By Matthias J.N.Junk
In his thesis, Matthias Junk takes an cutting edge method of investigate the neighborhood constitution and dynamics of organic and artificial amphiphilic macromolecules able to transporting small molecules. exchanging the latter with strong radicals, he makes use of state of the art electron paramagnetic resonance (EPR) spectroscopy to explain the hugely appropriate shipping functionality from the point of view of the visitor molecules. Such, he demonstrates that the sensible constitution of human serum albumin in resolution considerably differs from its crystal constitution – a outcome of the protein’s adaptability to host a number of endogenous compounds and drug molecules. additional, he indicates that the thermal cave in of thermoresponsive hydrogels and dendronized polymers ends up in static and dynamic heterogeneities at the nanoscale. those heterogeneities endure results for the material’s website hosting homes and allow unexpected complicated catalytic functionalities.
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Extra resources for Assessing the Functional Structure of Molecular Transporters by EPR Spectroscopy
Simulated powder spectra of a Jahn–Teller distorted copper(II) complex and a nitroxide are shown in Fig. 7, which exhibit both g and A anisotropy. The g tensor of the copper complex is axially symmetric due to four identical equatorial ligands, while the nitroxide shows unique orientational dependences along all molecular axes. The hyperfine anisotropy, however, is approximately axially symmetric in both cases. In either case, the principal axes of the g and the A tensor coincide. 4 Anisotropy in EPR Spectra 23 moiety (see also Sect.
Sect. 4). Between these two extremes, the spectral shape strongly depends on the time frame of the rotational diffusion. 6 Nitroxides as Spin Probes 29 1 2 3 EZ NZ HF NQ Fig. 10 Energy level diagram for an S ¼ 1=2; I ¼ 1=2 spin system in the strong coupling case jA=2j [ jXI j with allowed EPR transitions (blue) and nuclear single quantum (SQ) and double quantum (DQ) transitions (red). The nuclear quadrupole contribution is included sc ¼ Z1 hDlm;n ðXðtÞÞjDlm;n ðXðt0 ÞÞidt: ð2:65Þ t0 A detailed derivation is given in the literature [40, 41].
Due to this fact, all rotational correlation times in this thesis were obtained by fitting of spectral simulations (cf. Sect. 7). 30 2 Electron Paramagnetic Resonance Theory 2Azz 2Ayy z y x N O R Fig. 11 Definition of the molecular coordinate system of nitroxides and hypothetical spectra for orientations along the principal axes. Collinear g and A tensors with principal values gxx ¼ 2:0087; gyy ¼ 2:0065; gzz ¼ 2:0023 and Axx ¼ Ayy ¼ 18:2 MHz; Azz ¼ 100:9 MHz were assumed. g. due to chemical attachment), an anisotropy has to be introduced to the Brownian motion.