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This thesis work analyses aspects of dissipative quantum dynamics, with a view to look for further possibilities of controlling the dynamics with shaped laser pulses. The first part concerns the problem of efficient population transfer in mesoscopic zero-dimensional solid state systems - InAs quantum dots embedded in GaAs matrix. In these systems the consequences of laser driving induced dissipation of exciton dynamics are analyzed, in relation to adiabatic population transfer. Specifically, the problem of robust creation of exciton and biexciton states are addressed through numerical simulations and analytical approaches using a non-Markovian density matrix based analysis, suitable for dealing with dissipative quantum dynamics under strong laser fields. A physical picture describing phonon induced dissipation among dressed state has emerged as a consistent interpretation of the underlying dynamics. Furthermore, suitable parameter regimes where efficient population transfer can be achieved are proposed. The second part deals with the population transfer to high lying vibrational states of the CO stretching mode of carboxy-hemoglobin molecule in the native protein environment. On the basis of a fluctuating potential for the CO stretching mode, ultrafast pump-probe spectra are simulated using quantum wave packet propagation. To this end, Local Control Theory was employed to find design a set of laser pulses which accomplish the 'vibrational ladder climbing' and selective state preparation despite the detrimental fluctuations induced by the protein environment. These results will be providing benchmarks for the future experimental efforts.
This collection of lectures treats the dynamics of open systems with a strong emphasis on dissipation phenomena related to dynamical chaos. This research area is very broad, covering topics such as nonequilibrium statistical mechanics, environment-system coupling (decoherence) and applications of Markov semi-groups to name but a few. The book addresses not only experienced researchers in the field but also nonspecialists from related areas of research, postgraduate students wishing to enter the field and lecturers searching for advanced textbook material.
Marco Schröter investigates the influence of the local environment on the exciton dynamics within molecular aggregates, which build, e.g., the light-harvesting complexes of plants, bacteria or algae by means of the hierarchy equations of motion (HEOM) method. He addresses the following questions in detail: How can coherent oscillations within a system of coupled molecules be interpreted? What are the changes in the quantum dynamics of the system for increasing coupling strength between electronic and nuclear degrees of freedom? To what extent does decoherence govern the energy transfer properties of molecular aggregates?.
Knowledge of the excitation characteristics of matter is decisive for the descriptions of a variety of dynamical processes, which are of significant technological interest. E.g. transport properties and the optical response are controlled by the excitation spectrum. This self-contained work is a coherent presentation of the quantum theory of correlated few-particle excitations in electronic systems. It begins with a compact resume of the quantum mechanics of single particle excitations. Particular emphasis is put on Green function methods, which offer a natural tool to unravel the relations between the physics of small and large electronic systems. The book contains explicit expressions for the Coulomb Green function of two charge particles and a generalization to three-body systems. Techniques for the many-body Green function of finite systems are introduced and some explicit calculations of the Green functions are given. Concrete examples are provided and the theories are contrasted with experimental data, when available. The second volume presents an up-to-date selection of applications of the developed concepts and a comparison with available experiments is made
Mots-clés de l'auteur: Ultrafast Optical Spectroscopy ; Many-Body Physics ; Collective Excitations ; Strongly Correlated Electron Systems.
Finally, I investigate the dynamical interplay between the electron–electron interaction and the electron–phonon coupling within the Anderson–Holstein model via two complementary NCAs: the first is constructed around the weak-coupling limit and the second around the polaron limit. The influence of phonons on spectral and transport properties is explored in equilibrium, for non-equilibrium steady state and for transient dynamics after a quench. I find the two NCAs disagree in nontrivial ways, indicating that more reliable approaches to the problem are needed. The complementary frameworks used here pave the way for numerically exact methods based on inchworm dQMC algorithms capable of treating open systems simultaneously coupled to multiple fermionic and bosonic baths.