Coherent control in the presence of disorder

This thesis is about coherent control on disordered samples. Coherent control is the steering of processes with light of different frequencies. The relative phases between the frequencies determines in which di- rection the process is steered. When many frequencies are used, the light composes a short pulse. Changing the relative phases of the fre- quencies changes the shape of this pulse. We used such shaped pulses to guide processes on our samples. Pulse shaping and the different disordered samples are introduced in chapter 1, after which chapter 2 proceeds with the experimental details behind our studies. To perform a measurement with a shaped pulse, a nonlinear pro- cess is required. Second-harmonic generation (SHG) is one of the most straightforward nonlinear processes and plays an important role in this thesis. In chapter 3 theory of SHG is developed. Specifically, we deter- mine how to calculate the SHG intensity from shaped pulses on sam- ples with a resonance near the frequency of the illuminating light. We show that two mechanisms that broaden the line width of a resonance can not be distinguished by measuring the SHG signal. In the absence of resonances the maximum SHG intensity is produced by a transform- limited pulse. This pulse shape is required for many nonlinear optical spectroscopies and maximizing the SHG intensity is a useful method to obtain it. For such optimizations, algorithms are used that tune the coefficients for basis functions of the spectral phase. We looked at the fitness landscape of the SHG when a common basis set is used and by inspecting projections of the landscapewe constructed a more efficient basis set, that will make optimizations of SHG more efficient. In chapter 4 we describe simulations of the electric field in a ran- dom electrical network. The electrical network serves as a model for a film of randomly positioned gold islands, which we studied as re- ported in chapter 5. The simulations show that a metal density close to the percolation threshold results in a structure that has favourable properties for selective local excitation of the surface. In chapter 5 we proceed with this experiment on a random gold structure. The structure was coated with a layer of quantum dots. We imaged the fluorescence from this layer with a microscope and in this way were able to detect the local field intensities on the surface. We found that some control on the field intensity is possible, but the effect is minimal compared to the results of the simulations. The reason for this discrepancy is in the radiative damping of the oscillations, which was not included in the simulation. The radiative damping of plas- mons causes dephasing within �20 fs, making control with shaped pulses difficult. We further studied SHG from arrays of sub-wavelength holes in a gold film. The results of this study are presented in chapter 6. The amount of disorder in the positions of the holes in the arrays was var- ied. We found that the the SHG is produced in a resonance with a long lifetime of 55 fs. This lifetime is longer than most plasmonic resonances and shows that the effect of radiative damping is decreased on this structure. Furthermore, the SHG from all the structures has the same features. The disorder does not influence the SHG and the same reso- nance was found on all structures. Thus, it is likely that the resonance is a property of a single hole. Finally, we studied the coherent control of a dye in solution. Here the disorder is not in the structure, but in the transition frequency of the dye. Due to the interaction of the dye with the solvent, this fre- quency is constantly changing. These changes cause coherence to be lost in the system in a short time. We ran a closed-loop optimization to maximize the stimulated emission from the dye. All the pulse shapes tried in the optimization were saved and subsequently tried with the dye dissolved in other solvents. We found that the yield of the opti- mization varied greatly with the used solvent. These results formed a trend with the viscosity of the particular solvents. The viscosity can be related directly to the dephasing time, the time in which coherence is lost in the system. The trend of the optimization yield versus the vis- cosity shows directly that the fluctuations of the solvent are limiting the coherent control of the dye.