Exchange couplings in the magnetic molecular cluster Mn12Ac

The magnetic properties of the molecular cluster Mn12Ac are due to the four Mn3+ ions which have spins S=3/2 and the eight Mn4+ ions with spins S=2. These spins are coupled by superexchange mechanism. We determine the four exchange couplings assuming a Heisenberg-type interaction between the ions. We use exact diagonalization of the spin Hamiltonian by a Lanczos algorithm and we adjust the couplings to reproduce the magnetization curve of Mn12Ac. We also impose the constraint of reproducing a gap of 35K between a S=10 ground state and a first excited state with S=9. We predict that there is an excited level with S=8 at 37K above the ground state, only slightly above the S=9 excited state which lies at 35K and the next excited state is a S=9 multiplet at 67K above the S=10 ground state.Comment: 15 pages, 6 figures, submitted to Phys Rev B, corrected a misTeX: values of J1, J2 have changed, refs update

Spin Tunneling and Phonon-assisted Relaxation in Mn12-acetate

We present a comprehensive theory of the magnetization relaxation in a Mn12-acetate crystal in the high-temperature regime (T>1 K), which is based on phonon-assisted spin tunneling induced by quartic magnetic anisotropy and weak transverse magnetic fields. The overall relaxation rate as function of the longitudinal magnetic field is calculated and shown to agree well with experimental data including all resonance peaks measured so far. The Lorentzian shape of the resonances, which we obtain via a generalized master equation that includes spin tunneling, is also in good agreement with recent data. We derive a general formula for the tunnel splitting energy of these resonances. We show that fourth-order diagonal terms in the Hamiltonian lead to satellite peaks. A derivation of the effective linewidth of a resonance peak is given and shown to agree well with experimental data. In addition, previously unknown spin-phonon coupling constants are calculated explicitly. The values obtained for these constants and for the sound velocity are also in good agreement with recent data. We show that the spin relaxation in Mn12-acetate takes place via several transition paths of comparable weight. These transition paths are expressed in terms of intermediate relaxation times, which are calculated and which can be tested experimentally.Comment: 18 pages, 22 EPS figures, REVTe

Semiconductive and Photoconductive Properties of the Single Molecule Magnets Mn12_{12}-Acetate and Fe8_8Br8_8

Resistivity measurements are reported for single crystals of Mn$_{12}$-Acetate and Fe$_8$Br$_8$. Both materials exhibit a semiconductor-like, thermally activated behavior over the 200-300 K range. The activation energy, $E_a$, obtained for Mn$_{12}$-Acetate was 0.37 $\pm$ 0.05 eV, which is to be contrasted with the value of 0.55 eV deduced from the earlier reported absorption edge measurements and the range of 0.3-1 eV from intramolecular density of states calculations, assuming $2E_a$= $E_g$, the optical band gap. For Fe$_8$Br$_8$, $E_a$ was measured as 0.73 $\pm$ 0.1 eV, and is discussed in light of the available approximate band structure calculations. Some plausible pathways are indicated based on the crystal structures of both lattices. For Mn$_{12}$-Acetate, we also measured photoconductivity in the visible range; the conductivity increased by a factor of about eight on increasing the photon energy from 632.8 nm (red) to 488 nm (blue). X-ray irradiation increased the resistivity, but $E_a$ was insensitive to exposure.Comment: 7 pages, 8 figure

Low energy magnetic excitations of the Mn_{12}-acetate spin cluster observed by neutron scattering

We performed high resolution diffraction and inelastic neutron scattering measurements of Mn_{12}-acetate. Using a very high energy resolution, we could separate the energy levels corresponding to the splitting of the lowest S multiplet. Data were analyzed within a single spin model (S=10 ground state), using a spin Hamiltonian with parameters up to 4^{th} order. The non regular spacing of the transition energies unambiguously shows the presence of high order terms in the anisotropy (D= -0.457(2) cm^{-1}, B_4^0 = -2.33(4) 10^{-5}cm^{-1}). The relative intensity of the lowest energy peaks is very sensitive to the small transverse term, supposed to be mainly responsible for quantum tunneling. This allows an accurate determination of this term in zero magnetic field (B_4^4 = \pm 3.0(5) 10^{-5} cm^{-1}). The neutron results are discussed in view of recent experiments and theories.Comment: 4 pages ? 3 figures, submitted to Physical Review Lette

Entraves e desafios na construção recente da política indigenista no Brasil : arenas, problemas e interações (controvérsias) entre atores

Trabalho de Conclusão de Curso (graduação)—Universidade de Brasília, Faculdade de Economia, Administração, Contabilidade e Gestão de Políticas Públicas, Departamento de Gestão de Políticas Públicas, 2018.Esta monografia constrói um modelo explicativo para o travamento da política indigenista no Brasil recente, a partir da assunção dos conceitos de arena, problemas públicos, interações (controvérsias) entre os atores. A partir de um posicionamento cognitivo pós-positivista em uma abordagem pragmatista, a metodologia utiliza-se de uma análise qualitativa, de tipologia descritiva e explicativa entrevista, utilizando técnicas de pesquisa documental primária, secundária e entrevista. Percebeu-se que os retrocessos, em uma perspectiva de políticas indigenistas são uma constante enquanto os avanços foram poucos. Ao mesmo tempo, os problemas públicos que conformam as arenas orbitantes à questão indígena dificilmente conseguem sair da esfera do interesse especializado. Com isso, mostrou-se que a construção de uma matriz explicativa contendo avanços e retrocessos permitiu compreender que os retrocessos tinham também uma cara de continuidade

Role of dipolar and exchange interactions in the positions and widths of EPR transitions for the single-molecule magnets Fe8 and Mn12

We examine quantitatively the temperature dependence of the linewidths and line shifts in electron paramagnetic resonance experiments on single crystals of the single-molecule magnets Fe$_8$ and Mn$_{12}$, at fixed frequency, with an applied magnetic field along the easy axis. We include inter-molecular spin-spin interactions (dipolar and exchange) and distributions in both the uniaxial anisotropy parameter $D$ and the Land\'{e} $g$-factor. The temperature dependence of the linewidths and the line shifts are mainly caused by the spin-spin interactions. For Fe$_8$ and Mn$_{12}$, the temperature dependence of the calculated line shifts and linewidths agrees well with the trends of the experimental data. The linewidths for Fe$_8$ reveal a stronger temperature dependence than those for Mn$_{12}$, because for Mn$_{12}$ a much wider distribution in $D$ overshadows the temperature dependence of the spin-spin interactions. For Fe$_8$, the line-shift analysis suggests two competing interactions: a weak ferromagnetic exchange coupling between neighboring molecules and a longer-ranged dipolar interaction. This result could have implications for ordering in Fe$_8$ at low temperatures.Comment: published versio

Dislocation-induced spin tunneling in Mn-12 acetate

Comprehensive theory of quantum spin relaxation in Mn-12 acetate crystals is developed, that takes into account imperfections of the crystal structure and is based upon the generalization of the Landau-Zener effect for incoherent tunneling from excited energy levels. It is shown that linear dislocations at plausible concentrations provide the transverse anisotropy which is the main source of tunneling in Mn-12. Local rotations of the easy axis due to dislocations result in a transverse magnetic field generated by the field applied along the c-axis of the crystal, which explains the presence of odd tunneling resonances. Long-range deformations due to dislocations produce a broad distribution of tunnel splittings. The theory predicts that at subkelvin temperatures the relaxation curves for different tunneling resonances can be scaled onto a single master curve. The magnetic relaxation in the thermally activated regime follows the stretched-exponential law with the exponent depending on the field, temperature, and concentration of defects.Comment: 17 pages, 14 figures, 1 table, submitted to PR

Resonant Magnetization Tunneling in Mn12 Acetate: The Absence of Inhomogeneous Hyperfine Broadening

We present the results of a detailed study of the thermally-assisted-resonant-tunneling relaxation rate of Mn12 acetate as a function of an external, longitudinal magnetic field and find that the data can be fit extremely well to a Lorentzian function. No hint of inhomogeneous broadening is found, even though some is expected from the Mn nuclear hyperfine interaction. This inconsistency implies that the tunneling mechanism cannot be described simply in terms of a random hyperfine field.Comment: Some minor revisions, title changed, updated figures, two added notes, one added reference. RevTeX, 4 pages, 3 postscript figures. Submitted to Rapid Communication

Building on surface-active ionic liquids for the rescuing of the antimalarial drug chloroquine

Ionic liquids derived from classical antimalarials are emerging as a new approach towards the cost-effective rescuing of those drugs. Herein, we disclose novel surface-active ionic liquids derived from chloroquine and natural fatty acids whose antimalarial activity in vitro was found to be superior to that of the parent drug. The most potent ionic liquid was the laurate salt of chloroquine, which presented IC50 values of 4 and 110 nM against a chloroquine-sensitive and a chloroquine-resistant strain of Plasmodium falciparum, respectively, corresponding to an 11-and 6-fold increase in potency as compared to the reference chloroquine bisphosphate salt against the same strains. This unprecedented report opens new perspectives in both the fields of malaria chemotherapy and of surface-active ionic liquids derived from active pharmaceutical ingredients.publishersversionpublishe

The habitability of Proxima Centauri b I. Irradiation, rotation and volatile inventory from formation to the present

International audienceProxima b is a planet with a minimum mass of 1.3 MEarth orbiting within the habitable zone (HZ) of Proxima Centauri, a very low-mass, active star and the Sun's closest neighbor. Here we investigate a number of factors related to the potential habitability of Proxima b and its ability to maintain liquid water on its surface. We set the stage by estimating the current high-energy irradiance of the planet and show that the planet currently receives 30 times more EUV radiation than Earth and 250 times more X-rays. We compute the time evolution of the star's spectrum, which is essential for modeling the flux received over Proxima b's lifetime. We also show that Proxima b's obliquity is likely null and its spin is either synchronous or in a 3:2 spin-orbit resonance, depending on the planet's eccentricity and level of triaxiality. Next we consider the evolution of Proxima b's water inventory. We use our spectral energy distribution to compute the hydrogen loss from the planet with an improved energy-limited escape formalism. Despite the high level of stellar activity we find that Proxima b is likely to have lost less than an Earth ocean's worth of hydrogen before it reached the HZ 100-200 Myr after its formation. The largest uncertainty in our work is the initial water budget, which is not constrained by planet formation models. We conclude that Proxima b is a viable candidate habitable planet