Many-spin effects in inelastic neutron scattering and electron paramagnetic resonance of molecular nanomagnets

Many molecular magnetic clusters, such as single-molecule magnets, are characterized by spin ground states with defined total spin S exhibiting zero-field-splittings. In this work, the spectroscopic intensities of the transitions within the ground-state multiplet are analyzed. In particular, the effects of a mixing with higher-lying spin multiplets, which is produced by anisotropic interactions and is neglected in the standard single-spin description, are investigated systematically for the two experimental techniques of inelastic neutron scattering (INS) and electron paramagnetic resonance (EPR), with emphasis on the former technique. The spectroscopic transition intensities are calculated analytically by constructing corresponding effective spin operators perturbationally up to second order and consequently using irreducible tensor operator techniques. Three main effects of spin mixing are observed. Firstly, a pronounced dependence of the INS intensities on the momentum transfer Q, with a typical oscillatory behavior, emerges in first order, signaling the many-spin nature of the wave functions in exchange-coupled clusters. Secondly, as compared to the results of a first-order calculation, the intensities of the transitions within the spin multiplet are affected differently by spin mixing. This allows one, thirdly, to differentiate the higher-order contributions to the cluster magnetic anisotropy which come from the single-ion ligand-field terms and spin mixing, respectively. The analytical results are illustrated by means of the three examples of an antiferromagnetic heteronuclear dimer, the Mn-[3 x 3] grid molecule, and the single-molecule magnet Mn12.Comment: 18 pages, 3 figures, REVTEX4, to appear in PR

Direct Observation of Quantum Coherence in Single-Molecule Magnets

Direct evidence of quantum coherence in a single-molecule magnet in frozen solution is reported with coherence times as long as T2 = 630 ns. We can strongly increase the coherence time by modifying the matrix in which the single-molecule magnets are embedded. The electron spins are coupled to the proton nuclear spins of both the molecule itself and interestingly, also to those of the solvent. The clear observation of Rabi oscillations indicates that we can manipulate the spin coherently, an essential prerequisite for performing quantum computations.Comment: 5 Pages, 4 Figures, final version published in PR

Spin electric effects in molecular antiferromagnets

Molecular nanomagnets show clear signatures of coherent behavior and have a wide variety of effective low-energy spin Hamiltonians suitable for encoding qubits and implementing spin-based quantum information processing. At the nanoscale, the preferred mechanism for control of quantum systems is through application of electric fields, which are strong, can be locally applied, and rapidly switched. In this work, we provide the theoretical tools for the search for single molecule magnets suitable for electric control. By group-theoretical symmetry analysis we find that the spin-electric coupling in triangular molecules is governed by the modification of the exchange interaction, and is possible even in the absence of spin-orbit coupling. In pentagonal molecules the spin-electric coupling can exist only in the presence of spin-orbit interaction. This kind of coupling is allowed for both $s=1/2$ and $s=3/2$ spins at the magnetic centers. Within the Hubbard model, we find a relation between the spin-electric coupling and the properties of the chemical bonds in a molecule, suggesting that the best candidates for strong spin-electric coupling are molecules with nearly degenerate bond orbitals. We also investigate the possible experimental signatures of spin-electric coupling in nuclear magnetic resonance and electron spin resonance spectroscopy, as well as in the thermodynamic measurements of magnetization, electric polarization, and specific heat of the molecules.Comment: 31 pages, 24 figure

Single-ion and exchange anisotropy effects and multiferroic behavior in high-symmetry tetramer single molecule magnets

We study single-ion and exchange anisotropy effects in equal-spin $s_1$ tetramer single molecule magnets exhibiting $T_d$, $D_{4h}$, $D_{2d}$, $C_{4h}$, $C_{4v}$, or $S_4$ ionic point group symmetry. We first write the group-invariant quadratic single-ion and symmetric anisotropic exchange Hamiltonians in the appropriate local coordinates. We then rewrite these local Hamiltonians in the molecular or laboratory representation, along with the Dzyaloshinskii-Moriay (DM) and isotropic Heisenberg, biquadratic, and three-center quartic Hamiltonians. Using our exact, compact forms for the single-ion spin matrix elements, we evaluate the eigenstate energies analytically to first order in the microscopic anisotropy interactions, corresponding to the strong exchange limit, and provide tables of simple formulas for the energies of the lowest four eigenstate manifolds of ferromagnetic (FM) and anitiferromagnetic (AFM) tetramers with arbitrary $s_1$. For AFM tetramers, we illustrate the first-order level-crossing inductions for $s_1=1/2,1,3/2$, and obtain a preliminary estimate of the microscopic parameters in a Ni$_4$ from a fit to magnetization data. Accurate analytic expressions for the thermodynamics, electron paramagnetic resonance absorption and inelastic neutron scattering cross-section are given, allowing for a determination of three of the microscopic anisotropy interactions from the second excited state manifold of FM tetramers. We also predict that tetramers with symmetries $S_4$ and $D_{2d}$ should exhibit both DM interactions and multiferroic states, and illustrate our predictions for $s_1=1/2, 1$.Comment: 30 pages, 14 figures, submitted to Phys. Rev.

Bounding and approximating parabolas for the spectrum of Heisenberg spin systems

We prove that for a wide class of quantum spin systems with isotropic Heisenberg coupling the energy eigenvalues which belong to a total spin quantum number S have upper and lower bounds depending at most quadratically on S. The only assumption adopted is that the mean coupling strength of any spin w.r.t. its neighbours is constant for all N spins. The coefficients of the bounding parabolas are given in terms of special eigenvalues of the N times N coupling matrix which are usually easily evaluated. In addition we show that the bounding parabolas, if properly shifted, provide very good approximations of the true boundaries of the spectrum. We present numerical examples of frustrated rings, a cube, and an icosahedron.Comment: 8 pages, 3 figures. Submitted to Europhysics Letter

Nucleotide sequence of the structural gene (pyrB) that encodes the catalytic polypeptide of aspartate transcarbamoylase of Escherichia coli.

The deoxyribonucleotide sequence of pyrB, the cistron encoding the catalytic subunit of aspartate transcarbamoylase (carbamoylphosphate: L-aspartate carbamoyltransferase, EC 2.1.3.2), has been determined. The pyrB gene encodes a polypeptide of 311 amino acid residues initiated by an NH2-terminal methionine that is not present in the catalytically active polypeptide. The DNA sequence analysis revealed the presence of an eight-amino-acid sequence beginning at Met-219 that was not detected in previous analyses of amino acid sequence. This octapeptide sequence provides an additional component of the disordered loop in the equatorial domain of the catalytic polypeptide. It had been found previously that the catalytic polypeptide is expressed from a bicistronic operon that also produces the regulatory polypeptide encoded by pyrI. A single transcriptional control region precedes the structural gene of the catalytic polypeptide and a simple 15-base-pair region separates its COOH terminus from the structural gene of the regulatory polypeptide. The chain-terminating codon of the catalytic polypeptide may contribute to the ribosomal binding site for the regulatory polypeptide and thus assist coordinate expression of the two cistrons

Field-induced level crossings in spin clusters: Thermodynamics and magneto-elastic instability

Quantum spin clusters with dominant antiferromagnetic Heisenberg exchange interactions typically exhibit a sequence of field-induced level crossings in the ground state as function of magnetic field. For fields near a level crossing, the cluster can be approximated by a two-level Hamiltonian at low temperatures. Perturbations, such as magnetic anisotropy or spin-phonon coupling, sensitively affect the behavior at the level-crossing points. The general two-level Hamiltonian of the spin system is derived in first-order perturbation theory, and the thermodynamic functions magnetization, magnetic torque, and magnetic specific heat are calculated. Then a magneto-elastic coupling is introduced and the effective two-level Hamilitonian for the spin-lattice system derived in the adiabatic approximation of the phonons. At the level crossings the system becomes unconditionally unstable against lattice distortions due to the effects of magnetic anisotropy. The resultant magneto-elastic instabilities at the level crossings are discussed, as well as the magnetic behavior.Comment: 13 pages, 8 figures, REVTEX

Spin dynamics in the low-dimensional magnet TiOCl

We present detailed ESR investigations on single crystals of the low-dimensional quantum magnet TiOCl. The anisotropy of the g-factor indicates a stable orbital configuration below room temperature, and allows to estimate the energy of the first excited state as 0.3(1) eV ruling out a possible degeneracy of the orbital ground state. Moreover, we discuss the possible spin relaxation mechanisms in TiOCl and analyze the angular and temperature dependence of the linewidth up to 250 K in terms of anisotropic exchange interactions. Towards higher temperatures an exponential increase of the linewidth is observed, indicating an additional relaxation mechanism.Comment: 10 pages, 8 figures; accepted for publication in Phys. Rev.

Automatic Quantum Error Correction

Criteria are given by which dissipative evolution can transfer populations and coherences between quantum subspaces, without a loss of coherence. This results in a form of quantum error correction that is implemented by the joint evolution of a system and a cold bath. It requires no external intervention and, in principal, no ancilla. An example of a system that protects a qubit against spin-flip errors is proposed. It consists of three spin 1/2 magnetic particles and three modes of a resonator. The qubit is the triple quantum coherence of the spins, and the photons act as ancilla.Comment: 16 pages 12 fig LaTex uses multicol, graphicx expanded version of letter submitted to Phys Rev Let

High-field Electron Spin Resonance of Cu_{1-x}Zn_{x}GeO_{3}

High-Field Electron Spin Resonance measurements were made on powder samples of Cu_{1-x}Zn_{x}GeO_{3} (x=0.00, 0.01, 0.02, 0.03 and 0.05) at different frequencies (95, 110, 190, 220, 330 and 440 GHz) at low temperatures. The spectra of the doped samples show resonances whose positions are dependent on Zn concentration, frequency and temperature. The analysis of intensity variation of these lines with temperature allows us to identify them as originating in transitions within states situated inside the Spin Peierls gap. A qualitative explanation of the details of the spectra is possible if we assume that these states in the gap are associated with "loose" spins created near the Zn impurities, as recently theoreticaly predicted. A new phenomenon of quenching of the ESR signal across the Dimerized to Incommensurate phase-boundary is observed.Comment: 4 pages, 5 ps figures in the text, submitted to Phys. Rev. Let