Hidden order and multipolar exchange striction in a correlated f-electron system

Abstract

The nature of order in low-temperature phases of some materials is not directly seen by experiment. Such "hidden orders" (HO) may inspire decades of research to identify the mechanism underlying those exotic states of matter. In insulators, HO phases originate in degenerate many-electron states on localized f or d shells that may harbor high-rank multipole moments. Coupled by inter-site exchange, those moments form a vast space of competing order parameters. Here, we show how the ground state order and magnetic excitations of a prototypical HO system, neptunium dioxide NpO${}_2$, can be fully described by a low-energy Hamiltonian derived by a many-body ab initio force-theorem method. Superexchange interactions between the lowest crystal-field quadruplet of Np${}^{4+}$ ions induce a primary non-collinear order of time-odd rank-5 (triakontadipolar) moments with a secondary quadrupole order preserving the cubic symmetry of NpO${}_2$. Our study also reveals an unconventional multipolar exchange-striction mechanism behind the anomalous volume contraction of the NpO${}_2$ HO phase.

arXiv commentFinal version, 12 pages, 4 figures. For Supporting information etc. see the published version (Open Access)

References in corpus (31)

• Correlated quantum phenomena in the strong spin-orbit regime
• First-principles Calculations of the Electronic Structure and Spectra of Strongly Correlated Systems: Dynamical Mean-field Theory
• TRIQS: A Toolbox for Research on Interacting Quantum Systems
• Dynamical Mean-Field Theory within an Augmented Plane-Wave Framework: Assessing Electronic Correlations in the Iron Pnictide LaFeAsO
• Colloquium: Hidden Order, Superconductivity, and Magnetism -- The Unsolved Case of URu2Si2
• Plane-wave based electronic structure calculations for correlated materials using dynamical mean-field theory and projected local orbitals
• Arrested Kondo effect and hidden order in URu_2Si_2
• TRIQS/DFTTools: A TRIQS application for ab initio calculations of correlated materials
• Heavy Fermion Superconductivity in the Quadrupole Ordered State of PrV2Al20
• Triple-q octupolar ordering in NpO_2
• Self-consistency over the charge-density in dynamical mean-field theory: a linear muffin-tin implementation and some physical implications
• Importance of electronic correlations for structural and magnetic properties of the iron pnictide superconductor LaFeAsO
• Hastatic Order in URu2Si2
• Novel Magnetism and Local Symmetry Breaking in a Mott Insulator with Strong Spin Orbit Interactions
• Ferro-quadrupolar ordering in PrTi${}_2$Al${}_{20}$
• First-principles LDA+U and GGA+U study of neptunium dioxide
• Octupolar vs Néel Order in Cubic 5$d^2$ double perovskites
• Multipolar phases and magnetically hidden order: Review of the heavy-fermion compound Ce(1-x)La(x)B6
• Crystal field splittings in rare earth-based hard magnets: an ab initio approach
• Successive Symmetry Breaking in a Jeff = 3/2 Quartet in the Spin-Orbit Coupled Insulator Ba2MgReO6
• Microscopic theory of the insulating electronic ground states of actinide dioxides AnO2 (An=U, Np, Pu, Am, and Cm)
• A perturbative approach to J mixing in f-electron systems: Application to actinide dioxides
• Electronic structure and core-level spectra of light actinide dioxides in the dynamical mean-field theory
• Invariant Form of Hyperfine Interaction with Multipolar Moments - Observation of Octupolar Moments in NpO${}_2$ and CeB${}_6$ by NMR -
• First-Principles Theory of Multipolar Order in Neptunium Dioxide
• Multipole ordering in f-electron systems on the basis of a j-j coupling scheme
• Two-site fluctuations and multipolar superexchange interactions in strongly correlated systems
• High-order crystal field and rare-earth magnetism in RECo5 intermetallics
• Quadrupolar Superexchange Interactions, Multipolar Order and Magnetic Phase Transition in UO${}_2$
• Calculation of Multipolar Exchange Interactions in Spin-Orbital Coupled Systems
• Hidden order and multipolar exchange striction in a correlated f-electron system

Cited by in corpus (17)

• Ferro-octupolar order and low-energy excitations in d${}^2$ double perovskites of Osmium
• Synchrotron Radiation Techniques and their Application to Actinide Materials
• Hidden order and multipolar exchange striction in a correlated f-electron system
• Modelling Magnetic Multipolar Phases in Density Functional Theory
• Exchange interactions in iron and nickel: DFT+DMFT study in paramagnetic phase
• Hidden orders in spin-orbit entangled correlated insulators
• Structure of the normal state and origin of Schottky anomaly in the correlated heavy fermion superconductor UTe2
• Multipolar exchange interaction and complex order in insulating lanthanides
• Exploring energy landscapes of charge multipoles using constrained density functional theory
• Multipolar interactions and magnetic excitation gap in d${}^3$ spin-orbit Mott insulators
• Dipolar-octupolar correlations and hierarchy of exchange interactions in Ce${}_2$Hf${}_2$O${}_7$
• Cascade of magnetic-field-driven quantum phase transitions in Ce3Pd20Si6
• Non-collinear magnetism engendered by a hidden another order
• PULSEE: A software for the quantum simulation of an extensive set of magnetic resonance observables
• Dipolar and quadrupolar correlations in the $5d^2$ Re-based double perovskites Ba${}_2$YReO${}_6$ and Ba${}_2$ScReO${}_6$
• Multipolar ferroelectricity in the Mott regime
• 5d-mediated indirect exchange and effective spin Hamiltonians in Ce triangular-lattice delafossites