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Physical Review A

Quantum control and pathway manipulation in rubidium

Fang Gao, Yaoxiong Wang, Roberto Rey-de-Castro, HERSCHEL A. RABITZ, Feng Shuang

Published Sep 29, 2015• 9 citations
Publisher

Abstract

There is an increasing interest in the extraction and control of the interfering quantum pathway amplitudes induced by control fields during laser-matter interactions. The Hamiltonian-encoding and observable-decoding (HE-OD) technique has been introduced for extracting the amplitudes of the pathways present in the dynamics and has recently been experimentally applied to the pathway manipulation of atomic rubidium. This paper theoretically explores various strategies for manipulating pathway amplitudes in the context of a laser field interacting with a multilevel system similar to atomic rubidium for both narrow-band and broadband ultrafast fields. In the perturbation regime, two second-order quantum pathways connecting the Rb states $5{S}_{1/2}$ and $5{D}_{3/2}$ dominate the dynamics, namely, $5{S}_{1/2}\ensuremath{\rightarrow}5{P}_{3/2}\ensuremath{\rightarrow}5{D}_{3/2}$ (pathway 1) and $5{S}_{1/2}\ensuremath{\rightarrow}5{P}_{1/2}\ensuremath{\rightarrow}5{D}_{3/2}$ (pathway 2). For narrow-band field control, the analysis is carried out in the time domain with the laser field including only four narrow-band envelope subpulses centered at the resonant frequencies. When the two pathways cooperate constructively, temporal oscillations appear in the ratio of the two pathway amplitudes, and we conclude in this case that the period corresponds to the detuning between transitions $5{S}_{1/2}\ensuremath{\rightarrow}5{P}_{3/2}$ and $5{P}_{3/2}\ensuremath{\rightarrow}5{D}_{3/2}$. For broadband field control, the dynamics are treated in the frequency domain with the laser field including both resonant and continuous nonresonant frequency components. Various control strategies based on manipulating the phase of selected spectral components are tested. Compared to the outcome from a transform limited pulse, a $\frac{\ensuremath{\pi}}{2}$ step scheme can increase the dynamic range of the ratio between the two pathway amplitudes by a factor of $\ensuremath{\sim}3$. A scheme that manipulates eight spectral blocks, in which the spectral boundaries depend on the resonant frequencies, can increase the ratio by several orders of magnitude. Numerical simulations show that further dividing the spectrum into hundreds of evenly spaced blocks does not significantly enhance the pathway ratio over the eight-block scheme. The quantum control of pathways investigated in this work provides valuable insights on how to incorporate known information about the structure of quantum systems for the effective reduction of quantum control complexity.

DOI
10.1103/physreva.92.033423

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There is an increasing interest in the extraction and control of the interfering quantum pathway amplitudes induced by control fields during laser-matter interactions. The Hamiltonian-encoding and observable-decoding (HE-OD) technique has been introduced for extracting the amplitudes of the pathways present in the dynamics and has recently been experimentally applied to the pathway manipulation of atomic rubidium. This paper theoretically explores various strategies for manipulating pathway amplitudes in the context of a laser field interacting with a multilevel system similar to atomic rubidium for both narrow-band and broadband ultrafast fields. In the perturbation regime, two second-order quantum pathways connecting the Rb states 5S1/25{S}_{1/2}5S1/2​ and 5D3/25{D}_{3/2}5D3/2​ dominate the dynamics, namely, 5S1/2\ensuremath→5P3/2\ensuremath→5D3/25{S}_{1/2}\ensuremath{\rightarrow}5{P}_{3/2}\ensuremath{\rightarrow}5{D}_{3/2}5S1/2​\ensuremath→5P3/2​\ensuremath→5D3/2​ (pathway 1) and 5S1/2\ensuremath→5P1/2\ensuremath→5D3/25{S}_{1/2}\ensuremath{\rightarrow}5{P}_{1/2}\ensuremath{\rightarrow}5{D}_{3/2}5S1/2​\ensuremath→5P1/2​\ensuremath→5D3/2​ (pathway 2). For narrow-band field control, the analysis is carried out in the time domain with the laser field including only four narrow-band envelope subpulses centered at the resonant frequencies. When the two pathways cooperate constructively, temporal oscillations appear in the ratio of the two pathway amplitudes, and we conclude in this case that the period corresponds to the detuning between transitions 5S1/2\ensuremath→5P3/25{S}_{1/2}\ensuremath{\rightarrow}5{P}_{3/2}5S1/2​\ensuremath→5P3/2​ and 5P3/2\ensuremath→5D3/25{P}_{3/2}\ensuremath{\rightarrow}5{D}_{3/2}5P3/2​\ensuremath→5D3/2​. For broadband field control, the dynamics are treated in the frequency domain with the laser field including both resonant and continuous nonresonant frequency components. Various control strategies based on manipulating the phase of selected spectral components are tested. Compared to the outcome from a transform limited pulse, a \ensuremathπ2\frac{\ensuremath{\pi}}{2}2\ensuremathπ​ step scheme can increase the dynamic range of the ratio between the two pathway amplitudes by a factor of \ensuremath∼3\ensuremath{\sim}3\ensuremath∼3. A scheme that manipulates eight spectral blocks, in which the spectral boundaries depend on the resonant frequencies, can increase the ratio by several orders of magnitude. Numerical simulations show that further dividing the spectrum into hundreds of evenly spaced blocks does not significantly enhance the pathway ratio over the eight-block scheme. The quantum control of pathways investigated in this work provides valuable insights on how to incorporate known information about the structure of quantum systems for the effective reduction of quantum control complexity.
The manipulation of two 2nd-order quantum pathways has been successfully demonstrated experimentally in atomic Rubidium. This work would explore the coherent control of pathways in the quantum system with N intermediate states connecting the initial and target states. A 4N-block scheme is proposed to control the N 2nd-order pathways which are driven by a weak broadband pulse. The model with N=3 is given as an example to demonstrate our strategy. In this scheme, boundaries of the spectral blocks are functions of the resonant frequencies, and the resonant and non-resonant contributions interfere mutually to achieve the quantum pathway control effectively. The simple strategy may provide a practical choice for pathway manipulation experiments since there are only 2N phase variables to adjust.
We investigate coherent control of the two-photon transition pathways of a four-level atomic system in a diamond configuration. When an ultrashort laser pulse interacts with this system in the ground state 5S1/25{S}_{1/2}5S1/2​ of rubidium, the two-photon transition probability amplitude of 5D3/25{D}_{3/2}5D3/2​ is obtained by a summation of all possible resonant and nonresonant two-photon transition probability amplitudes via 5P1/25{P}_{1/2}5P1/2​ and 5P3/25{P}_{3/2}5P3/2​. Second-order perturbation theory predicts that the maximal constructive interference of the transition probability amplitudes occurs when the phases of eight different spectrum blocks satisfy four different phase relations. Experiments carried out with spectrally phase-coded laser pulses show good agreement with the theoretical prediction.
We analyze the behavior of a four-state, two-path atomic interferometer driven by shaped ultrafast laser pulses. The laser pulses interact with atomic rubidium, exciting the atoms to the 5D5D5D state via two intermediate resonances (the 5P1/25{P}_{1/2}5P1/2​ and 5P3/25{P}_{3/2}5P3/2​). The relative phase of the two paths can be modified by applying a varying spectral phase at the wavelength corresponding to one of the resonant transitions for each pathway. We trace out the behavior of the system from the simplest case of weak-field excitation with resonant fields to strong-field excitation with a broadband source. Our measurements and analysis reveal that while interference is observed for all field strengths and spectral widths, the character of the interference changes substantially.
The experimental work in this thesis is divided into two distinct parts. In both parts, broadband femtosecond laser pulses are "shaped" by adjusting the relative phase and amplitude of spectral components. In the first set of experiments, time-dependent perturbation theory is used to show that the probability of a quantum transition in atomic rubidium can be substantially enhanced or suppressed using pulse shaping, compared to the probability of transition observed when a transform-limited or "flat phase" optical pulse is used. These enhancement or suppression effects are also demonstrated experimentally. As quantum interference (the material phase having been transferred from the optical phase) is used to enhance or diminish a particular final quantum state, this can be classified as a quantum coherent control experiment. In the second set of experiments, an optical pulse is scattered into a train of pulses by a layered structure. The layered structure is used to simulate the effect of optical pulses travelling through certain types of complex media. One consequence of the disruption of a single pulse into a train of pulses is lower per-pulse peak intensity, and thus a greatly diminished nonlinear signal. It is shown that spectral pulse shaping (in phase only) is sufficient to pre-compensate for the scattering structure, allowing a single transform-limited pulse to be obtained at the output.
Abstract The dynamics of two two-photon absorption (TPA) pathways in a four-level quantum system driven by a laser pulse is investigated in this work. An analytical solution for pulse shaping is proposed to be globally optimal for constructive interference between the two pathways, and accurate spectral boundaries for phase modulation are obtained. The TPA rate can be enhanced by a factor of 8.33 with the optimal pulse instead of the transform limited pulse (TL pulse). Simple control strategies modulating both amplitudes and phases are also designed to increase the TPA amplitude along one pathway while decreasing that along the other simultaneously. The strategies are intuitive and the two pathway amplitudes can differ by two orders of magnitude.