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coupled metal Cd2Re2O7 tum (14, 18). In a cubic material, for example, this
order parameter can have either Eu or T2u sym-
metry. An example of a spin-polarized Fermi sur-
J. W. Harter,1,2 Z. Y. Zhao,3,4 J.-Q. Yan,3,5 D. G. Mandrus,3,5 D. Hsieh1,2* face distortion induced by T2u multipolar nematic
order is shown in Fig. 1A.
Strong electron interactions can drive metallic systems toward a variety of well-known The correlated metallic pyrochlore Cd2Re2O7
symmetry-broken phases, but the instabilities of correlated metals with strong spin-orbit has been proposed as a candidate for hosting
coupling have only recently begun to be explored. We uncovered a multipolar nematic multipolar nematic order because of the strong
phase of matter in the metallic pyrochlore Cd2Re2O7 using spatially resolved second- spin-orbit coupling of Re 5d valence electrons.
harmonic optical anisotropy measurements. Like previously discovered electronic nematic Detailed Raman scattering (19), x-ray (20, 21)
phases, this multipolar phase spontaneously breaks rotational symmetry while preserving
I
structure (space group I4m2) that breaks threefold
n the presence of strong Coulomb inter- in the context of classical bent-core liquid crystals rotational symmetry about the 111 axis (Fig. 1, B
actions, the fluid of mobile electrons in a (15). Theoretical models have shown that parity- and C). This phase transition has traditionally
metal can spontaneously break the point breaking nematic fluctuations can induce odd- been attributed to the freezing of a soft phonon
group symmetries of the underlying crystal parity p- or f-wave Cooper pairing and thus provide mode with Eu symmetry, dominated by the displace-
lattice, realizing the quantum analog of a a route to topological superconductivity (16, 17). ment of O(1) atoms (19, 24, 25). However, the ob-
nematic liquid crystal (1). Like their classical In addition, because inversion symmetry-breaking servation of extremely small changes in lattice
counterparts, quantum nematic phases generally necessarily lifts the spin degeneracy of bulk energy parameters (21, 22), an anomalous temperature
preserve spatial inversion symmetry and are there- bands in a spin-orbit coupled system, odd-parity dependence of superlattice Bragg peaks (20), and
fore anisotropic but centrosymmetric fluids. Ex- nematic order offers a potential mechanism for a dramatic reduction in the electronic density of
perimental evidence of such nematic order was generating topologically protected Weyl and nodal- states across Tc (2629) calls this interpretation
first detected in a two-dimensional (2D) GaAs/ line semimetals and for designing highly tunable into question and raises the possibility that a
AlGaAs quantum well interface on the basis of charge-to-spin current conversion technologies hitherto undetected electronic order is driving the
a pronounced resistivity anisotropy between the for spintronics applications. transition.
two principal directions of the underlying square
lattice (2, 3). Subsequently, similar behavior has
been reported in a number of quasi-2D square
lattice compounds, including Sr3Ru2O7 (4), URu2Si2
(5), and several families of both copper- (6, 7) and
iron-based (811) high-temperature superconduc-
tors, suggesting possible connections between
even-parity nematic fluctuations and unconven-
tional s- and d-wave Cooper pairing (12).
Extending earlier work on Fermi liquid in-
stabilities in the p-wave spin interaction channel
(13), it has recently been predicted that corre-
lated metals with strong spin-orbit coupling may
realize a fundamentally new class of electronic
nematic phases with spontaneously broken spa-
tial inversion symmetry (14), including a quantum
analog of the unusual NT nematic phase discussed
1
Department of Physics, California Institute of Technology, Fig. 1. Illustration of electronic and structural order parameters in Cd2Re2O 7. (A) T2u distortion of a
Pasadena, CA 91125, USA. 2Institute for Quantum spherical Fermi surface induced by a Qxy multipolar nematic order parameter.The Fermi surface is split into
Information and Matter, California Institute of Technology,
Pasadena, CA 91125, USA. 3Materials Science and
two nondegenerate surfaces of opposite spin texture (arrows), with the largest splitting at the equator and
Technology Division, Oak Ridge National Laboratory, Oak zero splitting at the poles. (B) The ideal pyrochlore structure of Cd2Re2O7 viewed along the (111) axis. Only
Ridge, TN 37831, USA. 4Department of Physics and Re (yellow tetrahedra) and O(1) (green octahedra) sublattices are shown. Dashed lines depict mirror
Astronomy, University of Tennessee, Knoxville, TN 37996, planes. For clarity, an enlarged view of two neighboring subunits from an alternative angle is also displayed.
USA. 5Department of Materials Science and Engineering,
University of Tennessee, Knoxville, TN 37996, USA. (C) The effect of the Eu lattice distortion.The vertical dashed line depicts the preserved (110) mirror plane,
*Corresponding author. Email: dhsieh@caltech.edu and arrows show the displacement directions of the O(1) atoms.
Unlike the previously studied even-parity ne- metry is broken. Because of this property, optical smooth area free of surface striations (Fig. 2B).
matic phases, multipolar nematic order cannot be SHG has been used recently to study noncentro- Next, wide-field SHG images [section S2 of (36)]
experimentally identified by using charge trans- symmetric Weyl semimetals (31) and odd-parity were acquired on this area both above and below
port anisotropy measurements because the loss order in correlated iridates and cuprates (32, 33). Tc (Fig. 2C). For T > Tc, the SHG signal is
of inversion symmetry is manifested in the spin To completely resolve the structure of cijk for dominated by the electric dipole response at
texture of the Fermi surface. Moreover, observa- Cd2Re2O7, we used a recently developed high- the surface (cSijk ), where inversion symmetry is
tions of conventional nematic order have often speed rotational anisotropy (RA) technique (34, 35) necessarily broken. The observed spatial uni-
relied on an alignment of nematic directors by that involves focusing a beam of light obliquely formity of the intensity indicates a single cubic
using applied magnetic (4) or uniaxial strain (9) onto the surface of a single crystal and measuring structural domain. For T < Tc, a strong bulk
fields in order to measure macroscopic symmetry- variations in the intensity of reflected SHG light response (cBijk ) develops owing to the inversion-
breaking responses, but neither magnetic nor as the scattering plane is rotated about the sur- symmetrybreaking tetragonal distortion. Three
strain fields couple linearly to Qij because they face normal. By projecting the SHG signal radiated types of tetragonal domains with sharply defined
are parity-even. Nonlinear optical anisotropy mea- at different scattering plane angles f onto a linear boundaries are clearly resolved, associated
surements can overcome these challenges because circular locus of points on a stationary 2D de- with orientations of the main tetragonal axis along
they probe the structure of higher-rank susceptibi- tector (Fig. 2A), the experiment can be carried each of the three equivalent cubic lattice directions
lity tensors that contain full point group information out at very high rotational frequencies (~4 Hz), [section S4 of (36)]. Last, we performed scanning
(30) and can be performed in a spatially resolved which greatly enhances the sensitivity to small RA-SHG measurements [section S3 of (36)] with-
manner. Optical SHG is particularly well-suited changes in symmetry by averaging over laser in a single tetragonal domain. Because inver-
to identifying odd-parity phases because the fluctuations. sion symmetry is spontaneously broken at the
leading-order electric dipole contribution, which In order to isolate a single-phase domain for phase transition, domains with opposite parity,
is described by a third-rank susceptibility ten- detailed RA-SHG study, we carried out three which we label (+) or (), will naturally form.
Because the sign of cBijk reverses upon spatial
Fig. 2. Spatially resolved optical SHG anisotropy measurements. (A) Schematic multiplying charge-coupled device (EMCCD) camera. The polarizers and phase
of the RA-SHG setup. A circularly polarized laser beam (red) with center wave- mask rotate rapidly (black arrows), causing the SHG beam to trace out a circle
length at 800 nm is sent through a linear polarizer (to select either Pin or Sin on the camera as the scattering plane angle f changes. (B) Optical micrograph
polarization) and onto a phase mask. The +1 diffracted order is isolated and of the (111) surface of a Cd2Re2O7 single crystal. (C) Wide-field SHG image of a
redirected parallel to the optical axis by a collimating lens. After passing through striation-free region measured at T = 210 K and T = 150 K. All three types of
a dichroic mirror, the beam is focused by an objective lens onto the stationary tetragonal domains [section S4 of (36)] are visible in the low-temperature image.
sample to a spot size of ~30 mm.The reflected SHG beam (blue) is recollimated (D) Enlarged SHG image of the region over which scanning RA-SHG was
by the objective, passes through a second linear polarizer (to select either Pout or performed. PinPout RA-SHG patterns for two opposite parity domains are shown,
Sout polarization), and is deflected by the dichroic mirror onto a 2D electron- and an approximate domain boundary is drawn.
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