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101.
102.
Detrital magnetic materials within cave stalagmitic formations, e.g., haematite or magnetite, carry remanence whose vector is of value in dating. Magnetometry measurements on a particular haematite‐bearing sample reveal that remanence was substantially restored and/or conserved on rewarming after cooling below the Morin transition temperature. Mössbauer measurements indicate the presence of two types of haematite, distinguished primarily by particle size. The majority is small in size, partially exhibiting superparamagnetism, and does not undergo a Morin transition above liquid nitrogen temperature. Superparamagnetic goethite is the second major component. Mine haematite samples of surface location with different color and mineralogical composition have also been studied. Possible relations between the mineralogical composition of the mine samples and detrital stalagmitic magnetic material, the modifications and the origin of this mineralization are discussed. Special attention is paid to the “irreversible” Morin transition in large enough (>20 nm) haematite particles and the possible loss of natural remanent magnetization and hence of palaeomagnetic records. 相似文献
103.
M. Haas E. Realo H. Winkler W. Meyer‐Klaucke A.X. Trautwein 《Hyperfine Interactions》2000,125(1-4):189-195
An expression for the amplitude of a pulse of synchrotron radiation coherently scattered in the forward direction by a Mössbauer absorber consisting of randomly oriented paramagnetic ironcontaining molecules (for example, a frozen solution of a 57Fe protein) in an applied magnetic field is derived from the theory of optics. It is assumed that the hyperfine splittings present in the Mössbauer nuclei can be described in the framework of the spinHamiltonian formalism. In the general case of a thick Mössbauer sample of this kind the response on an incident monochromatic and fully polarized beam cannot be given analytically because of the integrations involved. How nuclear forwardscattering for this general case is evaluated in the program package called SYNFOS is outlined. 相似文献
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Teschner T Yatsunyk L Schünemann V Paulsen H Winkler H Hu C Scheidt WR Walker FA Trautwein AX 《Journal of the American Chemical Society》2006,128(4):1379-1389
Crystalline samples of four low-spin Fe(III) octaalkyltetraphenylporphyrinate and two low-spin Fe(III) tetramesitylporphyrinate complexes, all of which are models of the bis-histidine-coordinated cytochromes of mitochondrial complexes II, III, and IV and chloroplast complex b(6)f, and whose molecular structures and EPR spectra have been reported previously, have been investigated in detail by M?ssbauer spectroscopy. The six complexes and the dihedral angles between axial ligand planes of each are [(TMP)Fe(1-MeIm)(2)]ClO(4) (0 degree), paral-[(OMTPP)Fe(1-MeIm)(2)]Cl (19.5 degrees), paral-[(TMP)Fe(5-MeHIm)(2)]ClO(4) (26 degrees, 30 degrees for two molecules in the unit cell whose EPR spectra overlap), [(OETPP)Fe(4-Me(2)NPy)(2)]Cl (70 degrees), perp-[(OETPP)Fe(1-MeIm)(2)]Cl (73 degrees), and perp-[(OMTPP)Fe(1-MeIm)(2)]Cl (90 degrees). Of these, the first three have been shown to exhibit normal rhombic EPR spectra, each with three clearly resolved g-values, while the last three have been shown to exhibit "large g(max)" EPR spectra at 4.2 K. It is found that the hyperfine coupling constants of the complexes are consistent with those reported previously for low-spin ferriheme systems, with the largest-magnitude hyperfine coupling constant, A(zz), being considerably smaller for the "parallel" complexes (400-540 kG) than for the strictly perpendicular complex (902 kG), A(xx) being negative for all six complexes, and A(zz) and A(xx) being of similar magnitude for the "parallel" complexes (for example, for [(TMP)Fe(1-MeIm)(2)]Cl, A(zz) = 400 kG, A(xx) = -400 kG). In all cases, A(yy) is small but difficult to estimate with accuracy. With results for six structurally characterized model systems, we find for the first time qualitative correlations of g(zz), A(zz), and DeltaE(Q) with axial ligand plane dihedral angle Deltavarphi. 相似文献
106.
Ronayne KL Paulsen H Höfer A Dennis AC Wolny JA Chumakov AI Schünemann V Winkler H Spiering H Bousseksou A Gütlich P Trautwein AX McGarvey JJ 《Physical chemistry chemical physics : PCCP》2006,8(40):4685-4693
The vibrational modes of the low-spin and high-spin isomers of the spin crossover complex [Fe(phen)(2)(NCS)(2)] (phen = 1,10-phenanthroline) have been measured by IR and Raman spectroscopy and by nuclear inelastic scattering. The vibrational frequencies and normal modes and the IR and Raman intensities have been calculated by density functional methods. The vibrational entropy difference between the two isomers, DeltaS(vib), which is--together with the electronic entropy difference DeltaS(el)--the driving force for the spin-transition, has been determined from the measured and from the calculated frequencies. The calculated difference (DeltaS(vib) = 57-70 J mol(-1) K(-1), depending on the method) is in qualitative agreement with experimental values (20-36 J mol(-1) K(-1)). Only the low energy vibrational modes (20% of the 147 modes of the free molecule) contribute to the entropy difference and about three quarters of the vibrational entropy difference are due to the 15 modes of the central FeN(6) octahedron. 相似文献
107.
E Witt F Witt N Trautwein D Fenske J Neumann H Borchert J Parisi J Kolny-Olesiak 《Physical chemistry chemical physics : PCCP》2012,14(33):11706-11714
Nearly monodisperse lead chalcogenide (PbE, E = S, Se, or Te) semiconductor quantum dots of controllable shape have been produced via a novel synthesis which includes the occurrence of in situ formed Pb(0) particles. Tunable size and shape are achieved through appropriate choice of the precursor type and the stabilizer. As precursor, we use, on the one hand, lead oxide or lead acetate, on the other hand, tellurium, selenium, or sulfur powder dissolved in trioctylphosphine (TOP), tributylphosphine (TBP), or 1-octadecene (ODE). Oleic acid (OA) and various amines, as well as TOP and TBP are used for stabilization. With respect to possible application in hybrid solar cells, the surface of as-synthesized spherical PbSe nanocrystals was investigated by nuclear magnetic resonance (NMR), mass spectrometry (MS) and thermogravimetric analysis (TGA). As an important result, it was found that the surface is not mostly covered by oleic acid after synthesis, but by a phosphorus compound. We also applied a ligand exchange procedure with hexylamine and found evidence for the successful attachment of hexylamine to the nanocrystal surface. Additionally, charge separation between these nanoparticles and the conjugated polymer poly(3-hexylthiophene) (P3HT) is studied by electron spin resonance and photoinduced absorption spectroscopy. The spectra obtained suggest that charges can be produced successfully by photoinduced charge transfer. 相似文献
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We consider the controlled stochastic Navier–Stokes equations in a bounded multidimensional domain, where the noise term allows jumps. In order to prove existence and uniqueness of an optimal control w.r.t. a given control problem, we first need to show the existence and uniqueness of a local mild solution of the considered controlled stochastic Navier–Stokes equations. We then discuss the control problem, where the related cost functional includes stopping times dependent on controls. Based on the continuity of the cost functional, we can apply existence and uniqueness results provided in [4], which enables us to show that a unique optimal control exists. 相似文献