In this thesis, we present work on coherent control of multilevelquantum systems in the strong field limit using shaped ultrafastlaser pulses. In recent years there have been numerous multiphotonabsorption experiments in two,three, and four-level atomic/molecularsystems and many are performed in the limit of weak fields whereperturbation theory is valid. Here, we describe a series ofexperiments aimed at exploring and understanding multiphotontransitions when the exciting field is strong and perturbationtheory breaks down. Our approach to strong field control utilizesboth parameterized scans of various pulse shapes and closed-looplearning control to identify a pulse shape that is optimal forpopulating a target quantum state. With this we will highlight thedifference between sequential population transfer and adiabaticrapid passage in multilevel systems with multiphoton couplingbetween levels. Additionally, we examine strong field control of afour-level atomic interferometer and show how interference in atarget state changes from resonant pathways in the frequency domainto time-domain interference via a singe path.Further, we use shaped femtosecond pulses to demonstrate aphenomenon in which a three-level atom becomes a modulator of anultrafast pulse. The results are based on a pump-probe scheme thatis very similar to Electromagnetically Induced Transparency (EIT).Important dynamics associated with a time-dependent coupling fieldare examined. Lastly, we extend previous work on two-photon drivensuperfluorescence from a shaped ultrafast drive laser and show howstimulated emission near threshold can turn modest coherent controlyields into essentially perfect discrimination between systems wherea control factor of about 104 is achieved between atomic andmolecular species.
Selective multiphoton excitations can be achieved by tailoring the driving pulses to manipulate the outcome of the light-matter interaction. While single-photon transitions of single atoms driven by ultrashort pulses, dependent mainly on the resonant frequency component, and thus possesses no optical selectivity no matter how the excitation pulse shapes [1]. Interestingly, when an ultrashort pulse interacts with an optically dense medium, quantum controllable optical selectivity can be achieved in a single-photon process.
We investigate optimal states of photon pairs to excite a target transition in a multilevel quantum system. With the help of coherent control theory for two-photon absorption with quantum light, we infer the maximal population achievable by optimal entangled vs separable states of light. Interference between excitation pathways as well as the presence of nearby states may hamper the selective excitation of a particular target state, but we show that quantum correlations can help to overcome this problem and enhance the achievable "selectivity" between two energy levels, i.e., the relative difference in population transferred into each of them. We find that the added value of optimal entangled states of light increases with broadening linewidths of the target states.
Wavefront shaping enables control of classical light through scattering media. Extending these techniques to spatially entangled photons promises new quantum applications, but their fundamental limits, especially when both photons scatter, remain unclear. Here, we theoretically and numerically investigate the enhancement of two-photon correlations through thick scattering media. We analyze configurations where a spatial light modulator shapes one or both photons, either before or after the medium, and show that the optimal enhancement differs fundamentally from classical expectations. For a system with
N modes, we show that shaping one photon yields the classical enhancement
η≈(π/4)N, while shaping both photons before the medium reduces it to
η≈(π/4)2N. However, in some symmetric detection schemes, when both photons are measured at the same mode, perfect correlations are restored with
η≈N, resembling digital optical phase conjugation. Conversely, shaping both photons after the medium leads to a complex, NP-hard-like optimization problem, yet achieves superior enhancements, up to
η≈4.6N. These results reveal unique quantum effects in complex media and identify strategies for quantum imaging and communication through scattering environments.
Ideally, strong nonlinearities could be used to implement quantum gates for photonic qubits by well-controlled two-photon interactions. However, the dependence of the nonlinear interaction on frequency and time makes it difficult to preserve a coherent pulse shape that could justify a single-mode model for the time-frequency degree of freedom of the photons. In this paper, we analyze the problem of temporal multimode effects by considering the pulse shape of the average output field obtained from a coherent input pulse. It is shown that a significant part of the two-photon state transformation can be derived from this semiclassical description of the optical nonlinearity. The effect of a nonlinear system on a two-photon state can then be determined from the density-matrix dynamics of the coherently driven system using input-output theory. As an example, the resonant nonlinearity of a single two-level atom is characterized. The results indicate that the most efficient nonlinear effect may not be the widely studied single-mode phase shift, but the transfer of one of the photons to an orthogonal mode distinguished by its temporal and spectral properties.