Optically Probing Unconventional Superconductivity in Atomically Thin Bi2Sr2Ca0.92Y0.08Cu2O8+δ.

Atomically thin cuprates exhibiting a superconducting phase transition temperature similar to that of the bulk have recently been realized, although the device fabrication remains a challenge and limits the potential for many novel studies and applications. Here, we use an optical pump-probe approach to noninvasively study the unconventional superconductivity in atomically thin Bi2Sr2Ca0.92Y0.08Cu2O8+δ (Y-Bi2212). Apart from finding an optical response due to the superconducting phase transition that is similar to that of bulk Y-Bi2212, we observe that the sign and amplitude of the pump-probe signal in atomically thin flakes vary significantly in different dielectric environments depending on the nature of the optical excitation. By exploiting the spatial resolution of the optical probe, we uncover the exceptional sensitivity of monolayer Y-Bi2212 to the environment. Our results provide the first optical evidence for the intralayer nature of the superconducting condensate in Bi2212 and highlight the role of double-sided encapsulation in preserving superconductivity in atomically thin cuprates.

Universal sheet resistance and revised phase diagram of the cuprate high-temperature superconductors.

Upon introducing charge carriers into the copper-oxygen sheets of the enigmatic lamellar cuprates, the ground state evolves from an insulator to a superconductor and eventually to a seemingly conventional metal (a Fermi liquid). Much has remained elusive about the nature of this evolution and about the peculiar metallic state at intermediate hole-carrier concentrations (p). The planar resistivity of this unconventional metal exhibits a linear temperature dependence (ρ ∝ T) that is disrupted upon cooling toward the superconducting state by the opening of a partial gap (the pseudogap) on the Fermi surface. Here, we first demonstrate for the quintessential compound HgBa2CuO4+δ a dramatic switch from linear to purely quadratic (Fermi liquid-like, ρ ∝ T(2)) resistive behavior in the pseudogap regime. Despite the considerable variation in crystal structures and disorder among different compounds, our result together with prior work gives insight into the p-T phase diagram and reveals the fundamental resistance per copper-oxygen sheet in both linear (ρ = A1T) and quadratic (ρ = A2T(2)) regimes, with A1 ∝ A2 ∝ 1/p. Theoretical models can now be benchmarked against this remarkably simple universal behavior. Deviations from this underlying behavior can be expected to lead to new insight into the nonuniversal features exhibited by certain compounds.

Spectroscopic evidence for Fermi liquid-like energy and temperature dependence of the relaxation rate in the pseudogap phase of the cuprates.

Cuprate high-Tc superconductors exhibit enigmatic behavior in the nonsuperconducting state. For carrier concentrations near "optimal doping" (with respect to the highest Tcs) the transport and spectroscopic properties are unlike those of a Landau-Fermi liquid. On the Mott-insulating side of the optimal carrier concentration, which corresponds to underdoping, a pseudogap removes quasi-particle spectral weight from parts of the Fermi surface and causes a breakup of the Fermi surface into disconnected nodal and antinodal sectors. Here, we show that the near-nodal excitations of underdoped cuprates obey Fermi liquid behavior. The lifetime τ(ω, T) of a quasi-particle depends on its energy ω as well as on the temperature T. For a Fermi liquid, 1/τ(ω, T) is expected to collapse on a universal function proportional to (ℏω)(2) + (pπk(B)T)(2). Magneto-transport experiments, which probe the properties in the limit ω = 0, have provided indications for the presence of a T(2) dependence of the dc (ω = 0) resistivity of different cuprate materials. However, Fermi liquid behavior is very much about the energy dependence of the lifetime, and this can only be addressed by spectroscopic techniques. Our optical experiments confirm the aforementioned universal ω- and T dependence of 1/τ(ω, T), with p ∼ 1.5. Our data thus provide a piece of evidence in favor of a Fermi liquid-like scenario of the pseudogap phase of the cuprates.

Mechanisms of Hysteresis and Reversibility across the Voltage-Driven Perovskite-Brownmillerite Transformation in Electrolyte-Gated Ultrathin La0.5Sr0.5CoO3-δ.

Perovskite cobaltites have emerged as archetypes for electrochemical control of materials properties in electrolyte-gate devices. Voltage-driven redox cycling can be performed between fully oxygenated perovskite and oxygen-vacancy-ordered brownmillerite phases, enabling exceptional modulation of the crystal structure, electronic transport, thermal transport, magnetism, and optical properties. The vast majority of studies, however, have focused heavily on the perovskite and brownmillerite end points. In contrast, here we focus on hysteresis and reversibility across the entire perovskite ↔ brownmillerite topotactic transformation, combining gate-voltage hysteresis loops, minor hysteresis loops, quantitative operando synchrotron X-ray diffraction, and temperature-dependent (magneto)transport, on ion-gel-gated ultrathin (10-unit-cell) epitaxial La0.5Sr0.5CoO3-δ films. Gate-voltage hysteresis loops combined with operando diffraction reveal a wealth of new mechanistic findings, including asymmetric redox kinetics due to differing oxygen diffusivities in the two phases, nonmonotonic transformation rates due to the first-order nature of the transformation, and limits on reversibility due to first-cycle structural degradation. Minor loops additionally enable the first rational design of an optimal gate-voltage cycle. Combining this knowledge, we demonstrate state-of-the-art nonvolatile cycling of electronic and magnetic properties, encompassing >105 transport ON/OFF ratios at room temperature, and reversible metal-insulator-metal and ferromagnet-nonferromagnet-ferromagnet cycling, all at 10-unit-cell thickness with high room-temperature stability. This paves the way for future work to establish the ultimate cycling frequency and endurance of such devices.

Doping- and Strain-Dependent Electrolyte-Gate-Induced Perovskite to Brownmillerite Transformation in Epitaxial La1-xSrxCoO3-δ Films.

Much recent attention has focused on the voltage-driven reversible topotactic transformation between the ferromagnetic metallic perovskite (P) SrCoO3-δ and oxygen-vacancy-ordered antiferromagnetic insulating brownmillerite (BM) SrCoO2.5. This is emerging as a paradigmatic example of the power of electrochemical gating (using, e.g., ionic liquids/gels), the wide modulation of electronic, magnetic, and optical properties generating clear application potential. SrCoO3 films are challenging with respect to stability, however, and there has been little exploration of alternate compositions. Here, we present the first study of ion-gel-gating-induced P → BM transformations across almost the entire La1-xSrxCoO3 phase diagram (0 ≤ x ≤ 0.70), under both tensile and compressive epitaxial strain. Electronic transport, magnetometry, and operando synchrotron X-ray diffraction establish that voltage-induced P → BM transformations are possible at essentially all x, including x ≤ 0.50, where both P and BM phases are highly stable. Under small compressive strain, the transformation threshold voltage decreases from approximately +2.7 V at x = 0 to negligible at x = 0.70. Both larger compressive strain and tensile strain induce further threshold voltage lowering, particularly at low x. The P → BM threshold voltage is thus tunable, via both composition and strain. At x = 0.50, voltage-controlled ferromagnetism, transport, and optical transmittance are then demonstrated, achieving Curie temperature and resistivity modulations of ∼220 K and at least 5 orders of magnitude, respectively, and enabling estimation of the voltage-dependent Co valence. The results are analyzed in the context of doping- and strain-dependent oxygen vacancy formation energies and diffusion coefficients, establishing that it is thermodynamic factors, not kinetics, that underpin the decrease in the threshold voltage with x, that is, with increasing formal Co valence. These findings substantially advance the practical and mechanistic understanding of this voltage-driven transformation, with fundamental and technological implications.

Emergence of superconductivity in the cuprates via a universal percolation process.

A pivotal step toward understanding unconventional superconductors would be to decipher how superconductivity emerges from the unusual normal state. In the cuprates, traces of superconducting pairing appear above the macroscopic transition temperature Tc, yet extensive investigation has led to disparate conclusions. The main difficulty has been to separate superconducting contributions from complex normal-state behaviour. Here we avoid this problem by measuring nonlinear conductivity, an observable that is zero in the normal state. We uncover for several representative cuprates that the nonlinear conductivity vanishes exponentially above Tc, both with temperature and magnetic field, and exhibits temperature-scaling characterized by a universal scale Ξ0. Attempts to model the response with standard Ginzburg-Landau theory are systematically unsuccessful. Instead, our findings are captured by a simple percolation model that also explains other properties of the cuprates. We thus resolve a long-standing conundrum by showing that the superconducting precursor in the cuprates is strongly affected by intrinsic inhomogeneity.

Dynamics of correlation-frozen antinodal quasiparticles in superconducting cuprates.

Many puzzling properties of high-critical temperature (Tc) superconducting (HTSC) copper oxides have deep roots in the nature of the antinodal quasiparticles, the elementary excitations with wave vector parallel to the Cu-O bonds. These electronic states are most affected by the onset of antiferromagnetic correlations and charge instabilities, and they host the maximum of the anisotropic superconducting gap and pseudogap. We use time-resolved extreme-ultraviolet photoemission with proper photon energy (18 eV) and time resolution (50 fs) to disclose the ultrafast dynamics of the antinodal states in a prototypical HTSC cuprate. After photoinducing a nonthermal charge redistribution within the Cu and O orbitals, we reveal a dramatic momentum-space differentiation of the transient electron dynamics. Whereas the nodal quasiparticle distribution is heated up as in a conventional metal, new quasiparticle states transiently emerge at the antinodes, similarly to what is expected for a photoexcited Mott insulator, where the frozen charges can be released by an impulsive excitation. This transient antinodal metallicity is mapped into the dynamics of the O-2p bands, thus directly demonstrating the intertwining between the low- and high-energy scales that is typical of correlated materials. Our results suggest that the correlation-driven freezing of the electrons moving along the Cu-O bonds, analogous to the Mott localization mechanism, constitutes the starting point for any model of high-Tc superconductivity and other exotic phases of HTSC cuprates.

Doping-dependent charge order correlations in electron-doped cuprates.

Understanding the interplay between charge order (CO) and other phenomena (for example, pseudogap, antiferromagnetism, and superconductivity) is one of the central questions in the cuprate high-temperature superconductors. The discovery that similar forms of CO exist in both hole- and electron-doped cuprates opened a path to determine what subset of the CO phenomenology is universal to all the cuprates. We use resonant x-ray scattering to measure the CO correlations in electron-doped cuprates (La2-x Ce x CuO4 and Nd2-x Ce x CuO4) and their relationship to antiferromagnetism, pseudogap, and superconductivity. Detailed measurements of Nd2-x Ce x CuO4 show that CO is present in the x = 0.059 to 0.166 range and that its doping-dependent wave vector is consistent with the separation between straight segments of the Fermi surface. The CO onset temperature is highest between x = 0.106 and 0.166 but decreases at lower doping levels, indicating that it is not tied to the appearance of antiferromagnetic correlations or the pseudogap. Near optimal doping, where the CO wave vector is also consistent with a previously observed phonon anomaly, measurements of the CO below and above the superconducting transition temperature, or in a magnetic field, show that the CO is insensitive to superconductivity. Overall, these findings indicate that, although verified in the electron-doped cuprates, material-dependent details determine whether the CO correlations acquire sufficient strength to compete for the ground state of the cuprates.

Revealing the high-energy electronic excitations underlying the onset of high-temperature superconductivity in cuprates.

In strongly correlated systems the electronic properties at the Fermi energy (E(F)) are intertwined with those at high-energy scales. One of the pivotal challenges in the field of high-temperature superconductivity (HTSC) is to understand whether and how the high-energy scale physics associated with Mott-like excitations (|E-E(F)|>1 eV) is involved in the condensate formation. Here, we report the interplay between the many-body high-energy CuO(2) excitations at 1.5 and 2 eV, and the onset of HTSC. This is revealed by a novel optical pump-supercontinuum-probe technique that provides access to the dynamics of the dielectric function in Bi(2)Sr(2)Ca(0.92)Y(0.08)Cu(2)O(8+δ) over an extended energy range, after the photoinduced suppression of the superconducting pairing. These results unveil an unconventional mechanism at the base of HTSC both below and above the optimal hole concentration required to attain the maximum critical temperature (T(c)).