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Using quantum optimal control to drive intramolecular vibrational redistribution and to perform quantum computing

Ludovic Santos, Nathalie Vaeck

Published Nov 28, 2017• 0 citations
OpenAlex

Abstract

Quantum optimal control theory is applied to find optimal pulses for controlling the motion of an ion and a molecule for two different applications. Those optimal pulses enable the control of the dynamics of the system by driving the atom or the molecule from an initial state to desired states.The evolution equations obtained by means of the quantum optimal control theory are resolved iteratively using a monotonic convergent algorithm. A number of simulation parameters are varied in order to get the optimal pulses including the duration of the pulses, the time step of the time grid, a penalty factor that limits the maximal intensity of the fields, and a guess pulse which is used to start the optimal control.The optimal pulses obtained for each application are analyzed by Fourier transform, and also by looking at the time evolution of the populations that they generate in the system.The first application is the preparation of specific vibrational states of acetylene that are usually not reachable from the ground state, and that would remain unpopulated by usual spectroscopy. Relevant state energies and transition dipole moments are extracted from the experimental literature and especially from the global acetylene Hamiltonian conferring an uncommon precision to the control simulation. The control starts from the ground state. The target states belongs to the polyad Ns=1, Nr=5 of acetylene which includes two vibrational dark states and one vibrational bright state. First, the simulation is performed with the Schrödinger equation and in a second step, with the Liouville--von Neumann equation, as mixed states are prepared. Indeed, the control starts from a Boltzmann distribution of population in the rotational levels of the vibrational ground state chosen in order to simulate an experimental condition. But the distribution is truncated to limit the computational effort. One of the dark states appears to be a potential target for a realistic experimental investigation because the average population of the Rabi oscillation remains high and decoherence is expected to be weak. The optimal pulses obtained have a high fidelity, have a spectrum with well-resolved peak frequencies, and their experimental feasibility seems achievable within the current abilities of experimental laboratories.The second application is to propose an experimental realization of a microscopic physical device able to simulate quantum dynamics. The idea is to use the motional states of a Cd^+ ion trapped in an anharmonic potential to realize a quantum dynamics simulator of a single-particle Schrödinger equation. In this way, the motional states store the information and the optimal pulse manipulates this information to realize operations. In the present case, the simulated dynamics was the propagation of a wave packet in a harmonic potential. Starting from an initial quantum state, the pulse acts on the system to modify the motional states of the ion in such a way that the final superposition of motional states corresponds to the results of the dynamics. This simulation is performed with the Liouville--von Neumann equation and also with the Lindblad equation as dissipation is included to test the robustness of the pulse against perturbations of the potential. The optimal pulses that are obtained have a high fidelity which shows that the ion trap system has correctly realized the quantum dynamics simulation. The optimal pulses are valid for any initial condition if the potential of the simulation or the mass of the propagated wave packet is unchanged.

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Quantum optimal control theory is applied to find optimal pulses for controlling the motion of an ion and a molecule for two different applications. Those optimal pulses enable the control of the dynamics of the system by driving the atom or the molecule from an initial state to desired states.The evolution equations obtained by means of the quantum optimal control theory are resolved iteratively using a monotonic convergent algorithm. A number of simulation parameters are varied in order to get the optimal pulses including the duration of the pulses, the time step of the time grid, a penalty factor that limits the maximal intensity of the fields, and a guess pulse which is used to start the optimal control.The optimal pulses obtained for each application are analyzed by Fourier transform, and also by looking at the time evolution of the populations that they generate in the system.The first application is the preparation of specific vibrational states of acetylene that are usually not reachable from the ground state, and that would remain unpopulated by usual spectroscopy. Relevant state energies and transition dipole moments are extracted from the experimental literature and especially from the global acetylene Hamiltonian conferring an uncommon precision to the control simulation. The control starts from the ground state. The target states belongs to the polyad Ns=1, Nr=5 of acetylene which includes two vibrational dark states and one vibrational bright state. First, the simulation is performed with the Schrödinger equation and in a second step, with the Liouville--von Neumann equation, as mixed states are prepared. Indeed, the control starts from a Boltzmann distribution of population in the rotational levels of the vibrational ground state chosen in order to simulate an experimental condition. But the distribution is truncated to limit the computational effort. One of the dark states appears to be a potential target for a realistic experimental investigation because the average population of the Rabi oscillation remains high and decoherence is expected to be weak. The optimal pulses obtained have a high fidelity, have a spectrum with well-resolved peak frequencies, and their experimental feasibility seems achievable within the current abilities of experimental laboratories.The second application is to propose an experimental realization of a microscopic physical device able to simulate quantum dynamics. The idea is to use the motional states of a Cd^+ ion trapped in an anharmonic potential to realize a quantum dynamics simulator of a single-particle Schrödinger equation. In this way, the motional states store the information and the optimal pulse manipulates this information to realize operations. In the present case, the simulated dynamics was the propagation of a wave packet in a harmonic potential. Starting from an initial quantum state, the pulse acts on the system to modify the motional states of the ion in such a way that the final superposition of motional states corresponds to the results of the dynamics. This simulation is performed with the Liouville--von Neumann equation and also with the Lindblad equation as dissipation is included to test the robustness of the pulse against perturbations of the potential. The optimal pulses that are obtained have a high fidelity which shows that the ion trap system has correctly realized the quantum dynamics simulation. The optimal pulses are valid for any initial condition if the potential of the simulation or the mass of the propagated wave packet is unchanged.
For practical realization of quantum information processing we need a quantum system that provides reliable preparation of the initial state, high-fidelity quantum gate operations, error tolerance, readout of the result of quantum computation and scalability of the system to increase the number of qubits. In this dissertation we show how these requirements can be addressed for molecular quantum computer. For computational study of quantum information processing with molecules we employ thiophosgene (SCCl2) molecule that has been used as a test system for quantum control experiments [Mol. Phys. 105, 1999 (2007)]. We investigate the gateway scheme of control in which transitions between the vibrational states that encode qubits are only allowed through the intermediate “gateway” state in the B electronic state. This scheme of control provides reliable preparation of the initial qubit state and allows using UV/vis laser pulses. We demonstrate that high-fidelity quantum gates are possible to achieve in molecular quantum computer. The optimal control theory is employed to obtain a shape of laser pulse that performs CNOT gate with ~0.9999 fidelity. Analysis of frequency profile of the optimal pulse shows that preparation of the high-fidelity computational pulse requires only 64 frequency channels. Error tolerance of the computational pulse is studied by modifying amplitudes and phases of frequency components. It is shown that gate fidelity remains high after small modifications are introduced to the optimal pulse. The scheme of readout of quantum information using quantum beat spectroscopy is proposed. The quantum beat signal is obtained from excitation of the final superposition of the qubit states to a readout state in the B electronic state with a time-delayed pulse. We find that fitting the quantum beat signal with a standard fitting expression produces a phase error and propose a new accurate expression that includes phase correction term. The system of two atomic ions trapped in a double-well potential is also studied as a first step towards scalable quantum computation with trapped molecular ions. The rigorous computational treatment of the system provides explanation of the vibrational energy transfer between the ions in terms of wave packet dynamics in the accurate asymmetric potential.
A time-dependent formulation of quantum control is employed to investigate optimally controlled vibrational population transfer in a diatomic quantum system. The problem of finding the optimal laser field needed to achieve a specific quantum transition from an initial state to the desired target goal is formulated using an iterative method and the conjugate gradient method (CGM). The time-dependent Schrödinger equation is solved with interaction of laser radiation with matter included within a dipole approximation in the Hamiltonian. Appropriate boundary conditions are chosen for the evolution problem. The control objective is chosen as the value of transition probability from an initial state to a target state. A comparison is made between the results obtained using the iterative method and the CGM for optimization. Finally, quantum bits are encoded using the vibrational states of the diatomic in the regime of low-vibrational excitation.
The dynamics of a quantum system driven by an external field is well described by a unitary transformation generated by a time-dependent Hamiltonian. The inverse problem of finding the field that generates a specific unitary transformation is the subject of study. The unitary transformation which can represent an algorithm in a quantum computation is imposed on a subset of quantum states embedded in a larger Hilbert space. Optimal control theory is used to solve the inversion problem irrespective of the initial input state. A unified formalism based on the Krotov method is developed leading to a different scheme. The schemes are compared for the inversion of a two-qubit Fourier transform using as registers the vibrational levels of the $X{}^{1}{\ensuremath{\Sigma}}_{g}^{+}$ electronic state of Na2.{\mathrm{Na}}_{2}.Na2​. Raman-like transitions through the $A{}^{1}{\ensuremath{\Sigma}}_{u}^{+}$ electronic state induce the transitions. Light fields are found that are able to implement the Fourier transform within a picosecond time scale. Such fields can be obtained by pulse-shaping techniques of a femtosecond pulse. Of the schemes studied, the square modulus scheme converges fastest. A study of the implementation of the Q qubit Fourier transform in the Na2{\mathrm{Na}}_{2}Na2​ molecule was carried out for up to five qubits. The classical computation effort required to obtain the algorithm with a given fidelity is estimated to scale exponentially with the number of levels. The observed moderate scaling of the pulse intensity with the number of qubits in the transformation is rationalized.
We investigate the problem of control of quantum systems. Various notions of controllability of quantum systems are discussed and Lie algebraic techniques are employed to derive necessary and sufficient conditions for the resulting degrees of controllability. The results are employed to study the degree of controllability for various model systems. The problem of optimal control is formulated as a problem of maximisation of the expectation value of an observable of the system subject to dynamical constraints and costs. A class of iterative algorithms is discussed, and shown to converge to a solution of the Euler-Lagrange equations, which is a necessary condition for optimality of a solution. A numerical realisation of the algorithm is presented and potential implementation of the resulting control fields in the laboratory is discussed. The algorithm is applied to find optimal control fields for a variety of applications including selective and simultaneous excitation of individual quantum dots in a globally addressed ensemble, creation of superposition states, and selective excitation of certain vibrational modes of a simple molecule such as Hydrogen Fluoride. In each case we systematically explore the parameter space of the algorithm to select solutions with desirable physical features from the multitude of possible choices. As there are many possible optimal control fields which give similar yields the question of whether some are more robust than others is investigated. A number of optimal fields are analysed quantitatively in terms of robustness with regard to temporal and spectral noise affecting the fields, uncertainty in the model parameters and the effect of experimental limitations such as restrictions on the bandwidth of the fields. It is shown that whilst the solutions tend to be sensitive to uncertainty in the energy levels chosen for the model, they appear to be surprisingly tolerant to even severe bandwidth limitations.
A method for encoding a multiqubit system into the quantized motional states of ion string in an anharmonic linear trap is proposed. Control over this system is achieved by applying oscillatory electric fields (rf) shaped optimally for desired state-to-state transitions. Anharmonicity of the vibrational spectrum of the system plays a key role in this approach to the control and quantum computation, since it allows resolving different state-to-state transitions and addressing them selectively. The anharmonic trap architecture proposed earlier [Phys. Rev. A 83, 022305 (2011)] is explored here and the optimal control theory is used to derive pulses for a set of universal quantum gates. An accurate choice of pulse parameters allows deriving gates that are both accurate and simple. A practical realization of this approach seems to be within the reach of today's technology.
We present a local optimal control strategy to produce desired unitary transformations. Unitary transformations are central to all quantum computational algorithms. Many realizations of quantum computation use a submanifold of states, comprising the quantum register, coupled by an external driving field to a collection of additional mediating excited states. Previous attempts to apply control theory to induce unitary transformations on the quantum register, while successful, produced pulses that drive the population out of the computational register at intermediate times. Leakage of population from the register is undesirable since often the states outside the register are prone to decay and decoherence, and populating them causes a decrease in the final fidelity. In this work we devise a local optimal control method for achieving target unitary transformations on a quantum register, while avoiding intermediate leakage out of the computational submanifold. The technique exploits a phase locking of the field to the system such as to eliminate the undesirable excitation. This method is then applied to produce an SU(6) Fourier transform on the vibrational levels of the ground electronic state of the Na2_22​ molecule. The emerging mechanism uses two photon resonances to create a transformation on the quantum register while blocking one photon resonances to excited states.