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Register a new userSpectroscopic determination of the atomic f-electron symmetry underlying hidden order in URu$_2$Si$_2$
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The low temperature hidden order state of URu$_2$Si$_2$ has long been a subject of intense speculation, and is thought to represent an as yet undetermined many-body quantum state not realized by other known materials. Here, X-ray absorption spectroscopy (XAS) and high resolution resonant inelastic X-ray scattering (RIXS) are used to observe electronic excitation spectra of URu$_2$Si$_2$, as a means to identify the degrees of freedom available to constitute the hidden order wavefunction. Excitations are shown to have symmetries that derive from a correlated $5f^2$ atomic multiplet basis that is modified by itinerancy. The features, amplitude and temperature dependence of linear dichroism are in agreement with ground states that closely resemble the doublet $Gamma_5$ crystal field state of uranium.
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Electrical resistivity measurements were performed on single crystals of URu$_2-x$Os$_x$Si$_2$ up to $x$ = 0.28 under hydrostatic pressure up to $P$ = 2 GPa. As the Os concentration, $x$ , is increased, (1) the lattice expands, creating an effective negative chemical pressure $P_{ch}$($x$), (2) the hidden order (HO) phase is enhanced and the system is driven toward a large-moment antiferromagnetic (LMAFM) phase, and (3) less external pressure $P_{c}$ is required to induce the HO to LMAFM phase transition. We compare the $T(x)$, $T(P)$ phase behavior reported here for the URu$_2-x$Os$_x$Si$_2$ system with previous reports of enhanced HO in URu$_2$Si$_2$ upon tuning with $P$, or similarly in URu$_2-x$Fe$_x$Si$_2$ upon tuning with positive $P_{ch}$($x$). It is noted that pressure, Fe substitution, and Os substitution are the only known perturbations that enhance the HO phase and induce the first order transition to the LMAFM phase in URu$_2$Si$_2$. We present a scenario in which the application of pressure or the isoelectronic substitution of Fe and Os ions for Ru results in an increase in the hybridization of the U-5$f$- and transition metal $d$-electron states which leads to electronic instability in the paramagnetic phase and a concurrent stability of HO (and LMAFM) in URu$_2$Si$_2$. Calculations in the tight binding approximation are included to determine the strength of hybridization between the U-5$f$ electrons and each of the isoelectronic transition metal $d$-electron states of Fe, Ru, and Os.
The observation of Ising quasiparticles is a signatory feature of the hidden order phase of URu$_2$Si$_2$. In this paper we discuss its nature and the strong constraints it places on current theories of the hidden order. In the hastatic theory such anisotropic quasiparticles are naturally described described by resonant scattering between half-integer spin conduction electrons and integer-spin Ising moments. The hybridization that mixes states of different Kramers parity is spinorial; its role as an symmetry-breaking order parameter is consistent with optical and tunnelling probes that indicate its sudden development at the hidden order transition. We discuss the microscopic origin of hastatic order, identifying it as a fractionalization of three body bound-states into integer spin fermions and half-integer spin bosons. After reviewing key features of hastatic order and their broader implications, we discuss our predictions for experiment and recent measurements. We end with challenges both for hastatic order and more generally for any theory of the hidden order state in URu$_2$Si$_2$.
A second-order phase transition is associated with emergence of an order parameter and a spontaneous symmetry breaking. For the heavy fermion superconductor URu$_2$Si$_2$, the symmetry of the order parameter associated with its ordered phase below 17.5 K has remained ambiguous despite 30 years of research, and hence is called hidden order (HO). Here we use polarization resolved Raman spectroscopy to specify the symmetry of the low energy excitations above and below the HO transition. These excitations involve transitions between interacting heavy uranium 5f orbitals, responsible for the broken symmetry in the HO phase. From the symmetry analysis of the collective mode, we determine that the HO parameter breaks local vertical and diagonal reflection symmetries at the uranium sites, resulting in crystal field states with distinct chiral properties, which order to a commensurate chirality density wave ground state.
At T$_0$ = 17.5 K an exotic phase emerges from a heavy fermion state in {ur}. The nature of this hidden order (HO) phase has so far evaded explanation. Formation of an unknown quasiparticle (QP) structure is believed to be responsible for the massive removal of entropy at HO transition, however, experiments and ab-initio calculations have been unable to reveal the essential character of the QP. Here we use femtosecond pump-probe time- and angle-resolved photoemission spectroscopy (tr-ARPES) to elucidate the ultrafast dynamics of the QP. We show how the Fermi surface is renormalized by shifting states away from the Fermi level at specific locations, characterized by vector $q_{<110>} = 0.56 pm 0.08$ {an}. Measurements of the temperature-time response reveal that upon entering the HO the QP lifetime in those locations increases from 42 fs to few hundred fs. The formation of the long-lived QPs is identified here as a principal actor of the HO.
Quantum materials are epitomized by the influence of collective modes upon their macroscopic properties. Relatively few examples exist, however, whereby coherence of the ground-state wavefunction directly contributes to the conductivity. Notable examples include the quantizing effects of high magnetic fields upon the 2D electron gas, the collective sliding of charge density waves subject to high electric fields, and perhaps most notably the macroscopic phase coherence that enables superconductors to carry dissipationless currents. Here we reveal that the low temperature hidden order state of URu$_2$Si$_2$ exhibits just such a connection between the quantum and macroscopic worlds -- under large voltage bias we observe non-linear contributions to the conductivity that are directly analogous to the manifestation of phase slips in one-dimensional superconductors [1], suggesting a complex order parameter for hidden order
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