The frequency-dependent transport through a nano-device containing a large-spin magnetic molecule is studied theoretically in the Kondo regime. Specifically, the effect of magnetic anisotropy on dynamical spin accumulation is of primary interest. Such accumulation arises due to finite off-diagonal in spin components of the dynamical conductance. Here, employing the Kubo formalism and the numerical renormalization group (NRG) method, we demonstrate that the dynamical transport properties strongly depend on magnetic configuration of the device and intrinsic parameters of the molecule. Specifically, the effect of dynamical spin accumulation is found to be greatly affected by the type of magnetic anisotropy exhibited by the molecule, and it develops for frequencies corresponding to the Kondo temperature. For the parallel magnetic configuration of the device, the presence of dynamical spin accumulation is conditioned by the interplay of ferromagnetic-lead-induced exchange field and the Kondo correlations.
The finite-frequency transport properties of a large-spin molecule attached to ferromagnetic contacts are studied theoretically in the Kondo regime. The focus is on the behavior of the dynamical conductance in the linear response regime, which is determined by using the numerical renormalization group method. It is shown that the dynamical conductance depends greatly on the magnetic configuration of the device and intrinsic parameters of the molecule. In particular, conductance exhibits characteristic features for frequencies corresponding to the dipolar and quadrupolar exchange fields resulti…
Dynamic response of spin accumulation to a time-dependent magnetic field has been investigated in a ferromagnetic/nonmagnetic bilayer under ferromagnetic resonance. In this system, magnetization precession driven by a microwave generates direct-current (dc) and alternate-current (ac) spin accumulation in the nonmagnetic layer by the spin pumping. The ac spin accumulation is coupled with the microwave magnetic field through a dynamical Hanle spin precession, giving rise to rectified spin accumulation comparable with the dc spin accumulation directly generated by the spin pumping.
We present a theoretical proposal for the Herzberg circuit and controlled accumulation of Berry's phase in a chirality-based coded qubit in a triangular triple quantum dot molecule with one electron spin each. The qubit is encoded in the two degenerate states of a three spin complex with total spin $S=1/2$. Using a Hubbard and Heisenberg model the Herzberg circuit encircling the degeneracy point is realized by adiabatically tuning the successive on-site energies of quantum dots and tunnel couplings across a pair of neighbouring dots. It is explicitly shown that encircling the degeneracy point …
Dynamical decoupling (DD) is an efficient tool for preserving quantum coherence in solid-state spin systems. However, the imperfections of real pulses can ruin the performance of long DD sequences. We investigate the accumulation and compensation of different pulse errors in DD using the electron spins of phosphorus donors in silicon as a test system. We study periodic DD sequences (PDD) based on spin rotations about two perpendicular axes, and their concatenated and symmetrized versions. We show that pulse errors may quickly destroy some spin states, but maintain other states with high fideli…
In this paper we investigate the spin-resolved thermoelectric properties of strongly correlated molecular junctions in the linear response regime. The magnetic molecule is modeled by a single orbital level to which the molecular core spin is attached by an exchange interaction. Using the numerical renormalization group method we analyze the behavior of the (spin) Seebeck effect, heat conductance and figure of merit for different model parameters of the molecule. We show that the thermopower strongly depends on the strength and type of the exchange interaction as well as the molecule's magnetic…
We study the spin and charge accumulation in junctions between a superconductor and a ferromagnet or a normal metal in the presence of a Zeeman magnetic field, when the junction is taken out of equilibrium by applying a voltage bias. We write down the most general form for the spin and charge current in such junctions, taking into account all spin-resolved possible tunneling processes. We make use of these forms to calculate the spin accumulation in NS junctions subjected to a DC bias, and to an AC bias, sinusoidal or rectangular. We observe that in the limit of negligeable changes on the supe…
Negative differential resistance - a decrease in current with increasing bias voltage - is a counter-intuitive effect that is observed in various molecular junctions. Here, we present a novel mechanism that may be responsible for such an effect, based on strong Coulomb interaction between electrons in the molecule and electrons on the atoms closest to the molecule. The Coulomb interaction induces electron-hole binding across the molecule-electrode interface, resulting in a renormalized and enhanced molecule-electrode coupling. Using a self-consistent non-equilibrium Green's function approach, …
Using the three-site Hubbard model and Floquet theorem, we investigate the dynamical behaviors of two electrons which are confined in a line-shape three quantum dot molecule driven by an AC electric field. Because the Hamiltonian contains no spin-flip terms, the six- dimension singlet state and nine-dimensional triplet state sub-spaces are decoupled and can be discussed respectively. In particular, the nine-dimensional triplet state sub-spaces can also be divided into 3 three-dimensional state sub-spaces which are fully decoupled. The analysis shows that the Hamiltonian in each three-dimension…
The dynamics of a molecular junction consisting of a PTCDA molecule between the tip of a scanning tunneling microscope and a Ag(111) surface have been investigated experimentally and theoretically. Repeated switching of a PTCDA molecule between two conductance states is studied by low-temperature scanning tunneling microscopy for the first time, and is found to be dependent on the tip-substrate distance and the applied bias. Using a minimal model Hamiltonian approach combined with density-functional calculations, the switching is shown to be related to the scattering of electrons tunneling thr…
The dynamical atom/molecule projection, recently used to probe fermion pairing, is fast compared to collective fermion times, but slow on the Feshbach resonance width scale. Theory of detuning-induced dynamics of molecules coupled to resonantly associating atom pairs, employing a time-dependent many-body Green's function approach, is presented. An exact solution is found, predicting a 1/3 power law for molecule production efficiency at fast sweep. The results for $s$- and p-wave resonances are obtained and compared. The predicted production efficiency agrees with experimental observations for …
We propose a nonequilibrium Monte Carlo (MC) approach to explore nonequilibrium dynamical ferromagnetism of interacting single molecule magnets (SMMs). Both quantum spin tunneling and thermally activated spin reversal are successfully implemented in the same MC simulation framework. Applied to a typical example, this simulation method satisfactorily reproduces experimental magnetization curves with experimental parameters. Our results show that both quantum and classical effects are essential to determine the hysteresis behaviors. This method is effective and reliable to gain deep insights int…
We present an experimental study of the {\em nonlinear} susceptibility of Mn$_{12}$ single-molecule magnets. We investigate both their thermal-equilibrium and dynamical nonlinear responses. The equilibrium results show the sensitivity of the nonlinear susceptibility to the magnetic anisotropy, which is nearly absent in the linear response for axes distributed at random. The nonlinear dynamic response of Mn$_{12}$ was recently found to be very large and displaying peaks reversed with respect to classical superparamagnets [F. Luis {\em et al.}, Phys. Rev. Lett. {\bf 92}, 107201 (2004)]. Here we …
We develop a nanoscale dynamical mean-field theory (nano-DMFT) to deal with strong Coulomb interaction effects in physical systems that are intermediate in size between atoms and bulk materials, taking into account the tunneling into nearby electrodes. Focusing on a simplified treelike geometry, the usual DMFT loop simply stops when the finite lattice is fully covered, starting with an initial seed provided by the electronic environment at the boundary. To illustrate this nano-DMFT, we investigate the disappearance of the quasiparticle weight in a correlated nano object near the Mott transitio…
In this paper, we combine thermal effects with Landau-Zener (LZ) quantum tunneling effects in a dynamical Monte Carlo (DMC) framework to produce satisfactory magnetization curves of single-molecule magnet (SMM) systems. We use the giant spin approximation for SMM spins and consider regular lattices of SMMs with magnetic dipolar interactions (MDI). We calculate spin reversal probabilities from thermal-activated barrier hurdling, direct LZ tunneling, and thermal-assisted LZ tunnelings in the presence of sweeping magnetic fields. We do systematical DMC simulations for Mn$_{12}$ systems with vario…
The generation and manipulation of carrier spin polarization in semiconductors solely by electric fields has garnered significant attention as both an interesting manifestation of spin-orbit physics as well as a valuable capability for potential spintronics devices. One realization of these spin-orbit phenomena, the spin Hall effect (SHE), has been studied as a means of all-electrical spin current generation and spin separation in both semiconductor and metallic systems. Previous measurements of the spin Hall effect have focused on steady-state generation and time-averaged detection, without d…
We study the influence of laser radiation on the electron transport through a molecular wire weakly coupled to two leads. In the absence of a generalized parity symmetry, the molecule rectifies the laser induced current, resulting in directed electron transport without any applied voltage. We consider two generic ways of dynamical symmetry breaking: mixing of different harmonics of the laser field and molecules consisting of asymmetric groups. For the evaluation of the nonlinear current, a numerically efficient formalism is derived which is based upon the Floquet solutions of the driven molecu…
Experimental measurements of electron transport properties of molecular junctions are often performed in solvents. Solvent-molecule coupling and physical properties of the solvent can be used as the external stimulus to control electric current through a molecule. In this paper, we propose a model, which includes dynamical effects of solvent-molecule interaction in the non-equilibrium Green's function calculations of electric current. The solvent is considered as a macroscopic dipole moment that reorients stochastically and interacts with the electrons tunnelling through the molecular junction…
