The specific heat $C$ of the single-layer cuprate superconductor HgBa$_2$CuO$_{4 + δ}$ was measured in an underdoped crystal with $T_{\rm c} = 72$ K at temperatures down to $2$ K in magnetic fields up to $35$ T, a field large enough to suppress superconductivity at that doping ($p \simeq 0.09$). In the normal state at $H = 35$ T, a residual linear term of magnitude $γ= 12 \pm 2$ mJ/K$^2$mol is observed in $C/T$ as $T \to 0$, a direct measure of the electronic density of states. This high value of $γ$ has two major implications. First, it is significantly larger than the value measured in overdoped cuprates outside the pseudogap phase ($p >p^\star$), such as La$_{2-x}$Sr$_x$CuO$_4$ and Tl$_2$Ba$_2$CuO$_{6 + δ}$ at $p \simeq 0.3$, where $γ\simeq 7$ mJ/K$^2$mol. Given that the pseudogap causes a loss of density of states, and assuming that HgBa$_2$CuO$_{4 + δ}$ has the same $γ$ value as other cuprates at $p \simeq 0.3$, this implies that $γ$ in HgBa$_2$CuO$_{4 + δ}$ must peak between $p \simeq 0.09$ and $p \simeq 0.3$, namely at (or near) the critical doping $p^\star$ where the pseudogap phase is expected to end ($p^\star\simeq 0.2$). Secondly, the high $γ$ value implies that the Fermi surface must consist of more than the single electron-like pocket detected by quantum oscillations in HgBa$_2$CuO$_{4 + δ}$ at $p \simeq 0.09$, whose effective mass $m^\star= 2.7\times m_0$ yields only $γ= 4.0$ mJ/K$^2$mol. This missing mass imposes a revision of the current scenario for how pseudogap and charge order respectively transform and reconstruct the Fermi surface of cuprates.
Using resonant X-ray diffraction and Raman spectroscopy, we study charge correlations and lattice dynamics in two model cuprates, HgBa$_{2}$CuO$_{4+δ}$ and HgBa$_{2}$CaCu$_{2}$O$_{6+δ}$. We observe a maximum of the characteristic charge order temperature around the same hole concentration ($p \approx 0.09$) in both compounds, and concomitant pronounced anomalies in the lattice dynamics that involve the motion of atoms in and/or adjacent to the CuO$_2$ layers. These anomalies are already present at room temperature, and therefore precede the formation of the static charge correlations, and we a…
The magnitude of the powder spin susceptibility of an optimally doped superconductor HgBa$_2$CuO$_{4+δ}$ (Hg1201) in the normal state is found to be nearly the same as that of La$_{2-x}$Sr$_{x}$CuO$_{4}$ near the optimally doped level. The Stoner enhancement factor of Hg1201 is larger than that of La$_{2-x}$Sr$_{x}$CuO$_{4}$. The magnitude correlation of the Stoner enhancement factor is inconsistent with the effect of the recent theoretical Coulomb repulsion between 3$d$ electrons and that of the superexchange intereraction of a charge transfer type.
Antiferromagnetic correlations have been argued to be the cause of the d-wave superconductivity and the pseudogap phenomena exhibited by the cuprates. Although the antiferromagnetic response in the pseudogap state has been reported for a number of compounds, there exists no information for structurally simple HgBa$_2$CuO$_{4+δ}$. Here we report neutron scattering results for HgBa$_2$CuO$_{4+δ}$ (superconducting transition temperature T$_c$ $\sim$ 71 K, pseudogap temperature T* $\sim$ 305 K) that demonstrate the absence of the two most prominent features of the magnetic excitation spectrum of t…
We report the transverse relaxation rates 1/$T_2$'s of the $^{63}$Cu nuclear spin-echo envelope for double-layer high-$T_c$ cuprate superconductors HgBa$_{2}$CaCu$_{2}$O$_{6+d}$ from underdoped to overdoped. The relaxation rate 1/$T_{2L}$ of the exponential function (Lorentzian component) shows a peak at 220$-$240 K in the underdoped ($T_c$ = 103 K) and the optimally doped ($T_c$ = 127 K) samples but no peak in the overdoped ($T_c$ = 93 K) sample. The enhancement in 1/$T_{2L}$ suggests development of the zero frequency components of local field fluctuations. Ultraslow fluctuations are hidden i…
The pseudogap phenomenon in cuprates is the most mysterious puzzle in the research of high-temperature superconductivity. In particular, whether the pseudogap is associated with a crossover or phase transition has been a long-standing controversial issue. The tetragonal cuprate HgBa$_2$CuO$_{4+δ}$, with only one CuO$_2$ layer per primitive cell, is an ideal system to tackle this puzzle. Here, we measure the anisotropy of magnetic susceptibility within the CuO$_2$ plane with exceptionally high-precision magnetic torque experiments. Our key finding is that a distinct two-fold in-plane anisotropy…
We develop a model for the angle-dependent magnetoresistance of HgBa$_2$CuO$_{4+δ}$ in the underdoped regime where the Fermi surface is thought to be reconstructed by an ordered state such as a charge density wave. We show that such measurements can be employed to unambiguously distinguish the form of the Fermi surface's interlayer warping, placing severe contraints on the symmetry and nature of the reconstructing order. We describe experimentally accessible conditions in which our calculations can be put to the test.
Anomalously high quasiparticle thermal conductivity in the underdoped cuprate superconductor HgBa$_{2}$CuO$_{4+δ}$
Université de Sherbrooke（舍布鲁克大学）；CEA Saclay（法国原子能和替代能源委员会萨克莱中心）；CNRS UPR3228, Univ. Grenoble Alpes, Univ. Toulouse, INSA-T（法国国家科学研究中心、格勒诺布尔阿尔卑斯大学、图卢兹大学）；IRL Frontières Quantiques, Université de Sherbrooke–CNRS（量子前沿研究所，舍布鲁克大学-法国国家科学研究中心）；Canadian Institute for Advanced Research（加拿大高级研究院）
The cuprates exhibit a prominent charge-density-wave (CDW) instability with wavevector along [100], i.e., the Cu-O bond direction. Whereas CDW order is most prominent at moderate doping and low temperature, there exists increasing evidence for dynamic charge correlations throughout a large portion of the temperature-doping phase diagram. In particular, signatures of incipient charge order have been observed as phonon softening and/or broadening near the CDW wavevector approximately half-way through the Brillouin zone. Most of this work has focused on moderately-doped cuprates, for which the CD…
Novel nanoscale probes are opening new venues for understanding unconventional electronic and magnetic functionalities driven by multiscale lattice complexity in doped high temperature superconducting perovskites. In this work we focus on the multiscale texture at supramolecular level of atomic oxygen interstitials (O-i) stripes in HgBa$_2$CuO$_{4+y}$ at optimal doping for the highest superconducting critical temperature $T_C$=94K. We report compelling evidence for the nematic phase of oxygen-interstitial O-i atomic wires with fractal-like spatial distribution over multiple scales by using sca…
We use neutron scattering to study magnetic excitations near the antiferromagnetic wave vector in the underdoped single-layer cuprate HgBa2CuO4+δ (superconducting transition temperature Tc ~ 88 K, pseudogap temperature T* ~ 220 K). The response is distinctly enhanced below T* and exhibits a Y-shaped dispersion in the pseudogap state, whereas the superconducting state features an X-shaped (hourglass) dispersion and a further resonance-like enhancement. A large spin gap of about 40 meV is observed in both states. This phenomenology is reminiscent of that exhibited by bilayer cuprates. The resona…
Various forms of spin and charge ordering have been identified in a wide range of cuprate superconducting materials, but whether these behaviors are ubiquitous phenomena is not established. In this work we focus on one of the simplest compounds, HgBa$_{2}$CuO$_{4+δ}$ (Hg1201), a superconductor with a high transition temperature, 97 K, having only a single layer and tetragonal structure, in contrast to one of the most extensively studied materials, YBa$_{2}$Cu$_{3}$O$_{6+y}$ (Y123). Using nuclear magnetic resonance we have discovered a coherent spatial modulation of both spin and charge that is…
While recent experiments have found that at optimum doping for the highest critical temperature in HgBa$_2$CuO$_{4+y}$ (Hg1201) the oxygen interstitials (O-i) are not homogeneously distributed but form one-dimensional atomic wires, there are no available information of its electronic structure considering self-organized O-i atomic wires. Here we report the calculated electronic structure of HgBa$_2$CuO$_{4+y}$ where oxygen interstitials form atomic wires along (1,0,0) crystal direction in the Hg layer. We find that at optimum doping for superconductivity the chemical potential is tuned near an…
We present an extensive study of vortex dynamics in a high-quality single crystal of HgBa$_2$CuO$_{4+δ}$ (Hg1201), a highly anisotropic superconductor that is a model system for studying the effects of anisotropy. From magnetization $M$ measurements over a wide range of temperatures $T$ and fields $H$, we construct a detailed vortex phase diagram. We find that the temperature-dependent vortex penetration field $H_p(T)$, second magnetization peak $H_{smp}(T)$, and irreversibility field $H_{irr}(T)$ all decay exponentially at low temperatures and exhibit an abrupt change in behavior at high temp…
We study the spin dynamics of the Resonant Excitonic State (RES) proposed, within the theory of an emergent SU(2) symmetry, to explain some properties of the pseudo-gap phase of cuprate superconductors. The RES can be described as a proliferation of particle-hole patches with an internal modulated structure. We model the RES modes as a charge order with multiple $2{\bf {p}}_{\text{F}}$ ordering vectors, where $2{\bf {p}}_{\text{F}}$ connects two opposite side of the Fermi surface. This simple modelization enables us to propose a comprehensive study of the collective mode observed at the antife…
Polarized-neutron diffraction experiments (PND) have revealed that the pseudogap state of the cuprates exhibits unusual intra-unit-cell (IUC) magnetism. At a qualitative level, the data indicate a moment direction that is neither perpendicular nor parallel to the CuO2 layers, yet an accurate measurement of a structurally simple compound has been lacking. Here we report PND results with unprecedented accuracy for the IUC magnetic order in the simple-tetragonal single-CuO$_2$-layer compound HgBa2CuO$_{4+δ}$. At the transition temperature, we find evidence for magnetic critical scattering. Deep i…
Two pseudogaps with different energy scales at the antinode of the high-temperature Bi$_2$Sr$_2$CuO$_6$ superconductor using angle-resolved photoemission spectroscopy
我们已经进行了高分辨率角分辨光电子能谱的单层铜酸盐Bi $_2$ Sr $_2$ CuO $_6$澄清的赝能隙的起源。通过使用不同的光子能量，我们已经成功地直接观察到两个不同的赝能隙与两个不同的能量尺度共存的波腹区域：一个反映了$d_{x^2-y^2}$波配对强度，而另一个具有较大的能量尺度，表明起源不同于超导。观察到的双赝能隙行为提供了一个关键，以充分理解赝能隙现象的铜酸盐。
We present a detailed synchrotron x-ray scattering study of the charge-density-wave (CDW) order in simple tetragonal HgBa$_2$CuO$_{4+δ}$ (Hg1201). Resonant soft x-ray scattering measurements reveal that short-range order appears at a temperature that is distinctly lower than the pseudogap temperature and in excellent agreement with a prior transient reflectivity result. Despite considerable structural differences between Hg1201 and YBa$_2$Cu$_3$O$_{6+δ}$, the CDW correlations exhibit similar doping dependencies, and we demonstrate a universal relationship between the CDW wave vector and the si…
We report the successful synthesis of single-crystalline cuprate superconductors HgBa$_{2}$CaCu$_{2}$O$_{6+δ}$ and HgBa$_{2}$Ca$_{2}$Cu$_{3}$O$_{8+δ}$. These compounds are well-known for their high optimal superconducting critical temperatures of $T_\mathrm{c}$ = 128 K and 134 K at ambient pressure, respectively, and for their challenging synthesis. Using a conventional quartz-tube encapsulation method and a two-layer encapsulation method that utilizes custom-built high-pressure furnaces, we are able to grow single crystals with linear dimensions up to several millimeters parallel to the CuO$_…
We studied local magnetic properties of triple-CuO$_2$-layer superconductors HgBa$_2$Ca$_2$Cu$_3$O$_{8+δ}$ with rich $^{63}$Cu isotope (underdoped $T_\mathrm{c}$ = 124 K and optimally doped $T_\mathrm{c}$ = 134 K) by $^{63}$Cu NMR spin-echo techniques. The temperature dependences of the $^{63}$Cu nuclear spin-lattice relaxation rate $^{63}$(1/$T_1$) and the spin Knight shift $^{63}K_\mathrm{spin}$ of the inner plane Cu(1) site were nearly the same as those of the outer plane Cu(2) site in the normal states. The pseudogap temperature $T^*$ defined as the maximum temperature of $^{63}$(1/$T_1T$)…
The lamellar cuprate superconductors exhibit the highest ambient-pressure superconducting transition temperatures (T$_C$) and, after more than three decades of extraordinary research activity, continue to pose formidable scientific challenges. A major experimental obstacle has been to distinguish universal phenomena from materials- or technique-dependent ones. Angle-resolved photoemission spectroscopy (ARPES) measures momentum-dependent single-particle electronic excitations and has been invaluable in the endeavor to determine the anisotropic momentum-space properties of the cuprates. HgBa$_2$…
Measurements of the $^{17}$O nuclear magnetic resonance (NMR) quadrupolar spectrum of apical oxygen in HgBa$_{2}$CuO$_{4+δ}$ were performed over a range of magnetic fields from 6.4 to 30\,T in the superconducting state. Oxygen isotope exchanged single crystals were investigated with doping corresponding to superconducting transition temperatures from 74\,K underdoped, to 78\,K overdoped. The apical oxygen site was chosen since its NMR spectrum has narrow quadrupolar satellites that are well separated from any other resonance. Non-vortex contributions to the spectra can be deconvolved in the ti…
In type-II superconductors exposed to magnetic fields between upper and lower critical values, $H_{c1}$ and $H_{c2}$, penetrating magnetic flux forms a lattice of vortices whose motion can induce dissipation. Consequently, the magnetization $M$ of superconductors is typically progressively weakened with increasing magnetic field $B \propto n_v$ (for vortex density $n_v$). However, some materials exhibit a non-monotonic $M(B)$, presenting a maximum in $M$ at what is known as the second magnetization peak. This phenomenon appears in most classes of superconductors, including low $T_c$ materials,…
Superconductivity studied by solving ab initio low-energy effective Hamiltonians for carrier doped CaCuO$_2$, Bi$_2$Sr$_2$CuO$_6$, Bi$_2$Sr$_2$CaCu$_2$O$_8$, and HgBa$_2$CuO$_4$
Observation of vortices and hidden pseudogap from scanning tunneling spectroscopic studies of electron-doped cuprate superconductor $Sr_{0.9}La_{0.1}CuO_2$
Superconductivity distorted by the coexisting pseudogap in the antinodal region of Bi$_{1.5}$Pb$_{0.55}$Sr$_{1.6}$La$_{0.4}$CuO$_{6+δ}$: A photon-energy-dependent angle-resolved photoemission study
超导电性和赝能隙之间的相互作用是铜氧化物物理的一个重要方面。然而，赝能隙的性质仍然存在争议，部分原因是不同的实验提出了不同的能隙函数。本文采用光子能量依赖角分辨光电子能谱（ARPES）研究了Bi $_{1.5}$ Pb $_{0.55}$ Sr $_{1.6}$ La $_{0.4}$ CuO $_{6+δ}$ .我们发现，在低光子能量的反节ARPES谱是由背景信号，这可能会导致一个错误的评估的光谱间隙的大小占主导地位。一旦背景是适当的占，独立的光子能量，在不同的能量下，主要归因于赝能隙和超导性，以及偏离一个简单的d-波形式的整体光谱间隙的波腹光谱鲁棒地显示两个共存的功能。这些结果支持了赝能隙和超导性之间的竞争导致能隙畸变的观点。
The charge-density-wave (CDW) instability in the underdoped, pseudogap part of the cuprate phase diagram has been a major recent research focus, yet measurements of dynamic, energy-resolved CDW correlations are still in their infancy. We report a high-resolution resonant inelastic X-ray scattering (RIXS) study of the underdoped cuprate superconductor HgBa$_{2}$CuO$_{4+δ}$ ($T_c = 70$ K). At $T=250$ K, above the CDW order temperature $T_\mathrm{CDW} \approx 200$ K, we observe significant dynamic CDW correlations at about 40 meV. This energy scale is comparable to both the superconducting gap an…
Multilayered cuprates possess not only the highest superconducting temperature transition but also offer a unique platform to study disorder-free CuO$_2$ planes and the interplay between competing orders with superconductivity. Here, we study the underdoped trilayer cuprate HgBa$_2$Ca$_2$Cu$_3$O$_{8+ δ}$ and we report the first quantum oscillation and Hall effect measurements in magnetic field up to 88 T. A careful analysis of the complex spectra of quantum oscillations strongly supports the coexistence of an antiferromagnetic order in the inner plane and a charge order in the outer planes. Th…
Thermopower across the pseudogap critical point of La(1.6-x)Nd(0.4)Sr(x)CuO(4): Evidence for a quantum critical point in a hole-doped high-Tc superconductor
Monotonic d-wave Superconducting Gap in Optimally-Doped Bi$_2$Sr$_{1.6}$La$_{0.4}$CuO$_6$ Superconductor by Laser-Based Angle-Resolved Photoemission Spectroscopy
利用超高分辨激光角分辨光电子能谱研究了最佳掺杂Bi $_2$ Sr $_{1.6}$ La $_{0.4}$ CuO $_6$超导体的超导能隙和赝能隙随动量和温度的变化关系。在超导状态下测得的能隙表现出标准的{ \it d}-波形。赝能隙在T $_c$以上的费米面的很大一部分打开，在结区附近形成“费米弧”。在“费米弧”以外的区域，赝能隙具有与超导态类似的能隙大小和动量依赖性，能隙随温度变化很小，在T_PDMATHABMR上没有突变。这些观测结果表明赝能隙和超导能隙是密切相关的，并支持赝能隙是超导能隙的先驱的观点。
The specific heat $C$ of the cuprate superconductors La$_{2-x}$Sr$_x$CuO$_4$ and Bi$_{2+y}$Sr$_{2-x-y}$La$_x$CuO$_{6+δ}$ was measured at low temperature (down to $0.5~{\rm K}$), for dopings $p$ close to $p^\star$, the critical doping for the onset of the pseudogap phase. A magnetic field up to $35~{\rm T}$ was applied to suppress superconductivity, giving direct access to the normal state at low temperature, and enabling a determination of $C_e$, the electronic contribution to the normal-state specific heat, at $T \to 0$. In La$_{2-x}$Sr$_x$CuO$_4$ at $x=p = 0.22$, $0.24$ and $0.25$, $C_e / T …
We report thermopower measurements under hydrostatic pressure on the cuprate superconductor La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ (Nd-LSCO), at low-temperature in the normal state accessed by suppressing superconductivity with a magnetic field up to $H = 31$ T. Using a newly developed AC thermopower measurement technique suitable for high pressure and high field, we track the pressure evolution of the Seebeck coefficient $S$. At ambient pressure and low temperature, $S/T$ was recently found to suddenly increase in Nd-LSCO at the pseudogap critical doping $p^{\star} = 0.23$, consistent with a dro…
