Field-angle resolved magnetic excitations as a probe of hidden-order symmetry in CeB6
P. Y. Portnichenko, A. Akbari, S. E. Nikitin, A. S. Cameron, A. V. Dukhnenko, V. B. Filipov, N. Yu. Shitsevalova, P. Cermak, I. Radelytskyi, A. Schneidewind, J.… 展开作者
P. Y. Portnichenko, A. Akbari, S. E. Nikitin, A. S. Cameron, A. V. Dukhnenko, V. B. Filipov, N. Yu. Shitsevalova, P. Cermak, I. Radelytskyi, A. Schneidewind, J. Ollivier, A. Podlesnyak, Z. Huesges, J. Xu, A. Ivanov, Y. Sidis, S. Petit, J. -M. Mignot, P. Thalmeier, D. S. Inosov
In contrast to magnetic order formed by electrons' dipolar moments, ordering phenomena associated with higher-order multipoles (quadrupoles, octupoles, etc.) are more difficult to characterize because of the limited choice of experimental probes that can distinguish different multipolar moments. The heavy-fermion compound CeB6 and its La-diluted alloys are among the best-studied realizations of the long-range-ordered multipolar phases, often referred to as "hidden order". Previously the hidden order in phase II was identified as primary antiferroquadrupolar (AFQ) and field-induced octupolar (AFO) order. Here we present a combined experimental and theoretical investigation of collective excitations in the phase II of CeB6. Inelastic neutron scattering (INS) in fields up to 16.5 T reveals a new high-energy mode above 14 T in addition to the low-energy magnetic excitations. The experimental dependence of their energy on the magnitude and angle of the applied magnetic field is compared to the results of a multipolar interaction model. The magnetic excitation spectrum in rotating field is calculated within a localized approach using the pseudo-spin presentation for the Gamma8 states. We show that the rotating-field technique at fixed momentum can complement conventional INS measurements of the dispersion at constant field and holds great promise for identifying the symmetry of multipolar order parameters and the details of inter-multipolar interactions that stabilize hidden-order phases.
We study, using high-resolution angle-resolved photoemission spectroscopy, the evolution of the electronic structure in URu2Si2 at the Gamma, Z and X high-symmetry points from the high-temperature Kondo-screened regime to the low-temperature `hidden-order' (HO) state. At all temperatures and symmetry points, we find structures resulting from the interaction between heavy and light bands, related to the Kondo lattice formation. At the X point, we directly measure a hybridization gap of 11 meV already open at temperatures above the ordered phase. Strikingly, we find that while the HO induces pro…
Nonequilibrium calculations in the presence of an electric field are usually performed in a gauge, and need to be transformed to reveal the gauge-invariant observables. In this work, we discuss the issue of gauge invariance in the context of time-resolved angle-resolved pump/probe photoemission. If the probe is applied while the pump is still on, one must ensure that the calculations of the observed photocurrent are gauge invariant. We also discuss the requirement of the photoemission signal to be positive and the relationship of this constraint to gauge invariance. We end by discussing some t…
We report angle resolved photoemission (ARPES) spectra of $η$-Mo$_4$O$_{11}$, a layered metal that undergoes two charge density wave (CDW) transitions at 109 K and 30 K. We have directly observed the ``hidden one-dimensional (hidden-1d)'' Fermi surface and an anisotropic gap opening associated with the 109 K transition, in agreement with the band theoretical description of the CDW transition. In addition, as in other hidden-1d materials such as NaMo$_6$O$_{17}$, the ARPES line shapes show certain anomalies, which we discuss in terms of non-Fermi liquid physics and possible roles of disorder.
We report thermoelectric measurements of the low carrier heavy fermion compound URu2Si2 at high fields up to 34T and at low temperatures down to 500mK. The field dependence of the thermoelectric power (TEP) and the Nernst signal shows successive anomalies deep inside the hidden order (HO) phase. The field position of these anomalies correspond to different changes in the Shubnikov-de Haas frequencies and effective masses around 12 T, 17 T, 23 T and 30 T. These results indicate successive reconstructions of the Fermi surface, which imply electronic phase transitions well within the HO phase.
The theory for time-resolved photoemission spectroscopy as applied to pump-probe experiments is developed and solved for the generic case of a strongly correlated material. The formal development incorporates all of the nonequilibrium effects of the pump pulse and the finite time width of the probe pulse. While our formal development is completely general, in our numerical illustration for the Hubbard model, we assume the pump pulse drives the electrons into a nonequilibrium configuration, which rapidly thermalizes to create a hot (quasi-equilibrium) electronic system, and we then study the ef…
Quasi-one-dimensional systems exhibit many-body effects elusive in higher dimensions. A prime example is spin-orbital separation, which has been measured by resonant inelastic X-ray scattering (RIXS) in Sr$_2$CuO$_3$. Here, we theoretically analyze the time-resolved RIXS spectrum of Sr$_2$CuO$_3$ under the action of a time-dependent electric field. We show that the external field can reversibly modify the parameters in the effective $t-J$ model used to describe spinon and orbiton dynamics in the material. For strong driving amplitudes, we find that the spectrum changes qualitatively as a resul…
We demonstrate that the volume of the Fermi surface, measured very precisely using de Haas-van Alphen oscillations, can be used to probe changes in the nature and occupancy of localized electronic states. In systems with unconventional ordered states, this allows an underlying electronic order parameter to be followed to very low temperatures. We describe this effect in the field-induced antiferroquadrupolar (AFQ) ordered phase of PrOs4Sb12, a heavy fermion intermetallic compound. We find that the phase of de Haas-van Alphen oscillations is sensitively coupled, through the Fermi volume, to the…
The dynamical properties of single crystal 1T-TaS$_{2}$ are investigated both in commensurate charge density wave state (CCDW state) and hidden charge density wave state (HCDW state). We develop a useful criterion in time-domain transmission terahertz measurement to judge whether the compound is driven into a metastable state or still in its virgin state. An increase of terahertz conductivity by two orders of magnitude from CCDW state to HCDW state is obtained by taking account of the penetration depth mismatch, which is in agreement with reported \emph{dc} transport measurement. Upon weak pum…
We show that a two-dimensional (2D) isotropic Fermi liquid harbors two new types of collective modes, driven by quantum fluctuations, in addition to conventional zero sound: "hidden" and "mirage" modes. The hidden modes occur for relatively weak attractive interaction both in the charge and spin channels with any angular momentum $l$. Instead of being conventional damped resonances within the particle-hole continuum, the hidden modes propagate at velocities larger than the Fermi velocity and have infinitesimally small damping in the clean limit, but are invisible to spectroscopic probes. The m…
In this work, we theoretically examine recent pump/probe photoemission experiments on the strongly correlated charge-density-wave insulator TaS\_2. We describe the general nonequilibrium many-body formulation of time-resolved photoemission in the sudden approximation, and then solve the problem using dynamical mean-field theory with the numerical renormalization group and a bare density of states calculated from density functional theory including the charge-density-wave distortion of the ion cores and spin-orbit coupling We find a number of interesting results: (i) the bare band structure act…
Broken symmetries in solids involving higher order multipolar degrees of freedom are historically referred to as "hidden orders" due to the formidable task of detecting them with conventional probes. Examples of such hidden orders include spin-nematic order in quantum magnets, and quadrupolar or higher multipolar orders in various correlated quantum materials. In this work, we theoretically propose that the study of magnetostriction provides a powerful and novel tool to directly detect higher-order multipolar symmetry breaking $-$ such as the elusive octupolar order $-$ by examining its scalin…
We demonstrated experimentally a direct way to probe a hidden propensity to the formation of spin density wave (SDW) in a non-magnetic metal with strong Fermi surface nesting. Substituting Fe for a tiny amount of Cu (1%) induced an incommensurate magnetic order below 20 K in heavily-overdoped La2-xSrxCuO4 (LSCO). Elastic neutron scattering suggested that this order cannot be ascribed to the localized spins on Cu or doped Fe. Angle-resolved photoemission spectroscopy (ARPES), combined with numerical calculations, revealed a strong Fermi surface nesting inherent in the pristine LSCO that likely …
We investigated the nonequilibrium electronic structure of 2H-NbSe$_2$ by time- and angle-resolved photoemission spectroscopy. We find that the band structure is distinctively modulated by strong photo-excitation, as indicated by the unusual increase in the photoelectron intensities around E$_F$. In order to gain insight into the observed photo-induced electronic state, we performed DFT calculations with modulated lattice structures, and found that the variation of the Se height from the Nb layer results in a significant change in the effective mass and band gap energy. We further study the mo…
The three-dimensional (3D) electronic structure of the hidden order compound URu$_2$Si$_2$ in a paramagnetic phase was revealed using a 3D angle-resolved photoelectron spectroscopy where the electronic structure of the entire Brillouin zone is obtained by scanning both incident photon energy and detection angles of photoelectrons. The quasi-particle bands with enhanced contribution from the $\mathrm{U}~5f$ state were observed near $E_\mathrm{F}$, formed by the hybridization with the $\mathrm{Ru}~4d$ states. The energy dispersion of the quasi-particle band is significantly depend on $k_z$, indi…
In this article we present high-resolution angle-resolved photoemission (ARPES) spectra of the heavy-fermion superconductor URu$_2$Si$_2$. Measurements as a function of both excitation energy and temperature allow us to disentangle a variety of spectral features, revealing the evolution of the low energy electronic structure across the hidden order transition. Already above the hidden order transition our measurements reveal the existence of weakly dispersive states below the Fermi level that exhibit a large scattering rate. Upon entering the hidden order phase, these states transform into a c…
Here we apply high resolution angle-resolved photoemission spectroscopy (ARPES) using a wide excitation energy range to probe the electronic structure and the Fermi surface topology of the Ba1-xKxFe2As2 (Tc = 32 K) superconductor. We find significant deviations in the low energy band structure from that predicted in calculations. A set of Fermi surface sheets with unexpected topology is detected at the Brillouin zone boundary. At the X-symmetry point the Fermi surface is formed by a shallow electron-like pocket surrounded by four hole-like pockets elongated in G-X and G-Y directions.
We investigate pump induced modulation in the temporal evolution of the excitonic coherent polarization generated by a probe pulse in GaAs multiple quantum wells. For this, we perform fs time resolved pump-probe reflectivity measurements using frequency upconversion at both positive and negative pump-probe delays. A contribution arising from interference of excitonic linear and nonlinear polarization, which is usually not considered in describing pump-probe experiments, is required to understand the results.
We present angle-resolved photoelectron spectroscopy data probing the electronic structure of the Nd-substituted high-$T_c$ cuprate La$_{1.48}$Nd$_{0.4}$Sr$_{0.12}$CuO$_4$ (Nd-LSCO). Data have been acquired at low and high photon energies, $hν$ = 55 and 500 eV, respectively. Earlier comparable low-energy studies of La$_{1.4-x}$Nd$_{0.6}$Sr$_{x}$CuO$_4$ ($x = 0.10, 0.12, 0.15$) have shown strongly suppressed photoemission intensity, or absence thereof, in large parts of the Brillouin zone. Contrary to these findings we observe spectral weight at all points along the entire Fermi surface contour…
The Charge-density-wave(CDW) in 2H-NbSe2(TCDW ~ 33 K), which coexists with superconductivity(Tc = 7.2 K), is investigated using Angle-resolved photoemission spectroscopy as a function of temperature. Across TCDW, energy and momentum(k) distribution curves show changes associated with the primary and secondary CDW vectors. The CDW is due to hidden charge order occurring at specific k-points on Fermi surfaces in the 2-dimensional Brillouin zone(2D BZ) with spectral weight suppression, but no gap formation. The study rules out nesting in the 2D BZ and the van Hove singularity driven CDW transitio…
We report angle-resolved photoemission spectroscopy (ARPES) experiments probing deep into the hidden order (HO) state of URu2Si2, utilizing tunable photon energies with sufficient energy and momentum resolution to detect the near Fermi surface (FS) behavior. Our results reveal: (i) the full itinerancy of the 5f electrons; (ii) the crucial three-dimensional (3D) k-space nature of the FS and its critical nesting vectors, in good comparison with density-functional theory calculations, and (iii) the existence of hot-spot lines and pairing of states at the FS, leading to FS gapping in the HO phase.
We present the development of a time- and angle-resolved photoemission spectroscopy based on a Yb-based femtosecond laser and a hemispherical electron analyzer. The energy of the pump photon is tunable between 1.4 and 1.9 eV, and the pulse duration is around 30 fs. We use a KBe$_2$BO$_3$F$_2$ non-linear optical crystal to generate probe pulses, of which the photon energy is up to 6.7 eV, and obtain an overall time resolution of 1 ps and energy resolution of 18 meV. In addition, $β$-BaB$_2$O$_4$ crystals are used to generate alternative probe pulses at 6.05 eV, giving an overall time resolution…
Since the discovery of charge disproportionation in the FeO$_2$ square-lattice compound Sr$_3$Fe$_2$O$_7$ by Mössbauer spectroscopy more than fifty years ago, the spatial ordering pattern of the disproportionated charges has remained "hidden" to conventional diffraction probes, despite numerous x-ray and neutron scattering studies. We have used neutron Larmor diffraction and Fe K-edge resonant x-ray scattering to demonstrate checkerboard charge order in the FeO$_2$ planes that vanishes at a sharp second-order phase transition upon heating above 332 K. Stacking disorder of the checkerboard patt…
Dynamics of depletion and recovery of superconducting state in La2-xSrxCuO_4 thin films is investigated utilizing optical pump-probe and optical pump - THz probe techniques as a function of temperature and excitation fluence. The absorbed energy density required to suppress superconductivity is found to be about 8 times higher than the thermodynamically determined condensation energy density and nearly temperature independent between 4 and 25 K. These findings indicate that during the time when superconducting state suppression takes place (~0.7 ps), a large part (nearly 90%) of the energy is …
Time-and-frequency resolved pump-probe optical spectroscopy is used to investigate the effect of the impulsive injection of delocalized excitations through a charge-transfer process in insulating CuGeO3. A large broadening of the charge-transfer edge is observed on the sub-ps timescale. The modification of this spectral feature can not be attributed to the local increase of the effective temperature, as a consequence of the energy absorbed by the pump pulse. The measured modifications of the optical properties of the system are consistent with the creation of a non-thermal state, metastable on…
Observation of hidden altermagnetism in Cs$_{1-δ}$V$_2$Te$_2$O
Zhejiang University（浙江大学）；Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences（中国科学院上海微系统与信息技术研究所）；Southern University of Science and Technology（南方科技大学）
The three-dimensional Fermi surface structure of hole-doped metallic layered nickelate Eu2-xSrxNiO4 (x=1.1), an important counterpart to the isostructural superconducting cuprate La2-xSrxCuO4, is investigated by energy-dependent soft-x-ray angle-resolved photoemission spectroscopy. In addition to a large cylindrical hole Fermi surface analogous to the cuprates, we observe a Gamma-centered 3z2-r2-derived small electron pocket. This finding demonstrates that in the layered nickelate the 3z2-r2 band resides close to the x2-y2 one in energy. The resultant multi-band feature with varying orbital ch…
Recently, kagome lattice metal AV$_3$Sb$_5$ (A = K, Rb, Cs) family has received wide attention due to its presence of superconductivity, charge density wave (CDW) and peculiar properties from topological nontrivial electronic structure. With time-resolved pump-probe spectroscopy, we show that the excited quasiparticle relaxation dynamics can be explained by formation of energy gap below the phase transition being similar to a usual second-order CDW condensate, by contrast, the structure change is predominantly first order phase transition. Furthermore, no CDW amplitude mode is identified in th…
High-resolution angle-resolved photoemission spectroscopy (ARPES) data reveal evidence of a crossover from one-dimensional (1D) to three-dimensional (3D) behavior in the prototypical charge density wave (CDW) material NbSe3. In the low-temperature 3D regime, gaps in the electronic structure are observed due to two incommensurate CDWs, in agreement with x-ray diffraction and electronic-structure calculations. At higher temperatures we observe a spectral weight depletion that approaches the power-law behavior expected in 1D. From the warping of the quasi-1D Fermi surface at low temperatures, we …
The superconducting gap structure of heavy fermion UPd_2Al_3, in which unconventional superconductivity coexists with antiferromagnetic (AF) order with atomic size local moments, was investigated by the thermal conductivity measurements in a magnetic field rotating in various directions relative to the crystal axes. The results provide strong evidence that the gap function Δ(k) has a single line node orthogonal to the c-axis located at the AF Brillouin zone boundary, while Δ(k) is isotropic within the basal plane. The determined nodal structure is compatible with the resonance peak in the dyna…
We investigate a momentum-resolved Raman spectroscopy technique which is able to probe the one-body spectral function and the quasi-particle states of a gas of strongly interacting ultracold atoms. This technique is inspired by Angle-Resolved Photo-Emission Spectroscopy, a powerful experimental probe of electronic states in solid-state systems. Quantitative examples of experimentally accessible spectra are given for the most significant regimes along the BEC-BCS crossover. When the theory is specialized to RF spectroscopy, agreement is found with recent experimental data. The main advantages o…
High-$T_c$ cuprate superconductors are characterized by a strong momentum-dependent anisotropy between the low energy excitations along the Brillouin zone diagonal (nodal direction) and those along the Brillouin zone face (antinodal direction). Most obvious is the d-wave superconducting gap, with the largest magnitude found in the antinodal direction and no gap in the nodal direction. Additionally, while antinodal quasiparticle excitations appear only below $T_c$, superconductivity is thought to be indifferent to nodal excitations as they are regarded robust and insensitive to $T_c$. Here we r…
Physicists have long debated whether the hidden order in URu2Si2 is itinerant or localized, and it remains inaccessible to direct external probes. Recent observation of an overdamped collective mode in this material (C. Weibe et al, Nature Physics 3, 96-100 (2007)), appears to resolve this outstanding issue.
We report the ultra-fast optical response of quasi-particles (QPs) in both the pseudogap (PG) and superconducting (SC) states of underdoped (UD) Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+δ}$ (Bi2212) single crystal measured with the time-resolved pump-probe technique. At a probe energy $\hbarω_{pr}$=1.55 eV, it is found that the reflectivity change $Δ$R/R changes its sign at exactly $T_{c}$, which allows the direct separation of the charge dynamics of PG and SC QPs. Further systematic investigations indicate that the transient signals associated with PG and SC QPs depend on the probe beam energy and pol…
Hidden Fermi liquid theory explicitly accounts for the effects of Gutzwiller projection in the t-J Hamiltonian, widely believed to contain the essential physics of the high-Tc superconductors. We derive expressions for the entire "strange metal", normal state relating angle-resolved photoemission, resistivity, Hall angle, and by generalizing the formalism to include the Fermi surface topology - angle-dependent magnetoresistance. We show this theory to be the first self-consistent description for the normal state of the cuprates based on transparent, fundamental assumptions. Our well-defined fo…
The insulating magnetic phase in graphene zigzag ribbons, predicted both by density functional and mean field Hubbard model calculations, is described without additional approximations with a BCS wave function of two phase-locked condensates of spin-polarized electron-hole pairs. The associated order parameter is the spin dipole operator that features both magnetic and electric order and accounts for the spin-resolved ferroelectricity of the system. Each condensate is associated to a spin-dependent dipole and their relative phase locking sets the total electric dipole and total magnetization e…
We present a probe-type scanning tunneling microscope (STM) with atomic resolution that is designed to be directly inserted and work in a harsh vibrational cryogen-free superconducting magnet system. When a commercial variable temperature insert (VTI) is installed in the magnet and the STM is in turn housed in the VTI, a lowest temperature of 1.6 K can be achieved, where the STM still operates well. We have tested it in an 8 T superconducting magnet cooled with the pulse-tube cryocooler (PTC) and obtained atomically revolved graphite and NiSe2 images as well as the scanning tunneling spectrum …
It is of central importance to probe the \emph{local} spectral function $A(\mathbf{k},ω)$ of a strongly interacting Fermi gas in a trap. Momentum resolved rf spectroscopy has been demonstrated to be able to probe the trap averaged $A(\mathbf{k},ω)$. However, the usefulness of this technique was limited by the trap inhomogeneity. Independent of a specific theory, here we propose that by studying the momentum resolved rf spectra of the minority fermions of a phase separated, population imbalanced Fermi gas at low temperature, one can effectively extract $A(\mathbf{k},ω)$ of a homogeneous superfl…
