Spin tunneling and topological selection rules for integer spins

We present topological interference effects for the tunneling of a single large spin, which are caused by the symmetry of a general class of magnetic anisotropies. The interference originates from spin Berry phases associated with different tunneling paths exposed to the same dynamics. Introducing a generalized path integral for coherent spin states, we evaluate transition amplitudes between ground as well as low-lying excited states. We show that these interference effects lead to topological selection rules and spin-parity effects for integer spins that agree with quantum selection rules and which thus provide a generalization of the Kramers degeneracy to integer spins. Our results apply to the molecular magnets Mn12 and Fe8.Comment: 4 pages, 3 EPS figures, REVTe

Berry-phase blockade in single-molecule magnets

We formulate the problem of electron transport through a single-molecule magnet (SMM) in the Coulomb blockade regime taking into account topological interference effects for the tunneling of the large spin of a SMM. The interference originates from spin Berry phases associated with different tunneling paths. We show that in the case of incoherent spin states it is essential to place the SMM between oppositely spin-polarized source and drain leads in order to detect the spin tunneling in the stationary current, which exhibits topological zeros as a function of the transverse magnetic field.Comment: 4 pages, Revtex 4, 4 EPS figure

Quantum Computing in Molecular Magnets

Shor and Grover demonstrated that a quantum computer can outperform any classical computer in factoring numbers and in searching a database by exploiting the parallelism of quantum mechanics. Whereas Shor's algorithm requires both superposition and entanglement of a many-particle system, the superposition of single-particle quantum states is sufficient for Grover's algorithm. Recently, the latter has been successfully implemented using Rydberg atoms. Here we propose an implementation of Grover's algorithm that uses molecular magnets, which are solid-state systems with a large spin; their spin eigenstates make them natural candidates for single-particle systems. We show theoretically that molecular magnets can be used to build dense and efficient memory devices based on the Grover algorithm. In particular, one single crystal can serve as a storage unit of a dynamic random access memory device. Fast electron spin resonance pulses can be used to decode and read out stored numbers of up to 10^5, with access times as short as 10^{-10} seconds. We show that our proposal should be feasible using the molecular magnets Fe8 and Mn12.Comment: 13 pages, 2 figures, PDF, version published in Nature, typos correcte

Crystal Field -AS_z^2 Does Not Produce One-Phonon Transitions With Delta S_z=+-2 [Comment on EPL 46, 692 (1999) by Leuenberger and Loss]

Recently Leuenbeger and Loss suggested a theory of phonon-assisted relaxation in a molecular nanomagnet Mn-12 that "contrary to previous results is in reasonably good agreement ... with all experimental parameter values known so far". The purpose of this Comment is to show that the model of Leuenberger and Loss and its comparison with experiment are premised upon their incorrect use of the linear formula for the strain tensor. The spin-phonon coupling introduced by Leuenberger and Loss disappears if the nonlinear term in the strain tensor is taken into account.Comment: 2 pages, no figures, submitted to EP

Spin relaxation in Mn12-acetate

We present a comprehensive derivation of the magnetization relaxation in a Mn12-acetate crystal based on thermally assisted spin tunneling induced by quartic anisotropy and weak transverse magnetic fields. The overall relaxation rate as function of the magnetic field is calculated and shown to agree well with data including all resonance peaks. The Lorentzian shape of the resonances is also in good agreement with recent data. A generalized master equation including resonances is derived and solved exactly. It is shown that many transition paths with comparable weight exist that contribute to the relaxation process. Previously unknown spin-phonon coupling constants are calculated explicitly.Comment: 4 pages,4 EPS figures,LaTeX(europhys.sty);final version accepted for EP

Multi-photon Rabi oscillations in high spin paramagnetic impurity

We report on multiple photon monochromatic quantum oscillations (Rabi oscillations) observed by pulsed EPR (Electron Paramagnetic Resonance) of Mn$^{2+}$ (S=5/2) impurities in MgO. We find that when the microwave magnetic field is similar or large than the anisotropy splitting, the Rabi oscillations have a spectrum made of many frequencies not predicted by the S=1/2 Rabi model. We show that these new frequencies come from multiple photon coherent manipulation of the multi-level spin impurity. We develop a model based on the crystal field theory and the rotating frame approximation, describing the observed phenomenon with a very good agreement.Comment: International Conference: Resonance in Condensed Matter Altshuler 10

Time-dependent density-matrix functional theory for biexcitonic phenomena

We formulate a time-dependent density-matrix functional theory (TDDMFT) approach for higher-order correlation effects like biexcitons in optical processes in solids based on the reduced two-particle density-matrix formalism within the normal orbital representation. A TDDMFT version of the Schr\"odinger equation for biexcitons in terms of one- and two-body reduced density matrices is derived, which leads to finite biexcitonic binding energies already with an adiabatic approximation. Biexcitonic binding energies for several bulk semiconductors are calculated using a contact biexciton model

Mode-selective coupling of coherent phonons to the Bi2212 electronic band structure

Cuprate superconductors host a multitude of low-energy optical phonons. Using time- and angle-resolved photoemission spectroscopy, we study coherent phonons in Bi$_{2}$Sr$_{2}$Ca$_{0.92}$Y$_{0.08}$Cu$_{2}$O$_{8+\delta}$. Sub-meV modulations of the electronic band structure are observed at frequencies of $3.94\pm 0.01$ and $5.59\pm 0.06$ THz. For the dominant mode at 3.94 THz, the amplitude of the band energy oscillation weakly increases as a function of momentum away from the node. Theoretical calculations allow identifying the observed modes as CuO$_{2}$-derived $A_{1g}$ phonons. The Bi- and Sr-derived $A_{1g}$ modes which dominate Raman spectra in the relevant frequency range are absent in our measurements. This highlights the mode-selectivity for phonons coupled to the near-Fermi-level electrons, which originate from CuO$_{2}$ planes and dictate thermodynamic properties.Comment: 7 pages, 3 figure

Analytical approach to semiconductor Bloch equations

Although semiconductor Bloch equations have been widely used for decades to address ultrafast optical phenomena in semiconductors, they have a few important drawbacks: (i) Coulomb terms between free electron-hole pairs require Hartree-Fock treatment which, in its usual form, preserves excitonic poles but loses biexcitonic resonances. (ii) Solving the resulting coupled differential equations imposes heavy numerics which completely hide the physics. This can be completely avoided if, instead of free electron-hole pairs, we use correlated pairs, i.e., excitons. Their interactions are easy to handle through the recently constructed composite-exciton many-body theory, which allows us to \emph{analytically} obtain the time evolution of the polarization induced by a laser pulse. This polarization comes from Coulomb interactions between virtual excitons, but also from Coulomb-free fermion exchanges, which are dominant at large detuning

Magnetic quantum coherence effect in Ni4 molecular transistors

We consider the electron transport in single molecule magnet transistors in the presence of Zeeman spin splitting and magnetic quantum coherence (MQC). The Zeeman interaction is extended along the leads, thereby producing gaps in the energy spectrum which allow electron transport with spin polarized along a certain direction. The MQC induces an effective coupling between localized spin states and continuum spin states in the single molecule magnet and leads, respectively. We investigate the conductance at zero temperature as a function of the applied bias and magnetic field, and show that the MQC is responsible for the appearence of resonances. Accordingly, we name them MQC resonances.Comment: 5 pages, Revtex