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Angle-resolved photoemission spectroscopy, visualizing the superconducting gap in k-space, plays a pivotal role in research on cuprates and other high-Tc superconducting materials. However, there has always been an imminent doubt whether this technique truly represents the intrinsic bulk spectral function, whose response can be distorted by energy- and k-dependence of the photoexcitation matrix element, and by a small photoelectron escape depth of few surface atomic layers. Here, we address this fundamental question with soft-X-ray photoemission measurements of the superconducting gap in the paradigm high-Tc cuprate Bi2Sr2CaCu2O8. We vary the matrix element by spanning a dense k-space grid, formed by the lattice superstructure, and the probing depth by changing the emission angle. The measured gap appears independent of the matrix element effects, probing depth or photoexcitation energy. This fact proves the relevance of photoemission studies for the bulk superconductivity in Bi2Sr2CaCu2O8, and calls for similar verification experiments on other high-Tc compounds, in particular more three-dimensional ones. Bi2Sr2CaCu2O8 shows an anomalously fast decay of the coherent spectral weight with photon energy, tracing back to strong electron–phonon interaction or relaxation of the lattice coherence.

Cuprate superconductors have long been thought of as having strong electronic correlations but negligible spin-orbit coupling. Using spin- and angle-resolved photoemission spectroscopy, we discovered that one of the most studied cuprate superconductors, Bi2212, has a nontrivial spin texture with a spin-momentum locking that circles the Brillouin zone center and a spin-layer locking that allows states of opposite spin to be localized in different parts of the unit cell. Our findings pose challenges for the vast majority of models of cuprates, such as the Hubbard model and its variants, where spin-orbit interaction has been mostly neglected, and open the intriguing question of how the high-temperature superconducting state emerges in the presence of this nontrivial spin texture.

Many puzzling properties of high-critical temperature (T-c) 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-T-c superconductivity and other exotic phases of HTSC cuprates.

Cuprate superconductors have long been thought of as having strong electronic correlations but negligible spin-orbit coupling. Using spin- and angle-resolved photoemission spectroscopy, we discovered that one of the most studied cuprate superconductors, Bi2212, has a nontrivial spin texture with a spin-momentum locking that circles the Brillouin zone center and a spin-layer locking that allows states of opposite spin to be localized in different parts of the unit cell. Our findings pose challenges for the vast majority of models of cuprates, such as the Hubbard model and its variants, where spin-orbit interaction has been mostly neglected, and open the intriguing question of how the high-temperature superconducting state emerges in the presence of this nontrivial spin texture.

Many puzzling properties of high-critical temperature (T-c) 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-T-c superconductivity and other exotic phases of HTSC 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 non-thermal 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.

One of the pivotal questions in the physics of high-temperature superconductors is whether the low-energy dynamics of the charge carriers is mediated by bosons with a characteristic timescale. This issue has remained elusive as electronic correlations are expected to greatly accelerate the electron–boson scattering processes, confining them to the very femtosecond timescale that is hard to access even with state-of-the-art ultrafast techniques. Here we simultaneously push the time resolution and frequency range of transient reflectivity measurements up to an unprecedented level, enabling us to directly observe the ∼16 fs build-up of the effective electron–boson interaction in hole-doped copper oxides. This extremely fast timescale is in agreement with numerical calculations based on the t–J model and the repulsive Hubbard model, in which the relaxation of the photo-excited charges is achieved via inelastic scattering with short-range antiferromagnetic excitations.

この論文は国立情報学研究所の電子図書館事業により電子化されました。

この論文は国立情報学研究所の電子図書館事業により電子化されました。

この論文は国立情報学研究所の電子図書館事業により電子化されました。

この論文は国立情報学研究所の電子図書館事業により電子化されました。

この論文は国立情報学研究所の電子図書館事業により電子化されました。

この論文は国立情報学研究所の電子図書館事業により電子化されました。

In strongly correlated materials the electronic and optical properties are significantly affected by the coupling of fermionic quasiparticles to different degrees of freedom, such as lattice vibrations and bosonic excitations of electronic origin. Broadband ultrafast spectroscopy is emerging as the premier technique to unravel the subtle interplay between quasiparticles and electronic or phononic collective excitations, by their different characteristic timescales and spectral responses. By investigating the femtosecond dynamics of the optical properties of Y-Bi2212)crystals over the 0.5-2 eV energy range, we disentangle the electronic and phononic contributions to the generalized electron-boson Eliashberg function, showing that the spectral distribution of the electronic excitations, such as spin fluctuations and current loops, and the strength of their interaction with quasiparticles can account for the high critical temperature of the superconducting phase transition [5]. Finally, we discuss how the use of this technique can be extended to the underdoped region of the phase diagram of cuprates, in which a pseudogap in the quasiparticle density of states opens. The microscopic modeling of the interaction of ultrashort light pulses with unconventional superconductors will be one of the key challenges of the next-years materials science, eventually leading to the full understanding of the role of the electronic correlations in controlling the dynamics on the femtosecond timescale.

In strongly correlated materials the electronic and optical properties are significantly affected by the coupling of fermionic quasiparticles to different degrees of freedom, such as lattice vibrations and bosonic excitations of electronic origin. Broadband ultrafast spectroscopy is emerging as the premier technique to unravel the subtle interplay between quasiparticles and electronic or phononic collective excitations, by their different characteristic timescales and spectral responses. By investigating the femtosecond dynamics of the optical properties of Y-Bi2212)crystals over the 0.5-2 eV energy range, we disentangle the electronic and phononic contributions to the generalized electron-boson Eliashberg function, showing that the spectral distribution of the electronic excitations, such as spin fluctuations and current loops, and the strength of their interaction with quasiparticles can account for the high critical temperature of the superconducting phase transition [5]. Finally, we discuss how the use of this technique can be extended to the underdoped region of the phase diagram of cuprates, in which a pseudogap in the quasiparticle density of states opens. The microscopic modeling of the interaction of ultrashort light pulses with unconventional superconductors will be one of the key challenges of the next-years materials science, eventually leading to the full understanding of the role of the electronic correlations in controlling the dynamics on the femtosecond timescale.

Ultrafast broadband transient reflectivity experiments are performed to study the interplay between the non-equilibrium dynamics of the pseudogap and the superconducting phases in Y-Bi2212. Once superconductivity is established the relaxation of the pseudogap proceeds 2 times faster than in the normal state, and the corresponding transient reflectivity variation changes sign after 0.5 ps. The results can be described by a set of coupled differential equations for the pseudogap and for the superconducting order parameter. The sign and strength of the coupling term suggest a remarkably weak competition between the two phases, allowing their coexistence.

Here we report extensive ultrafast time-resolved reflectivity experiments on overdoped Y-Bi2212 single crystals (Tc=78 K) aimed to clarify the nature of the superconducting-to-normal-state photoinduced phase transition. The experimental data show the lack of the quasiparticles decay time divergence at the fluence required to induce this phase transition, in contrast to the thermally-driven phase transition observed at Tc and at variance with recently reported photoinduced charge-density-wave and spin-density-wave to metal phase transitions. Our data demonstrate the non-thermal character of the superconducting-to-normal-state photoinduced phase transition. The data have been analyzed using an ad-hoc developed timedependent Rothwarf-Taylor model, opening the question on the order of this non-equilibrium phase transition.

In strongly-correlated systems the electronic properties at the Fermi energy (EF) 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-EF|>1 eV) is involved in the condensate formation. Here we show the interplay between the many-body high-energy CuO2 excitations at 1.5 and 2 eV and the onset of HTSC. This is revealed by a novel optical pump supercontinuum-probe technique, which provides access to the dynamics of the dielectric function in Y-Bi2212 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 (Tc).

type:text, Low energy ultrahigh momentum resolution angle resolved photoemission spectroscopy study on four-layer self-doped high T-c superconductor Ba2Ca3Cu4O8F2 (F0234) revealed fine structure in the band dispersion, identifying the unconventional association of hole and electron doping with the inner and outer CuO2 layers, respectively. For the states originating from two inequivalent CuO2 layers, different energy scales are observed in dispersion kinks associated with the collective mode coupling, with the larger energy scale found in the electron (n-) doped state which also has stronger coupling strength. Given the earlier finding that the superconducting gap is substantially larger along the n-type Fermi surface, our observations connect the mode coupling energy and strength with magnitude of the pairing gap.

Low energy ultrahigh momentum resolution angle resolved photoemission spectroscopy study on four-layer self-doped high T-c superconductor Ba2Ca3Cu4O8F2 (F0234) revealed fine structure in the band dispersion, identifying the unconventional association of hole and electron doping with the inner and outer CuO2 layers, respectively. For the states originating from two inequivalent CuO2 layers, different energy scales are observed in dispersion kinks associated with the collective mode coupling, with the larger energy scale found in the electron (n-) doped state which also has stronger coupling strength. Given the earlier finding that the superconducting gap is substantially larger along the n-type Fermi surface, our observations connect the mode coupling energy and strength with magnitude of the pairing gap.

Low energy ultrahigh momentum resolution angle resolved photoemission spectroscopy study on four-layer self-doped high T-c superconductor Ba2Ca3Cu4O8F2 (F0234) revealed fine structure in the band dispersion, identifying the unconventional association of hole and electron doping with the inner and outer CuO2 layers, respectively. For the states originating from two inequivalent CuO2 layers, different energy scales are observed in dispersion kinks associated with the collective mode coupling, with the larger energy scale found in the electron (n-) doped state which also has stronger coupling strength. Given the earlier finding that the superconducting gap is substantially larger along the n-type Fermi surface, our observations connect the mode coupling energy and strength with magnitude of the pairing gap.

Low energy ultrahigh momentum resolution angle resolved photoemission spectroscopy study on four-layer self-doped high T-c superconductor Ba2Ca3Cu4O8F2 (F0234) revealed fine structure in the band dispersion, identifying the unconventional association of hole and electron doping with the inner and outer CuO2 layers, respectively. For the states originating from two inequivalent CuO2 layers, different energy scales are observed in dispersion kinks associated with the collective mode coupling, with the larger energy scale found in the electron (n-) doped state which also has stronger coupling strength. Given the earlier finding that the superconducting gap is substantially larger along the n-type Fermi surface, our observations connect the mode coupling energy and strength with magnitude of the pairing gap.