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Physical Review A

Rovibrational controlled-NOT gates using optimized stimulated Raman adiabatic passage techniques and optimal control theory

Dominique Sugny, L. Bomble, T. Ribeyre, Olivier Dulieu, Michèle Desouter-Lecomte

Published Oct 23, 2009• 31 citations
Publisher

Abstract

Implementation of quantum controlled-NOT (CNOT) gates in realistic molecular systems is studied using stimulated Raman adiabatic passage (STIRAP) techniques optimized in the time domain by genetic algorithms or coupled with optimal control theory. In the first case, with an adiabatic solution (a series of STIRAP processes) as starting point, we optimize in the time domain different parameters of the pulses to obtain a high fidelity in two realistic cases under consideration. A two-qubit CNOT gate constructed from different assignments in rovibrational states is considered in diatomic (NaCs) or polyatomic $({\text{SCCl}}_{2})$ molecules. The difficulty of encoding logical states in pure rotational states with STIRAP processes is illustrated. In such circumstances, the gate can be implemented by optimal control theory and the STIRAP sequence can then be used as an interesting trial field. We discuss the relative merits of the two methods for rovibrational computing (structure of the control field, duration of the control, and efficiency of the optimization).

DOI
10.1103/physreva.80.042325

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arXiv:0906.1989•Physical Review A•Jul 27, 2009•123 citations
Implementation of quantum controlled-NOT (CNOT) gates in realistic molecular systems is studied using stimulated Raman adiabatic passage (STIRAP) techniques optimized in the time domain by genetic algorithms or coupled with optimal control theory. In the first case, with an adiabatic solution (a series of STIRAP processes) as starting point, we optimize in the time domain different parameters of the pulses to obtain a high fidelity in two realistic cases under consideration. A two-qubit CNOT gate constructed from different assignments in rovibrational states is considered in diatomic (NaCs) or polyatomic (SCCl2)({\text{SCCl}}_{2})(SCCl2​) molecules. The difficulty of encoding logical states in pure rotational states with STIRAP processes is illustrated. In such circumstances, the gate can be implemented by optimal control theory and the STIRAP sequence can then be used as an interesting trial field. We discuss the relative merits of the two methods for rovibrational computing (structure of the control field, duration of the control, and efficiency of the optimization).
We have numerically examined optimization of the experimentally achievable shapes of mid-infrared femtosecond laser pulses to construct elementary quantum gates using molecular rovibrational states of a single molecule. Instead of optimizing the electric field by optimal control theory, the method generally used in theoretical studies of coherent control, the transmittance and the phase shift of conventional pulse shapers were optimized in the frequency domain by a genetic algorithm. The target molecular system we examined was the rotation-vibration states of CO in the $X({^{1}\ensuremath{\Sigma}}^{+})$ ground electronic state. Although the existence of the rotational degrees of freedom makes the quantum gate operation complicated, high fidelity of over 0.95 was achieved for one-rovibrational-qubit systems, which indicates that a molecular quantum computer may be feasible for at least one-qubit calculations on a diatomic molecule. On the other hand, two-qubit calculations are more difficult to achieve in a single CO molecule using rotational and vibrational degrees of freedom as different qubits. The importance of the control of the rotational in addition to the vibrational wave packet in order to realize a molecular quantum computer is discussed.
We explore theoretically the rovibrational dynamics of stimulated Raman adiabatic passage (STIRAP) in molecular electronic states including both the rotational and the vibrational degrees of freedom, with the LiH molecule as an example. By using a pure rovibrational state as initial state, we find that, under the condition of two-photon resonance, an efficient rovibrational population transfer can be achieved via STIRAP in molecular electronic states and the desired target state can be selected by adjusting laser-pulse parameters. Besides the interested rovibrational states, however, some unwanted rovibrational states may affect population transfer process, especially while the two-photon detuning is taken into account. By inspecting the evolution process of wave packet, we can easily search these unwanted rovibrational states and study their influences. Moreover, the effect of rotational temperature on the population transfer process is discussed using thermal mixed state as initial state.
The intent of this study is to determine the feasibility of diatomics as molecular quantum computing candidates and shed insight into the use of such experimental laser pulse shaping methods to represent quantum logic gates. Four appropriate rovibrational states of model diatomic molecules are encoded as the qubit states. A set of 2-qubit quantum logic gates (ACNOT, CNOT, NOT, Hadamard) are represented by amplitude and phase shaped laser pulses. The combinations of amplitudes and phases that produce the optimal laser pulse representation, for each quantum logic gate, are determined by a Genetic Algorithm optimization routine. The theoretical laser pulse shaping is analogous to current experimental frequency-domain pulse shaping apparatus with amplitude and phase control at individual frequencies. A model set of diatomics is sampled in order to determine a relationship between optimal laser pulse shaping and the choice of diatomic molecule. We show that the choice of diatomic molecule greatly influences the ability to produce optimal laser pulse shapes to represent quantum logic gates. Tuneable parameters specific to laser pulse shaping instruments are varied to determine their effect on optimal pulse production. They include varying the number of amplitude and phase components, adjusting the number of frequency components, and altering the frequency resolution which is synonymous with altering the laser pulse duration. A time domain analytic form of the original frequency domain laser pulse function is derived, providing a useful means to infer the laser pulse dependencies on these parameters. Initially, we show that the appropriate choice of rovibrational state qubits of carbon monoxide (12C16O) and the use of simple shaped binary pulses, 2 amplitude and 2 phase components, can provide significant control for specific quantum gates. Further amplitude variation at each frequency component is shown to be a crucial requirement for optimal laser pulse shaping, whereas phase variation provides minimal contribution. We show that the generation of optimal laser pulse shapes is highly dependent upon the frequency resolution and increasing the number of frequency components provides incremental improvements to optimal laser pulses.
Based on the quantum Zeno dynamics, we propose two approaches for directly implementing a CNOT gate in a cavity QED system instead of constructing it from elementary gates. The first approach works in the decoherence-free subspaces (DFS) due to the quantum Zeno effect, which is robust against cavity decay. Based on the first model, we then propose the second approach which takes advantage of stimulated Raman adiabatic passage (STIRAP) with only six pulses; thus it is insensitive to the atomic spontaneous emission. The two schemes are suitable for different decoherence parameters. The strictly numerical simulation shows that the average gate fidelities for the two methods are relatively high.
Quantum control of lossy systems is known to be achieved by adiabatic passage via an approximate dark state relatively immune to loss, such as the emblematic example of stimulated Raman adiabatic passage (STIRAP) featuring a lossy excited state. By systematic optimal control study, via the Pontryagin maximum principle, we design alternative more efficient routes that, for a given admissible loss, feature an optimal transfer with respect to the cost defined as (i) the pulse energy (energy minimization) or (ii) the pulse duration (time minimization). The optimal controls feature remarkably simple sequences in the respective cases: (i) operating far from a dark state, of π-pulse type in the limit of low admissible loss, or (ii) close to the dark state with a counterintuitive pulse configuration sandwiched by sharp intuitive sequences, referred to as the intuitive/counterintuitive/intuitive (ICI) sequence. In the case of time optimization, the resulting stimulated Raman exact passage (STIREP) outperforms STIRAP in term of speed, accuracy, and robustness for low admissible loss.
Stimulated Raman adiabatic passage (STIRAP) driven with pulses of optimum shape and delay has the potential of reaching fidelities high enough to make it suitable for quantum-information processing. The optimum pulse shapes are obtained upon reduction of STIRAP to effective two-state systems. We use the Dykhne-Davis-Pechukas (DDP) method to minimize nonadiabatic transitions and to maximize the fidelity of STIRAP. This results in a particular relation between the pulse shapes of the two fields driving the Raman process. The DDP-optimized version of STIRAP maintains its robustness against variations in the pulse intensities and durations, the single-photon detuning, and possible losses from the intermediate state.