alcohol, acetone, HCl, and KOH. The morphology of Bi-2212 flakes is relatively stable in organic solvents. However, the flakes are etched relatively quick in HCl and KOH, especially in an acidic environment. Our results imply that hydrogen ions are primarily responsible for the deterioration of their properties. Both TEM and calculation results demonstrate that the atoms in the Bi-O plane are relatively stable when compared to the inner atoms in Sr-O, Ca-O, and Cu-O planes. This work contributes toward understanding the chemical stability of a Bi-2212 superconducting device in environmental medium, which is important for both fundamental studies and practical applications of copper oxide high-temperature superconductors.
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We use neutron scattering to show that spin waves in the iron chalcogenide Fe(1.05)Te display novel dispersion clearly different from both the first principles density functional calculations and recent observations in the related iron pnictide CaFe(2)As(2). By fitting to a Heisenberg Hamiltonian, we find that although the nearest-neighbor exchange couplings in the two systems are quite different, their next-nearest-neighbor (NNN) couplings are similar. This suggests that superconductivity in the pnictides and chalcogenides share a common magnetic origin that is intimately associated with the NNN magnetic coupling between the irons.
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Ultra-broadband photodetection is crucial for various applications like imaging and sensing and has become a hot research topic in recent years. However, most of the reported ultra-broadband photodetectors can only cover the range from ultraviolet to infrared, which is insufficient. Herein, a photothermoelectric (PTE) detector made of NbS3 is reported. The device shows a considerable performance from ultraviolet to terahertz. For all examined wavelengths, the photoresponsivities are all larger than 1 V W-1 while the response time is less than 10 ms, much shorter than the reported ultra-broadband photodetectors made of millimetric scale graphene, ternary chalcogenide single crystal, and other materials. The extraordinary performance is fully discussed and can be attributed to the thermal localization enhanced PTE effect. Because of the short thermal decay length and low thermal loss, the heat generated by the illumination is localized in only a micrometer scale along the channel, and thus a strong PTE response is produced. In addition, the fabricated device also demonstrates robust flexibility and stability. Thanks to the quasi-one-dimensional (quasi-1D) structure, the NbS3 crystal is easy to be scaled down and thus intrinsically facilitate the integration of detectors. With these favorable merits, the quasi-1D NbS3 crystal holds a promising potential in high-performance, ultra-broadband photodetectors.
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The experimental discovery of Weyl semimetals offers unprecedented opportunities to study Weyl physics in condensed matters. Unique electromagnetic response of Weyl semimetals such as chiral magnetic effect has been observed and presented by the axial θ E · B term in electromagnetic Lagrangian (E and B are the electric and magnetic field, respectively). But till now, the experimental progress in this direction in Weyl semimetals is restricted to the DC regime. Here we report experimental access to the dynamic regime in Weyl semimetal NbAs by combining the internal deformation potential of coupled phonons with applied static magnetic field. While the dynamic E · B field is realized, it produces an anomalous phonon activity with a characteristic angle-dependence. Our results provide an effective approach to achieve the dynamic regime beyond the widely-investigated DC limit which enables the coupling between the Weyl fermions and the electromagnetic wave for further study of novel light-matter interactions in Weyl semimetals.
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Ionic evolution-induced phase transformation can lead to wide ranges of novel material functionalities with promising applications. Here, using the gating voltage during ionic liquid gating as a tuning knob, the brownmillerite SrCoO2.5 is transformed into a series of protonated H x SrCoO2.5 phases with distinct hydrogen contents. The unexpected electron to charge-neutral doping crossover along with the increase of proton concentration from x = 1 to 2 suggests the formation of exotic charge neutral H-H dimers for higher proton concentration, which is directly visualized at the vacant tetrahedron by scanning transmission electron microscopy and then further supported by first principles calculations. Although the H-H dimers cause no change of the valency of Co2+ ions, they result in clear enhancement of electronic bandgap and suppression of magnetization through lattice expansion. These results not only reveal a hydrogen chemical state beyond anion and cation within the complex oxides, but also suggest an effective pathway to design functional materials through tunable ionic evolution.
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The high-pressure angle-dispersive X-ray diffraction experiments on the iron-based superconductor Nd(O0.88F0.12)FeAs were performed up to 32.7 GPa at room temperature. An isostructural phase transition starts at approximately 10 GPa. When pressure is higher than 13.5 GPa, Nd(O0.88F0.12)FeAs completely transforms to a high-pressure phase, which remains the same tetragonal structure with a larger a-axis and smaller c-axis than those of the low-pressure phase. The ambient conditions isothermal bulk moduli B0 are derived as 102(2) and 245(9) GPa for the low-pressure phase and high-pressure phase, respectively. The structure analysis based on the Rietveld refinement methods shows the difference of pressure dependence of the Fe-As and Nd-(O, F) bonding distances, as well as As-Fe-As and Nd-(O, F)-Nd angles between the low-pressure phase and high-pressure phase.