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We study theoretically the formation of the nuclear-spin polaron state in semiconductor nanosystems within the Lindblad equation approach. To this end, we derive a general Lindblad equation for the density operator that complies with the symmetry of the system Hamiltonian and address the nuclear-spin polaron formation for localized charge carriers subject to an arbitrarily anisotropic hyperfine interaction when optically cooling the nuclei. The steady-state solution of the density matrix for an anisotropic central spin model is presented as a function of the electron and nuclear spin bath temperature. Results for the electron-nuclear spin correlator as well as data for the nuclear spin distribution function serve as a measure of spin-entanglement. The features in both of them clearly indicate the formation of the nuclear polaron state at low temperatures where the crossover regime coincides with an enhancement of quantum fluctuations and agrees with the mean-field prediction of the critical temperature line. We can identify two distinct polaron states dependent upon the hyperfine anisotropy which are separated by a quantum phase transition at the isotropic point. These states are reflected in the temporal spin auto-correlation functions accessible in experiment via spin-noise measurements., 19 pages, 8 figures

Two-color spin-noise spectroscopy of interacting electron spins in singly charged semiconductor quantum dots provides information on the inter quantum dot interactions. We investigate the spin cross-correlation function in a quantum dot ensemble using a modified semiclassical approach. Spin-correlation functions are calculated using a Hamilton quaternion approach maintaining local quantum mechanical properties of the spins. This method takes into account the effects of the nuclear-electric quadrupolar interactions, the randomness of the coupling constants, and the electron g factor on the spin-noise power-spectra. We demonstrate that the quantum dot ensemble can be mapped on an effective two-quantum dot problem and discuss how the characteristic length scale of the inter-dot interaction modifies the low-frequency cross-correlation spectrum. We argue that details on the interaction strength distribution can be extracted from the cross-correlation spectrum when applying a longitudinal or a transversal external magnetic field., 19 pages, 7 figures

The antiferromagnetic ordering in Mott insulators upon lowering the temperature is accompanied by a transfer of the single-particle spectral weight to lower energies and a shift of the Mott gap to higher energies (magnetic blue shift, MBS). The MBS is governed by the double exchange and the exchange mechanisms. Both mechanisms enhance the MBS upon increasing the number of orbitals. By performing a polynomial fit to numerical dynamical mean-field theory data we provide an expansion for the MBS in terms of hopping and exchange coupling of a prototype Hubbard-Kondo-Heisenberg model and discuss how the results can be generalized for application to realistic Mott or charge-transfer insulator materials. This allows estimating the MBS of the charge gap in real materials in an extremely simple way avoiding extensive theoretical calculations. The approach is exemplarily applied to $\alpha$-MnTe, NiO, and BiFeO$_3$ and an MBS of about $130$ meV, $360$ meV, and $157$ meV is found, respectively. The values are compared with the previous theoretical calculations and the available experimental data. Our ready-to-use formula for the MBS simplifies the future studies searching for materials with a strong coupling between the antiferromagnetic ordering and the charge excitations, which is paramount to realize a coupled spin-charge coherent dynamics at a femtosecond time scale., Comment: 17 pages, 13 figures

We present a microscopic model for a singly charged quantum dot (QD) ensemble to reveal the origin of the long-range effective interaction between the electron spins in the QDs. Wilson's numerical renormalization group (NRG) is used to calculate the magnitude and the spatial dependency of the effective spin-spin interaction mediated by the growth induced wetting layer. Surprisingly, we found an antiferromagnetic Heisenberg coupling for very short inter-QD distances that is caused by the significant particle-hole asymmetry of the wetting layer band at very low filling. Using the NRG results obtained from realistic parameters as input for a semiclassical simulation for a large QD ensemble, we demonstrate that the experimentally reported phase shifts in the coherent spin dynamics between single and two color laser pumping can be reproduced by our model, solving a longstanding mystery of the microscopic origin of the inter QD electron spin-spin interaction., Comment: 4 pages, 3 figure and a supplement

The light-induced femtosecond dynamics of the sublattice magnetizations in the antiferromagnetically ordered phase of the semiconductor $\alpha$-MnTe is investigated theoretically as function of an external driving field. The electromagnetic field is coupled to optical modes and the concomitant atomic displacements modulate the Heisenberg exchange couplings. We derive the equations of motion for the time-dependent sublattice magnetization in spin wave theory and analyze the contributions from the driven magnon modes. The antiferromagnetic order parameter exhibits coherent longitudinal oscillations determined by the external driving frequency which decay due to dephasing. Including a phenomenological dissipative term to mimic spin-lattice relaxation processes leads to relaxation back to thermal equilibrium. We provide approximate analytic solutions of the resulting differential equations which allow us to understand the effect of the driving light pulse on the amplitude, frequency, and lifetime of the coherent spin dynamics., Comment: 20 pages, 15 figures

The emerging and screening of local magnetic moments in solids have been investigated for more than 60 years. Local vacancies as in graphene or in heavy fermions can induce decoupled bound states that lead to the formation of local moments. In this paper, we address the puzzling question how these local moments can be screened and what determines the additionally emerging low-temperature scale. We review the initial problem for half-filled conduction bands from two complementary perspectives: By a single-particle supercell analysis in the uncorrelated limit and by the Lieb-Mathis theorem for systems with a large Coulomb interaction $U$. Applying Wilson's numerical renormalization group approach to a recently developed mapping of the problem onto an effective low-energy description of a Kondo hole with up to ${N}_{f}=7$ correlated impurities as background, we proof that the stable local moments are subject to screening by three different mechanisms. Firstly the local moments are delocalized by a finite $U$ beyond the single-particle bound state. We find a Kosterlitz-Thouless type transition governed by an exponentially suppressed low-energy scale of a counterintuitive Kondo form with ${J}_{\mathrm{eff}}\ensuremath{\propto}{U}^{n}$ for small $U$, where $ng1$ depends on the precise model. Secondly, we show that away from half-filling the local moment phase becomes unstable and is replaced by two types of singlet phases that are adiabatically connected. At a critical value for the band center, the physics is governed by an exponentially suppressed Kondo scale approaching the strong coupling phase that is replaced by a singlet formation via antiferromagnetic RKKY interaction for large deviation from the critical values. Thirdly, we show that the local magnetic moment can be screened by a Kondo hole orbital at finite energy, even though the orbital occupation is negligible: An additional low-energy scale emerges below which the localized moment is quenched. Similarities to the experimental findings in ${\mathrm{Ce}}_{1\ensuremath{-}x}{\mathrm{La}}_{x}{\mathrm{Pd}}_{3}$ are pointed out.

We investigate the real-space spectral properties of strongly-correlated multi-impurity arrays in the Kondo insulator regime. Employing a recently developed mapping onto an effective correlated cluster problem makes the problem accessible to the numerical renormalization group. The evolution of the spectrum as function of cluster size and cluster site is studied. We applied the extended Lieb-Mattis theorem to predict whether the spectral function must vanish at the Fermi energy developing a true pseudo-gap or whether the spectral function remains finite at $\w=0$. Our numerical renormalization group spectra confirm the predictions of the theorem and shows a metallic behavior at the surface of a cluster prevailing in arbitrary spatial dimensions. We present a conventional minimal extension of a particle-hole symmetric Anderson lattice model at $U=0$ that leads to a gapped bulk band but a surface band with mainly $f$-orbital character for weak and moderate hybridization strength. The change in the site-dependent spectra upon introducing a Kondo hole in the center of the cluster are presented as a function of the hole-orbital energy. In particular the spectral signatures across the Kosterlitz-Thouless type quantum phase transition from a singlet to a local moment fixed point are discussed., Comment: 15 pages,15 figures

We present a mapping of correlated multi-impurity Anderson models to a cluster model coupled to a number of effective conduction bands capturing its essential low-energy physics. The major ingredient is the complex single-particle self energy matrix of the uncorrelated problem that encodes the influence to the host conduction band onto the dynamics of a set of correlated orbitals. While the real part of the self-energy matrix generates an effective hopping between the cluster orbitals, the imaginary part determines the coupling to the effective conduction bands in the mapped model. The rank of the imaginary part determines the number of independent screening channels of the problem, and allows the replacement of the phenomenological exhaustion criterion by a rigorous mathematical statement. This rank provides a distinction between multi-impurity models of first kind and of second kind. For the latter, there are insufficient screening channels available, so that a singlet ground state must be driven by the inter-cluster spin correlations. This classification provides a fundamental answer to the question of why ferromagnetic correlations between local moments are irrelevant for the spin compensated ground state in dilute impurity models, whereas they compete with the Kondo-scale in dense impurity arrays, without evoking a spin density wave. The low-temperature physics of three examples taken from the literature are deduced from the analytic structure of the mapped model, demonstrating the potential power of this approach. NRG calculations are presented for up to five site cluster. We investigate the appearance of frustration induced non-Fermi liquid fixed points in the trimer, and demonstrate the existence of several critical points of KT type at which ferromagnetic correlations suppress the screening of an additional effective spin-$1/2$ degree of freedom.

Under optical cooling of nuclei, a strongly correlated nuclear-spin polaron state can form in semiconductor nanostructures with localized charge carriers due to the strong hyperfine interaction of the localized electron spin with the surrounding nuclear spins. Here we develop a kinetic-equation formalism describing the nuclear-spin polaron formation. We present a derivation of the kinetic equations for an electron-nuclear spin system coupled to reservoirs of different electron and nuclear spin temperatures which generate the exact thermodynamic steady state for equal temperatures independent of the system size. We illustrate our approach using the analytical solution of the central spin model in the limit of an Ising form of the hyperfine coupling. For homogeneous hyperfine coupling constants, i.e., the box model, the model is reduced to an analytically solvable form. Based on the analysis of the nuclear-spin distribution function and the electron-nuclear spin correlators, we derive a relation between the electron and nuclear spin temperatures, where the correlated nuclear-spin polaron state is formed. In the limit of large nuclear baths, this temperature line coincides with the critical temperature of the mean-field theory for polaron formation. The criteria of the polaron formation in a finite-size system are discussed. We demonstrate that the system's behavior at the transition temperature does not depend on details of the hyperfine-coupling distribution function but only on the effective number of coupled bath spins. In addition, the kinetic equations enable the analysis of the temporal formation of the nuclear-polaron state, where we find the build-up process predominated by the nuclear spin-flip dynamics., 11 pages, 5 figures

The continuous coupling function in quantum impurity problems is exactly partitioned into a part represented by a finite size Wilson chain and a part represented by a set of additional reservoirs, each coupled to one Wilson chain site. These additional reservoirs represent high-energy modes of the environment neglected by the numerical renormalization group and are required to restore the continuum limit of the original problem. We present a hybrid time-dependent numerical renormalization group approach which combines an accurate numerical renormalization group treatment of the non-equilibrium dynamics on the finite size Wilson chain with a Bloch-Redfield formalism to include the effect of these additional reservoirs. Our approach overcomes the intrinsic shortcoming of the time-dependent numerical renormalization group approach induced by the bath discretization with a Wilson parameter $\Lambda > 1$. We analytically prove that for a system with a single chemical potential, the thermal equilibrium reduced density operator is the steady-state solution of the Bloch-Redfield master equation. For the numerical solution of this master equation a Lanczos method is employed which couples all energy shells of the numerical renormalization group. The presented hybrid approach is applied to the real-time dynamics in correlated fermionic quantum-impurity systems. An analytical solution of the resonant-level model serves as a benchmark for the accuracy of the method which is then applied to non-trivial models, such as the interacting resonant-level model and the single impurity Anderson model., Comment: 27 papes, 18 figures

We analyze the ground-state energy, local spin correlation, impurity spin polarization, impurity-induced magnetization, and corresponding zero-field susceptibilities of the symmetric single-impurity Kondo model on a tight-binding chain with bandwidth $W=2{\cal D}$ and coupling strength $J_{\rm K}$. We compare perturbative results and variational upper bounds from Yosida, Gutzwiller, and first-order Lanczos wave functions to the numerically exact data obtained from the Density-Matrix Renormalization Group (DMRG) and from the Numerical Renormalization Group (NRG) methods. The Gutzwiller variational approach becomes exact in the strong-coupling limit and reproduces the ground-state properties from DMRG and NRG for large couplings. We calculate the impurity spin polarization and its susceptibility in the presence of magnetic fields that are applied globally/locally to the impurity spin. The Yosida wave function provides qualitatively correct results in the weak-coupling limit. In DMRG, chains with about $10^3$ sites are large enough to describe the susceptibilities down to $J_{\rm K}/{\cal D}\approx 0.5$. For smaller Kondo couplings, only the NRG provides reliable results for a general host-electron density of states $\rho_0(\epsilon)$. To compare with results from Bethe Ansatz, we study the impurity-induced magnetization and zero-field susceptibility. For small Kondo couplings, the zero-field susceptibilities at zero temperature approach $\chi_0(J_{\rm K}\ll {\cal D})/(g\mu_{\rm B})^2\approx \exp[1/(\rho_0(0)J_{\rm K})]/(2C{\cal D}\sqrt{\pi e \rho_0(0)J_{\rm K}})$, where $\ln(C)$ is the regularized first inverse moment of the density of states. Using NRG, we determine the universal sub-leading corrections up to second order in $\rho_0(0)J_{\rm K}$., Comment: 66 pages (26 pages main text, 12 pages appendices, 28 pages supplemental material), 23 figures

We study the conductance of a time-reversal symmetric helical electronic edge coupled antiferromagnetically to a magnetic impurity, employing analytical and numerical approaches. The impurity can reduce the perfect conductance $G_0$ of a noninteracting helical edge by generating a backscattered current. The backscattered steady-state current tends to vanish below the Kondo temperature $T_K$ for time-reversal symmetric setups. We show that the central role in maintaining the perfect conductance is played by a global $U(1)$ symmetry. This symmetry can be broken by an anisotropic exchange coupling of the helical modes to the local impurity. Such anisotropy, in general, dynamically vanishes during the renormalization group (RG) flow to the strong coupling limit at low-temperatures. The role of the anisotropic exchange coupling is further studied using the time-dependent Numerical Renormalization Group (TD-NRG) method, uniquely suitable for calculating out-of-equilibrium observables of strongly correlated setups. We investigate the role of finite bias voltage and temperature in cutting the RG flow before the isotropic strong-coupling fixed point is reached, extract the relevant energy scales and the manner in which the crossover from the weakly interacting regime to the strong-coupling backscattering-free screened regime is manifested. Most notably, we find that at low temperatures the conductance of the backscattering current follows a power-law behavior $G\sim (T/T_K)^2$, which we understand as a strong nonlinear effect due to time-reversal symmetry breaking by the finite-bias.

We present an extension of the tunneling theory for scanning tunneling microcopy (STM) to include different types of vibrational-electronic couplings responsible for inelastic contributions to the tunnel current in the strong-coupling limit. It allows for a better understanding of more complex scanning tunneling spectra of molecules on a metallic substrate in separating elastic and inelastic contributions. The starting point is the exact solution of the spectral functions for the electronic active local orbitals in the absence of the STM tip. This includes electron-phonon coupling in the coupled system comprising the molecule and the substrate to arbitrary order including the anti-adiabatic strong coupling regime as well as the Kondo effect on a free electron spin of the molecule. The tunneling current is derived in second order of the tunneling matrix element which is expanded in powers of the relevant vibrational displacements. We use the results of an ab-initio calculation for the single-particle electronic properties as an adapted material-specific input for a numerical renormalization group approach for accurately determining the electronic properties of a NTCDA molecule on Ag(111) as a challenging sample system for our theory. Our analysis shows that the mismatch between the ab-initio many-body calculation of the tunnel current in the absence of any electron-phonon coupling to the experiment scanning tunneling spectra can be resolved by including two mechanisms: (i) a strong unconventional Holstein term on the local substrate orbital leads to reduction of the Kondo temperature and (ii) a different electron-vibrational coupling to the tunneling matrix element is responsible for inelastic steps in the $dI/dV$ curve at finite frequencies., 34 pages, 26 figure

In normal metals, the magnetic-moment of impurity-spins disappears below a characteristic Kondo temperature, TK. This marks the formation of a polarized cloud of conduction band electrons that screen the magnetic moment . In contrast, moments embedded in insulators remain unscreened at all temperatures. This raises the question about the fate of magnetic-moments in intermediate, pseudogap systems, such as graphene. In these systems coupling between the local moment and the conduction band electrons is predicted to drive a quantum phase-transition between a local-moment phase and a Kondo-screened singlet phase as illustrated in Fig. 1A. However, attempts to experimentally confirm these predictions and their intriguing consequences such as the ability to electrostatically tune magnetic-moments, have been elusive. Here we report the observation of Kondo screening and the quantum phase-transition between screened and unscreened phases of vacancy magnetic-moments in graphene. Using scanning-tunneling-microscopy (STM), spectroscopy (STS) and numerical-renormalization-group (NRG) calculations, we identified Kondo-screening by its spectroscopic signature and mapped the quantum phase-transition as a function of coupling strength and chemical potential. We show that the coupling strength can be tuned across this transition by variations in the local curvature and furthermore that the transition makes it possible to turn the magnetic-moment on and off with a gate voltage., 28 pages 9 figures. arXiv admin note: substantial text overlap with arXiv:1711.06942

Spin noise spectroscopy has developed into a very powerful tool to access the electron spin dynamics. While the spin-noise power spectrum in an ensemble of quantum dots in a magnetic field is essentially understood, we argue that the investigation of the higher order cumulants promises to provide additional information not accessible by the conventional power noise spectrum. We present a quantum mechanical approach to the correlation function of the spin-noise power operators at two different frequencies for small spin bath sizes and compare the results with a simulation obtained from the classical spin dynamics for large number of nuclear spins. This bispectrum is defined as a two-dimensional frequency cut in the parameter space of the fourth-order spin correlation function. It reveals information on the influence of the nuclear-electric quadrupolar interactions on the long-time electron spin dynamics dominated by a magnetic field. For large bath sizes and spin lengths the quantum mechanical spectra converge to those of the classical simulations. The broadening of the bispectrum across the diagonal in the frequency space is a direct measure of the quadrupolar interaction strength. A narrowing is found with increasing magnetic field indicating a suppression of the influence of quadrupolar interactions in favor of the nuclear Zeeman effect., Comment: 15 pages, 14 figures

We study theoretically the electron spin noise in quantum dots under non-equilibrium conditions caused by the pumping by a train of circularly polarized optical pulses. In such a situation, the nuclear spins are known to adjust in such a way, that the electron spin precession frequencies become multiples of the pump pulse repetition frequency. This so called phase synchronization effect was uncovered in [Science {\bf 317}, 1896 (2007)] and termed nuclei-induced frequency focusing of electron spin coherence. Using the classical approach to the central spin model we evaluate the nuclear spin distribution function and the electron spin noise spectrum. We show that the electron spin noise spectrum consists of sharp peaks corresponding to the phase synchronization conditions and directly reveal the distribution of the nuclear spins. We discuss the effects of nuclear spin relaxation after the pumping is over and analyze the corresponding evolution of nuclear spin distributions and electron spin noise spectra., 8 pages, 5 figures

Periodic laser pulsing of singly charged semiconductor quantum dots in an external magnetic field leads to a synchronization of the spin dynamics with the optical excitation. The pumped electron spins partially rephase prior to each laser pulse, causing a revival of electron spin polarization with its maximum at the incidence time of a laser pulse. The amplitude of this revival is amplified by the frequency focusing of the surrounding nuclear spins. Two complementary theoretical approaches for simulating up to 20 million laser pulses are developed and employed that are able to bridge between 11 orders of magnitude in time: a fully quantum mechanical description limited to small nuclear bath sizes and a technique based on the classical equations of motion applicable for a large number of nuclear spins. We present experimental data of the nonmonotonic revival amplitude as function of the magnetic field applied perpendicular to the optical axis. The dependence of the revival amplitude on the external field with a profound minimum at $4\;$T is reproduced by both of our theoretical approaches and is ascribed to the nuclear Zeeman effect. Since the nuclear Larmor precession determines the electronic resonance condition, it also defines the number of electron spin revolutions between pump pulses, the orientation of the electron spin at the incidence time of a pump pulse, and the resulting revival amplitude. The magnetic field of $4\;$T, for example, corresponds to half a revolution of nuclear spins between two laser pulses., 21 pages, 16 figures

We investigate the equilibrium and real-time properties of the spin-correlation function $\ensuremath{\langle}{\stackrel{P\vec}{S}}_{1}{\stackrel{P\vec}{S}}_{2}\ensuremath{\rangle}$ in the two-impurity Kondo model for different distances $R$ between the two-impurity spins. It is shown that the competition between the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction and the Kondo effect governs the amplitude of $\ensuremath{\langle}{\stackrel{P\vec}{S}}_{1}{\stackrel{P\vec}{S}}_{2}\ensuremath{\rangle}$. For distances $R$ exceeding the Kondo length scale, the Kondo effect also has a profound effect on the sign of the correlation function. For ferromagnetic Heisenberg couplings $J$ between the impurities and the conduction band, the Kondo effect is absent and the correlation function only decays for distances beyond a certain length scale introduced by finite temperature. The real-time dynamics after a sudden quench of the system reveals that correlations propagate through the conduction band with Fermi velocity. We identify two distinct timescales for the long-time behavior, which reflects that for small $J$ the system is driven by the RKKY interaction while for large $J$ the Kondo effect dominates. Interestingly, we find that at certain distances a one-dimensional dispersion obeying $\ensuremath{\epsilon}(k)=\ensuremath{\epsilon}(\ensuremath{-}k)$ may lead to a local parity conservation of the impurities such that $\ensuremath{\langle}{\stackrel{P\vec}{S}}_{1}{\stackrel{P\vec}{S}}_{2}\ensuremath{\rangle}$ becomes a conserved quantity for long times and does not decay to its equilibrium value.

We study theoretically the spin fluctuations of nuclei in quantum dots. We employ the central spin model which accounts for the hyperfine interaction of the nuclei with the electron spin. We present an analytical solution in the frame of the box model approximation where all hyperfine coupling constants are assumed to be equal. These results are in good agreement with numerical simulations. We demonstrate that in rather high magnetic field the nuclear spin noise spectra has a two-peak structure centered at the nuclear Zeeman frequency with the shape of the spectrum controlled by the distribution of the hyperfine constants., 9 pages, 10 figures

We show that the RKKY interaction in the two-impurity Anderson model comprise two contributions: a ferromagnetic part stemming from the symmetrized hybridization functions and an anti-ferromagnetic part. We demonstrate that this anti-ferromagnetic contribution can also be generated by an effective local tunneling term between the two impurities. This tunneling can be analytically calculated for particle-hole symmetric impurities. Replacing the full hybridization functions by the symmetric part and this tunneling term leads to the identical low-temperature fixed point spectrum in the numerical renormalization group. Compensating this tunneling term is used to restore the Varma-Jones quantum critical point between a strong coupling phase and a local singlet phase even in the absence of particle-hole symmetry in the hybridization functions. We analytically investigate the spatial frequencies of the effective tunneling term based on the combination of the band dispersion and the shape of the Fermi surface. Numerical renormalization group calculations provide a comparison of the distance dependent tunneling term and the local spin-spin correlation function. Derivations between the spatial dependency of the full spin-spin correlation function and the textbook RKKY interaction are reported.

We present an investigation of the electron spin dynamics in an ensemble of singly charged semiconductor quantum dots subject to an external magnetic field and laser pumping with circularly polarized light. The spectral laser width is tailored such that ensembles with an increasing number of quantum dots are coherently pumped. Surprisingly, the dephasing time ${T}^{*}$ of the electron spin polarization depends only weakly on the laser spectral width. These findings can be consistently explained by a cluster theory of coupled quantum dots with a long-range electronic spin-spin interaction. We present a numerical simulation of the spin dynamics based on the central spin model that includes a quantum mechanical description of the laser pulses as well as a time-independent Heisenberg interaction between each pair of electron spins. We discuss the individual dephasing contributions stemming from the Overhauser field, the distribution of the electron $g$ factors, and the electronic spin-spin interaction as well as the spectral width of the laser pulse. This analysis reveals counterbalancing effects on the total dephasing time when increasing the spectral laser width. On one hand, the increasing deviations of the electron $g$ factors reduce the dephasing time. On the other hand, more electron spins are coherently pumped and synchronize due to the electronic spin-spin interaction which extends the dephasing time. We find an excellent agreement between the experimental data and the dephasing time in the simulation using an exponential distribution of Heisenberg couplings with a mean value $\overline{J}\ensuremath{\approx}0.26\phantom{\rule{0.16em}{0ex}}\ensuremath{\mu}\mathrm{eV}$.

We study the magnetic properties in the vicinity of a single carbon defect in a monolayer of graphene. We include the unbound $\sigma$ orbital and the vacancy induced bound $\pi$ state in an effective two-orbital single impurity model. The local magnetic moments are stabilized by the Coulomb interaction as well as a significant ferromagnetic Hund's rule coupling between the orbitals predicted by a density functional theory calculation. A hybridization between the orbitals and the Dirac fermions is generated by the curvature of the graphene sheet in the vicinity of the vacancy. We present results for the local spectral function calculated using Wilson's numerical renormalization group approach for a realistic graphene band structure and find three different regimes depending on the filling, the controlling chemical potential, and the hybridization strength. These different regions are characterized by different magnetic properties. The calculated spectral functions qualitatively agree with recent scanning tunneling spectra on graphene vacancies., Comment: 18 pages, 15 figures

Electron spin dephasing in a singly charged semiconductor quantum dot can partially be suppressed by periodic laser pulsing. We propose a semi-classical approach describing the decoherence of the electron spin polarization governed by the hyperfine interaction with the nuclear spins as well as the probabilistic nature of the photon absorption. We use the steady-state Floquet condition to analytically derive two subclasses of resonance conditions excellently predicting the peak locations in the part of the Overhauser field distribution which is projected in the direction of the external magnetic field. As a consequence of the periodic pulsing, a non-equilibrium distribution develops as a function of time. The numerical simulation of the coupled dynamics reveals the influence of the hyperfine coupling constant distribution onto the evolution of the electron spin polarisation before the next laser pulse. Experimental indications are provided for both subclasses of resonance conditions., Comment: 21 pages, 21 figures

The coherence of the electron spin in a semiconductor quantum dot is strongly enhanced by mode locking through nuclear focusing, where the synchronization of the electron spin to periodic pulsing is slowly transferred to the nuclear spins of the semiconductor material, mediated by the hyperfine interaction between these. The external magnetic field that drives the Larmor oscillations of the electron spin also subjects the nuclear spins to a Zeeman-like coupling, albeit a much weaker one. For typical magnetic fields used in experiments, the energy scale of the nuclear Zeeman effect is comparable to that of the hyperfine interaction, so that it is not negligible. In this work, we analyze the influence of the nuclear Zeeman effect on mode locking quantitatively. Within a perturbative framework, we calculate the Overhauser-field distribution after a prolonged period of pulsing. We find that the nuclear Zeeman effect can exchange resonant and non-resonant frequencies. We distinguish between models with a single type and with multiple types of nuclei. For the latter case, the positions of the resonances depend on the individual $g$ factors, rather than on the average value., 11 pages, 6 figures

We study the long-time decay of fourth-order electron spin correlation functions for an isolated singly charged semi-conductor quantum dot. The electron spin dynamics is governed by the applied external magnetic field as well as the hyperfine interaction. While the long-time coherent oscillations in the correlation functions can be understood within an semi-classical approach treating the Overhauser field as frozen, the field dependent decay of its amplitude reported in different experiments cannot be explained by the central-spin model indicating the insufficiency of such a description. By incorporating the nuclear Zeeman splitting and the strain induced nuclear-electric quadrupolar interaction, we find the correct crossover from a fast decay in small magnetic fields to a slow exponential asymptotic in large magnetic fields. It originates from a competition between the quadrupolar interaction inducing an enhanced spin decay and the nuclear Zeeman term that suppressed the spin-flip processes. We are able to explain the magnetic field dependency of the characteristic long-time decay time $T_2$ depending on the experimental setups. The calculated asymptotic values of $T_2 = 3 -4\,\mu$s agree qualitatively well with the experimental data., Comment: 13 pages, 9 figures

We show that the two-impurity Anderson model exhibits an additional quantum critical point at infinitely many specific distances between both impurities for an inversion symmetric one-dimensional dispersion. Unlike the quantum critical point previously established, it is robust against particle-hole or parity symmetry breaking. The quantum critical point separates a spin doublet from a spin singlet ground state and is, therefore, protected. A finite single-particle tunneling $t$ or an applied uniform gate voltage will drive the system across the quantum critical point. The discriminative magnetic properties of the different phases cause a jump in the spectral functions at low temperature, which might be useful for future spintronics devices. A local parity conservation will prevent the spin-spin correlation function from decaying to its equilibrium value after spin manipulations.

We employ density-functional theory (DFT) in the generalized gradient approximation (GGA) and its extensions GGA+$U$ and GGA+Gutzwiller to calculate the magnetic exchange couplings between pairs of Mn ions substituting Cd in a CdTe crystal at very small doping. DFT(GGA) overestimates the exchange couplings by a factor of three because it underestimates the charge-transfer gap in Mn-doped II-VI semiconductors. Fixing the nearest-neighbor coupling $J_1$ to its experimental value in GGA+$U$, in GGA+Gutzwiller, or by a simple scaling of the DFT(GGA) results provides acceptable values for the exchange couplings at 2nd, 3rd, and 4th neighbor distances in Cd(Mn)Te, Zn(Mn)Te, Zn(Mn)Se, and Zn(Mn)S. In particular, we recover the experimentally observed relation $J_4>J_2,J_3$. The filling of the Mn 3$d$-shell is not integer which puts the underlying Heisenberg description into question. However, using a few-ion toy model the picture of a slightly extended local moment emerges so that an integer $3d$-shell filling is not a prerequisite for equidistant magnetization plateaus, as seen in experiment., 12 pages, 10 figures

Spin noise spectroscopy is a promising technique for revealing the microscopic nature of spin dephasing processes in quantum dots (QDs). We compare the spin-noise in an ensemble of singly charged QDs calculated by two complementary approaches. The Chebyshev polynomial expansion technique (CET) accounts for the full quantum mechanical fluctuation of the nuclear spin bath and a semi-classical approach (SCA) is based on the averaging the electron spin dynamics over all different static Overhauser field configurations. We observe a remarkable agreement between both methods in the high-frequency part of the spectra determined by static nuclear fields. The low-frequency part is determined by the long time fluctuations of the Overhauser field. We find small differences in the spectra depending on the distribution of hyperfine couplings. The spin-noise spectra in strong enough magnetic fields where the nuclear dynamics is quenched calculated by two complimentary approaches are in perfect agreement.

Before transport data can be understood quantitatively, a few prerequisites have to be fulfilled: the geometric and the electronic structures of the metal/molecule contacts have to be known, and electron correlation effects have to be taken into account. Here we discuss experimental and theoretical approaches to tackle these challenges. On the theoretical side, density-functional theory (including van der Waals-corrections for structural optimization) is combined with many-body perturbation theory and numerical renormalization group theory in order to include all relevant correlation effects. We had already discussed such features in a previous study [Phys. Rev. B 84, 125413 (2011)], but some remaining differences between our calculated spectra and our experimental data from a scanning-tunnelling microscope remained unexplained. Here we show that the explicit incorporation of van der Waals interaction in the calculations, that had been negleted before, yields improved geometric structure and leads to much better agreement with our measured spectra. This clearly demonstrates the significant sensitivity of electronic transport to structural details.PTCDA molecule in a junction between a silver surface and an STM tip.

When constructing a Wilson chain to represent a quantum impurity model, the effects of truncated bath modes are neglected. We show that their influence can be kept track of systematically by constructing an "open Wilson chain" in which each site is coupled to a separate effective bath of its own. As a first application, we use the method to cure the so-called mass-flow problem that can arise when using standard Wilson chains to treat impurity models with asymmetric bath spectral functions at finite temperature. We demonstrate this for the strongly sub-Ohmic spin-boson model at quantum criticality where we directly observe the flow towards a Gaussian critical fixed point., 4 + 12 pages, 4 + 6 figures (published version)

Quantum dots in GaAs/InGaAs structures have been proposed as a candidate system for realizing quantum computing. The short coherence time of the electronic quantum state that arises from coupling to the nuclei of the substrate is dramatically increased if the system is subjected to a magnetic field and to repeated optical pulsing. This enhancement is due to mode locking: Oscillation frequencies resonant with the pulsing frequencies are enhanced, while off-resonant oscillations eventually die out. Because the resonant frequencies are determined by the pulsing frequency only, the system becomes immune to frequency shifts caused by the nuclear coupling and by slight variations between individual quantum dots. The effects remain even after the optical pulsing is terminated. In this work, we explore the phenomenon of mode locking from a quantum mechanical perspective. We treat the dynamics using the central spin model, which includes coupling to 10-20 nuclei and incoherent decay of the excited electronic state, in a perturbative framework. Using scaling arguments, we extrapolate our results to realistic system parameters. We find that the synchronization to the pulsing frequency needs time scales in the order of 1 s., 20.1 pages, including appendices; 7 figures; with Erratum and corrected Figs. 2 and 3

We employ the Gutzwiller variational approach to investigate the interplay of Coulomb interaction and spin-orbit coupling in a three-orbital Hubbard model. Already in the paramagnetic phase we find a substantial renormalization of the spin-orbit coupling that enters the effective single-particle Hamiltonian for the quasi-particles. Only close to half band-filling and for sizable Coulomb interaction we observe clear signatures of Hund's atomic rules for spin, orbital, and total angular momentum. For a finite local Hund's-rule exchange interaction we find a ferromagnetically ordered state. The spin-orbit coupling considerably reduces the size of the ordered moment, it generates a small ordered orbital moment, and it induces a magnetic anisotropy. To investigate the magnetic anisotropy energy, we use an external magnetic field that tilts the magnetic moment away from the easy axis $(1,1,1)$., Comment: 16 pages, 14 figures

The spin fluctuations of electron and hole doped self-assembled quantum dot ensembles are measured optically in the low-intensity limit of a probe laser in absence and presence of longitudinal or transverse static magnetic fields. The experimental results are modeled by two complementary approaches based either on semiclassical or quantum mechanical descriptions. This allows us to characterize the hyperfine interaction of electron and hole spins with the surrounding bath of nuclei on time scales covering several orders of magnitude. Our results demonstrate (i) the intrinsic precession of the electron spin fluctuations around the effective nuclear Overhauser field caused by the host lattice nuclear spins, (ii) the comparably long time scales for electron and hole spin decoherence, as well as (iii) the dramatic enhancement of the spin lifetimes induced by a longitudinal magnetic field due to the decoupling of nuclear and charge carrier spins., 16 pages, 9 figures

Decoherence of a central spin coupled to an interacting spin bath via inhomogeneous Heisenberg coupling is studied by two different approaches, namely an exact equations of motion (EOMs) method and a Chebyshev expansion technique (CET). By assuming a wheel topology of the bath spins with uniform nearest-neighbor $XX$-type intrabath coupling, we examine the central spin dynamics with the bath prepared in two different types of bath initial conditions. For fully polarized baths in strong magnetic fields, the polarization dynamics of the central spin exhibits a collapse-revival behavior in the intermediate-time regime. Under an antiferromagnetic bath initial condition, the two methods give excellently consistent central spin decoherence dynamics for finite-size baths of $N\leq14$ bath spins. The decoherence factor is found to drop off abruptly on a short time scale and approach a finite plateau value which depends on the intrabath coupling strength non-monotonically. In the ultrastrong intrabath coupling regime, the plateau values show an oscillatory behavior depending on whether $N/2$ is even or odd. The observed results are interpreted qualitatively within the framework of the EOM and perturbation analysis. The effects of anisotropic spin-bath coupling and inhomogeneous intrabath bath couplings are briefly discussed. Possible experimental realization of the model in a modified quantum corral setup is suggested., 11 pages, 7 figures, to appear in Phys. Rev. B

By means of low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS), we have investigated the adsorption of single Au atoms on a PTCDA monolayer physisorbed on the Au(111) surface. A chemical reaction between the Au atom and the PTCDA molecule leads to the formation of a radical that has an unpaired electron in its highest occupied orbital. This orbital is a $\ensuremath{\pi}$ orbital that extends over the whole Au-PTCDA complex. Because of the large Coulomb repulsion in this orbital, the unpaired electron generates a local moment when the molecule is adsorbed on the Au(111) surface. We demonstrate the formation of the radical and the existence of the local moment after adsorption by observing a zero-bias differential conductance peak that originates from the Kondo effect. By temperature dependent measurements of the zero-bias differential conductance, we determine the Kondo temperature to be ${T}_{\mathrm{K}}=(38\ifmmode\pm\else\textpm\fi{}8)\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. For the theoretical description of the properties of the Au-PTCDA complex we use a hierarchy of methods, ranging from density functional theory (DFT) including a van der Waals correction to many-body perturbation theory (MBPT) and the numerical renormalization group (NRG) approach. Regarding the high-energy orbital spectrum, we obtain an excellent agreement with experiments by both spin-polarized DFT/MBPT and NRG. Moreover, the NRG provides an accurate description of the low-energy excitation spectrum of the spin degree of freedom, predicting a Kondo temperature very close to the experimental value. This is achieved by a detailed analysis of the universality of various definitions of ${T}_{\mathrm{K}}$ and by taking into account the full energy dependence of the coupling function between the molecule-metal complex and the metallic substrate.

The real-time spin dynamics and the spin noise spectra are calculated for p and n-charged quantum dots within an anisotropic central spin model extended by additional nuclear electric quadrupolar interactions (QC) and augmented by experimental data studied using identical excitation conditions. Using realistic estimates for the distribution of coupling constants including an anisotropy parameter, we show that the characteristic long time scale is of the same order for electron and hole spins strongly determined by the QC even though the analytical form of the spin decay differs significantly consistent with our measurements. The low frequency part of the electron spin noise spectrum is approximately $1/3$ smaller than those for hole spins as a consequence of the spectral sum rule and the different spectral shapes. This is confirmed by our experimental spectra measured on both types of quantum dot ensembles in the low power limit of the probe laser., Comment: 5 pages, 3 figures, submitted to PRL

We use the scattering states numerical renormalization group (SNRG) approach to calculate the current $I(V)$ through a single molecular level coupled to a local molecular phonon. The suppression of $I$ for asymmetric junctions with increasing electron-phonon coupling, the hallmark of the Franck-Condon blockade, is discussed. We compare the SNRG currents with recently published data obtained by an iterative summation of path integrals approach (ISPI). Our results excellently agree with the ISPI currents for small and intermediate voltages. In the linear response regime $I(V)$ approaches the current calculated from the equilibrium spectral function. We also present the temperature and voltage evolution of the non-equilibrium spectral functions for a particle-hole asymmetric junction with symmetric coupling to the lead., Comment: 7 pages, 7 figures

The ionic Hubbard model on a cubic lattice is investigated using analytical approximations and Wilson's renormalization group for the charge excitation spectrum. Near the Mott insulating regime, where the Hubbard repulsion starts to dominate all energies, the formation of correlated bands is described. The corresponding partial spectral weights and local densities of states show characteristic features, which compare well with a hybridized-band picture appropriate for the regime at small $U$, which at half-filling is known as a band insulator. In particular, a narrow charge gap is obtained at half-filling, and the distribution of spectral quasi-particle weight reflects the fundamental hybridization mechanism of the model.

The energy-dependent scattering of fermions from a localized orbital at an energy-dependent rate $\ensuremath{\Gamma}(\ensuremath{\varepsilon})\ensuremath{\propto}{|\ensuremath{\varepsilon}|}^{r}$ gives rise to quantum critical points (QCPs) in the pseudogap single-impurity Anderson model separating a local moment phase with an unscreened spin moment from a strong-coupling phase which slightly deviates from the screened phase of standard Kondo problem. Using the time-dependent numerical renormalization group (TD-NRG) approach we show that local dynamic properties always equilibrate towards a steady-state value even for quenches across the QCP but with systematic deviations from the thermal equilibrium depending on the distance to the critical coupling. Local nonequilibrium properties are presented for interaction quenches and hybridization quenches. We augment our numerical data by an analytical calculation that becomes exact at short times and find excellent agreement between the numerics and the analytical theory. For interaction quenches within the screened phase we find a universal function for the time-dependent local double occupancy. We trace back the discrepancy between our results and the data obtained by a time-dependent Gutzwiller variational approach to restrictions of the wave-function ansatz in the Gutzwiller theory: while the NRG ground states properly account for the formation of an extended spin moment which decouples from the system in the unscreened phase, the Gutzwiller ansatz only allows the formation of the spin moment on the local impurity orbital.

We develop a low-order conserving approximation for the interacting resonant-level model (IRLM), and apply it to (i) thermal equilibrium, (ii) nonequilibrium steady state, and (iii) nonequilibrium quench dynamics. Thermal equilibrium is first used to carefully gauge the quality of the approximation by comparing the results with other well-studied methods, and finding good agreement for small values of the interaction. We analytically show that the power-law exponent of the renormalized level width usually derived using renormalization group approaches can also be correctly obtained in our approach in the weak interaction limit. A closed expression for the nonequilibrium steady-state current is derived and analytically and numerically evaluated. We find a negative differential conductance at large voltages, and the exponent of the power-law suppression of the steady-state current is calculated analytically at zero-temperature. The response of the system to quenches is investigated for a single-lead as well as for two-lead setup at finite voltage bias at particle-hole symmetry using a self-consistent two-times Keldysh Green function approach, and results are presented for the time-dependent current for different bias and contact interaction strength.

We address the fundamental question how the spatial Kondo correlations are building up in time assuming an initially decoupled impurity spin ${\stackrel{P\vec}{S}}_{\mathrm{imp}}$. We investigate the time-dependent spin-correlation function $\ensuremath{\chi}(\stackrel{P\vec}{r},t)=\ensuremath{\langle}{\stackrel{P\vec}{S}}_{\mathrm{imp}}\stackrel{P\vec}{s}(\stackrel{P\vec}{r})\ensuremath{\rangle}(t)$ in the Kondo model with antiferromagnetic and ferromagnetic couplings, where $\stackrel{P\vec}{s}(\stackrel{P\vec}{r})$ denotes the spin density of the conduction electrons after switching on the Kondo coupling at time $t=0$. We present data obtained from a time-dependent numerical renormalisation group (TD-NRG) calculation. We gauge the accuracy of our two-band NRG by the spatial sum rules of the equilibrium correlation functions and the reproduction of the analytically exactly known spin-correlation function of the decoupled Fermi sea. We find a remarkable building up of Kondo correlation outside of the light cone defined by the Fermi velocity of the host metal. By employing a perturbative approach exact in second-order of the Kondo coupling, we connect these surprising correlations to the intrinsic spin-density entanglement of the Fermi sea. The thermal wavelength supplies a cutoff scale at finite temperatures beyond which correlations are exponentially suppressed. We present data for the frequency dependent retarded spin-spin susceptibility and use the results to calculate the real-time response of a weak perturbation in linear response: within the spatial resolution no response outside of the light cone is found.

Mazur's inequality renders statements about persistent correlations possible. We generalize it in a convenient form applicable to any set of linearly independent constants of motion. This approach is used to show rigorously that a fraction of the initial spin correlations persists indefinitely in the isotropic central spin model unless the average coupling vanishes. The central spin model describes a major mechanism of decoherence in a large class of potential realizations of quantum bits. Thus the derived results contribute significantly to the understanding of the preservation of coherence. We will show that persisting quantum correlations are not linked to the integrability of the model, but caused by a finite operator overlap with a finite set of constants of motion., Comment: 5 pages, 1 figure, +2 pages supplemental material Small changes and some additional explicit calculations in the supplement

Motivated by the recent observation of the Kondo effect in graphene in transport experiments, we investigate the resistivity and dephasing rate in the Kondo regime due to magnetic impurities in graphene with different chemical potentials ($\ensuremath{\mu}$). The Kondo effect due to either carbon vacancies or magnetic adatoms in graphene is described by the single-orbital pseudogap asymmetric Anderson impurity model which is solved by the accurate numerical renormalization group method. We find that although the Anderson impurity model considered here is a mixed-valence system, it can be driven into either the Kondo [$\ensuremath{\mu}g{\ensuremath{\mu}}_{c}$ (critical value) $g0$], mixed-valency ($\ensuremath{\mu}\ensuremath{\approx}{\ensuremath{\mu}}_{c}$), or empty-orbital ($\ensuremath{\mu}l{\ensuremath{\mu}}_{c}$) regime by a gate voltage, giving rise to characteristic features in resistivity and dephasing rate in each regime. Specifically, in the case of $\ensuremath{\mu}l{\ensuremath{\mu}}_{c}$, the shapes of the resistivity (dephasing rate) curves for different $\ensuremath{\mu}$ are nearly identical. However, as temperature decreases, they start to increase to their maxima at a lower $T/{T}_{K}$, but more rapidly [as ${({T}_{K}/T)}^{3/2}$] than in normal metals [here, $T$ (${T}_{K}$) denotes the (Kondo) temperature]. As $T$ further decreases, after reaching the maximum, the dephasing rate drops more quickly than in normal metals, behaving as ${(T/{T}_{K})}^{3}$ instead of ${(T/{T}_{K})}^{2}$. Furthermore, the resistivity has a distinct peak above the saturation value near ${T}_{K}$. In the case of $\ensuremath{\mu}g{\ensuremath{\mu}}_{c}$, in contrast, the resistivity curve has an additional broad shoulder above 10${T}_{K}$ and the dephasing rate exhibits an interesting shoulder-peak shape. In the narrow boundary region ($\ensuremath{\mu}\ensuremath{\approx}{\ensuremath{\mu}}_{c}$), both the resistivity and dephasing rate curves are similar to the corresponding ones in normal metals. This explains the conventional Kondo-like resistivity from recent experiments on graphene with defects, although the distinct features in the resistivity in the other cases ($\ensuremath{\mu}l{\ensuremath{\mu}}_{c}$ or $\ensuremath{\mu}g{\ensuremath{\mu}}_{c}$) were not seen in the experiments. The interesting features in the resistivity and dephasing rate are analyzed in terms of the calculated $T$-dependent spectral function, correlation self-energy, and renormalized impurity level.

We present calculations of the electronic transport properties of heavy-fermion systems within a semi-phenomenological approach to the dynamical mean field theory. In this approach the dynamics of the Hund's rules 4f (5f )-ionic multiplet split in a crystalline environment is taken into account. Within the scope of this calculation we use the linear response theory to reproduce qualitative features of the temperature-dependent resistivity and hall conductivity, the magneto-resistivity and the thermoelectric power typical for heavy-fermion systems. The model calculations are directly compared with experimental results on CeCu2Si2.

We show that the optical response of metals with strong electron-electron correlation consists of two excitations, a renormalized Drude response at zero energy and a mid-infrared peak occurring at frequencies around 2000 cm-1. The latter originates from a dynamical, correlation-induced gap, as evinced from a many body theoretical approach based on the periodic Anderson model. At very low temperatures, it can be viewed as optical gap between two renormalized quasi-particle bands. The gap size is proportional to the geometric mean of the characteristic lattice Kondo temperature of the material and its bandwidth.

The RCSJ model of resistively and capacitively shunted Josephson junctions is used to describe superconducting point contacts over a wide range of resistances up to the metallic–tunneling transition. Their small dynamic capacitance of order C = 0.1 fF due to the point-contact geometry results in a huge plasma frequency. The critical current is then strongly suppressed and the contact resistance becomes finite because of quantum-mechanical zero-point fluctuations of the Josephson plasma and the rather large escape rate out of the zero-voltage state due to quantum tunneling. We test the predictions of the RCSJ model on the classical superconductors lead, indium, aluminum, and cadmium.