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Isoelectronic perturbations to $f$-$d$-electron hybridization and the enhancement of hidden order in URu$_2$Si$_2$

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 Added by Christian Wolowiec
 Publication date 2020
  fields Physics
and research's language is English




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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.



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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.
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.
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.
We measured the polarized optical conductivity of URu$_2$Si$_2$ from room temperature down to 5 K, covering the Kondo state, the coherent Kondo liquid regime, and the hidden-order phase. The normal state is characterized by an anisotropic behavior between the ab plane and c axis responses. The ab plane optical conductivity is strongly influenced by the formation of the coherent Kondo liquid: a sharp Drude peak develops and a hybridization gap at 12 meV leads to a spectral weight transfer to mid-infrared energies. The c axis conductivity has a different behavior: the Drude peak already exists at 300 K and no particular anomaly or gap signature appears in the coherent Kondo liquid regime. When entering the hidden-order state, both polarizations see a dramatic decrease in the Drude spectral weight and scattering rate, compatible with a loss of about 50 % of the carriers at the Fermi level. At the same time a density-wave like gap appears along both polarizations at about 6.5 meV at 5 K. This gap closes respecting a mean field thermal evolution in the ab plane. Along the c axis it remains roughly constant and it fills up rather than closing.
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