Mott localization in the correlated superconductor Cs3C60 resulting from the molecular Jahn-Teller effect
Katalin Kamaras, Gyongyi Klupp, Peter Matus, Alexey Y. Ganin, Alec McLennan, Matthew J. Rosseinsky, Yasuhiro Takabayashi, Martin T. McDonald, Kosmas Prassides
备注：
6 pages, 4 figures, 1 supplementary movie; XXI International Symposium on the Jahn-Teller Effect, Tsukuba, Japan, August 26-31, 2012
发表信息：
Journal of Physics: Conference Series 428 (2013) 012002
Cs3C60 is a correlated superconductor under pressure, but an insulator under ambient conditions. The mechanism causing this insulating behavior is the combination of Mott localization and the dynamic Jahn-Teller effect. We show evidence from infrared spectroscopy for the dynamic Jahn-Teller distortion. The continuous change with temperature of the splitting of infrared lines is typical Jahn-Teller behavior, reflecting the change in population of solid-state conformers. We conclude that the electronic and magnetic solid-state properties of the insulating state are controlled by molecular phenomena. We estimate the time scale of the dynamic Jahn-Teller effect to be above 10^(-11) s and the energy difference between the conformers less than 20 cm-1.
We present a theoretical study on the relation between the size of the rare earth ions, often known as chemical pressure, and the stability of the coherent Jahn-Teller distortions in undoped perovskite manganites. Using a Keating model expressed in terms of atomic scale symmetry modes, we show that there exists a coupling between the uniform shear distortion and the staggered buckling distortion within the Jahn-Teller energy term. It is found that this coupling provides a mechanism by which the coherent Jahn-Teller distortion is more stabilized by smaller rare earth ions. We analyze the appear…
The charge order of CE phase in half-doped manganites is studied, based on an argument that the charge-ordering is caused by the Jahn-Teller distortions of MnO6 octahedra rather than Coulomb repulsion between electrons. The uantitative calculation on the ferromagnetic zigzag chain as the basic structure unit of CE phase within the framework of two-orbital double exchange model including Jahn-Teller effect is performed, and it is shown that the charge-disproportionation of Mn cations in the charge-ordered CE phase is less than 13%. In addition, we predict the negative charge-disproportionation …
The Jahn-Teller effect is a fascinating and ubiquitous phenomenon in modern quantum physics and chemistry. We propose a class of oxides with melilite structure Ba$_2$TGe$_2$O$_7$ (T=V,Ni) where Jahn-Teller distortions are the main responsibles for the appearance of electric polarization. At the hearth of the proposed mechanism lies the lack of inversion symmetry displayed by tetrahedrally coordinated transition-metal ions, which allows for the condensation of polar Jahn-Teller distortions, at odds with octahedral coordination typical of conventional ferroelectric oxides with perovskite structu…
Distortions of the oxygen sublattice couple to $e_g$ orbitals of Mn$^{3+}$ and drive a cooperative Jahn-Teller (orbital ordering) transition in LaMnO$_3$. A simple model for this transition is studied. Without further adjustment, the model predicts the shape and stability of small (anti-Jahn-Teller) polarons which form when holes are doped into the material. This leads to a new description of the lightly doped insulator, the anti-ferromagnetic to ferromagnetic transition, and the metal-insulator transition.
The role of elastic interactions between Jahn-Teller ions in formation of various orbital- and charge-ordered structures in manganites and related compounds is analyzed. It is shown that such interactions alone are often sufficient to reproduce the structures observed in different regions of the phase diagram. A special attention is focused on stripe structures at high doping levels.
The presence/absence of a Berry phase depends on the topology of the manifold of dynamical Jahn-Teller potential minima. We describe in detail the relation between these topological properties and the way the lowest two adiabatic potential surfaces get locally degenerate. We illustrate our arguments through spherical generalizations of the linear T x h and H x h cases, relevant for the physics of fullerene ions. Our analysis allows us to classify all the spherical Jahn-Teller systems with respect to the Berry phase. Its absence can, but does not necessarily, lead to a nondegenerate ground stat…
We report the temperature dependent mid- and near-infrared spectra of K4C60, Rb4C60 and Cs4C60. The splitting of the vibrational and electronic transitions indicates a molecular symmetry change of C604- which brings the fulleride anion from D2h to either a D3d or a D5d distortion. In contrast to Cs4C60, low temperature neutron diffraction measurements did not reveal a structural phase transition in either K4C60 and Rb4C60. This proves that the molecular transition is driven by the molecular Jahn-Teller effect, which overrides the distorting potential field of the surrounding cations at high te…
Absorption spectra fine structure of $KDy(MoO_4)_2$ in the region of cooperative Jahn-Teller type ordering was studied. Temperature anomalies in the spectra occurring at phase transformation correlate with the ultrasound peculiarities observed earlier. Based on the symmetry approaching, possible activity of the irreducible representations of the rhombic $D_{2h}$ point group was discussed, which lead to the incommensurate phase at cooperative ordering. It was supposed, that coupled $A_u$-type phonon mode may lead to the incommensurate phase existence, which is possible at least in the temperatu…
We discuss the Kondo effect in a spinless two-orbital conduction electron system coupled with anharmonic Jahn-Teller vibration by employing a numerical renormalization group technique. When a temperature $T$ is decreased, we encounter a plateau of $\log 3$ entropy due to quasi-triple degeneracy of local low-energy states, composed of vibronic ground states and the first excited state with an excitation energy of $ΔE$. Around at $T$$\approx$$ΔE$, we observe an entropy change from $\log 3$ to $\log 2$. This $\log 2$ entropy originates from the rotational degree of freedom of the vibronic state a…
The Jahn-Teller effect is one of the most fundamental phenomena important not only for physics, but also for chemistry and material science. Solving the Jahn-Teller problem and taking into account strong electron correlations we show that quantum entanglement of the spin and orbital degrees of freedom via spin--orbit coupling strongly affects this effect. Depending on the number of $d$ electrons it may quench (electronic configurations $t_{2g}^2$, $t_{2g}^4$, and $t_{2g}^5$), partially suppress ($t_{2g}^1$) or in contrast induce ($t_{2g}^3$) Jahn-Teller distortions. Moreover, in certain situat…
Epitaxial thin films of stoichiometric ${\rm LaMnO_3}$ were grown on ${\rm SrTiO_3(110)}$ substrates using the pulsed laser deposition technique. From the high resolution x-ray diffraction measurements, the lattice parameters were determined as a function of temperature and the cooperative Jahn-Teller transition was found to occur at $T_{JT}$=573.0 K. Also measured was resonant x-ray scattering intensity of the orthorhombic (100) peak of ${\rm LaMnO_3}$ near the Mn K edge from low temperatures to above $T_{JT}$. We demonstrate that the integrated intensity of the (100) peak is proportional to …
We have studied the temperature dependence of crystal and magnetic structures of the Jahn-Teller distorted transition metal difluorides CrF$_2$ and CuF$_2$ by neutron powder diffraction in the temperature range 2-280 K. The lattice parameters and the unit cell volume show magnetoelastic effects below the Néel temperature. The lattice strain due to the magnetostriction effect couples with the square of the order parameter of the antiferromagnetic phase transition. We also investigated the temperature dependence of the Jahn-Teller distortion which does not show any significant effect at the anti…
The origin of the cooperative Jahn-Teller distortion and orbital-order in LaMnO3 is central to the physics of the manganites. The question is complicated by the simultaneous presence of tetragonal and GdFeO3-type distortions and the strong Hund's rule coupling between e_g and t_2g electrons. To clarify the situation we calculate the transition temperature for the Kugel-Khomskii superexchange mechanism by using the local density approximation+dynamical mean-field method, and disentangle the effects of super-exchange from those of lattice distortions. We find that super-exchange alone would yiel…
Based on previously computed parameters for the electron-phonon couplings and the Coulomb exchange, we compute and classify the static Jahn-Teller distortions, i.e. the minima of the lowest adiabatic potential energy surface, of C60(n+), for all values of charge 1 <= n <= 9 and spin. We compute the intra-band electronic excitation energies in the different optimal geometries in the sudden approximation, and find a spread of the electronic states of roughly 1 eV. We also obtain the leading vibronic quantum corrections to the ground-state energy, equal to zero-point energy lowering due to the so…
Single crystals of electron-doped SrMnO3 with a cubic perovskite structure have been systematically investigated as the most canonical (orbital-degenerate) double-exchange system, whose ground states have been still theoretically controversial. With only 1-2% electron doping by Ce substitution for Sr, a G-type antiferromagnetic metal with a tiny spin canting in a cubic lattice shows up as the ground state, where the Jahn-Teller polarons with heavy mass are likely to form. Further electron doping above 4%, however, replaces this isotropic metal with an insulator with tetragonal lattice distorti…
We present an ab-initio study of the Mn substitution for Ga in GaN using the Heyd-Scuseria-Ernzerhof hybrid functional (HSE). Contrary to semi-local functionals, the majority Mn t$_{2}$ manifold splits into an occupied doublet and an unoccupied singlet well above the Fermi-level resulting in an insulating groundstate, which is further stabilized by a sizeable Jahn-Teller distortion. The predictions are confirmed using $GW$ calculations and are in agreement with experiment. A transition from a localized to a delocalized Mn hole state is predicted from GaN to GaAs.
We analyze fulleride superconductivity at experimental doping levels, treating the electron-electron and electron-phonon interactions on an equal footing, and establish the existence of novel physics which helps explain the unusually high superconducting transition temperatures in these systems. The Jahn-Teller phonons create a local (intramolecular) pairing that is surprisingly resistant to the Coulomb repulsion, despite the weakness of retardation in these low-bandwidth systems. The requirement for coherence throughout the solid to establish superconductivity then yields a very strong doping…
Ultrasound velocity measurements of magnesium chromite spinel MgCr$_2$O$_4$ reveal elastic anomalies in the paramagnetic phase that are characterized as due to geometrical frustration. The temperature dependence of the tetragonal shear modulus $(C_{11}-C_{12})/2$ exhibits huge Curie-type softening, which should be the precursor to spin Jahn-Teller distortion in the antiferromagnetic phase. The trigonal shear modulus $C_{44}$ exhibits nonmonotonic temperature dependence with a characteristic minimum at $\sim$50 K, indicating a coupling of the lattice to dynamical molecular spin state. These res…
A recent Letter reports photoemission data for the free C60 molecule, showing an interesting three-peak structure, presented as evidence of dynamic Jahn-Teller (DJT) effect in the C60+ ion. Those data constitute, along with earlier spectra by the Uppsala group, the best available piece of experimental evidence about the spectrum of a hole in fullerene. DJT must indeed affect the fivefold-degenerate h_u hole molecular orbital, but we contend that the energy separation of these three peaks is far too large for the proposed tunneling interpretation to be correct.
Dynamical Jahn-Teller (DJT) effect in a spin-orbital coupled system on a honeycomb lattice is examined, motivated from recently observed spin-liquid behavior in Ba$_3$CuSb$_2$O$_9$. An effective vibronic Hamiltonian, where the superexchange interaction and the DJT effect are taken into account, is derived. We find that the DJT effect induces a spin-orbital resonant state where local spin-singlet states and parallel orbital configurations are entangled with each other. This spin-orbital resonant state is realized in between an orbital ordered state, where spin-singlet pairs are localized, and a…
LaMnO$_3$ is considered as a prototypical Jahn-Teller perovskite compound, exhibiting a metal to insulator transition at $T_{JT} = 750K$ related to the joint appearance of an electronic orbital ordering and a large lattice Jahn-Teller distortion. From first-principles, we revisit the behavior of LaMnO$_3$ and show that it is not only prone to orbital ordering but also to charge ordering. Both charge and orbital orderings appear to be enabled by rotations of the oxygen octahedra and the subtle competition between them is monitored by a large tetragonal compressive strain, that is itself a Jahn-…
We report on high-temperature electron spin resonance studies of a detwinned LaMnO$_3$ single crystal across the Jahn-Teller transition at $T_{\rm JT}$ = 750 K. The anisotropy of the linewidth and g-factor reflects the local Jahn-Teller distortions in the orbitally ordered phase. A clear jump in the linewidth accompanies the Jahn-Teller transition at $T_{\rm JT}$ = 750 K confirming that the transition is of first order. Already at $T^*$ = 550 K a significant decrease of the reduced linewidth is observed. This temperature scale is discussed with respect to the interaction of the $e_g$-electrons…
We introduce an effective model for $e_g$ electrons to describe quasi-two-dimensional layered La$_{2-x}$Sr$_{x}$NiO$_4$ nickelates and study it using correlated wave functions on $8 \times 8 $ and $6 \times 6 $ clusters. The effective Hamiltonian includes the kinetic energy, on-site Coulomb interactions for $e_g$ electrons (intraorbital $U$ and Hund's exchange $J_H$) and the coupling between $e_g$ electrons and Jahn-Teller distortions (static modes). The experimental ground state phases with inhomogeneous charge, spin and orbital order at the dopings $x=1/3$ and $x=1/2$ are reproduced very wel…
We present a thorough analysis of the interplay of magnetic moment and the Jahn-Teller effect in the $Γ_8$ cubic multiplet. We find that in the presence of dynamical Jahn-Teller effect, the Zeeman interaction remains isotropic, whereas the $g$ and $G$ factors can change their signs. The static Jahn-Teller distortion also can change the sign of these $g$ factors as well as the nature of the magnetic anisotropy. Combining the theory with state-of-the-art {\it ab initio} calculations, we analyzed the magnetic properties of Np$^{4+}$ and Ir$^{4+}$ impurity ions in cubic environment. The calculated…
Ultrasound velocity measurements of cubic spinel GeCo$_2$O$_4$ in single crystal were performed for the investigation of shear and compression moduli. The shear moduli in the paramagnetic state reveal an absence of Jahn-Teller activity despite the presence of orbital degeneracy in the Co$^{2+}$ ions. Such a Jahn-Teller inactivity indicates that the intersite orbital-orbital interaction is much stronger than the Jahn-Teller coupling. The compression moduli in the paramagnetic state near the N$\acute{e}$el temperature $T_N$ reveal that the most relevant exchange path for the antiferromagnetic tr…
We argue that the Jahn-Teller theorem, if applied to 3d-ion compounds, has to be considered in the orbital+spin space. It is despite of the weakness of the intraatomic spin-orbit coupling.
We propose a mechanism for A-type antiferromagnetism in orthorombic LaMnO_3, compatible with the large Jahn-Teller splitting inferred from structural data. Orbital ordering resulting from Jahn-Teller distortions effectively leads to A-type ordering (antiferromagnetic in the c axis and ferromagnetic in the ab plane) provided the in-plane distorsion Q_2 is large enough, a condition generally fulfilled in existing data.
We investigate how Kondo phenomenon occurs in the Anderson model dynamically coupled with local Jahn-Teller phonons. It is found that the total angular moment composed of electron pseudo-spin and phonon angular moments is screened by conduction electrons. Namely, phonon degrees of freedom essentially contribute to the formation of singlet ground state. A characteristic temperature of the Kondo effect due to dynamical Jahn-Teller phonons is explained by an effective $s$-$d$ Hamiltonian with anisotropic exchange interaction obtained from the Jahn-Teller-Anderson model in a non-adiabatic region.
Narrow-band conductors may turn insulating and magnetic as a consequence of strong electron-electron correlation. In molecular conductors, the concomitance of a strong Jahn-Teller coupling may give rise to the alternative possibility of a non-magnetic insulator, with or without a static cooperative Jahn-Teller distortion. In the latter case the insulator has Mott-like properties, with an interesting interplay between electron-electron repulsion and the Jahn-Teller effect, which is dynamical. We study this kind of non-magnetic insulator in a very simple $E\otimes e$ Jahn-Teller model and we dis…
The formation of a long-range Jahn-Teller distortion in undoped manganites is studied within the dynamical mean-field theory taking both electron-phonon and electron-electron interactions into account. We find that the observed insulating behavior at temperatures above the Jahn-Teller transition and the bond-length changes below it can most naturally by explained by assuming a strong electronic repulsion and a rather weak electron-phonon coupling.
We observe two consecutive transitions in La1-xCaxMnO3, x=0.19: ferromagnetic ordering at Tc = 177 K and Jahn-Teller orbital ordering at T_JT = 150 K. The presence of a ferromagnetic insulating state below T_JT shows that the metallic phase is bound by ferromagnetic and Jahn- Teller ordering, and not induced by a critical doping concentration. The A-site shift is found to be a good indicator of Jahn-Teller ordering. Furthermore, the A-site shift does not disapppear above T_JT, indicating a dynamical behaviour of the distorted MnO6 octahedra.
Temperature dependences of a magnetic and an orbital Bragg reflection at the Mn L2 and L3 edges of La0.5Sr1.5MnO4 have been collected. The temperature evolution of the orbital reflection depend strongly on the x-ray energy and reflects the different order parameteres for orbitals and Jahn-Teller distortions. The gradual increase of the orbital order parameter indicates that the orbital order and not the Jahn-Teller distortion drives the metal-insulator transition. Correspondingly, the orbital-orbital (super) exchange interaction dominates over the Jahn-Teller strain-field interaction.
In contrary to customarily consideration of the Jahn-Teller theorem for 3d-ion compounds in the orbital space only we point out that it has to be considered in the spin-orbital space. It is despite the weakness of the intraatomic spin-orbit coupling. A direct motivation for this paper is an erroneous claim of a recent Phys. Rev. Lett. 96 (2006) 027201 paper that the high-spin t2g4eg2 state of the 3d6 configuration is not Jahn-Teller active.
A realistic modeling of manganites should include the Coulomb repulsion between $e_g$ electrons, the Hund's rule coupling to $t_{2g}$ spins, and Jahn-Teller phonons. Solving such a model by dynamical mean field theory, we report large magnetoresistances and spectra in good agreement with experiments. The physics of the unusual, insulating-like paramagnetic phase is determined by correlated electrons which are-due to strong correlations-easily trapped as Jahn-Teller polarons.
Dynamical Jahn-Teller effect has escaped so far direct observation in metallic systems. It is particularly believed to be quenched also in correlated conductors with orbitally degenerate sites such as cubic fullerides. Here the Gutzwiller approach is extended to treat electron correlation over metals with Jahn-Teller active sites and applied to the investigation of the ground state of K$_3$C$_{60}$. It is shown that dynamical Jahn-Teller instability fully develops in this material when the interelectron repulsion $U$ on C$_{60}$ sites exceeds some critical value. The latter is found to be lowe…
We study the influence of the lattice structure, the Jahn-Teller effect and the Hund's rule coupling on a metal-insulator transition in AnC60 (A= K, Rb). The difference in lattice structure favors A3C60 (fcc) being a metal and A4C60 (bct) being an insulator, and the coupling to Hg Jahn-Teller phonons favors A4C60 being nonmagnetic. The coupling to Hg (Ag) phonons decreases (increases) the value Uc of the Coulomb integral at which the metal-insulator transition occurs. There is an important partial cancellation between the Jahn-Teller effect and the Hund's rule coupling.
In a two orbital double exchange model we formulate Jahn-Teller coupled charge density wave in one electron per lattice site limit. Softening of Jahn-Teller phonons corresponding to distortion modes $Q_2$ or $Q_3$ associated with perfect nesting of Fermi surface leads to this instability at low temperature. The gap equation for charge density wave state and its dependences on electron-lattice coupling are calculated explicitly when any one of the Jahn-Teller modes is excited cooperatively. We find that the $Q_2$ distortion mode yields lowest free energy. The calculated heat capacity for each m…
We investigate the electronic properties of multi-domain configurations in models for undoped manganites by means of variational and Monte Carlo techniques. These materials display simultaneous Jahn-Teller distortions and magnetic ordering. We find that a band of electronic states appears associated with Jahn-Teller domain walls, and this band is localized in the direction perpendicular to the walls. The energy and width of this band depends on the conformational properties of the domain walls. At finite temperatures, the conductance along the domain walls, induced by the localized domain wall…
The quadratic Jahn-Teller effect of C$_{60}^{n-}$ ($n=$ 1-5) is investigated from the first principles. Employing the density functional theory calculations with hybrid functional, the quadratic vibronic coupling constants of C$_{60}^-$ were derived. The warping of the adiabatic potential energy surface of C$_{60}^-$ by the quadratic vibronic coupling is estimated about 2 meV, which is much smaller than the Jahn-Teller stabilization energy ($\approx$ 50 meV). Because of the selection rule and the vibronic reduction, the quadratic coupling slightly modifies the vibronic states of C$_{60}$ anion…
It is shown that the layered antiferromagnetic order in stoechiometric LaMnO_3 cannot be understood purely from electronic interactions. On the contrary, it mainly results from strong cooperative Jahn-Teller deformations. Those involve a compression of the Mn-O octahedron along the c-axis (mode Q_3 < 0), while alternate Jahn-Teller deformations occur in the ab-plane (mode Q_2). These deformations stabilize a certain type of orbital ordering. The resulting superexchange couplings are calculated by exact diagonalization, taking into account both e_g and t_{2g} orbitals. The main result is that a…
Based on the magnetoresistance, magnetization, ultrasound, and crystallographic data, we studied the role of the cooperative Jahn-Teller effect in the charge ordered (CO) state for La1-xCaxMnO3. We found that, with increasing the fraction of Q3 mode of Jahn-Teller distortion and decreasing that of Q2 mode in the CO state, the magnetic structure evolves from CE-type to C-type and the orbital ordering changes from 3d(x2-r2)/3d(y2-r2)-type to 3d(x2-z2)-type, with the strength of ferromagnetism and the phase separation tendency being suppressed. At the same time, the stability of the CO state and …
The Raman scattering (RS) spectra of rhombohedral $LaMnO_3$ is considered. It is shown that broad high intensity RS line at 640 $cm^{-1}$ could be explained in the framework of cooperative dynamical Jahn-Teller effect. This hypothesis is illustrated through the lattice dynamics calculations explicitly allowing for the electron-phonon term both in crystal energy and in dynamical matrix. The averaging scheme for the one mode cooperative dynamical effect is proposed
The Jahn-Teller effect in the charge-ordered (CO) state for La1-xCaxMnO3 (0.5<x<0.87) was studied by measuring the low-temperature powder x-ray diffraction, internal friction, and shear modulus. We find that the electron-lattice interaction with the static Jahn-Teller distortion is the strongest near x=0.75 in the CO state. It was particularly observed that a crossover of the Jahn-Teller vibration mode from Q2 to Q3 near x=0.75 induces crossovers of the crystal structure from tetragonally compressed to tetragonally elongated orthorhombic, and of the magnetic structure from CE-type to C-type ne…
It is shown that the d8 electron system occurring in the Ni2+ ion can have the non-magnetic ground state in the atomic scale formed by the Jahn-Teller effect. The tetragonal/trigonal off-cubic lattice distortion for the octahedral site causes the splitting of the triplet 3A2g into a singlet-doublet structure with the non-magnetic singlet lying lower provided the intra-atomic spin-orbit coupling is taken into account.
When strong spin-orbit coupling removes orbital degeneracy, it would at the same time appear to render the Jahn-Teller mechanism ineffective. We discuss such a situation, the t_2g manifold of iridates, and show that, while the Jahn-Teller effect does indeed not affect the j_eff=1/2 antiferromagnetically ordered ground state, it leads to distinctive signatures in the j_eff=3/2 spin-orbit exciton. It allows for a hopping of the spin-orbit exciton between the nearest neighbor sites without producing defects in the j_eff=1/2 antiferromagnet. This arises because the lattice-driven Jahn-Teller mecha…
We study the unconventional insulating state in A_4C_{60} with a variety of approaches, including density functional calculations and dynamical mean-field theory. While the former predicts a metallic state, in disagreement with experiment, the latter yields a (paramagnetic) Mott-Jahn-Teller insulator. In that state, conduction between molecules is blocked by on-site Coulomb repulsion, magnetism is suppressed by intra-molecular Jahn-Teller effect, and important excitations (such as optical and spin gap) should be essentially intra-molecular. Experimental gaps of 0.5 eV and 0.1 eV respectively c…
We investigate the bipolaronic crossover and the pairing transition for a two-orbital model with Jahn-Teller coupling to a two-fold degenerate phonon mode. The evolution from weak to strong coupling is reminiscent of the behavior of the single-band Holstein model: The polaron crossover in which the electrons and phonons become strongly entangled occurs for a weaker coupling than the binding of bipolarons, which gives rise to a metal-insulator transition. Interestingly, a single bipolaronic transition takes place also when the two bands have significantly different bandwidths, as opposed to the…
The dynamical Jahn--Teller effect on fullerene sites in insulating Cs$_3$C$_{60}$ is investigated fully ab initio. The vibronic excitations of rotational type are at $\ge$65 cm$^{-1}$ while the net kinetic contribution to the Jahn--Teller stabilization energy constitutes ca 90 meV. This means that no localization of distortions by intermolecular interactions is possible in these fullerides, therefore, free rotations of deformations take place independently on each C$_{60}$. The latter destroy the orbital ordering and establish a conventional exchange interaction between $S=1/2$ on fullerene si…
We analyze the electronic structure of a mixed-valence ladder system. We find that structural anisotropy and complex electron correlations lead to on-rung charge localization and insulating character. Charge fluctuations within the rung of the ladder interact strongly to the lattice degrees of freedom, which gives rise to large pseudo Jahn--Teller effects. The phase transition in NaV$_2$O$_5$ should be driven by this kind of mechanism.
We employ a combination of density functional theory and dynamical mean-field theory to investigate the electronic structure of the recently synthesized insulator BaCrO$_3$. Our calculations show that Hund's coupling is responsible for strong correlation effects, which are however not sufficient to turn the system insulating. A finite Jahn-Teller distortion lifting the orbital degeneracy is necessary to stabilize an insulating state with orbital ordering and consequent magnetic ordering.
The properties of the polaron and bipolaron are explored in the 1D Jahn-Teller model with dynamical quantum phonons. The ground-state properties of the polaron and bipolaron are computed using a recently developed variational method. Dynamical properties of the ground state of a polaron are investigated by calculating the optical conductivity $σ(ω)$. Our numerical results suggest that the Jahn-Teller and Holstein polarons are similar. However, in the strong-coupling regime qualitative differences in $σ(ω)$ between the two models are found and discussed. The influence of the electron-phonon cou…
We have synthesized a new spinel oxide LiRh2O4 with a mixed-valent configuration of Rh3+ and Rh4+. At room temperature it is a paramagnetic metal, but on cooling, a metal-insulator transition occurs and a valence bond solid state is formed below 170 K. We argue that the formation of valence bond solid is promoted by a band Jahn-Teller transition at 230 K and the resultant confinement of t2g holes within the xy band. The band Jahn-Teller instability is also responsible for the observed enhanced thermoelectric power in the orbital disordered phase above 230 K.
The effect of Jahn-Teller phonons on the magnetic and orbital structure of LaMnO$_3$ is investigated using a combination of relaxation and Monte Carlo techniques on three-dimensional clusters of MnO$_6$ octahedra. In the physically relevant region of parameter space for LaMnO$_3$, and after including small corrections due to tilting effects, the A-type antiferromagnetic and C-type orbital structures were stabilized, in agreement with experiments.
The two-orbital Kondo model with classical Jahn-Teller phonons is studied using Monte Carlo techniques. The observed phase diagram is rich, and includes a novel regime of phase separation induced by the orbital degrees of freedom. Experimental consequences of our results are discussed. In addition, the optical conductivity $σ(ω)$ of the model is presented. It is shown to have several similarities with experimental measurements for manganites.
A synchrotron x-ray diffraction study of the crystallographic structure of PrO2 in the Jahn-Teller distorted phase is reported. The distortion of the oxygen sublattice, which was previously ambiguous, is shown to be a chiral structure in which neighbouring oxygen chains have opposite chiralities. A temperature dependent study of the magnetic excitation spectrum, probed by neutron inelastic scattering, is also reported. Changes in the energies and relative intensities of the crystal field transitions provide an insight into the interplay between the static and dynamic Jahn-Teller effects.
A recursive method is developed to treat electrons coupled to phonons. It is applied to small systems with $E\otimesβ$ Jahn-Teller coupling. Two cases are considered, a model with one electron and two orbitals on a single site (related to the Rabi Hamiltonian) and a model with two electrons on two sites. The corresponding Green's functions are represented by rational functions. It is found that the spectra change substantially when one phonon couples to the electron but are relatively robust under an increasing number of phonons.
We investigate the stability of the charge exchange (CE) phase within a microscopic model which describes a single plane as in La$_{0.5}$Sr$_{1.5}$MnO$_4$. The model includes Coulomb interactions (on-site and intersite), the Jahn-Teller term and the superexchange interactions due to $e_g$ and $t_{2g}$ electrons. By investigating the phase diagram at T=0 in mean-field approximation we conclude that the superexchange interactions can stabilize the CE phase, but only if they are stronger than estimated from spectroscopy.
