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Calculation of vibrational SFG spectra from molecular dynamics simulations
MUSIL, Patrik
In this thesis, implementation of calculation vibrational Sum-Frequency Generation (SFG) spectra from classical molecular simulations of aqueous solutions in the O-H vibrations region is presented. The key part of the thesis was significant improvement of the original codes used by the group of Prof. Marie-Pierre Gaigeot to post-process ab initio molecular dynamics trajectories to predict vibrational SFG spectra and apply it to classical molecular dynamics simulations. Particular attention was paid to modifying and optimizing the code for processing much larger systems (number of molecules) and much longer trajectories (longer simulation times), allowing to take advantage of classical simulations to work on larges scales than the ab initio simulations. The code also integrates calculations of contributions from water O-H bonds and surface hydroxyls. As a new feature, calculation of cross-correlations among molecules was implemented. The performance of the resulting codes is verified and the influence of classical molecular simulation parameters, as well as parameters entering the SFG spectra calculations, on the calculated vibrational SFG spectra is studied for fluorite/water interface.
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Sum-frequency generation in far-UV spectral region
Martínek, Miroslav
;
Kozák, Martin
(advisor) ;
Ondič, Lukáš
(referee)
Nonlinear optics is the area of high field optics, where the dependence of polarization of matter on the electric field of optical radiation cannot be considered as linear. This has important implications for practise, since the superposition principle is no longer valid in nonlinear optics. Thus it is possible to influence light, propagating through material, by another intensive radiation. Nonlinear optical phenomena are important especially for laser technology because they allow to generate light at different wavelengths using various interactions. This thesis is focused on the study of the sum-frequency generation in the far ultraviolet (UV) region of the spectrum. As the radiation source the femtosecond laser system was used. The aim of the study was to theoretically describe generation by nonlinear wave equation and to calculate the dependence of phase-matching angle on generated wavelength. Theoretical results were then verified experimentally in the laboratory. Also the energy of generated pulses and sum-frequency generation efficiency were measured for pulses in spectral region 215-250 nm. The generated pulses will further serve to excite electron-hole pairs in the diamond.
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