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Physical Review Letters

Manipulating Quantum Pathways on the Fly

Roberto Rey-de-Castro, Zaki Leghtas, HERSCHEL A. RABITZ

Published May 29, 2013• 16 citations
Publisher

Abstract

The expectation value of a quantum system observable can be written as a sum over interfering pathway amplitudes. In this Letter, we demonstrate for the fist time adaptive manipulation of quantum pathways using the Hamiltonian encoding-observable decoding (HE-OD) technique. The principles of HE-OD are illustrated for population transfer in atomic rubidium using shaped femtosecond laser pulses. The ability to manipulate multiple pathway amplitudes is of fundamental importance in all quantum control applications.

DOI
10.1103/physrevlett.110.223601

Related papers

Pathway dynamics in the optimal quantum control of rubidium: Cooperation and competition

Fang Gao, Roberto Rey-de-Castro, Ashley Donovan +4 more

The dynamics that take place in the optimal quantum control of atomic rubidium upon population transfer from state 5${S}_{1/2}$ to state 5${D}_{3/2}$ are investigated with Hamiltonian-encoding--observable-decoding (HE-OD). For modest laser powers two second-order pathways, 5${S}_{1/2}$$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}$5${P}_{3/2}$$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}$5${D}_{3/2}$ (pathway 1) and 5${S}_{1/2}$$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}$5${P}_{1/2}$$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}$5${D}_{3/2}$ (pathway 2), govern the population transfer process. Pathway 1 has larger transition dipoles than pathway 2. However, state 5${P}_{3/2}$ along pathway 1 may also be excited to an undesired state 5${D}_{5/2}$, which can result in population ``leakage.'' Thus, the two pathways may either cooperate or compete with each other in various dynamical regimes. An important feature in the case of cooperation is that the ratio between the amplitudes of pathways 1 and 2 oscillates over time with a frequency equal to the detuning between transitions 5${S}_{1/2}$$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}$5${P}_{3/2}$ and 5${P}_{3/2}$$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}$5${D}_{3/2}$. We also study the regime in which pathway 2 dominates the dynamics when the larger transition dipoles of pathway 1 can no longer compensate for its population leakage. The overall analysis illustrates the utility of HE-OD as a tool to reveal the quantum control mechanism.

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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 $5{S}_{1/2}$ 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.

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Optimal control of quantum dynamics in the laboratory is proving to be increasingly successful. The control fields can be complex, and the mechanisms by which they operate have often remained obscure. Hamiltonian encoding (HE) has been proposed as a method for understanding mechanisms in quantum dynamics. In this context mechanism is defined in terms of the dominant quantum pathways leading to the final state of the controlled system. HE operates by encoding a special modulation into the Hamiltonian and decoding its signature in the dynamics to determine the dominant pathway amplitudes. Earlier work encoded the modulation directly into the Hamiltonian operators. This present work introduces the alternative scheme of field based HE, where the modulation is encoded into the control field and not directly into the Hamiltonian operators. This distinct form of modulation yields a new perspective on mechanism and is computationally faster than the earlier approach. Field based encoding is also an important step towards a laboratory based algorithm for HE as it is the only form of encoding that may be experimentally executed. HE is also extended to cover systems with noise and uncertainty and finally, a hierarchical algorithm is introduced to reveal mechanism in a stepwise fashion of ever increasing detail as desired. This new hierarchical algorithm is an improvement over earlier approaches to HE where the entire mechanism was determined in one stroke. The improvement comes from the use of less complex modulation schemes, which leads to fewer evaluations of Schrodinger's equation. A number of simulations are presented on simple systems to illustrate the new field based encoding technique for mechanism assessment.

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Efficient Hamiltonian encoding algorithms for extracting quantum control mechanism as interfering pathway amplitudes in the Dyson series

Erez Abrams, Michael Kasprzak, Gaurav Bhole +2 more

Hamiltonian encoding is a methodology for revealing the mechanism behind the dynamics governing controlled quantum systems. In this paper, following Mitra and Rabitz \cite{abhra_1}, we define mechanism via pathways of eigenstates that describe the evolution of the system, where each pathway is associated with a complex-valued amplitude corresponding to a term in the Dyson series. The evolution of the system is determined by the constructive and destructive interference of these pathway amplitudes. Pathways with similar attributes can be grouped together into pathway classes. The amplitudes of pathway classes are computed by modulating the Hamiltonian matrix elements and decoding the subsequent evolution of the system rather than by direct computation of the individual terms in the Dyson series. The original implementation of Hamiltonian encoding was computationally intensive and became prohibitively expensive in large quantum systems. This paper presents two new encoding algorithms that calculate the amplitudes of pathway classes by using techniques from graph theory and algebraic topology to exploit patterns in the set of allowed transitions, greatly reducing the number of matrix elements that need to be modulated. These new algorithms provide an exponential decrease in both computation time and memory utilization with respect to the Hilbert space dimension of the system. To demonstrate the use of these techniques, they are applied to two illustrative state-to-state transition problems.

arXiv:2406.05585•Quantum•Feb 10, 2025•1 citation
The expectation value of a quantum system observable can be written as a sum over interfering pathway amplitudes. In this Letter, we demonstrate for the fist time adaptive manipulation of quantum pathways using the Hamiltonian encoding-observable decoding (HE-OD) technique. The principles of HE-OD are illustrated for population transfer in atomic rubidium using shaped femtosecond laser pulses. The ability to manipulate multiple pathway amplitudes is of fundamental importance in all quantum control applications.
The dynamics that take place in the optimal quantum control of atomic rubidium upon population transfer from state 5S1/2{S}_{1/2}S1/2​ to state 5D3/2{D}_{3/2}D3/2​ are investigated with Hamiltonian-encoding--observable-decoding (HE-OD). For modest laser powers two second-order pathways, 5S1/2{S}_{1/2}S1/2​$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}555{P}_{3/2}$$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}$5${D}_{3/2}$ (pathway 1) and 5${S}_{1/2}$$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}555{P}_{1/2}$$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}$5${D}_{3/2}$ (pathway 2), govern the population transfer process. Pathway 1 has larger transition dipoles than pathway 2. However, state 5${P}_{3/2}$ along pathway 1 may also be excited to an undesired state 5${D}_{5/2}$, which can result in population ``leakage.'' Thus, the two pathways may either cooperate or compete with each other in various dynamical regimes. An important feature in the case of cooperation is that the ratio between the amplitudes of pathways 1 and 2 oscillates over time with a frequency equal to the detuning between transitions 5${S}_{1/2}$$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}555{P}_{3/2}$ and 5P3/2{P}_{3/2}P3/2​$\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}555{D}_{3/2}$. We also study the regime in which pathway 2 dominates the dynamics when the larger transition dipoles of pathway 1 can no longer compensate for its population leakage. The overall analysis illustrates the utility of HE-OD as a tool to reveal the quantum control mechanism.
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, $5{S}_{1/2}\ensuremath{\rightarrow}5{P}_{3/2}\ensuremath{\rightarrow}5{D}_{3/2}$ (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.
The Hamiltonian encoding observable decoding (HE-OD) technique is experimentally demonstrated for process tomography of laser-induced dynamics in atomic Rb vapor. With the assistance of a laser pulse truncation method, a time dependent reconstruction of the quantum evolution is achieved. HE-OD can perform full as well as partial process tomography with appropriate measurements to characterize the system. The latter feature makes HE-OD tomography suitable for analyzing quantum processes in complex systems.
We report on the laboratory implementation of quantum-control-mechanism identification through Hamiltonian encoding and observable decoding (HE-OD). Over a sequence of experiments, HE-OD introduces a special encoded signature into the components of a previously determined control field expressed in a chosen representation. The outcome appears as a modulated signal in the controlled system observable. Decoding the modulated signal identifies the hierarchy of correlations between components of the control field in a particular representation. In cases where the initial quantum state and observable operator are fully known, then HE-OD can also identify the transition amplitudes of the various Dyson expansion orders contributing to the controlled dynamics. The basic principles of HE-OD are illustrated for second harmonic generation when the components of the field representation are simply taken as the pixels in the pulse shaper. The outcome of HE-OD agrees well with simulations, verifying the concept.
Optimal control of quantum dynamics in the laboratory is proving to be increasingly successful. The control fields can be complex, and the mechanisms by which they operate have often remained obscure. Hamiltonian encoding (HE) has been proposed as a method for understanding mechanisms in quantum dynamics. In this context mechanism is defined in terms of the dominant quantum pathways leading to the final state of the controlled system. HE operates by encoding a special modulation into the Hamiltonian and decoding its signature in the dynamics to determine the dominant pathway amplitudes. Earlier work encoded the modulation directly into the Hamiltonian operators. This present work introduces the alternative scheme of field based HE, where the modulation is encoded into the control field and not directly into the Hamiltonian operators. This distinct form of modulation yields a new perspective on mechanism and is computationally faster than the earlier approach. Field based encoding is also an important step towards a laboratory based algorithm for HE as it is the only form of encoding that may be experimentally executed. HE is also extended to cover systems with noise and uncertainty and finally, a hierarchical algorithm is introduced to reveal mechanism in a stepwise fashion of ever increasing detail as desired. This new hierarchical algorithm is an improvement over earlier approaches to HE where the entire mechanism was determined in one stroke. The improvement comes from the use of less complex modulation schemes, which leads to fewer evaluations of Schrodinger's equation. A number of simulations are presented on simple systems to illustrate the new field based encoding technique for mechanism assessment.
Hamiltonian encoding is a methodology for revealing the mechanism behind the dynamics governing controlled quantum systems. In this paper, following Mitra and Rabitz \cite{abhra_1}, we define mechanism via pathways of eigenstates that describe the evolution of the system, where each pathway is associated with a complex-valued amplitude corresponding to a term in the Dyson series. The evolution of the system is determined by the constructive and destructive interference of these pathway amplitudes. Pathways with similar attributes can be grouped together into pathway classes. The amplitudes of pathway classes are computed by modulating the Hamiltonian matrix elements and decoding the subsequent evolution of the system rather than by direct computation of the individual terms in the Dyson series. The original implementation of Hamiltonian encoding was computationally intensive and became prohibitively expensive in large quantum systems. This paper presents two new encoding algorithms that calculate the amplitudes of pathway classes by using techniques from graph theory and algebraic topology to exploit patterns in the set of allowed transitions, greatly reducing the number of matrix elements that need to be modulated. These new algorithms provide an exponential decrease in both computation time and memory utilization with respect to the Hilbert space dimension of the system. To demonstrate the use of these techniques, they are applied to two illustrative state-to-state transition problems.