arXiv subjects

R. Liang

Publications and source records attributed to R. Liang.

At least 19 recordsLinked to original sources

arXiv2026

Persistent short-range charge correlations revealed by ultrafast melting of electronic order in YBa$_2$Cu$_3$O$_{6+x}$

Charge density waves (CDW) are ubiquitous in the complex phase diagram of cuprate superconductors and exhibit both short- and long-range correlations. Using time-resolved resonant X-ray scattering, we investigate the photo-induced dynamics of CDW in YBa$_2$Cu$_3$O$_{6.67}$. We discover an excitation threshold ($\Phi$$_\mathrm{C}$ $\approx$ 65 $\mu$J/cm$^2$) above which long-range CDW disappear, revealing a persistent CDW peak with short-range correlation length. Ultrafast photo-excitation promptly uncovers this residual short-range CDW correlations, appearing within $\approx$ 0.2 ps. Long-range CDW coherence recovers within $\approx$ 0.6 ps, while the peak intensity remains partially suppressed. We rationalize the dichotomic behavior in the fluence and temporal dependencies as the signature of two coexisting CDW peaks, arising from short- and long-range correlations, which we disentangle through their distinct response to photo-excitation. We provide evidence that the collapse of long-range correlations is driven by an electronic process, while short-range correlations are characterized by distinct timescales and stiffness against photo-excitation. This approach establishes ultrafast X-ray scattering as an effective tool for disentangling coexisting density waves and correlations in quantum materials.

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arXiv2024

Signatures of two gaps in the spin susceptibility of a cuprate superconductor

A major obstacle to understanding high-Tc cuprates is that superconductivity precludes observing normal-state properties at low temperatures. One prime example is the normal-state spin susceptibility \c{hi}spin: although its decrease upon cooling far above Tc typifies pseudogap behavior, its behavior at low temperatures is generally unknown. Here, our measurements in high magnetic fields expose \c{hi}spin of YBa2Cu3Oy down to low temperatures. Even though superconductivity is suppressed by the field, we uncover two thermally-activated contributions alongside a residual \c{hi}spin(T=0) due to gapless excitations. We relate these two distinct gaps to short-range charge-density waves and to the formation of singlets as in certain quantum spin systems. Both phenomena thus contribute to the pseudogap at low temperature, supplementing short-lived antiferromagnetism that initiates pseudogap behavior at high temperatures. We therefore propose that the pseudogap ought to be regarded as a composite property and that, when not undergoing spin-stripe ordering, underdoped cuprates tend to form short-ranged spin singlets.

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arXiv2022

No nematicity at the onset temperature of the pseudogap phase in the cuprate superconductor YBCO

Electronic nematicity is the spontaneous loss of rotational symmetry in a metal, without breaking translational symmetry. In the cuprate superconductors, there is experimental evidence for nematicity, but its origin remains unclear. Here we investigate the onset of nematicity in the transport of charge by means of electric and thermoelectric measurements in underdoped YBa$_{\rm 2}$Cu$_{\rm 3}$O$_{\rm y}$, performed by passing the current (electrical or thermal) first along the $a$ axis then the $b$ axis of the orthorhombic structure in the same crystal, with a hole doping $p = 0.12$. Upon cooling, we observe no additional in-plane anisotropy -- beyond the background anisotropy due to the CuO chains -- in either the resistivity $\rho$ or the Seebeck coefficient $S$ as the temperature $T^{\star}$~for the onset of the pseudogap phase is crossed. We conclude that the pseudogap phase of cuprates is not nematic. However, at temperatures much lower than $T^{\star}$, a strong additional anisotropy is observed, most clearly in the Peltier coefficient $\alpha = S / \rho$. We interpret it as nematicity associated with the development of charge order.

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arXiv2021

Locally commensurate charge-density wave with three-unit-cell periodicity in YBCO

In order to identify the mechanism responsible for the formation of charge-density waves (CDW) in cuprate superconductors, it is important to understand which aspects of the CDW's microscopic structure are generic and which are material-dependent. Here, we show that, at the local scale probed by NMR, long-range CDW order in YBa2Cu3Oy is unidirectional with a commensurate period of three unit cells (lambda = 3b), implying that the incommensurability found in X-ray scattering is ensured by phase slips (discommensurations). Furthermore, NMR spectra reveal a predominant oxygen character of the CDW with an out-of-phase relationship between certain lattice sites but no specific signature of a secondary CDW with lambda = 6b associated with a putative pair-density wave. These results shed light on universal aspects of the cuprate CDW. In particular, its spatial profile appears to generically result from the interplay between an incommensurate tendency at long length scales, possibly related to properties of the Fermi surface, and local commensuration effects, due to electron-electron interactions or lock-in to the lattice.

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arXiv2021

Unconventional short-range structural fluctuations in cuprate high-$T_c$ superconductors

The interplay between structural and electronic degrees of freedom in complex materials is the subject of extensive debate in physics and materials science. Particularly interesting questions pertain to the nature and extent of pre-transitional short-range order in diverse systems ranging from shape-memory alloys to unconventional superconductors, and how this microstructure affects macroscopic properties. Here we use neutron and X-ray diffuse scattering to uncover universal structural fluctuations in La$_{2-x}$Sr$_x$CuO$_4$ and Tl$_2$Ba$_2$CuO$_{6+\delta}$, two cuprate superconductors with distinct point disorder effects and optimal superconducting transition temperatures. The fluctuations are present in wide doping and temperature ranges, including compositions that maintain high average structural symmetry, and they exhibit unusual, yet simple scaling behavior. The scaling regime is robust and universal, similar to the well-known critical fluctuations close to second-order phase transitions, but with a distinctly different physical origin. We relate this behavior to pre-transitional phenomena in a broad class of systems with structural and magnetic transitions, and propose an explanation based on rare structural fluctuations caused by intrinsic nanoscale inhomogeneity. We also uncover parallels with superconducting fluctuations, which indicates that the underlying inhomogeneity plays an important role in cuprate physics.

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arXiv2020

Thermal Hall conductivity in the cuprate Mott insulators Nd$_2$CuO$_4$ and Sr$_2$CuO$_2$Cl$_2$

The heat carriers responsible for the unexpectedly large thermal Hall conductivity of the cuprate Mott insulator La$_2$CuO$_4$ were recently shown to be phonons. However, the mechanism by which phonons in cuprates acquire chirality in a magnetic field is still unknown. Here, we report a similar thermal Hall conductivity in two cuprate Mott insulators with significantly different crystal structures and magnetic orders - Nd$_2$CuO$_4$ and Sr$_2$CuO$_2$Cl$_2$ - and show that two potential mechanisms can be excluded - the scattering of phonons by rare-earth impurities and by structural domains. Our comparative study further reveals that orthorhombicity, apical oxygens, the tilting of oxygen octahedra and the canting of spins out of the CuO$_2$ planes are not essential to the mechanism of chirality. Our findings point to a chiral mechanism coming from a coupling of acoustic phonons to the intrinsic excitations of the CuO$_2$ planes.

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arXiv2020

Enhanced charge density wave coherence in a light-quenched, high-temperature superconductor

Superconductivity and charge density waves (CDW) are competitive, yet coexisting orders in cuprate superconductors. To understand their microscopic interdependence, a probe capable of discerning their interaction on its natural length and time scales is necessary. We use ultrafast resonant soft x-ray scattering to track the transient evolution of CDW correlations in YBa$_{2}$Cu$_{3}$O$_{6+x}$ following the quench of superconductivity by an infrared laser pulse. We observe a non-thermal response of the CDW order characterized by a near doubling of the correlation length within $\approx$ 1 picosecond of the superconducting quench. Our results are consistent with a model in which the interaction between superconductivity and CDW manifests inhomogeneously through disruption of spatial coherence, with superconductivity playing the dominant role in stabilizing CDW topological defects, such as discommensurations.

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arXiv2019

Spatially Inhomogeneous Competition between Superconductivity and the Charge Density Wave in YBa$_2$Cu$_3$O$_{6.67}$

The charge density wave in the high-temperature superconductor YBa$_2$Cu$_3$O$_{7-x}$ (YBCO) is now known to have two different ordering tendencies differentiated by their $c$-axis correlations. These correspond to ferro- (F-CDW) and antiferro- (AF-CDW) couplings between CDW in neighbouring CuO$_2$ bilayers. This discovery has prompted a number of fundamental questions. For example, how does superconductivity adjust to two competing orders and are either of these orders responsible for the electronic reconstruction? Here we use high-energy x-ray diffraction to study YBa$_2$Cu$_3$O$_{6.67}$ as a function of magnetic field and temperature. We show that regions of the sample with F-CDW correlations suppress superconductivity more strongly than those with AF-CDW correlations. This implies that an inhomogeneous superconducting state exists, in which some regions show a weak or fragile form of superconductivity. By comparison of F-CDW and AF-CDW correlation lengths, it is furthermore concluded that F-CDW ordering is sufficiently long-range to modify the electronic structure. Our study thus suggests that F-CDW correlations have an important impact on superconducting and normal state properties of underdoped YBCO.

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arXiv2019

NMR study of charge density waves under hydrostatic pressure in YBa2Cu3Oy

The effect of hydrostatic pressure (P) on charge density waves (CDW) in YBa2Cu3Oy has recently been controversial. Using NMR, we find that both the short-range CDW in the normal state and the long-range CDW in high fields are, at most, slightly weakened at P=1.9 GPa. This result is in contradiction with x-ray scattering results finding complete suppression of the CDW at ~1 GPa and we discuss possible explanations of this discrepancy. Quantitative analysis, however, shows that the NMR data is not inconsistent with a disappearance of the CDW on a larger pressure scale, typically ~10-20 GPa. We also propose a simple model reconciling transport data with such a hypothesis, provided the pressure-induced change in doping is taken into account. We conclude that it is therefore possible that most of the spectacular increase in Tc upon increasing pressure up to ~15~GPa arises from a concomitant decrease of CDW strength.

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arXiv2019

Resolving the nature of electronic excitations in resonant inelastic x-ray scattering

The study of elementary bosonic excitations is essential toward a complete description of quantum electronic solids. In this context, resonant inelastic X-ray scattering (RIXS) has recently risen to becoming a versatile probe of electronic excitations in strongly correlated electron systems. The nature of the radiation-matter interaction endows RIXS with the ability to resolve the charge, spin and orbital nature of individual excitations. However, this capability has been only marginally explored to date. Here, we demonstrate a systematic method for the extraction of the character of excitations as imprinted in the azimuthal dependence of the RIXS signal. Using this novel approach, we resolve the charge, spin, and orbital nature of elastic scattering, (para-)magnon/bimagnon modes, and higher energy dd excitations in magnetically-ordered and superconducting copper-oxide perovskites (Nd2CuO4 and YBa2Cu3O6.75). Our method derives from a direct application of scattering theory, enabling us to deconstruct the complex scattering tensor as a function of energy loss. In particular, we use the characteristic tensorial nature of each excitation to precisely and reliably disentangle the charge and spin contributions to the low energy RIXS spectrum. This procedure enables to separately track the evolution of spin and charge spectral distributions in cuprates with doping. Our results demonstrate a new capability that can be integrated into the RIXS toolset, and that promises to be widely applicable to materials with intertwined spin, orbital, and charge excitations.

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arXiv2018

Influence of Spin Orbit Coupling in the Iron-Based Superconductors

We report on the influence of spin-orbit coupling (SOC) in the Fe-based superconductors (FeSCs) via application of circularly-polarized spin and angle-resolved photoemission spectroscopy. We combine this technique in representative members of both the Fe-pnictides and Fe-chalcogenides with ab initio density functional theory and tight-binding calculations to establish an ubiquitous modification of the electronic structure in these materials imbued by SOC. The influence of SOC is found to be concentrated on the hole pockets where the superconducting gap is generally found to be largest. This result contests descriptions of superconductivity in these materials in terms of pure spin-singlet eigenstates, raising questions regarding the possible pairing mechanisms and role of SOC therein.

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arXiv2018

Sensitivity of $T_{\rm c}$ to pressure and magnetic field in the cuprate superconductor YBa$_{2}$Cu$_{3}$O$_{y}$: evidence of charge order suppression by pressure

Cuprate superconductors have a universal tendency to form charge density-wave (CDW) order which competes with superconductivity and is strongest at a doping $p \simeq 0.12$. Here we show that in the archetypal cuprate YBa$_{2}$Cu$_{3}$O$_{y}$ (YBCO) pressure suppresses charge order, but does not affect the pseudogap phase. This is based on transport measurements under pressure, which reveal that the onset of the pseudogap at $T^*$ is independent of pressure, while the negative Hall effect, a clear signature of CDW order in YBCO, is suppressed by pressure. We also find that pressure and magnetic field shift the superconducting transition temperature $T_{\rm c}$ of YBCO in the same way as a function of doping - but in opposite directions - and most effectively at $p \simeq 0.12$. This shows that the competition between superconductivity and CDW order can be tuned in two ways, either by suppressing superconductivity with field or suppressing CDW order by pressure. Based on existing high-pressure data and our own work, we observe that when CDW order is fully suppressed at high pressure, the so-called "1/8 anomaly" in the superconducting dome vanishes, revealing a smooth $T_{\rm c}$ dome which now peaks at $p \simeq 0.13$. We propose that this $T_{\rm c}$ dome is shaped by the competing effects of the pseudogap phase below its critical point $p^{\star} \sim 0.19$ and spin order at low doping.

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arXiv2018

Unusual interplay between superconductivity and field-induced charge order in YBa2Cu3Oy

We present a detailed study of the temperature (T) and magnetic field (H) dependence of the electronic density of states (DOS) at the Fermi level, as deduced from specific heat and Knight shift measurements in underdoped YBa2Cu3Oy. We find that the DOS becomes field-independent above a characteristic field H_{DOS} and that the H_{DOS}(T) line displays an unusual inflection near the onset of the long range 3D charge-density wave order. The unusual S-shape of H_{DOS}(T) is suggestive of two mutually-exclusive orders that eventually establish a form of cooperation in order to coexist at low T. On theoretical grounds, such a collaboration could result from the stabilisation of a pair-density wave state, which calls for further investigations in this region of the phase diagram

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arXiv2018

Pseudogap temperature $T^\star$ of cuprate superconductors from the Nernst effect

We use the Nernst effect to delineate the boundary of the pseudogap phase in the temperature-doping phase diagram of cuprate superconductors. New data for the Nernst coefficient $ν(T)$ of YBa$_{2}$Cu$_{3}$O$_{y}$ (YBCO), La$_{1.8-x}$Eu$_{0.2}$Sr$_x$CuO$_4$ (Eu-LSCO) and La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ (Nd-LSCO) are presented and compared with previous data including La$_{2-x}$Sr$_x$CuO$_4$ (LSCO). The temperature $T_ν$ at which $ν/T$ deviates from its high-temperature behaviour is found to coincide with the temperature at which the resistivity deviates from its linear-$T$ dependence, which we take as the definition of the pseudogap temperature $T^\star$- in agreement with gap opening detected in ARPES data. We track $T^\star$ as a function of doping and find that it decreases linearly vs $p$ in all four materials, having the same value in the three LSCO-based cuprates, irrespective of their different crystal structures. At low $p$, $T^\star$ is higher than the onset temperature of the various orders observed in underdoped cuprates, suggesting that these orders are secondary instabilities of the pseudogap phase. A linear extrapolation of $T^\star(p)$ to $p=0$ yields $T^\star(p\to 0)\simeq T_N(0)$, the Néel temperature for the onset of antiferromagnetic order at $p=0$, suggesting that there is a link between pseudogap and antiferromagnetism. With increasing $p$, $T^\star(p)$ extrapolates linearly to zero at $p\simeq p_{\rm c2}$, the critical doping below which superconductivity emerges at high doping, suggesting that the conditions which favour pseudogap formation also favour pairing. We also use the Nernst effect to investigate how far superconducting fluctuations extend above $T_{\rm c}$, as a function of doping, and find that a narrow fluctuation regime tracks $T_{\rm c}$, and not $T^\star$. This confirms that the pseudogap phase is not a form of precursor superconductivity.

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arXiv2017

Spin susceptibility of charge ordered YBa2Cu3Oy across the upper critical field

The value of the upper critical field Hc2, a fundamental characteristic of the superconducting state, has been subject to strong controversy in high-Tc copper-oxides. Since the issue has been tackled almost exclusively by macroscopic techniques so far, there is a clear need for local-probe measurements. Here, we use 17O NMR to measure the spin susceptibility $\chi_{spin}$ of the CuO2 planes at low temperature in charge ordered YBa2Cu3Oy. We find that $\chi_{spin}$ increases (most likely linearly) with magnetic field H and saturates above field values ranging from 20 to 40 T. This result is consistent with Hc2 values claimed by G. Grissonnanche et al. [Nat. Commun. 5, 3280 (2014)] and with the interpretation that the charge-density-wave (CDW) reduces Hc2 in underdoped YBa2Cu3Oy. Furthermore, the absence of marked deviation in $\chi_{spin}(H)$ at the onset of long-range CDW order indicates that this Hc2 reduction and the Fermi-surface reconstruction are primarily rooted in the short-range CDW order already present in zero field, not in the field-induced long-range CDWorder. Above Hc2, the relatively low values of $\chi_{spin}$ at T=2 K show that the pseudogap is a ground-state property, independent of the superconducting gap.

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arXiv2017

Crossover from Collective to Incoherent Spin Excitations in Superconducting Cuprates Probed by Detuned Resonant Inelastic X-ray Scattering

Spin excitations in the overdoped high temperature superconductors Tl$_2$Ba$_2$CuO$_{6+δ}$ and (Bi,Pb)$_2$(Sr,La)$_{2}$CuO$_{6+δ}$ were investigated by resonant inelastic x-ray scattering (RIXS) as functions of doping and detuning of the incoming photon energy above the Cu-$L_3$ absorption peak. The RIXS spectra at optimal doping are dominated by a paramagnon feature with peak energy independent of photon energy, similar to prior results on underdoped cuprates. Beyond optimal doping, the RIXS data indicate a sharp crossover to a regime with a strong contribution from incoherent particle/hole excitations whose maximum shows a fluorescence-like shift upon detuning. The spectra of both compound families are closely similar, and their salient features are reproduced by exact-diagonalization calculations of the single-band Hubbard model on a finite cluster. The results are discussed in the light of recent transport experiments indicating a quantum phase transition near optimal doping.

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arXiv2017

Anomalous Thermal Diffusivity in Underdoped YBa$_2$Cu$_3$O$_{6+x}$

We present local optical measurements of thermal diffusivity in the $ab$ plane of underdoped YBCO crystals. We find that the diffusivity anisotropy is comparable to reported values of the electrical resistivity anisotropy, suggesting that the anisotropies have the same origin. The anisotropy drops sharply below the charge order transition. We interpret our results through a strong electron-phonon scattering picture and find that both electronic and phononic contributions to the diffusivity saturate a proposed bound. Our results suggest that neither well-defined electron nor phonon quasiparticles are present in this material.

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arXiv2017

Anisotropy of the Seebeck Coefficient in the Cuprate Superconductor YBa$_{2}$Cu$_{3}$O$_{y}$: Fermi-Surface Reconstruction by Bidirectional Charge Order

The Seebeck coefficient $S$ of the cuprate YBa$_{2}$Cu$_{3}$O$_{y}$ was measured in magnetic fields large enough to suppress superconductivity, at hole dopings $p = 0.11$ and $p = 0.12$, for heat currents along the $a$ and $b$ directions of the orthorhombic crystal structure. For both directions, $S/T$ decreases and becomes negative at low temperature, a signature that the Fermi surface undergoes a reconstruction due to broken translational symmetry. Above a clear threshold field, a strong new feature appears in $S_{\rm b}$, for conduction along the $b$ axis only. We attribute this feature to the onset of 3D-coherent unidirectional charge-density-wave modulations seen by x-ray diffraction, also along the $b$ axis only. Because these modulations have a sharp onset temperature well below the temperature where $S/T$ starts to drop towards negative values, we infer that they are not the cause of Fermi-surface reconstruction. Instead, the reconstruction must be caused by the quasi-2D bidirectional modulations that develop at significantly higher temperature.

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