Selective resonant excitations can be realized with a shaped ultrashort pulse in an optically dense collection of multilevel individual atoms, where the near dipole-dipole interactions induce intrinsic frequency shifts of the atomic resonance. A proper transform-limited pulse and modulation of excitation pulses can be controlled to establish constructive or destructive quantum interference between different excitation pathways towards a desired selective resonant excitation, even driven by pulses with broadband spectral components.
Selective resonant excitations can be realized with a shaped ultrashort pulse in an optically dense collection of multilevel individual atoms, where the near dipole-dipole interactions induce intrinsic frequency shifts of the atomic resonance. A proper transform-limited pulse and modulation of excitation pulses can be controlled to establish constructive or destructive quantum interference between different excitation pathways towards a desired selective resonant excitation, even driven by pulses with broadband spectral components.
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 theoretically demonstrate that selective resonant excitation can be achieved in a dense collection of V-type three-level atoms by optimizing the pulse delay and peak intensity ratio of an applied phase-tailored ultrashort pulse pair. Near-dipole-dipole interaction plays an important role in the quantum control of selective excitations since it brings about an intrinsic frequency shift in the atomic resonance, which builds up various excitation pathways. As a consequence, we can control the quantum interference between various pathways by shaping the excitation pulse pair to steer the atomic excitation selectively toward a desired quantum state.
A selective excitation technique based on light interference is proposed to control quantum systems by frequency-chirped laser fields. Interference of two identical, delayed and phase-shifted pulses is used to modulate the laser spectrum and project it onto the time domain. By adjusting the delay and phase shift, selected transitions can be brought into the ``holes'' of the spectrum and thus remain nonexcited. The possibility to selectively manipulate or even ``shut down'' resonant transitions, making the medium transparent to the field, is shown for the Rb atom.
The resonant absorption, emission, and scattering of light are the fundamental optical processes that have been used both to probe matter and to manipulate light itself. In the last decade there has been essential progress in coherent control of both linear and nonlinear optical responses based on resonant excitation of atomic coherence in multilevel quantum systems. Some interesting and useful phenomena, resulting from coherent control of absorption and the group index, such as electromagnetically induced transparency, lasing without inversion, and ultra-slow group velocity of light have been widely studied. This work is focused on coherent control of refractive index and resonant fluorescence in multilevel medium. \n \nWe suggest two promising schemes for resonant enhancement of the refractive index with eliminated absorption and propose their implementation in transition element doped crystals with excited state absorption and in a cell of Rb atoms at natural abundance. We show how to use one of these schemes for spatial variation of the refractive index via its periodic resonant increase/decrease, remarkably keeping at the same time zero absorption/gain. It opens the way to production of transparent photonic structures (such as distributed Bragg reflectors, holey fibers, or photonic crystals) in a homogeneous resonant atomic media such as dielectrics with homogeneously distributed impurities, atomic, or molecular gases. These optically produced photonic structures could easily be controlled (including switching on/off, changing amplitude and period of modulation) and would be highly selective in frequency, naturally limited by the width of the optical resonance. \n \nWe also derive the optical fluorescence spectra of a three-level medium driven by two coherent fields at the adjacent transitions in a general case when all three transitions are allowed. We show that coherent driving can efficiently control the distribution of intensities between the fluorescent channels. In particular, the total intensity of fluorescence at the transition which is not driven by the optical fields may essentially exceed the fluorescence intensity at the driven transitions under the condition of two-photon resonance. This counter-intuitive effect is due to depletion of the intermediate state via atomic interference.
The coherent control of atomic energy level population is important for several areas physics and engineering including fluorescent spectroscopy, resonantly enhanced multiphoton ionization, harmonic generation, remote sensing and lasing. At low intensities where the Stark shift can be neglected, coherent control mechanisms usually exploit resonances created from stationary energy states dressed by integer multiples of the photon energy. However, in the strong field limit where large laser pulse intensities lead to significant Stark shifts, the resonant conditions are dynamic both in time and space and will likely not be satisfied for the entire laser pulse or beam.\n\nIn this research, we experimentally and theoretically demonstrate coherent control of atomic energy level population in sodium vapor as well as the selective excitation of sodium Rydberg levels using high intensity laser pulses. We also make a direct measurement of the ponderomotive shift of the continuum. While techniques based on resonance interferences and rapid adiabatic passage have been introduced for selective excitation, the conditions that must be satisfied for these phenomena can be hampered by short femtosecond pulse durations and large Stark shifts. In contrast, a technique referred to here as Resonance Sampling, uses the AC Stark shifts to selectively induce Freeman resonances and is resilient to changes in the spectral phase. Freeman resonances established in this way can result in population inversion of the excited state, and may lead to new lasing mediums and remote sensing applications.\n\n\nIn this research, we experimentally and theoretically demonstrate coherent control of atomic energy level population in sodium vapor as well as the selective excitation of sodium Rydberg levels using high intensity laser pulses. While techniques based on resonance interferences and rapid adiabatic passage have been introduced for selective excitation, the conditions that must be satisfied for these phenomena can be hampered by short femtosecond pulse durations and large Stark shifts. In contrast, a technique referred to here as Resonance Sampling, uses the AC Stark shifts to selectively induce Freeman resonances and is resilient to changes in the spectral phase. Freeman resonances established in this way can result in population inversion of the excited state, and may lead to new lasing mediums and remote sensing applications.
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.