We study equilibrium and non-equilibrium properties of a two-level quantum dot close to the singlet-triplet transition. We treat the on-site Coulomb interaction and Hund's rule coupling perturbatively within the Keldysh formalism. We compute the spectral functions and the differential conductance of the dot. For moderate interactions our perturbative approach captures the Kondo effect and many of the experimentally observed properties.
The low-lying singlet and triplet spectrum in conjugated polymers clearly show that the mechanism proposed by Lin et al. to explain their electric field dependence of singlet to triplet yield ratios is wrong. This comment, from theoretical spectrum obtained for long polyenes, shows that the phonon bottleneck proposed by Lin et al. for triplets in polyenes cannot exist.
New data for the two-dimensional J1-J2 model shows that the critical points for singlet and triplet excitations near J2/J1=0.38 are very close together, or coincident. We propose that this is a more general result: in strongly frustrated spin systems the critical dynamics of singlet and triplet excitations are closely related. An effective field theory for such a critical point, or points, is developed, and its implications discussed. The analysis suggests the existance of gapless or almost gapless singlet excitations in the magnetically disordered phase.
The t-J model is regarded as a canonical model of spin-singlet pairing induced by the {\em kinetic exchange interaction} responsible also for an antiferromagnetic ordering in the strongly correlated narrow-band systems. In the orbitally degenerate systems both ferromagnetic and antiferromagnetic kinetic exchange interactions occur. I review briefly the analogy between the singlet and triplet types of pairing, as well as draw some general conclusions about the pairing induced by these exchange interactions. The general discussion is also illustrated with a concrete case of a two-dimensional lat…
We have performed time-of-flight neutron scattering measurements on powder samples of the unconventional spin-Peierls compound TiOBr using the fine-resolution Fermi chopper spectrometer (SEQUOIA) at the SNS. These measurements reveal two branches of magnetic excitations within the commensurate and incommensurate spin-Peierls phases, which we associate with n = 1 and n = 2 triplet excitations out of the singlet ground state. These measurements represent the first direct measure of the singlet-triplet energy gap in TiOBr, which is determined to be Eg = 21.2 +/- 1.0 meV.
The spinel, MgTi$_2$O$_4$, undergoes a transition into a dimerized state at low temperatures that is expected to be a spin singlet. However, no signature of a singlet-triplet transition has been discovered, in part due to the difficulty of predicting the energy of the transition from theory. We find that the dimers of MgTi$_2$O$_4$ can be described by a Heisenberg model with very small interactions between different dimers. Using high-accuracy first-principles quantum Monte Carlo combined with a novel model-fitting approach, we predict the singlet-triplet gap of these dimers to be 350(50) meV,…
Dynamical properties are studied numerically for a variant of the Kondo model with singlet and triplet crystalline electric field (CEF) levels where Kondo and CEF singlets compete for the ground state. Using the continuous-time quantum Monte Carlo method, we derive the $t$-matrix of conduction electrons and dynamical susceptibilities of local electrons without encountering the negative sign problem. When the CEF splitting is comparable to the Kondo temperature, the dynamical response has only a quasi-elastic peak. Nevertheless, the local single-particle spectrum shows an energy gap in strong c…
As a continuation of a previous work [B. Horváth et al., Phys. Rev. B {\bf 82}, 165129 (2010)], here we extend the so-called Fluctuation Exchange Approximation (FLEX) to study the non-equilibrium singlet-triplet transition. We show that, while being relatively fast and a conserving approximation, FLEX is able to recover all important features of the transition, including the evolution of the linear conductance throughout the transition, the two-stage Kondo effect on the triplet side, and the gradual opening of the singlet-triplet gap on the triplet side of the transition. A comparison with num…
Dynamics of the singlet-triplet crystalline electric field (CEF) system at finite temperatures is discussed by use of the non-crossing approximation. Even though the Kondo temperature is smaller than excitation energy to the CEF triplet, the Kondo effect appears at temperatures higher than the CEF splitting, and accordingly only quasi-elastic peak is found in the magnetic spectra. On the other hand, at lower temperatures the CEF splitting suppresses the Kondo effect and inelastic peak develops. The broad quasi-elastic neutron scattering spectra observed in PrFe_4P_{12} at temperatures higher t…
We use a simple iterative perturbation theory to study the singlet-triplet (ST) transition in lateral and vertical quantum dots, modeled by the non-equilibrium two-level Anderson model. To a great surprise, the region of stable perturbation theory extends to relatively strong interactions, and this simple approach is able to reproduce all experimentally-observed features of the ST transition, including the formation of a dip in the differential conductance of a lateral dot indicative of the two-stage Kondo effect, or the maximum in the linear conductance around the transition point. Choosing t…
Have you been lying awake wondering what symmetries determine whether a superconductor is spin singlet, triplet, or both? We show that if BCS theory is supplied with additional degrees of freedom, spin singlet can coexist with spin triplet superconductivity. In the first part, we didactically guide the reader to the most general superconducting state using symmetry arguments. If both singlet and triplet pairing channels are present, a magnetic field can convert between spin singlet and triplet states. In the second part, we discuss two possible singlet-triplet superconductors: CeRh$_2$As$_2$ a…
Superconductivity of quasi-one-dimensional organic conductors with a quarter-filled band is investigated using the two-loop renormalization group approach to the extended Hubbard model for which both the single electron hopping t_{\perp} and the repulsive interaction V_{\perp} perpendicular to the chains are included. For a four-patches Fermi surface with deviations to perfect nesting, we calculate the response functions for the dominant fluctuations and possible superconducting states. By increasing V_{\perp}, it is shown that a d-wave (singlet) to f-wave (triplet) superconducting state cross…
In a previous article, we have investigated the non-equilibrium two-level Anderson model with a simple iterative perturbation theory. Here we use here a more sophisticated perturbative method, the fluctuation-exchange (FLEX) approximation. The great advantage of FLEX is its \textit{conserving} nature, and that it can describe well the Kondo energy scale, the Kondo-temperature, $T_{K}$. As it was expected from the results obtained with iterative perturbation theory, the FLEX description can give back also the relevant features of the spectral properties.
We present single crystal inelastic neutron scattering measurements of the S=1 dimerized quasi-two-dimensional antiferromagnet Ba$_3$Mn$_2$O$_8$. The singlet-triplet dispersion reveals nearest-neighbor and next-nearest-neighbor ferromagnetic interactions between adjacent bilayers that compete against each other. Although the inter-bilayer exchange is comparable to the intra-bilayer exchange, this additional frustration reduces the effective coupling along the c-axis and leads to a quasi-two dimensional behavior. In addition, the obtained exchange values are able to reproduce the four critical …
We discuss the pairing symmetry of a cobaltate superconductor Na$_x$CoO$_2\cdot y$ H$_2$O by adopting an effective single band model that takes into account the $e_g'$ hole pockets, as discussed in our previous paper [to appear in Phys. Rev. Lett.] Here we consider the off-site repulsions in addition to the on-site repulsion considered in our previous study. We show that the spin-triplet f-wave pairing proposed in our previous study is robust to some extent even in the presence of off-site repulsions. However, f-wave pairing gives way to singlet pairings for sufficiently large values of off-si…
In order to clarify magnetic properties of filled skutterudites, we analyze the Anderson model including seven $f$ orbitals hybridized with an $a_{\rm u}$ conduction band using a numerical technique. For $n$=2 corresponding to Pr-based filled skutterudites, where $n$ is the local $f$-electron number, even if the ground state is a singlet, there remain significant magnetic fluctuations from a triplet state with a small excitation energy. This result can be understood by the fact that $f$-electron states are clearly distinguished as itinerant and localized ones in the filled skutterudite structu…
High resolution neutron scattering measurements on a single crystal of SrCu(2-x)Mgx(BO3)2 with x=0.05 reveal the presence of new spin excitations within the gap of this quasi-two dimensional, singlet ground state system. Application of a magnetic field induces Zeeman-split states associated with S=1/2 unpaired spins which are antiferromagnetically correlated with the bulk singlet. Substantial broadening of both the one and two-triplet excitations in the doped single crystal is observed, as compared with pure SrCu2(BO3)2. Theoretical calculations using a variational algorithm and a single quenc…
We study spin relaxation in a two-electron quantum dot in the vicinity of the singlet-triplet crossing. The spin relaxation occurs due to a combined effect of the spin-orbit, Zeeman, and electron-phonon interactions. The singlet-triplet relaxation rates exhibit strong variations as a function of the singlet-triplet splitting. We show that the Coulomb interaction between the electrons has two competing effects on the singlet-triplet spin relaxation. One effect is to enhance the relative strength of spin-orbit coupling in the quantum dot, resulting in larger spin-orbit splittings and thus in a s…
Recent advances in singlet-fission research make it imperative that structure-property correlations that determine optical signatures of the triplet-triplet spin biexciton as well as its binding energy be understood precisely. We report many-body calculations of excited state absorptions from the triplet exciton and the triplet-triplet biexciton from two transversally linked dimers of pentacene derivatives. Comparison of experiment against theory leads to new interpretations of experiments performed earlier. We show that in the para-linked isomer the triplet-triplet does not dissociate to free…
We consider two interacting electrons in a semiconductor quantum dot structure which consists of a small dot within a larger dot, and demonstrate a singlet-triplet filtering mechanism which involves spin-dependent resonances and can generate entanglement. By studying the exact time evolution of singlet and triplet states we show how the degree of both filtering and spin entanglement can be tuned using a time-dependent gate voltage.
We show how in principle a coherent coupling between two superconductors of opposite parity can be realized in a three-layer oxide heterostructure. Due to strong intraionic spin-orbit coupling in the middle layer, singlet Cooper pairs are converted into triplet ones and vice versa. This results in a large enhancement of the triplet superconductivity, persisting well above the native triplet critical temperature.
We discuss transport through a lateral quantum dot in the vicinity of a singlet-triplet spin transition in its ground state. Extracting the scattering phase shifts from the numerical renormalization group spectra, we determine the linear conductance at zero temperature as a function of a Zeeman field and the splitting of the singlet and triplet states. We find reduced low-energy transport, and a non-monotonic magnetic field dependence both in the singlet and the triplet regime. For a generic set of dot parameters and no Zeeman splitting, the singlet-triplet transition may be identified with th…
Within the framework of periodic asymmetric Anderson model for Kondo isoulators an effective singlet-triplet Hamiltonian with indirect antiferromagnetic f-f exchange interaction is introduced which allows to study analytically the dynamic magnetic susceptibilities of f-electrons. The approach allows to describe the three-level spin excitation spectrum with a specific dispersion in $YbB_{12}$. Distinctive feature of the consideration is the introduction of small radius singlet and triplet collective f-d excitations which at movement on a lattice form low - and high-energy spin bands.
In present work the effective singlet-triplet model for CuO2-layer on the grounds of multiband p-d model of strongly correlated electrons is obtained. The resulting Hamiltonian has a form of generalized singlet-triplet t-t'-J model for p-type superconductors and form of usual t-t'-J model for n-type superconductors. In the mean field approximation in X-operator representation we derived equations for Gorkov type Green functions. The symmetry classification of the superconducting order parameter in case of tetragonal lattice resulted in d_{x^2-y^2}- and d_{xy}-types of singlet pairing for both …
We study the Anderson model in which a configuration with a doublet is hybridized with another with a singlet and a triplet. We calculate the conductance through the system as a function of temperature and bias voltage, near the quantum critical line for which the system is exactly solvable. The results explain recent transport measurements in a single-molecule quantum dot.
Based on symmetry constraint that leads to the appearance of nodes in the wave functions of 3-electron systems at regular triangle configurations, it was found that, if the parameters of confinement are skillfully given and if a magnetic field is tuned around the critical point of the singlet-triplet transition, a 2-electron quantum dot can be used as a highly sensitive switch for single-electron transport.
We propose a theoretical model of quasi-one-dimensional superconductors, with attractive electron-electron interactions dominant in the singlet d-wave channel and sub-dominant in the p-wave channel. We discuss, in the mean field approximation, the effect of a magnetic field applied perpendicularly to the direction of the lowest conductivity. The lowest free energy phase corresponds to a singlet d-wave symmetry in low fields, but to a triplet symmetry in high fields. A first order singlet-triplet phase transition is expected at moderate applied fields of a few teslas. We propose to ascribe the …
Recent experiments in quantum critical heavy fermion metals have pushed to the fore the question about whether antiferromagnetic fluctuations can promote both spin-singlet and spin-triplet superconductivity. Here we address the issue through non-perturbative calculations in antiferromagnetically correlated Kondo systems. We identify Kondo-destruction quantum critical points in both the SU(2) symmetric and Ising-anisotropic cluster Bose-Fermi Anderson models. The spin-singlet pairing correlations are significantly enhanced near the quantum critical point in the SU(2) case; however, with adequat…
We derive gap equations for superconductivity in coexistence with ferromagnetism. We treat singlet states and triplet states with either equal spin pairing (ESP) or opposite spin pairing (OSP) states, and study the behaviour of these states as a function of exchange splitting. For the s-wave singlet state we find that our gap equations correctly reproduce the Clogston--Chandrasekhar limiting behaviour and the phase diagram of the Baltensperger--Sarma equation (excluding the FFLO region). The singlet superconducting order parameter is shown to be independent of exchange splitting at zero temper…
We study the Coulomb-Fröhlich model on a triangular lattice, looking in particular at states with angular momentum. We examine a simplified model of crab bipolarons with angular momentum by projecting onto the low energy subspace of the Coulomb-Fröhlich model with large phonon frequency. Such a projection is consistent with large long-range electron-phonon coupling and large repulsive Hubbard $U$. Significant differences are found between the band structure of singlet and triplet states: The triplet state (which has a flat band) is found to be significantly heavier than the singlet state (whic…
We propose a two-dimensional exciton model showing the possibility of two-exciton pairing in cuprates, both in singlet and in triplet states. The former is assumed to be responsible for the superconductivity and the latter for the unusual normal state properties. The ground state is found to be a projection of the Bose condensation of N/2 mobile bosons with a ηprojection operator which is a generalization of the Gutzwiller projection operator. The phase diagram of the model shows insulator-superconductivity and superconductivity-metal transitions with doping.
We study two-electron states confined in two coupled quantum dots formed by a short-range potential in a two-dimensional topological insulator. It is shown that there is a fairly wide range of the system parameters, where the ground state is a tripletlike state formed by a superposition of two spin-polarized states. Outside this range, the ground state is a singlet. A transition between the singlet and triplet states can be realized by changing the potential of the quantum dots. The effect is caused by a significant change in the energies of the Coulomb repulsion and the exchange interaction o…
We present precise measurements of the upper critical field (Hc2) in the recently discovered cobalt oxide superconductor. We have found that the critical field has an unusual temperature dependence; namely, there is an abrupt change of the slope of Hc2(T) in a weak field regime. In order to explain this result we have derived and solved Gor'kov equations on a triangular lattice. Our experimental results may be interpreted in terms of the field-induced transition from singlet to triplet superconductivity.
By measuring the THz electron spin resonance (ESR) transmission spectra and high-field magnetization on the spin-gapped system CuTe$_2$O$_5$, we identified the singlet-triplet excitations in the dimerized non-magnetic ground state. The determined spin-gap value of $hν_0=4.94$ meV at the $Γ$ point ($\mathbf{Q}\simeq\mathbf{0}$) is significantly smaller than the strongest antiferromagnetic exchange interaction between the Cu ions predicted by theoretical investigations. We also observed the critical field $H_{c1}^{a^*}=37.6$ T for \textbf{H} $\bot$ \emph{bc}-plane and $H_{c1}^{bc}=40.6$ T for \t…
We have studied the competition and coexistence of staggered triplet SC with d-wave singlet SC and SDW in the mean-field approximation. Detailed numerical studies demonstrate that particle-hole asymmetry mixes these states and therefore they are simultaneously present. Even more interesting were the results of our study of the influence of a uniform magnetic field. We observe novel transitions that show the characteristics of Fulde-Ferrel phases, yet they concern transitions to different combinations of the above orders. For example, above a given field, in a particle-hole symmetric system we …
In the present paper, we propose the parity even,orbital singlet and spin triplet pairing state as the ground state of the newly discovered super-conductor $LaO_{1-x}F_xFeAs$.The pairing mechanism involves both the special shape of the electron fermi surface and the strong ferromagnetic fluctuation induced by Hund's rule coupling.The special behavior of the Bogoliubov quasi-particle spectrum may leads to "Fermi arc" like anisotropy super-conducting gap, which can be detected by angle resolved photo emission(ARPES).The impurity effects are also discussed.
The linear and nonlinear transport through a multi-level lateral quantum dot connected to two leads is investigated using a generalized finite-$U$ slave-boson mean field approach. For a two-level quantum dot, our calculation demonstrates a substantial conductance enhancement near the degeneracy point of the spin singlet and triplet states, a non-monotonic temperature-dependence of conductance and a sharp dip and nonzero bias maximum of the differential conductance. These agree well with recent experiment observations. This two-stage Kondo effect in an out-of-equilibrium situation is attributed…
We consider a Josephson junction with an arbitrary transmission coefficient $\mathcal{D}$ between a singlet and a triplet superconductor with the latter order parameter characterized by a d-vector of the form ($k_x\hat{y}-k_y\hat{x}$). Various quantities such as the tunnelling current, spin accumulation, and spin current are calculated via the quasiclassical Green's functions. We also present a symmetry argument on the existence of these quantities and their dependencies on the phase difference across the junction. A physical picture is also given in terms of the Andreev states near the juncti…
We investigate two serially-aligned quantum dots in the molecular regime of large tunnel couplings t. A Zeeman field B is used to tune the energy difference of singlet and triplet spin configurations. Attaching this geometry to BCS source and drain leads with gap Delta and phase difference phi gives rise to an equilibrium supercurrent J. To compute J in presence of Coulomb interactions U between the dot electrons, we employ the functional renormalization group (FRG). For B\simt -- where the singlet and lowest-lying triplet spin states are equal in energy -- the current exhibits characteristics…
Probing extended polyene systems with energy in excess of the bright state ($1^1B_u^+$/$S_2$) band edge generates triplets via singlet fission. This process is not thought to involve the $2^1A_g^-$/$S_1$ state, suggesting that other states play a role. Using density matrix renormalisation group (DMRG) calculations of the Pariser-Parr-Pople-Peierls Hamiltonian, we investigate candidate states that could be involved in singlet fission. We find that the relaxed $1^1B_u^-$, and $3^1A_g^-$ singlet states and $1^5A_g^-$ quintet state lie below the $S_2$ state. The $1^1B_u^-$, $3^1A_g^-$ and $1^5A_g^…
This work explores the possibility to transfer the parity law of the singlet-triplet gap established for square ladders (gapped for even number of legs, gapless for odd number of legs) to fused polyacenic 1-D systems, i.e., graphite ribbons. Qualitative arguments are presented in favor of a gapped character when the number $n\_ω$ of benzene rings along the ribbon width is odd. A series of numerical calculations (quantitative mapping on spin 1/2 chains, renormalized excitonic treatments and Quantum Monte Carlo) confirm the parity law and the gapless character of the ribbon for even $n\_ω$.
Employing a spin-parameterized Kleldysh-Usadel technique for the diffusive regime, we demonstrate that even in the low proximity limit, considerable long-ranged triplet supercurrents can be effectively generated by spin-singlet supercurrents flowing \textit{parallel} to the interfaces of uniform double ferromagnet interlayers with noncollinear exchange fields "{\it independent}" of actual junction geometry. The triplet supercurrents are found to be most pronounced when the thicknesses of the ferromagnet strips are unequal. To experimentally verify this generic phenomenon, we propose an accessi…
