We present a comparative study of magnetic excitations in the first two Ruddlesden-Popper members of the Hg-family of high-temperature superconducting cuprates, which are chemically nearly identical and have the highest critical temperature ($T_\mathrm{c}$) among all cuprate families. Our inelastic photon scattering experiments reveal that the two compounds' paramagnon spectra are nearly identical apart from an energy scale factor of $\sim130\%$ that matches the ratio of $T_\mathrm{c}$'s, as expected in magnetic Cooper pairing theories. By relating our observations to other cuprates, we infer that the strength of magnetic interactions determines how high $T_\mathrm{c}$ can reach. Our finding can be viewed as a magnetic analogue of the isotope effect, thus firmly supporting models of magnetically mediated high-temperature superconductivity.
We report the self-energy associated with RPA magnetic susceptibility in the hole-doped Bi_2Sr_2CuO_6 (Bi2201) and the electron-doped Nd_{2-x}Ce_xCuO_4 (NCCO) in the overdoped regime within the framework of a one-band Hubbard model. Strong weight is found in the magnetic spectrum around (pi, 0) at about 360 meV in Bi2201 and 640 meV in NCCO, which yields dispersion anomalies in accord with the recently observed `waterfall' effects in the cuprates.
Paramagnon softening upon doping in oxychloride cuprate superconductors
Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院）；Univ. Grenoble Alpes（格勒诺布尔阿尔卑斯大学）；CNRS（法国国家科学研究中心）；Grenoble INP（格勒诺布尔国立理工学院）；Institut Néel（奈尔研究所）；Sorbonne Université（索邦大学）；MNHN（法国国家自然历史博物馆）；IBM（国际商业机器公司）；Université de Strasbourg（斯特拉斯堡大学）；Institut de Physique et Chimie des Matériaux de Strasbourg（斯特拉斯堡材料物理与化学研究所）；Université de Sherbrooke（舍布鲁克大学）；Univ Rennes（雷恩大学）；Institut des Sciences Chimiques de Rennes（雷恩化学科学研究所）；Synchrotron SOLEIL（SOLEIL同步辐射装置）；European Synchrotron Radiation Facility (ESRF)（欧洲同步辐射装置（ESRF））
In the search for the mechanism of high-temperature superconductivity, intense research has been focused on the evolution of the spin excitation spectrum upon doping from the antiferromagnetic insulating to the superconducting states of the cuprates. Because of technical limitations, the experimental investigation of doped cuprates has been largely focused on low-energy excitations in a small range of momentum space. Here we use resonant inelastic x-ray scattering to show that a large family of superconductors, encompassing underdoped YBa$_2$Cu$_4$O$_8$ and overdoped YBa$_2$Cu$_3$O$_{7}$, exhi…
Recently, spin excitations in doped cuprates are measured using the resonant inelastic X-ray scattering (RIXS). The paramagnon dispersions show the large hardening effect in the electron-doped systems and seemingly doping-independence in the hole-doped systems, with the energy scales comparable to that of the antiferromagnetic magnons. This anomalous hardening effect was partially explained by using the strong coupling t-J model but with a three-site term(Nature communications 5, 3314 (2014)). However we show that hardening effect is a signature of strong coupling physics even without includin…
Ultrafast Two-Dimensional Spectroscopy Uncovers Ubiquitous Electron-Paramagnon Coupling in Cuprate Superconductors
Università Cattolica del Sacro Cuore（天主教神圣之心大学）；ILAMP (Interdisciplinary Laboratories for Advanced Materials Physics), Università Cattolica del Sacro Cuore（天主教神圣之心大学先进材料物理跨学科实验室）；KU Leuven（荷语鲁汶大学）；CNR-INO (National Institute of Optics)（意大利国家研究委员会光学研究所）；University of Brescia（布雷西亚大学）；“Sapienza” University of Rome（罗马第一大学）；Swinburne University of Technology（斯威本科技大学）
We show that low-energy spectral features in the cuprates can be separated into different components by the measurement of the recombination dynamics of different low-energy excitations in real-time using femtosecond laser spectroscopy. Quasiparticle (QP) recombination across the gap and intra-gap localized state relaxation processes exhibit qualitatively different time- and temperature-dependences. The relaxation measurements also show the existence of two distinct coexisting energy gaps near optimum doping and in the overdoped region, one more or less temperature independent (which exists ab…
We provide a unified interpretation of both paramagnon and plasmon modes in high-$T_c$ copper-oxides, and verify it quantitatively against available resonant inelastic $x$-ray scattering (RIXS) data across the hole-doped phase diagram. Three-dimensional extended Hubbard model, with included long-range Coulomb interactions and doping-independent microscopic parameters for both classes of quantum fluctuations, is used. Collective modes are studied using VWF+$1/\mathcal{N}_f$ approach which extends variational wave function (VWF) scheme by means of an expansion in inverse number of fermionic flav…
Resonant X-ray scattering experiments on high-temperature superconductors and related cuprates have revealed the presence of intense paramagnon scattering at high excitation energies, of the order of several hundred meV. The excitation energies appear to show very similar behavior across all compounds, ranging from magnetically ordered, via superconductors, to heavy fermion systems. However, we argue that this apparent behavior has been inferred from the data through model fitting which implicitly imposes such similarities. Using model fitting that is free from such restrictions, we show that …
Since the discovery of the high-T$_{c}$ cuprate superconductor La$_{2-x}$BaCuO$_{4}$ in 1986 by Bednorz and Müller, controversy regarding the nature or origin of this remarkable superconductivity has continued. However, d-wave superconductivity in the hole-doped cuprates, arising due to the anti-paramagnon exchange, was established around 1994. More recently we have shown that the mean field theory, like the BCS theory of superconductivity and Landau's Fermi liquid theory are adequate to describe the cuprates. The keys for this development are the facts that a)the pseudogap phase is d-wave den…
A microscopic theory of spin excitations in strongly-correlated electronic systems within the t-J model is discussed. An exact representation for the dynamic spin susceptibility is derived. In the normal state, the excitation spectrum reveals a crossover from spin-wave-like excitations at low doping to overdamped paramagnons above the optimal doping. At low temperatures, the resonance mode at the antiferromagnetic wave vector Q = π(1,1) emerges which is explained by a strong suppression of the spin excitation damping caused by a spin gap at Q rather than by opening of a superconducting gap. A …
Charge order has now been observed in several cuprate high-temperature superconductors. We report a resonant inelastic x-ray scattering experiment on the electron-doped cuprate Nd$_{2-x}$Ce$_{x}$CuO$_4$ that demonstrates the existence of dynamic correlations at the charge order wave vector. Upon cooling we observe a softening in the electronic response, which has been predicted to occur for a d-wave charge order in electron-doped cuprates. At low temperatures, the energy range of these excitations coincides with that of the dispersive magnetic modes known as paramagnons. Furthermore, measureme…
The charge and spin correlations in La$_{1.875}$Ba$_{0.125}$CuO$_4$ (LBCO 1/8) are studied using Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS). The static charge order (CO) is observed at a wavevector of $(0.24,0)$ and its charge nature confirmed by measuring the dependence of this peak on the incident x-ray polarization. The paramagnon excitation in LBCO 1/8 is then measured as it disperses through the CO wavevector. Within the experimental uncertainty no changes are observed in the paramagnon due to the static CO, and the paramagnon seems to be similar to that measured in other cu…
Using Cu-$L_3$ edge resonant inelastic x-ray scattering (RIXS) we measured the dispersion and damping of spin excitations (magnons and paramagnons) in the high-$T_\mathrm{c}$ superconductor (Bi,Pb)$_{2}$(Sr,La)$_{2}$CuO$_{6+δ}$ (Bi2201), for a large doping range across the phase diagram ($0.03\lesssim p\lesssim0.21$). Selected measurements with full polarization analysis unambiguously demonstrate the spin-flip character of these excitations, even in the overdoped sample. We find that the undamped frequencies increase slightly with doping for all accessible momenta, while the damping grows rapi…
The $t$-$J$-$U$ model of high-$T_c$ copper-oxide superconductors incorporates both the on-site Coulomb repulsion and kinetic exchange interaction and yields a semi-quantitative description of the static properties of those materials. We extend this analysis to dynamic quantities and address collective spin- and charge excitations in the correlated metallic state of the $t$-$J$-$U$ model. We employ VWF+$1/\mathcal{N}_f$ approach that combines the variational wave function (VWF) approach with the expansion in the inverse number of fermionic flavors ($1/\mathcal{N}_f$). It is shown that the reson…
The organizers of the Memorial Session for Herman Rietschel asked that I review some of the history of the interplay of superconductivity and spin fluctuations. Initially, Berk and Schrieffer showed how paramagnon spin fluctuations could suppress superconductivity in nearly-ferromagnetic materials. Following this, Rietschel and various co-workers wrote a number of papers in which they investigated the role of spin fluctuations in reducing the T_c of various electron-phonon superconductors. Paramagnon spin fluctuations are also believed to provide the p-wave pairing mechanism responsible for th…
The Fermi energy, Ef of newly discovered high-Tc superconductor MgB2 and cuprates is estimated from the measured London penetration depth using a parameter-free expression. Ef of MgB2 and more than 30 lanthanum, yttrium and mercury-based cuprates appears to be about or below 100 meV, depending on doping. There is every evidence that the remarkable low value of Ef and the strong coupling of carriers with high-frequency phonons is the cause of high Tc in all newly discovered superconductors. Taking into account that the carriers mainly reside on oxygen in cuprates, on boron in magnesium diborade…
A parameter-free expression for the superconducting critical temperature of layered cuprates is derived which allows us to express Tc in terms of experimentally measured parameters. It yields Tc values observed in about 30 lanthanum, yttrium and mercury-based samples for different levels of doping. This remarkable agreement with the experiment as well as the unusual critical behaviour and the normal-state gap indicate that many cuprates are close to the Bose-Einstein condensation regime.
Despite decades of search for the pairing boson in cuprate high-Tc superconductors, its identity still remains debated to date. For this reason, spectroscopic signatures of electron-boson interactions in cuprates have always been a center of attention. For example, the kinks in the quasiparticle dispersion observed by angle-resolved photoemission spectroscopy (ARPES) studies have motivated a decade-long investigation of electron-phonon as well as electron-paramagnon interactions in cuprates. On the other hand, the overlap between the charge-order correlations and the pseudogap in the cuprate p…
The cuprate high temperature superconductors exhibit a pronounced trend in which the superconducting transition temperature, $T_{\rm c}$, increases with the number of CuO$_2$ planes, $n$, in the crystal structure. We compare the magnetic excitation spectrum of Bi$_{2+x}$Sr$_{2-x}$CuO$_{6+δ}$ (Bi-2201) and Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10 + δ}$ (Bi-2223), with $n=1$ and $n=3$ respectively, using Cu $L_3$-edge resonant inelastic x-ray scattering (RIXS). Near the anti-nodal zone boundary we find the paramagnon energy in Bi-2223 is substantially higher than that in Bi-2201, indicating that multilaye…
We consider the Pseudo-Gap (PG) state of high-$T_c$ superconductors in form of a composite order parameter fluctuating between 2$p_F$-charge ordering and superconducting (SC) pairing. In the limit of linear dispersion and at the hotspots, both order parameters are related by a SU(2) symmetry and the eight hotspot model of Efetov $\textit{et al.}$ [Nat. Phys. $\bf{9}$, 442 (2013)] is recovered. In the general case however, curvature terms of the dispersion will break this symmetry and the degeneracy between both states is lifted. Taking the full momentum dependence of the order parameter into a…
We have performed neutron inelastic scattering and resonant inelastic X-ray scattering (RIXS) at the Cu-$L_3$ edge to study high-energy magnetic excitations at energy transfers of more than 100 meV for overdoped La$_{2-x}$Sr$_{x}$CuO$_{4}$ with $x=0.25$ ($T_c=15$ K) and $x=0.30$ (non-superconducting) using identical single crystal samples for the two techniques. From constant-energy slices of neutron scattering cross-sections, we have identified magnetic excitations up to ~250 meV for $x=0.25$. Although the width in the momentum direction is large, the peak positions along the (pi, pi) directi…
Magnetic fluctuations is the leading candidate for pairing in cuprate, iron-based and heavy fermion superconductors. This view is challenged by the recent discovery of nodeless superconductivity in CeCu$_2$Si$_2$, and calls for a detailed understanding of the corresponding magnetic fluctuations. Here, we mapped out the magnetic excitations in \ys{superconducting (S-type)} CeCu$_2$Si$_2$ using inelastic neutron scattering, finding a strongly asymmetric dispersion for $E\lesssim1.5$~meV, which at higher energies evolve into broad columnar magnetic excitations that extend to $E\gtrsim 5$ meV. Whi…
We report an original procedure for the elaboration of very high quality single crystals of superconducting HgBa2Ca2Cu3O8+δ mercury cuprates. These single crystals are unique with very high quality surface paving the way for spectroscopic, transport and thermodynamic probes in order to understand the hole-doped cuprate phase diagram. The superconductivity transition width of about 2 K indicates they are homogeneous. Annealing allows to optimize Tc up to Tc$^{max}$ = 133 K. We show for the first time that with adequate heat treatment, Hg-1223 can be largely under-doped and its doping level cont…
The evolution of electronic (spin and charge) excitations upon carrier doping is an extremely important issue in superconducting layered cuprates and the knowledge of its asymmetry between electron- and hole-dopings is still fragmentary. Here we combine x-ray and neutron inelastic scattering measurements to track the doping dependence of both spin and charge excitations in electron-doped materials. Copper L3 resonant inelastic x-ray scattering spectra show that magnetic excitations shift to higher energy upon doping. Their dispersion becomes steeper near the magnetic zone center and deeply mix…
We report a comprehensive study of magnetic correlations in LaNiO$_{2}$, a parent compound of the recently discovered family of infinite-layer (IL) nickelate superconductors, using multiple experimental and theoretical methods. Our specific heat, muon-spin rotation ($μ$SR), and magnetic susceptibility measurements on polycrystalline LaNiO$_{2}$ show that long-range magnetic order remains absent down to 2 K. Nevertheless, we detect residual entropy in the low-temperature specific heat, which is compatible with a model fit that includes paramagnon excitations. The $μ$SR and low-field static and …
Unveiling the Interplay of Charge and Magnetic Excitations in HgBa$_2$Ca$_2$Cu$_3$O$_{8+δ}$
Chalmers University of Technology（查尔姆斯理工大学）；Politecnico di Milano（米兰理工大学）；ESRF, The European Synchrotron（欧洲同步辐射装置）；CEA Saclay（法国原子能和替代能源委员会萨克雷中心）；Université Paris Cité（巴黎西岱大学）；BTU Cottbus-Senftenberg（科特布斯-森夫滕贝格勃兰登堡工业大学）
Magnetic excitations in the optimally doped high-$T_\mathrm{c}$ superconductor Bi$_{1.5}$Pb$_{0.55}$Sr$_{1.6}$La$_{0.4}$CuO$_{6+δ}$ (OP-Bi2201, $T_\mathrm{c}\simeq 34$ K) are investigated by Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS), below and above the pseudogap opening temperature. At both temperatures the broad spectral distribution disperses along the (1,0) direction up to $\sim$350~meV at zone boundary, similarly to other hole-doped cuprates. However, above $\sim$0.22 reciprocal lattice units, we observe a concurrent intensity decrease for magnetic excitations and quasi-ela…
Superconductivity was discovered in 1911 by Kamerlingh Onnes and Holst in mercury at the temperature of liquid helium (4.2 K). It took almost 50 years until in 1957 a microscopic theory of superconductivity, the so-called BCS theory, was developed. Since the discovery a number of superconducting materials were found with transition temperatures up to 23 K. A breakthrough in the field happened in 1986 when Bednorz and Müller discovered a new class of superconductors, the so-called cuprate high-temperature superconductors with transition temperatures as high as 135 K. This surprising discovery i…
