Laser-plasma accelerators are of great interest because of their ability to sustain extremely large acceleration gradients, enabling compact accelerating structures. Laser-plasma acceleration is realized by using a high-intensity short pulse laser to drive a large plasma wave or wakefield in an underdense plasma. This thesis considers the effect of axial plasma density upramps on laser wakefield acceleration. Theoretical groundwork shows that tapered plasma channels can be used to mitigate one of the main limitations of laser plasma acceleration, that is, dephasing of an electron beam with respect to the plasma wave. It is shown that it is possible to maintain an electron bunch at constant phase in the longitudinal electric fields of the laser wake field. This leads to an increased energy gain of an electron trapped in the wakefield. The required shape of the density slope is difficult to implement in experiments. Therefore, a linear density ramp is also considered which is predicted to also increase the energy gain beyond that possible in a uniform density plasma. Towards an experimental implementation it was studied how a suitable gas density profile can be established in a capillary. This was done employing simulations using the computational fluid dynamics tool kit OpenFoam and comparing these to measurements of the axial density profile based on Raman scattering. It was demonstrated that a linear density ramp could be established by applying different pressures on the capillary gas inlets. The dependence of the density profile on the capillary parameters, such as, capillary diameter and length and inlet diameter were also studied. The results of the simulations and the measurement showed excellent agreement and demonstrate that approximately linear density ramps can be generated by flowing gas along a capillary of constant cross-section Laser wakefield acceleration in plasmas with longitudinally varying density was investigated in an experiment at the Astra Laser at Rutherford Laboratories. The experiment utilised ionisation injection in order to operate in the mildly non-linear regime of laser-wakefield acceleration. The measured electron energies agree well with the theoretical predictions. It was demonstrated that an increase in the energy gain can be obtained by driving the accelerator in a ramped plasma, the electron spectrum is more narrow and the injected charge increases significantly. Measurements of the X-ray spectrum emitted by the betatron motion of the accelerated electron bunch allowed the transverse radius of the bunch to be deduced. These measurements showed that retrieved electron bunch radius is inversely proportional to the longitudinal density gradient, that is a plasma density upramp (downramp) has a decreased (increased) electron bunch radius.

Based on the superposition principle, any two states of a quantum system may be coherently superposed to yield a novel state. Such a simple construction is at the heart of genuinely quantum phenomena such as interference of massive particles or quantum entanglement. Yet, these superpositions are susceptible to environmental influences, eventually leading to a complete disappearance of the system's quantum character. In principle, two distinct mechanisms responsible for this process of decoherence may be identified. In a classical decoherence setting, on the one hand, stochastic fluctuations of classical, ambient fields are the relevant source. This approach leads to a formulation in terms of stochastic Hamiltonians; the dynamics is unitary, yet stochastic. In a quantum decoherence scenario, on the other hand, the system is described in the language of open quantum systems. Here, the environmental degrees of freedom are to be treated quantum mechanically, too. The loss of coherence is then a direct consequence of growing correlations between system and environment. The purpose of the present thesis is to clarify the distinction between classical and quantum decoherence. It is known that there exist decoherence processes that are not reconcilable with the classical approach. We deem it desirable to have a simple, feasible model at hand of which it is known that it cannot be understood in terms of fluctuating fields. Indeed, we find such an example of true quantum decoherence. The calculation of the norm distance to the convex set of classical dynamics allows for a quantitative assessment of the results. In order to incorporate genuine irreversibility, we extend the original toy model by an additional bath. Here, the fragility of the true quantum nature of the dynamics under increasing coupling strength is evident. The geometric character of our findings offers remarkable insights into the geometry of the set of non-classical decoherence maps. We give a very intuitive geometrical measure---a volume---for the quantumness of dynamics. This enables us to identify the decoherence process of maximum quantumness, that is, having maximal distance to the convex set of dynamics consistent with the stochastic, classical approach. In addition, we observe a distinct correlation between the decoherence potential of a given dynamics and its achievable quantumness. In a last step, we study the notion of quantum decoherence in the context of a bipartite system which couples locally to the subsystems' respective environments. A simple argument shows that in the case of a separable environment the resulting dynamics is of classical nature. Based on a realistic experiment, we analyze the impact of entanglement between the local environments on the nature of the dynamics. Interestingly, despite the variety of entangled environmental states scrutinized, no single instance of true quantum decoherence is encountered. In part, the identification of the classical nature relies on numerical schemes. However, for a large class of dynamics, we are able to exclude analytically the true quantum nature.

In spite of being the subject of intense research, several key but complex questions on the nonequilibrium physics of correlated quantum systems remain controversial. For example, the nature of particle and energy transport in different interacting regimes, the relevance of integrability and the impact of environmental coupling are still under active debate. These problems can now be approached numerically, due to the development of powerful algorithms which allow the efficient simulation of the dynamics of correlated systems. In the present thesis we study numerically and analytically the transport properties of low-dimensional quantum systems. In particular, we consider the steady-state spin and energy conduction through XXZ boundary-driven spin-1/2 chains. In the first part, we analyse the transport through chains with only coherent processes in the bulk. For spin transport induced by a magnetisation imbalance between the boundaries, previously identified ballistic, diffusive and negative differential conductivity regimes are reproduced. We provide a comprehensive explanation of the latter. The energy conduction induced by this driving scheme features the same properties as spin transport. For thermally-driven chains, we discuss the nature of energy transport and the emergence of local thermal states when the integrability of the Hamiltonian is broken. In the second part of the thesis we analyse the effect of bulk incoherent effects on the transport properties previously discussed. First we find that for weak particle-particle interactions, pure dephasing degrades spin and energy conduction. In contrast, for strong interactions dephasing induces a significant transport enhancement. We identify the underlying mechanism and discuss its generality. Finally, motivated by the lattice structure of several organic conductors, we study the interplay between coherent and incoherent processes in systems of weakly-coupled chains. We find an enhancement effect due to incoherent interchain hopping, stronger than that by dephasing, which increases with the chain length and relates to superdiffusive transport.

Atomically thin, semiconducting transition metal dichalogenides (TMDs), a special class of layered semiconductors, that can be shaped as a perfect two dimensional material, have garnered a lot of attention owing to their fascinating electronic properties which are achievable at the extreme nanoscale. In contrast to graphene, the most celebrated two-dimensional (2D) material thus far; TMDs exhibit a direct band gap in the monolayer regime. The presence of a non-zero bandgap along with the broken inversion symmetry in the monolayer limit brands semiconducting TMDs as the perfect candidate for future optoelectronic and valleytronics-based device application. These remarkable discoveries demand exploration of different materials that possess similar properties alike TMDs. Recently, III-VI layered semiconducting materials (example: InSe, GaSe etc.) have also emerged as potential materials for optical device based applications as, similar to TMDs, they can be shaped into a perfect two-dimensional form as well as possess a sizable band gap in their nano-regime. The perfect 2D character in layered materials cause enhancement of strong Coulomb interaction. As a result, excitons, a coulomb bound quasiparticle made of electron-hole pair, dominate the optical properties near the bandgap. The basis of development for future optoelectronic-based devices requires accurate characterization of the essential properties of excitons. Two fundamental parameters that characterize the quantum dynamics of excitons are: a) the dephasing rate, 𝛾, which represents the coherence loss due to the interaction of the excitons with their environment (for example- phonons, impurities, other excitons, etc.) and b) excited state population decay rate arising from radiative and non-radiative relaxation processes. The dephasing rate is representative of the time scale over which excitons can be coherently manipulated, therefore accurately probing the source of exciton decoherence is crucial for understanding the basic unexplored science as well as creating technological developments. The dephasing dynamics in semiconductors typically occur in the picosecond to femtosecond timescale, thus the use of ultrafast laser spectroscopy is a potential route to probe such excitonic responses. The focus of this dissertation is two-fold: firstly, to develop the necessary instrumentation to accurately probe the aforementioned parameters and secondly, to explore the quantum dynamics and the underlying many-body interactions in different layered semiconducting materials. A custom-built multidimensional optical non-linear spectrometer was developed in order to perform two-dimensional spectroscopic (2DFT) measurements. The advantages of this technique are multifaceted compared to regular one-dimensional and non-linear incoherent techniques. 2DFT technique is based on an enhanced version of Four wave mixing experiments. This powerful tool is capable of identifying the resonant coupling, probing the coherent pathways, unambiguously extracting the homogeneous linewidth in the presence of inhomogeneity and decomposing a complex spectra into real and imaginary parts. It is not possible to uncover such crucial features by employing one dimensional non-linear technique. Monolayers as well as bulk TMDs and group III-VI bulk layered materials are explored in this dissertation. The exciton quantum dynamics is explored with three pulse four-wave mixing whereas the phase sensitive measurements are obtained by employing two-dimensional Fourier transform spectroscopy. Temperature and excitation density dependent 2DFT experiments unfold the information associated with the many-body interactions in the layered semiconducting samples.

Based on the superposition principle, any two states of a quantum system may be coherently superposed to yield a novel state. Such a simple construction is at the heart of genuinely quantum phenomena such as interference of massive particles or quantum entanglement. Yet, these superpositions are susceptible to environmental influences, eventually leading to a complete disappearance of the system's quantum character. In principle, two distinct mechanisms responsible for this process of decoherence may be identified. In a classical decoherence setting, on the one hand, stochastic fluctuations of classical, ambient fields are the relevant source. This approach leads to a formulation in terms of stochastic Hamiltonians; the dynamics is unitary, yet stochastic. In a quantum decoherence scenario, on the other hand, the system is described in the language of open quantum systems. Here, the environmental degrees of freedom are to be treated quantum mechanically, too. The loss of coherence is then a direct consequence of growing correlations between system and environment. The purpose of the present thesis is to clarify the distinction between classical and quantum decoherence. It is known that there exist decoherence processes that are not reconcilable with the classical approach. We deem it desirable to have a simple, feasible model at hand of which it is known that it cannot be understood in terms of fluctuating fields. Indeed, we find such an example of true quantum decoherence. The calculation of the norm distance to the convex set of classical dynamics allows for a quantitative assessment of the results. In order to incorporate genuine irreversibility, we extend the original toy model by an additional bath. Here, the fragility of the true quantum nature of the dynamics under increasing coupling strength is evident. The geometric character of our findings offers remarkable insights into the geometry of the set of non-classical decoherence maps. We give a very intuitive geometrical measure---a volume---for the quantumness of dynamics. This enables us to identify the decoherence process of maximum quantumness, that is, having maximal distance to the convex set of dynamics consistent with the stochastic, classical approach. In addition, we observe a distinct correlation between the decoherence potential of a given dynamics and its achievable quantumness. In a last step, we study the notion of quantum decoherence in the context of a bipartite system which couples locally to the subsystems' respective environments. A simple argument shows that in the case of a separable environment the resulting dynamics is of classical nature. Based on a realistic experiment, we analyze the impact of entanglement between the local environments on the nature of the dynamics. Interestingly, despite the variety of entangled environmental states scrutinized, no single instance of true quantum decoherence is encountered. In part, the identification of the classical nature relies on numerical schemes. However, for a large class of dynamics, we are able to exclude analytically the true quantum nature.

No description available.

This thesis describes theoretical and experimental work whose main aim is the development of techniques for using trapped ⁴³Ca⁺ ions for quantum information processing. I present a rate equations model of ⁴³Ca⁺, and compare it with experimental data. The model is then used to investigate and optimise an electron-shelving readout method from a ground-level hyperfine qubit. The process is robust against common experimental imperfections. A shelving fidelity of up to 99.97% is theoretically possible, taking 100 μs. The laser pulse sequence can be greatly simplified for only a small reduction in the fidelity. The simplified method is tested experimentally with fidelities up to 99.8%. The shelving procedure could be applied to other commonly-used species of ion qubit. An entangling two-qubit quantum controlled-phase gate was attempted between a ⁴⁰Ca⁺ and a ⁴³Ca⁺ ion. The experiment did not succeed due to frequent decrystallisation of the ion pair, and strong motional decoherence. The source of the problems was never identified despite significant experimental effort, and the decision was made to suspend the experiments and continue them in an improved ion trap which is under construction. A sequence of pi-pulses, inspired by the Hahn spin-echo, was derived that is capable of greatly reducing dephasing of any qubit. If the qubit precession frequency varies with time as an nth-order polynomial, an (n+1) pulse sequence is theoretically capable of perfectly cancelling the resulting phase error. The sequence is used on a 43Ca+ magnetic-field-sensitive hyperfine qubit, with 20 pulses increasing the coherence time by a factor of 75 compared to an experiment without any spin-echo. In our ambient noise environment the well-known Carr-Purcell-Meiboom-Gill dynamic-decoupling method was found to be comparably effective.

Methoden der transienten Vierwellenmischung mit Femtosekunden-Zeitauflösung werden angewendet, um die Phasen- und Energierelaxation optisch selektiv erzeugter Anregungszustände im Lichtsammelkomplex II höherer Pflanzen (LHC II) sowie im Halbleiter Cadmiumsulfid (CdS) bei verschiedenen Temperaturen zu untersuchen. Für den LHC II werden die Ergebnisse der Messungen des zeitaufgelösten und integrierten Zweipuls-Photonenechos mit Resultaten aus Pump-Test-Experimenten verglichen, um unter Einbeziehung von Literaturdaten Rückschlüsse über den Charakter der phasenzerstörenden Prozesse zu ziehen und Zusammenhänge zu Strukturdaten des Komplexes aufzudecken. Die vorliegende Arbeit liefert erstmals einen systematischen Überblick über die totalen Phasenrelaxationszeiten T2 im Bereich der Qy-Bande des LHC II von 640 bis 685 nm bei 5 K. Das bei 5 K beobachtete Photonenechosignal am LHC II zeigt in Abhängigkeit von der Verzögerung der beiden Anregungsimpulse ein multiexponentielles Abklingen, das auf die Überlagerung der Einflüsse mehrerer Relaxationsprozesse zurückgeführt wird. Dabei lassen sich drei charakteristische Bereiche der Phasenrelaxationszeit unterscheiden, die verschiedenen phasenzerstörenden Prozessen zugeordnet werden. Ein Vergleich mit Resultaten aus Pump-Test-Experimenten führt zu der Schlußfolgerung, daß die Phasenrelaxation im LHC II bei 5 K für Wellenlängen £ 675 nm im wesentlichen durch den Energietransfer auf einer sub-ps Zeitskala bestimmt wird. Für Wellenlängen > 675 nm steigt die Phasenrelaxationszeit stark an und wird insbesondere im Bereich der tiefsten Anregungszustände um 680 nm durch reine Phasenzerstörung dominiert. Ab 20 K setzt bei dieser Wellenlänge ein zusätzlicher phasenzerstörender Prozeß ein, der mit steigender Temperatur zu einem mäßigen linearen Anstieg der Phasenrelaxationsrate (T2)-1 führt. Die Ursache ist vermutlich ein Aufwärts-Energietransfer. Im Bereich der Chlorophyll a-Absorption vernichten außerdem (physiologisch irrelevante) Multiexzitoneneffekte die Kohärenz der angeregten Zustände, verursacht durch die hohe Anregungsintensität. Zusammenfassend kann festgestellt werden, daß die Erhaltung der Kohärenz für die Funktionalität des LHC II eine untergeordnete Rolle spielt. Die wesentlichen Prozesse sind der schnelle räumliche Energietransfer und die Energierelaxation auf das Niveau des primären Elektrondonators P680 im Reaktionszentrum. Am Halbleiter CdS wird erstmals ein mittels Zwei-Photonen-Absorption angeregtes Photonenecho beschrieben, das in Abhängigkeit von der Wellenlänge charakteristische Quantenbeats mit einer Periode von 700 bis 800 fs zeigt. Das stark gedämpfte periodische Echosignal tritt sowohl für positive als auch für negative Verzögerungszeiten t der Anregungsimpulse auf, wobei die Abklingzeit für t>0 mit 170±10 fs doppelt so groß ist wie für t / Transient four-wave-mixing experiments with femtosecond resolution are performed in order to investigate phase and energy relaxation processes of optically excited states in the light harvesting complex II of higher plants (LHC II) and in the semiconductor cadmium sulfide (CdS) at different wavelengths and temperatures. Extensive studies of the time resolved and integrated two-pulse photon echo on LHC II are combined with pump-probe experiments. Results of both methods together with literature data are used to characterize the nature of dephasing processes and to reveal connections with structural data of the complex. This study gives the first systematic survey of total dephasing times T2 in the spectral region of the Qy-absorption band of LHC II from 640 to 685 nm at 5 K. In the case of LHC II, the photon echo signal at 5 K monitored as a function of delay between both excitation pulses shows a multi-exponential decay which is attributed to the superposition of several relaxation processes. Three characteristic dephasing time domains can be distinguished, ascribed to different dephasing processes. Comparing photon echo and pump-probe results it can be concluded that dephasing in LHC II at 5 K and for wavelengths £ 675 nm is dominated by the fast excitation energy transfer on a sub-ps time scale. At wavelengths > 675 nm the total dephasing time increases drastically. The loss of coherence of the lowest excited states around 680 nm at 5 K is mainly determined by pure dephasing. An additional dephasing process, probably uphill energy transfer, occurs at temperatures higher than 20 K leading to a moderate linear rise of the dephasing rate (T2)-1 with increasing temperature. Furthermore, the dephasing in the spectral region of chlorophyll a absorption is affected by (physiologically irrelevant) multi-excitonic effects caused by the high excitation energy. In summary, it can be concluded that the preservation of coherence plays a minor role in the functionality of LHC II. The main processes are the fast spatial excitation energy transfer and the energy relaxation down to the energetic level of the primary electron donor P680 of the reaction center. Investigations of four-wave mixing signals of the semiconductor CdS resulted in the first description of a two-photon excited photon echo in CdS showing characteristic quantum beats with a period of 700 to 800 fs in dependence on wavelength. The strongly damped periodical echo signal is found for both positive and negative delay times t between the excitation pulses. The decay time for t>0 amounts to 170±10 fs and is twice as large as for t

A espectroscopia Raman é utilizada para obtenção de informações dinâmicas de líquidos. A habilidade do ânion croconato como sonda das interações é testada no estudo do processo de transição vítrea no sal croconato de tetra-n-butilamônio (CTBA), [(C4H9)4N]2C5O5.4H2O, um líquido muito viscoso com temperatura de transição vítrea, Tg, em cerca de 298K. As funções de correlação temporais foram obtidas pela transformada de Fourier do contorno dos modos do croconato, C5O5-2. Posteriormente, foram ajustados modelos teóricos para o defasamento vibracional a essas funções de correlação, como o modelo de Kubo. Nesse estudo foi possível encontrar assinaturas espectroscópicas da transição vítrea que são interpretadas do ponto de vista da dinâmica do ânion croconato e das interações deste ânion com o ambiente em que ele se insere. A miscibilidade do CTBA em acetonitrila permitiu que fossem feitos estudos do defasamento do ânion croconato neste solvente. Nestes estudos, nota-se um contraste com os resultados obtidos para a solução aquosa saturada do sal Li2C5O5. O valor encontrado para tempo de correlação da flutuação da freqüência vibracional, τc, na solução diluída em acetonitrila (τc ≈ 0,5 ps) é superior ao respectivo valor encontrado no CTBA. A relaxação lenta e o ambiente homogêneo experimentado pelo oxocarbono na solução diluída de CTBA em acetonitrila corroboram que as interações de curto alcance entre as moléculas de acetonitrila e o croconato não são decisivas para o defasamento neste sistema, já que na solução aquosa o valor de τc é determinado pela estrutura de gaiola das moléculas de água em torno do C5O5-2 unidas por ligações de hidrogênio fortes. / Raman spectroscopy is used for attainment of dynamic information of liquids. The ability of the croconate anion as a probe of the interactions is tested in the study of the glass transition in the salt tetra-n-butilammonium croconate (CTBA), [n-(C4H9)4N]2C5O5.4H2O, a very viscous liquid with glass transition temperature, Tg, at ca. 298K. The time correlation functions were obtained by Fourier transforming the contour of the Raman bands of the croconate\'s modes, C5O5-2. Theoretical models for vibrational dephasing were adjusted to these vibrational time correlation functions by the Kubo\'s equation. In this study, it was possible to find spectroscopic signatures of the glass transition that are interpreted in the light of the dynamics of the croconate anion, and the interactions of this anion with the surrounding environment. The miscibility of the CTBA with acetonitrile allowed for studies of the anion dephasing in this solvent. In these studies, a contrast with the results obtained for the saturated aqueous solution of the simple salt Li2C5O5 was noticed. The value of the correlation time of the fluctuation of the vibrational frequency, τc, in the diluted acetonitrile solution (τc ≈ 0,5 ps) is higher than the respective value in pure CTBA despite the high viscosity of the latter. The slow relaxation and the homogeneous environment probed by oxocarbon in the diluted solution of CTBA in acetonitrile corroborate the physical picture in which the short-range interactions between the molecules of acetonitrile and the croconate are not essential for the vibrational dephasing in this system, since the τc value in the aqueous solution is mainly determined by the tight structure of water molecules around the C5O5-2 due to the hydrogen bonds.

A espectroscopia Raman é utilizada para obtenção de informações dinâmicas de líquidos. A habilidade do ânion croconato como sonda das interações é testada no estudo do processo de transição vítrea no sal croconato de tetra-n-butilamônio (CTBA), [(C4H9)4N]2C5O5.4H2O, um líquido muito viscoso com temperatura de transição vítrea, Tg, em cerca de 298K. As funções de correlação temporais foram obtidas pela transformada de Fourier do contorno dos modos do croconato, C5O5-2. Posteriormente, foram ajustados modelos teóricos para o defasamento vibracional a essas funções de correlação, como o modelo de Kubo. Nesse estudo foi possível encontrar assinaturas espectroscópicas da transição vítrea que são interpretadas do ponto de vista da dinâmica do ânion croconato e das interações deste ânion com o ambiente em que ele se insere. A miscibilidade do CTBA em acetonitrila permitiu que fossem feitos estudos do defasamento do ânion croconato neste solvente. Nestes estudos, nota-se um contraste com os resultados obtidos para a solução aquosa saturada do sal Li2C5O5. O valor encontrado para tempo de correlação da flutuação da freqüência vibracional, τc, na solução diluída em acetonitrila (τc ≈ 0,5 ps) é superior ao respectivo valor encontrado no CTBA. A relaxação lenta e o ambiente homogêneo experimentado pelo oxocarbono na solução diluída de CTBA em acetonitrila corroboram que as interações de curto alcance entre as moléculas de acetonitrila e o croconato não são decisivas para o defasamento neste sistema, já que na solução aquosa o valor de τc é determinado pela estrutura de gaiola das moléculas de água em torno do C5O5-2 unidas por ligações de hidrogênio fortes. / Raman spectroscopy is used for attainment of dynamic information of liquids. The ability of the croconate anion as a probe of the interactions is tested in the study of the glass transition in the salt tetra-n-butilammonium croconate (CTBA), [n-(C4H9)4N]2C5O5.4H2O, a very viscous liquid with glass transition temperature, Tg, at ca. 298K. The time correlation functions were obtained by Fourier transforming the contour of the Raman bands of the croconate\'s modes, C5O5-2. Theoretical models for vibrational dephasing were adjusted to these vibrational time correlation functions by the Kubo\'s equation. In this study, it was possible to find spectroscopic signatures of the glass transition that are interpreted in the light of the dynamics of the croconate anion, and the interactions of this anion with the surrounding environment. The miscibility of the CTBA with acetonitrile allowed for studies of the anion dephasing in this solvent. In these studies, a contrast with the results obtained for the saturated aqueous solution of the simple salt Li2C5O5 was noticed. The value of the correlation time of the fluctuation of the vibrational frequency, τc, in the diluted acetonitrile solution (τc ≈ 0,5 ps) is higher than the respective value in pure CTBA despite the high viscosity of the latter. The slow relaxation and the homogeneous environment probed by oxocarbon in the diluted solution of CTBA in acetonitrile corroborate the physical picture in which the short-range interactions between the molecules of acetonitrile and the croconate are not essential for the vibrational dephasing in this system, since the τc value in the aqueous solution is mainly determined by the tight structure of water molecules around the C5O5-2 due to the hydrogen bonds.