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Structural dynamics of solvated metal complexes with anisotropy-enhanced X-ray scattering
| Content Provider | Semantic Scholar |
|---|---|
| Author | Biasin, Elisa Nielsen, Martin Meedom Haldrup, Kristoffer |
| Copyright Year | 2016 |
| Abstract | Transition metal complexes undergo photochemical and photophysical processes that can be exploited in applications such as solar energy conversion, catalysis, and water splitting. Understanding such processes involves the investigation of the photoinduced dynamics at the fundamental time scale of atomic motions. This thesis describes the use of time-resolved X-ray scattering at X-ray free electron lasers to study the photoinduced structural dynamics of solvated transition metal complexes at the femtosecond time scale. First, the thesis describes the formalism necessary for the analysis of asymmetric scattering patterns arising from an aligned ensemble of molecules. The scattering signal is expanded in a sum of the zero-order (isotropic) and second-order (anisotropic) Legendre polynomials. Secondly, the thesis describes and applies methods to: correct raw measured anisotropic scattering patterns, especially from artefacts dependent on the X-ray source; extract isotropic and anisotropic di erence scattering curves from the scattering patterns; quantitatively analyse the isotropic and anisotropic signals. Focus is given to the information gained from the anisotropic signal. The rst application of these methods gives insight into the ultrafast (< 3 ps) electronic and structural dynamics of [Co(terpy)2] in water upon photoinduced spin state transition. Density Functional Theory calculations and Molecular Dynamics simulations are used to interpret the ultrafast elongation of the Co-N bonds, the vibrational coherences arising from Co-N stretching and decaying on a sub-picosecond time scale, the population kinetics, and the changes in the rst solvation shell. From the anisotropic component of the signal, the transient response of the water molecules to the linearly polarized laser eld is observed and provides an accurate estimate of the Instrument Response Func- |
| File Format | PDF HTM / HTML |
| Alternate Webpage(s) | http://orbit.dtu.dk/ws/files/127665899/PhDThesis_BiasinElisa_Oct2016..pdf |
| Alternate Webpage(s) | https://backend.orbit.dtu.dk/ws/portalfiles/portal/127665899/PhDThesis_BiasinElisa_Oct2016..pdf |
| Alternate Webpage(s) | https://orbit.dtu.dk/ws/files/127665899/PhDThesis_BiasinElisa_Oct2016..pdf |
| Alternate Webpage(s) | http://orbit.dtu.dk/files/127665899/PhDThesis_BiasinElisa_Oct2016..pdf |
| Language | English |
| Access Restriction | Open |
| Content Type | Text |
| Resource Type | Article |
