The subtle and fundamental issue of indistinguishability and interference between independent pathways to the same target state is examined in the context of coherent control of atomic and molecular processes, with emphasis placed on possible "which-way" information due to quantum entanglement established in the quantum dynamics. Because quantum interference between independent pathways to the same target state occurs only when the independent pathways are indistinguishable, it is first shown that creating useful coherence between nondegenerate states of a molecule for subsequent quantum interference manipulation cannot be achieved by collisions between atoms or molecules that are prepared in momentum and energy eigenstates. Coherence can, however, be transferred from light fields to atoms or molecules. Using a particular coherent control scenario, it is shown that this coherence transfer and the subsequent coherent phase control can be readily realized by the most classical states of light, i.e., coherent states of light. It is further demonstrated that quantum states of light may suppress the extent of phase-sensitive coherent control by leaking out some which-way information while "incoherent interference control" scenarios proposed in the literature have automatically ensured the indistinguishability of multiple excitation pathways. The possibility of quantum coherence in photodissociation product states is also understood in terms of the disentanglement between photodissociation fragments. Results offer deeper insights into quantum coherence generation in atomic and molecular processes.
The subtle and fundamental issue of indistinguishability and interference between independent pathways to the same target state is examined in the context of coherent control of atomic and molecular processes, with emphasis placed on possible "which-way" information due to quantum entanglement established in the quantum dynamics. Because quantum interference between independent pathways to the same target state occurs only when the independent pathways are indistinguishable, it is first shown that creating useful coherence between nondegenerate states of a molecule for subsequent quantum interference manipulation cannot be achieved by collisions between atoms or molecules that are prepared in momentum and energy eigenstates. Coherence can, however, be transferred from light fields to atoms or molecules. Using a particular coherent control scenario, it is shown that this coherence transfer and the subsequent coherent phase control can be readily realized by the most classical states of light, i.e., coherent states of light. It is further demonstrated that quantum states of light may suppress the extent of phase-sensitive coherent control by leaking out some which-way information while "incoherent interference control" scenarios proposed in the literature have automatically ensured the indistinguishability of multiple excitation pathways. The possibility of quantum coherence in photodissociation product states is also understood in terms of the disentanglement between photodissociation fragments. Results offer deeper insights into quantum coherence generation in atomic and molecular processes.
Wave-mechanical phenomena such as resonance and interference, in both light and matter, are central to the principles of quantum coherent control over molecular processes. Focusing on the dynamical aspects, this dissertation is a compilation of studies on the interaction physics involving wave packets in molecules, the driving light field, and the underlying coherence and control. In each work, we will demonstrate interesting correlations between the properties of a carefully designed excitation light field and desirable outcomes of the molecules quantum dynamics. We will analyze the dynamical effect of a Feshbach resonance in the adiabatic Raman photoassociation for ultracold diatomic molecule formation from ultracold atoms. A narrow resonance is shown to be able to increase the effective number of collisions, in an ultracold atomic gas, that are available for photoassociation. This results in an optimal resonance width much smaller than the atomic collision energy bandwidth, due to the balance between the effective collision rate and single-collision transfer probability. Next, we demonstrate the linear molecular response to high-intensity, broadband, shaped optical fields. We show that this originates from interferences based on intra-pulse Raman excitations, and thus response linearity is not unique to the first-order perturbative limit and can not be used to infer the strength of the field. In the last study, we simulate the stochastic vibrational wave packet and dissociation-flux dynamics in a molecule excited by light with temporal and spectral incoherent properties. Between this case and that using a coherent pulse with the same spectral profile, we compare the vibrational wave functions and the loss of electronic and vibrational coherence, and demonstrate the qualitative difference between coherently and incoherently driven dynamics in molecules.
Preface. Part I: Atomic and Molecular systems. Scenarios in Coherent Control P. Brumer, M. Shapiro. Quantum Control in Atomic Systems D. Charalambidis, et al. Laser-phase-sensitive Coherent Control of Photoion Product States in 2-Photon vs. 2-Photon Ionization of Atomic Barium, F. Wang, et al. Coherent Phase control of Photoionization and Photodissociation R.J. Gordon, et al. Coherent Control of Atomic Photoionization and Autoionization P. Lambropoulos, T. Nakajima. Lasing Without Inversion via Interference of Double-Dark Resonances in Atomic and Quantum Well Systems M.O. Scully, et al. Part II: Coherent Control in Semiconductors. Coherence Control of Free Carriers in Bulk Semiconductors H.M. van Driel, et al. Coherent Control of 2D Excitons Probed by Time-Resolved Secondary Emission X. Marie, et al. Many-Body Effects in the Ultrafast Population Transfer in p-Doped Semiconductor Quantum Wells R. Binder, M. Lindberg. Coherent Control of Heavy-Light Hole and Phonon Quantum Beats T. Kuhn, et al. Coherent Control Schemes in Semiconductor Double Wells X. Hu, W. Poetz. Terahertz-Control of Charge-Carrier Wavepackets in Semiconductor Quantum Wells S. Hughes, D.S. Citrin. Microcavity Exciton-Polariton H. Cao. Part III: Coherent Phenomena and Related Topics. Coherent Control of Quantum Localization M. Holthaus. Tunneling of Low-Energetic Electrons in the Presence of Intense Laser Fields: The Formation of Dynamical Barrier States M. Wagner. Hopping Mechanism of Coherent Photovoltaic Effect and Photoinduced Polar Anisotropy in Glass E.M. Baskin, M.V. Entin. Heterodyning Scheme Employing Quantum Interference J.B. Khurgin, et al. Generation of Widely Tunable THz-Wave Using Nonlinear Optics K. Kawase, H.Ito. List of Participants.
Quantum mechanics, though a probabilistic theory, gives a 'deterministic' answer to the question of how the present determines the future. In essence, in order to predict future probabilities, we need to (numerically) propagate the time-dependent Schrödinger equation from the present to the future. It is interesting to note that classical mechanics of macroscopic bodies, though reputed to be a deterministic theory, does not allow, due to chaos (which unfortunately is more prevalent than integrability), such clear insights into the future. In contrast, small (e.g., atomic, molecular and photonic) systems which are best understood using the tools of quantum mechanics, do not suffer from chaos, rendering the prediction of the probability-distributions of future events possible. The field of quantum control deals with an important modification of this task, namely, it asks: given a wave function in the present, what dynamics, i.e. what Hamiltonian, guarantees a desired outcome or 'objective' in the future? In practice one may achieve this goal of modifying and finding the desired Hamiltonian by introducing external fields, e.g. laser light. It is then possible to reach the objective in a 'trial-and-error' fashion, performed either numerically or in the laboratory. We can guess or build a Hamiltonian, do an experiment, or propagate the initial wave function to the future, compare the result with the desirable objective, and correct the guess for the Hamiltonian until satisfactory agreement with the objective is reached. A systematic way of executing this procedure is the sub-field called 'optimal control'. The trial-and-error method is often very time consuming and rarely provides mechanistic insight. There are situations where analytical solutions exist, rendering the control strategies more transparent. This is especially so when one can identify quantum interferences as the heart of quantum control, the essence of the field called 'coherent control'. The experience accumulated so far by many groups is that quantum interferences are the mechanism underlying most successful control scenarios and control experiments. The identification of the control mechanism is especially facile when the time-dependence of the Hamiltonian merely serves to prepare a state which then evolves in the absence of external fields. Analytical theories also exist when the explicit time dependence of the Hamiltonian can be treated adiabatically. Under these circumstances one can identify the quantum interfering pathways that lead to control, allowing for the simultaneous exploration of entire 'landscapes' (and not just a single 'desirable' objective) resulting from varying all the experimental 'knobs' at our disposal, e.g., relative- and envelope-phases, intensities, polarizations, and pulse-sequencing. Such 'pulse-shaping' knobs are now available down to the sub-femtosecond regime in broad spectral regions ranging from the UV to the IR. We expect that comprehensive investigations of the quantum interference required to control dynamical processes will result in a more detailed understanding of the dynamics themselves. Together with experimental progress---the stage is now set for many exciting applications in fundamental and applied sciences by 'tailoring' light--matter interactions essentially at will.
Laser light has been used as a probe of atoms, molecules, and solids since the invention of the laser. The use of laser light in a more active role, to modify and process surfaces, and initiate chemical reactions, followed shortly thereafter. But usually it is the intensity and the directionality of the laser light that is employed, not necessarily its coherence, and not particularly the fact that it has a well-defined phase. 'Coherence control' can be broadly understood as the set of processes whereby light modifies matter in a way that is critically dependent on the incident light beams possessing well-defined phases. While in a laser matter is manipulated to produce light of the desired properties, in coherent control light is manipulated -- in particular, its phase and intensity is adjusted -- to produce a material response of the desired type. Of the various coherent control processes that are currently being investigated, some involve a transition in the material medium from an initial state to a final state by two or more possible processes. With each of these is associated a quantum mechanical amplitude, and hence the probability for the transition can show interference effects between the two amplitudes, just as in the familiar two-slit interference experiment the probability for the electron to be observed at a given position involves a probability that is the square of the sum of two amplitudes. In quantum interference control (QUIC), the relative phase of the two amplitudes is adjusted by adjusting the relative phase of two polarizations of a single beam, or the relative phase of two beams at different frequencies. It is this particular type of coherent control that is of interest in this communication.
A new scheme is suggested to manipulate the probe transitions (and hence the optical properties of atomic vapors) via double-control destructive and constructive quantum interferences. The influence of phase coherence between the two control transitions on the probe transition is also studied. The most remarkable feature of the present scheme is that the optical properties (absorption, transparency and dispersion) of an atomic system can be manipulated using this double-control multi-pathway interferences (multiple routes to excitation). It is also shown that a four-level system will exhibit a two-level resonant absorption because the two control levels (driven by the two control fields) form a dark state (and hence a destructive quantum interference occurs between the two control transitions). However, the present four-level system will exhibit electromagnetically induced transparency to the probe field when the three lower levels (including the probe level and the two control levels) form a three-level dark state. The present scenario has potential applications in new devices (e.g. logic gates and sensitive optical switches) and new techniques (e.g. quantum coherent information storage).
The generation and control of entanglement in a quantum mechanical system are critical elements of nearly all quantum applications. Molecular systems are promising candidates, with numerous degrees of freedom able to be targeted. However, knowledge of intersystem entanglement mechanisms in such systems is limited. In this work, we demonstrate the generation of entanglement between vibrational degrees of freedom in molecules via strong coupling to a cavity mode driven by a weak coherent field. In a bimolecular system, we show that entanglement can be generated not only between the cavity and molecular system but also between molecules. This process also results in the generation of nonclassical states of light, providing potential pathways for harnessing entanglement in molecular systems.