Quasi-one-dimensional iron-based ladders and chains, with the 3$d$ iron electronic density $n = 6$, are attracting considerable attention. Recently, a new iron chain system Ba$_2$FeS$_3$, also with $n = 6$, was prepared under high-pressure and high-temperature conditions. Here, the magnetic and electronic phase diagrams are theoretically studied for this quasi-one-dimensional compound. Based on first-principles calculations, a strongly anisotropic one-dimensional electronic band behavior near the Fermi level was observed. In addition, a three-orbital electronic Hubbard model for this chain was constructed. Introducing the Hubbard and Hund couplings and studying the model via the density matrix renormalization group (DMRG) method, we studied the ground-state phase diagram. A robust staggered $uparrow$-$downarrow$-$uparrow$-$downarrow$ AFM region was unveiled in the chain direction, consistent with our density functional theory (DFT) calculations. Furthermore, at intermediate Hubbard $U$ coupling strengths, this system was found to display an orbital selective Mott phase (OSMP) with one localized orbital and two itinerant metallic orbitals. At very large $U/W$ ($W$ = bandwidth), the system displays Mott insulator characteristics, with two orbitals half-filled and one doubly occupied. Our results for high pressure Ba$_2$FeS$_3$ provide guidance to experimentalists and theorists working on this one-dimensional iron chalcogenide chain material.
An insulating ferromagnetic (FM) phase exists in the quasi-one-dimensional iron chalcogenide Ce$_2$O$_2$FeSe$_2$ but its origin is unknown. To understand the FM mechanism, here a systematic investigation of this material is provided, analyzing the competition between ferromagnetic and antiferromagnetic tendencies and the interplay of hoppings, Coulomb interactions, Hunds coupling, and crystal-field splittings. Our intuitive analysis based on second-order perturbation theory shows that large entanglements between doubly-occupied and half-filled orbitals play a key role in stabilizing the FM order in Ce$_2$O$_2$FeSe$_2$. In addition, via many-body computational techniques applied to a multi-orbital Hubbard model, the phase diagram confirms the proposed FM mechanism, in agreement with experiments.
We investigate spin chains with bilinear-biquadratic spin interactions as a function of an applied magnetic field $h$. At the Uimin-Lai-Sutherland (ULS) critical point we find a remarkable hierarchy of fractionalized excitations revealed by the dynamical structure factor $S(q,omega)$ as a function of magnetic field yielding a transition from a gapless phase to another gapless phase before reaching the fully polarized state. At $h=0$, the envelope of the lowest energy excitations goes soft at two points $q_1=2pi/3$ and $q_2=4pi/3$, dubbed the A-phase. With increasing field, the spectral peaks at each of the gapless points bifurcate and combine to form a new set of fractionalized excitations that soften at a single point $q=pi$ at $h_{c1}approx 0.94$. Beyond $h_{c1}$ the system remains in this phase dubbed the B-phase until the transition at $h_{c2}=4$ to the fully polarized phase. We discuss the central charge of these two gapless phases and contrast the behavior with that of the gapped Haldane phase in a field.
The entropy stabilized oxide Mg$_{0.2}$Co$_{0.2}$Ni$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$O exhibits antiferromagnetic order and magnetic excitations, as revealed by recent neutron scattering experiments. This observation raises the question of the nature of spin wave excitations in such disordered systems. Here, we investigate theoretically the magnetic ground state and the spin-wave excitations using linear spin-wave theory in combination with the supercell approximation to take into account the extreme disorder in this magnetic system. We find that the experimentally observed antiferromagnetic structure can be stabilized by a rhombohedral distortion together with large second nearest neighbor interactions. Our calculations show that the spin-wave spectrum consists of a well-defined low-energy coherent spectrum in the background of an incoherent continuum that extends to higher energies.
The biaxial van der Waals semiconductor $alpha$-phase molybdenum trioxide ($alpha$-MoO$_3$) has recently received significant attention due to its ability to support highly anisotropic phonon polaritons (PhPs) -infrared (IR) light coupled to lattice vibrations in polar materials-, offering an unprecedented platform for controlling the flow of energy at the nanoscale. However, to fully exploit the extraordinary IR response of this material, an accurate dielectric function is required. Here, we report the accurate IR dielectric function of $alpha$-MoO$_3$ by modelling far-field, polarized IR reflectance spectra acquired on a single thick flake of this material. Unique to our work, the far-field model is refined by contrasting the experimental dispersion and damping of PhPs, revealed by polariton interferometry using scattering-type scanning near-field optical microscopy (s-SNOM) on thin flakes of $alpha$-MoO$_3$, with analytical and transfer-matrix calculations, as well as full-wave simulations. Through these correlative efforts, exceptional quantitative agreement is attained to both far- and near-field properties for multiple flakes, thus providing strong verification of the accuracy of our model, while offering a novel approach to extracting dielectric functions of nanomaterials, usually too small or inhomogeneous for establishing accurate models only from standard far-field methods. In addition, by employing density functional theory (DFT), we provide insights into the various vibrational states dictating our dielectric function model and the intriguing optical properties of $alpha$-MoO$_3$.
Theoretical studies recently predicted the condensation of spin-orbit excitons at momentum $q$=$pi$ in $t_{2g}^4$ spin-orbit coupled three-orbital Hubbard models at electronic density $n=4$. In parallel, experiments involving iridates with non-integer valence states for the Ir ions are starting to attract considerable attention. In this publication, using the density matrix renormalization group technique we present evidence for the existence of a novel excitonic condensate at $n=3.5$ in a one-dimensional Hubbard model with a degenerate $t_{2g}$ sector, when in the presence of spin-orbit coupling. At intermediate Hubbard $U$ and spin-orbit $lambda$ couplings, we found an excitonic condensate at the unexpected momentum $q$=$pi/2$ involving $j_{textrm{eff}}=3/2,m=pm1/2$ and $j_{textrm{eff}}=1/2,m=pm1/2$ bands in the triplet channel, coexisting with an also unexpected block magnetic order. We also present the entire $lambda$ vs $U$ phase diagram, at a fixed and robust Hund coupling. Interestingly, this new `block excitonic phase is present even at large values of $lambda$, unlike the $n=4$ excitonic phase discussed before. Our computational study helps to understand and predict the possible magnetic phases of materials with $d^{3.5}$ valence and robust spin-orbit coupling.
We examine the accuracy of the microcanonical Lanczos method (MCLM) developed by Long, {it et al.} [Phys. Rev. B {bf 68}, 235106 (2003)] to compute dynamical spectral functions of interacting quantum models at finite temperatures. The MCLM is based on the microcanonical ensemble, which becomes exact in the thermodynamic limit. To apply the microcanonical ensemble at a fixed temperature, one has to find energy eigenstates with the energy eigenvalue corresponding to the internal energy in the canonical ensemble. Here, we propose to use thermal pure quantum state methods by Sugiura and Shimizu [Phys. Rev. Lett. {bf 111}, 010401 (2013)] to obtain the internal energy. After obtaining the energy eigenstates using the Lanczos diagonalization method, dynamical quantities are computed via a continued fraction expansion, a standard procedure for Lanczos-based numerical methods. Using one-dimensional antiferromagnetic Heisenberg chains with $S=1/2$, we demonstrate that the proposed procedure is reasonably accurate even for relatively small systems.
We report a quantum phase transition between orbital-selective Mott states, with different localized orbitals, in a Hunds metals model. Using the density matrix renormalization group, the phase diagram is constructed varying the electronic density and Hubbard $U$, at robust Hunds coupling. We demonstrate that this transition is preempted by charge fluctuations and the emergence of free spinless fermions, as opposed to the magnetically-driven Mott transition. The Luttinger correlation exponent is shown to have a universal value in the strong-coupling phase, whereas it is interaction dependent at intermediate couplings. At weak coupling we find a second transition from a normal metal to the intermediate-coupling phase.
The orbital-selective Mott phase (OSMP) of multiorbital Hubbard models has been extensively analyzed before using static and dynamical mean-field approximations. In parallel, the properties of Block states (antiferromagnetically coupled ferromagnetic spin clusters) in Fe-based superconductors have also been much discussed. The present effort uses numerically exact techniques in one-dimensional systems to report the observation of Block states within the OSMP regime, connecting two seemingly independent areas of research, and providing analogies with the physics of Double-Exchange models.
The undoped three-orbital spin fermion model for the Fe-based superconductors is studied via Monte Carlo techniques in two-dimensional clusters. At low temperatures, the magnetic and one-particle spectral properties are in good agreement with neutron and photoemission experiments. Our most important results are the resistance vs. temperature curves that display all the features experimentally observed in BaFe$_2$As$_2$ detwinned single crystals (under uniaxial stress), including a low-temperature anisotropy between the two directions followed by a peak at the magnetic ordering temperature, here induced by short-range spin order and concomitant Fermi Surface orbital order.
