The electronic nematic phase emerging with spontaneous rotation symmetry breaking is a central issue of modern condensed matter physics. In particular, various nematic phases in iron-based superconductors and high-$T_{\rm c}$ cuprate superconductors are extensively studied recently. Electric quadrupole moments (EQMs) are one of the order parameters characterizing these nematic phases in a unified way, and elucidating EQMs is a key to understanding these nematic phases. However, the quantum-mechanical formulation of the EQMs in crystals is a nontrivial issue because the position operators are non-periodic and unbound. Recently, the EQMs have been formulated by local thermodynamics, and such {\it thermodynamic EQMs} may be used to characterize the fourfold rotation symmetry breaking in materials. In this paper, we calculate the thermodynamic EQMs in iron-based superconductors LaFeAsO and FeSe as well as a cuprate superconductor La$_2$CuO$_4$ by a first-principles calculation. We show that owing to the orbital degeneracy the EQMs in iron-based superconductors are mainly determined by the geometric properties of wave functions. This result is in sharp contrast to the cuprate superconductor, in which the EQMs are dominated by distortion of the Fermi surface.
Linear Response Theory for Shear Modulus $C_{66}$ and Raman Quadrupole Susceptibility: Significant Evidence for Orbital Nematic Fluctuations in Fe-Based Superconductors
We report a study of the Mott insulator La$_2$O$_3$Fe$_2$Se$_2$ by means of $^{139}$La nuclear quadrupole resonance (NQR). The NQR spectra evidence a single La site in the paramagnetic phase and two inequivalent La sites, La1 and La2, in the antiferromagnetically-ordered phase (Néel temperature $T_{\rm{N}} \simeq 90$ K). These two sites are characterized by different quadrupole couplings, indicative of distinct lattice and/or charge configurations likely segregated in domains. The dependence of the quadrupole coupling for La2 on temperature suggests that the magnetic order parameter drives the…
Ferroquadrupole order associated with local $4f$ atomic orbitals of rare earth ions is a realization of electronic nematic order. However, there are relatively few examples of intermetallic materials which exhibit continuous ferroquadrupole phase transitions, motivating the search for additional materials that fall in to this category. Furthermore, it is not clear a priori whether experimental approaches based on transport measurements which have been successfully used to probe the nematic susceptibility in materials such as the Fe-based superconductors, will be as effective in the case of $4f…
In this Rapid Communication, a set of $^{209}$Bi-nuclear magnetic resonance (NMR)/nuclear quadrupole resonance (NQR) measurements has been performed to investigate the physical properties of superconducting (SC) BaTi$_2$Bi$_2$O from a microscopic point of view. The NMR and NQR spectra at 5~K can be reproduced with a non-zero in-plane anisotropic parameter $η$, indicating the breaking of the in-plane four-fold symmetry at the Bi site without any magnetic order, i.e., `the electronic nematic state'. In the SC state, the nuclear spin-lattice relaxation rate divided by temperature, $1/T_1T$, does …
A central issue in the quest to understand the superconductivity in cuprates is the nature and origin of the pseudogap state, which harbours anomalous electronic states such as Fermi arc, charge density wave (CDW), and $d$-wave superconductivity. A fundamentally important, but long-standing controversial problem has been whether the pseudogap state is a distinct thermodynamic phase characterized by broken symmetries below the onset temperature $T^*$. Electronic nematicity, a fourfold ($C_4$) rotational symmetry breaking, has emerged as a key feature inside the pseudogap regime, but the presenc…
We investigate quantum phase transitions and quantum coherence in infinite biquadratic spin-1 and -2 XY chains with rhombic single-ion anisotropy. All considered coherence measures such as the $l_1$ norm of coherence, the relative entropy of coherence, and the quantum Jensen-Shannon divergence, and the quantum mutual information show consistently that singular behaviors occur for the spin-1 system, which enables to identity quantum phase transitions. For the spin-2 system, the relative entropy of coherence and the quantum mutual information properly detect no singular behavior in the whole sys…
The elastocaloric effect (ECE) is a thermodynamic quantity relating changes in entropy to changes in strain experienced by a material. As such, ECE measurements can provide valuable information about the entropy landscape proximate to strain-tuned phase transitions. For ordered states that break only point symmetries, bilinear coupling of the order parameter with strain implies that the ECE can also provide a window on fluctuations above the critical temperature, and hence, in principle, can also provide a thermodynamic measure of the associated susceptibility. To demonstrate this, we use the …
We study numerically the thermodynamic properties of the spin nematic phases in a magnetic field in the spin-1 bilinear-biquadratic model. When the field is applied, the phase transition temperature once goes up and then decreases rapidly toward zero, which is detected by the peak-shift in the specific heat. The underlying mechanism of the reentrant behavior is the entropic effect. In a weak field the high temperature paramagnetic phase rapidly loses its entropy while the ferroquadrupolar nematic phase remains robust by modifying the shape of the ferroquadrupolar moment. This feature serves as…
Unconventional superconductivity is characterized by the spontaneous symmetry breaking of the macroscopic superconducting wavefunction in addition to the gauge symmetry breaking, such as rotational-symmetry breaking with respect to the underlying crystal-lattice symmetry. Particularly, superconductivity with spontaneous rotational-symmetry breaking in the wavefunction amplitude and thus in bulk properties, not yet reported previously, is intriguing and can be termed "nematic" superconductivity in analogy to nematic liquid-crystal phases. Here, based on specific-heat measurements of the single-…
We discuss the results of $^{75}$As Nuclear Quadrupole Resonance (NQR) and muon spin relaxation measurements in AFe$_2$As$_2$ (A= Cs, Rb) iron-based superconductors. We demonstrate that the crossover detected in the nuclear spin-lattice relaxation rate $1/T_1$ (around 150 K in RbFe$_2$As$_2$ and around 75 K in CsFe$_2$As$_2$), from a high temperature nearly localized to a low temperature delocalized behaviour, is associated with the onset of an inhomogeneous local charge distribution causing the broadening or even the splitting of the NQR spectra as well as an increase in the muon spin relaxat…
Higher-rank electric/magnetic multipole moments are attracting attention these days as candidate order parameters for exotic material phases. However, quantum-mechanical formulation of those multipole moments is still an ongoing issue. In this paper, we propose a thermodynamic definition of electric quadrupole moments as a measure of symmetry breaking, following previous studies of orbital magnetic dipole moments and magnetic quadrupole moments. The obtained formulas are illustrated with a model of orbital-ordered nematic phases of iron-based superconductors.
The exotic normal state of iron chalcogenide superconductor FeSe, which exhibits vanishing magnetic order and possesses an electronic nematic order, triggered extensive explorations of its magnetic ground state. To understand its novel properties, we study the ground state of a highly frustrated spin-$1$ system with bilinear-biquadratic interactions using unbiased large-scale density matrix renormalization group. Remarkably, with increasing biquadratic interactions, we find a paramagnetic phase between Néel and stripe magnetic ordered phases. We identify this phase as a candidate of nematic qu…
Spin liquid crystals are magnetic analogs of liquid crystals, possessing properties of both liquids and solids, a typical example of which are spin nematics. Spin nematics share many features with spin liquids, and the interplay between them is a promising, but little explored, route to uncovering new phases of matter. Here, we address this question in the context of a spin-$1$ magnet on the honeycomb lattice, by considering a model with both biquadratic interactions, favouring spin-nematic states, and Kitaev-like interactions, supporting spin liquids. Accompanying these, where dipole and quad…
We report the results of our in-depth analysis of spectroscopic and thermodynamic properties of a multi-orbital metal, like FeSe, which first develops a nematic order and then undergoes a transition into a superconducting state, which co-exists with nematicity. We analyze the angular dependence of the gap function and specific heat $C_V (T)$ of such nematic superconductor. We specifically address three issues: (i) angular dependence of the gap in light of the competition between nematicity-induced $s$-$d$ mixture and orbital transmutation of low-energy excitations in the nematic state, (ii) th…
Phononic enhancement and detection of hidden spin-nematicity and dynamics in quantum magnets
International Center for Quantum Materials, School of Physics, Peking University（北京大学物理学院量子材料国际中心）；Collaborative Innovation Center of Quantum Matter（量子物质协同创新中心）
Charge stripe order has recently been established as an important ingredient of the physics of cuprate high-T$_c$ superconductors. However, due to the complex interplay between competing phases and the influence of disorder, it is unclear how it emerges from the parent metallic state. Here we report on the discovery of an unconventional electronic ordered phase between charge-stripe order and (pseudogapped) metal in the cuprate La$_{2-x-y}$Eu$_{y}$Sr$_x$CuO$_4$ with $y = 0.2$ (LESCO). The peculiar properties of the intermediate phase are revealed through three complementary experiments: nuclea…
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 explore several classes of quadrupolar ordering in a system of antiferromagnetically coupled quantum spin-1 dimers, which are stacked in the triangular lattice geometry forming a bilayer. Low-energy properties of this model is described by an $\mathcal{S}=1$ hard-core bosonic degrees of freedom defined on each dimer-bond, where the singlet and triplet states of the dimerized spins are interpreted as the vacuum and the occupancy of boson, respectively. The number of bosons per dimer and the magnetic and density fluctuations of bosons are controlled by the inter-dimer Heisenberg interactions.…
At ambient pressure and zero field, tetragonal CeAuSb$_{2}$ hosts stripe antiferromagnetic order at $T_{N} = 6.3$ K. Here we first show via bulk thermodynamic probes and x-ray diffraction measurements that this magnetic order is connected with a structural phase transition to a superstructure which likely breaks $C_{4}$ symmetry, thus signaling nematic order. The temperature-field-pressure phase diagram of CeAuSb$_{2}$ subsequently reveals the emergence of additional ordered states under applied pressure at a multicritical point. Our phenomenological model supports the presence of a vestigial …
The bond-nematic state has both long-range ordering of magnetic quadrupoles and the high entanglement typical of spin liquids, and as such can be thought of as a spin liquid crystal. One of the most promising materials in which to find such a state is BaCdVO(PO$_4$)$_2$, in which a magnetically silent phase has been found between a magnetically ordered low-field phase and the high-field polarised phase. Here I study the magnetic Hamiltonian of BaCdVO(PO$_4$)$_2$, and, for the Hamiltonian-parameters determined by fits to inelastic neutron scattering experiments, show that magnons condense out o…
The Kitaev model is a remarkable spin model with gapped and gapless spin liquid phases, which are potentially realized in iridates and $α$-RuCl$_3$. In the recent experiment of $α$-RuCl$_3$, the signature of a nematic transition to the gapped toric code phase, which breaks the $C_3$ symmetry of the system, has been observed through the angle dependence of the heat capacity. We here propose a mechanism by which the nematic transition can be detected electrically. This is seemingly impossible because $J_\textrm{eff}=1/2$ spins do not have an electric quadrupole moment (EQM). However, in the seco…
Quantum criticality has been invoked as being essential to the understanding of a wide range of exotic electronic behavior, including heavy Fermion and unconventional superconductivity, but conclusive evidence of quantum critical fluctuations has been elusive in many materials of current interest. An expected characteristic feature of quantum criticality is power law behavior of thermodynamic quantities as a function of a non-thermal tuning parameter close to the quantum critical point (QCP). In the present work, we observe power law behavior of the critical temperature of the coupled nematic/…
We demonstrate how first-principles calculations of many competing low-energy states of a correlated material, here a cuprate, can be used to develop a thermodynamic model of Mott and pseudogap transitions in terms of magnetic short-range order. Mott physics is found in this picture to be driven by an unbinding of the antiphase domain walls, while the pseudogap phenomenon represents local moment formation. We provide explanations for nematicity and Fermi arc formation, and find a striking correspondence with many-body perturbation theory predictions.
We study the excitation spectrum in the dimer phase of the Shastry-Sutherland model by using an unbiased variational method that works in the thermodynamic limit. The method outputs dynamical correlation functions in all possible channels. This output is exploited to identify the order parameters with the highest susceptibility (single or multitriplon condensation in a specific channel) upon approaching a quantum phase transition in the magnetic field versus the $J'/J$ phase diagram. We find four different instabilities: antiferro spin nematic, plaquette spin nematic, stripe magnetic order, an…
We report the magnetic and calorimetric measurements in single crystal samples of the square lattice $J_{1}-J_{2}$ quantum antiferromagnet BaCdVO(PO$_4$)$_2$. An investigation of the scaling of magnetization reveals a "dimensionality reduction" indicative of a strong degree of geometric frustration. Below a characteristic temperature of $T^{\ast}\simeq150$~mK we observe the emergence of an additional strongly fluctuating quantum phase close to full magnetic saturation. It is separated from the magnetically ordered state by first- and second-order phase transitions, depending on the orientation…
Theoretical studies of magnets have traditionally concentrated on either classical spins, or the extreme quantum limit of spin-1/2. However, magnets built of spin-1 moments are also intrinsically interesting, not least because they can support quadrupole, as well as dipole moments, on a single site. For this reason, spin-1 models have been extensively studied as prototypes for quadrupolar (spin-nematic) order in magnetic insulators, and Fe-based superconductors. At the same time, because of the presence of quadrupoles, the classical limit of a spin-1 moment is not an $O(3)$ vector, a fact whic…
