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Register a new userTin-DNA Complexes Investigated by Nuclear Inelastic Scattering of Synchrotron Radiation
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Nuclear inelastic scattering (NIS) of synchrotron radiation has been used to investigate the dynamics of tin ions chelated by DNA. Theoretical NIS spectra have been simulated with the help of density functional theory (DFT) calculations using 12 models for different binding sites of the tin ion in (CH3)Sn(DNAPhosphate)2. The simulated spectra are compared with the measured spectrum of the tin-DNA complex.
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Nuclear inelastic scattering (NIS) spectra were recorded for the spin-crossover complexes STP and ETP (STP = [Fe(1,1,1-trisf[N-(2-pyridylmethyl)-N-methylamino]methylg- ethane)](ClO4)2 and ETP = [Fe(1,1,1-trisf[N-(2-pyridylmethyl)-N-methylamino]methylg-butane)](ClO4)2) at 30 K and at room temperature and also at ambient pressure and applied pressure (up to 2.6 GPa). Spin transition from the high-spin (HS) to the low-spin (LS) state was observed by lowering temperature and also by applying pressure at room temperature and has been assigned to the hardening of iron-bond stretching modes due to the smaller volume in the LS isomer.
The theory of incoherent nuclear resonant scattering of synchrotron radiation accompanied by absorption or emission of phonons in a crystal lattice is developed. The theory is based on the Maxwells equations and time-dependent quantum mechanics under the condition of incoherent scattering of radiation by various nuclei. A concept of coherence in scattering processes, properties of the synchrotron radiation, and conditions of measurement are discussed. We show that employing the monochromator with a narrow bandwidth plays a decisive role.
Nuclear inelastic scattering of synchrotron radiation has been used now since 10 years as a tool for vibrational spectroscopy. This method has turned out especially useful in case of large molecules that contain a Mossbauer active metal center. Recent applications to iron-sulfur proteins, to iron(II) spin crossover complexes and to tin-DNA complexes are discussed. Special emphasis is given to the combination of nuclear inelastic scattering and density functional calculations.
The nanoscale fluctuation dynamics of semi dilute high molecular weight polymer solutions of Polyethylenoxide (PEO) in D2O under non-equilibrium flow conditions were studied by the neutron spin-echo technique. The sample cell was in contraction flow geometry and provided a pressure driven flow with a high elongational component that stretched the polymers most efficiently. The experiments suggest that the mobility on the scale of a few monomers, comparable to the Kuhn segment length, becomes highly anisotropic and is enhanced perpendicular to the flow direction. Diffraction data show a weak structural correlation along the chains on a length scale of about 17 Angstroems, which might be related to the Kuhn length in this system.
Nuclear resonant forward scattering (NFS) and nuclear inelastic scattering (NIS) of synchrotron radiation are fairly recent spectroscopic methods for the investigation of complexes containing Mossbauer-active transition metal ions. NFS, which can be regarded as Mossbauer spectroscopy in the time domain, overcomes some limitations of conventional Mossbauer spectroscopy as has been demonstrated especially for bioinorganic compounds. NIS extends the energy range of conventional Mossbauer spectroscopy to the range of molecular vibrations. Since NIS is sensitive only to the mean-square displacement of Mossbauer nuclei it can be used as site-selective vibrational spectroscopy. It complements usefully comparable techniques such as IR or Raman spectroscopy. Examples are given for applications to spin crossover complexes, nitroprusside compounds, heme model complexes and myoglobin.
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