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The Journal of Chemical Physics

Time-optimal excitation of maximum quantum coherence: Physical limits and pulse sequences

S. Kocher, Thomas Heydenreich, Y. Zhang, G. N. Manjunatha Reddy, Stéfano Caldarelli, Haidong Yuan, Steffen J. Glaser

Published Apr 22, 2016• 20 citations
Publisher

Abstract

Here we study the optimum efficiency of the excitation of maximum quantum (MaxQ) coherence using analytical and numerical methods based on optimal control theory. The theoretical limit of the achievable MaxQ amplitude and the minimum time to achieve this limit are explored for a set of model systems consisting of up to five coupled spins. In addition to arbitrary pulse shapes, two simple pulse sequence families of practical interest are considered in the optimizations. Compared to conventional approaches, substantial gains were found both in terms of the achieved MaxQ amplitude and in pulse sequence durations. For a model system, theoretically predicted gains of a factor of three compared to the conventional pulse sequence were experimentally demonstrated. Motivated by the numerical results, also two novel analytical transfer schemes were found: Compared to conventional approaches based on non-selective pulses and delays, double-quantum coherence in two-spin systems can be created twice as fast using isotropic mixing and hard spin-selective pulses. Also it is proved that in a chain of three weakly coupled spins with the same coupling constants, triple-quantum coherence can be created in a time-optimal fashion using so-called geodesic pulses.

DOI
10.1063/1.4945781

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Here we study the optimum efficiency of the excitation of maximum quantum (MaxQ) coherence using analytical and numerical methods based on optimal control theory. The theoretical limit of the achievable MaxQ amplitude and the minimum time to achieve this limit are explored for a set of model systems consisting of up to five coupled spins. In addition to arbitrary pulse shapes, two simple pulse sequence families of practical interest are considered in the optimizations. Compared to conventional approaches, substantial gains were found both in terms of the achieved MaxQ amplitude and in pulse sequence durations. For a model system, theoretically predicted gains of a factor of three compared to the conventional pulse sequence were experimentally demonstrated. Motivated by the numerical results, also two novel analytical transfer schemes were found: Compared to conventional approaches based on non-selective pulses and delays, double-quantum coherence in two-spin systems can be created twice as fast using isotropic mixing and hard spin-selective pulses. Also it is proved that in a chain of three weakly coupled spins with the same coupling constants, triple-quantum coherence can be created in a time-optimal fashion using so-called geodesic pulses.
We study multiple-spin coherence transfers in linear Ising spin chains with nearest-neighbor couplings. These constitute a model for efficient information transfers in future quantum computing devices and for many multidimensional experiments for the assignment of complex spectra in nuclear magnetic resonance spectroscopy. We complement prior analytic techniques for multiple-spin coherence transfers with a systematic numerical study where we obtain strong evidence that a certain analytically motivated family of restricted controls is sufficient for time optimality. In the case of a linear three-spin system, additional evidence suggests that prior analytic pulse sequences using this family of restricted controls are time optimal even for arbitrary local controls. In addition, we compare the pulse sequences for linear Ising spin chains to pulse sequences for more realistic spin systems with additional long-range couplings between nonadjacent spins. We experimentally implement the derived pulse sequences in three- and four-spin systems and demonstrate that they are applicable in realistic settings under relaxation and experimental imperfections---in particular---by deriving broadband pulse sequences which are robust with respect to frequency offsets.
In this paper, we study the design of pulse sequences for nuclear magnetic resonance spectroscopy as a problem of time optimal control of the unitary propagator. Radio-frequency pulses are used in coherent spectroscopy to implement a unitary transfer between states. Pulse sequences that accomplish a desired transfer should be as short as possible in order to minimize the effects of relaxation and to optimize the sensitivity of the experiments. Here, we give an analytical characterization of such time optimal pulse sequences applicable to coherence transfer experiments in multiple-spin systems. We have adopted a general mathematical formulation, and present many of our results in this setting, mindful of the fact that new structures in optimal pulse design are constantly arising. From a general control theory perspective, the problems we want to study have the following character. Suppose we are given a controllable right invariant system on a compact Lie group. What is the minimum time required to steer the system from some initial point to a specified final point? In nuclear magnetic resonance (NMR) spectroscopy and quantum computing, this translates to, what is the minimum time required to produce a unitary propagator? We also give an analytical characterization of maximum achievable transfer in a given time for the two-spin system.
In this thesis, we study methods for optimal manipulation of coupled spin dynamics in the presence of relaxation. We use these methods to compute analytical upper bounds for the efficiency of coherence and polarization transfer between coupled nuclear spins in multidimensional nuclear magnetic resonance (NMR) experiments, under the presence of relaxation. We derive relaxation optimized pulse sequences which achieve or approach these bounds and maximize the sensitivity of the experiments. The two systems examined in detail in this thesis, arising in the context of protein NMR spectroscopy, are a coupled heteronuclear spin pair and an Ising spin chain. New schemes for coherence and polarization transfer are found, which yield substantial gains in transfer efficiency, compared to the traditionally used pulse sequences. From the standpoint of mathematical control theory, the problems arising in connection with optimal manipulation of dissipative quantum dynamics, motivate the study of a class of dissipative bilinear control systems and the computation of their reachable sets. For these systems we show that the optimal solution, corresponding to the maximization of transfer efficiency, and the reachable set can be found by solving a semidefinite program.
Relaxation effects impose fundamental limitations on our ability to coherently control quantum mechanical phenomena. In this paper, we solve a new class of optimal control problems, which helps establish physical limits on how closely a quantum mechanical system can be steered to a desired target state in the presence of relaxation. In particular, we explicitly compute the maximum coherence or polarization that can be transferred between coupled nuclear spins in the presence of very general decoherence mechanisms that include cross-correlated relaxation. We give analytical expressions for the optimal control laws (pulse sequences). Exploitation of cross-correlation effects has recently led to the development of powerful methods in NMR spectroscopy to study very large biomolecules in solution. We demonstrate that the optimal pulse sequences provide significant gains over these state of the art methods, opening new avenues for spectroscopy of much larger proteins. It is shown that in spite of very large relaxation rates, optimal control can transfer coherence without any loss when cross-correlated relaxation rates are tuned to auto-correlated relaxation rates.
In this article, we study optimal control of dynamics of a linear chain of three spin 1∕21∕21∕2, weakly coupled with unequal Ising couplings. We address the problem of time-optimal synthesis of multiple spin quantum coherences. We derive time-optimal pulse sequences for creating desired spin order by computing geodesics on a sphere under a special metric. The solution to the geodesic equation is related to the nonlinear oscillator equation and the minimum time to create multiple spin order can be expressed in terms of an elliptic integral. These techniques are used for efficient creation of multiple spin coherences in Ising spin chains with unequal couplings.
Radio-frequency pulses are used in nuclear-magnetic-resonance spectroscopy to produce unitary transfer of states. Pulse sequences that accomplish a desired transfer should be as short as possible in order to minimize the effects of relaxation, and to optimize the sensitivity of the experiments. Many coherence-transfer experiments in NMR, involving a network of coupled spins, use temporary spin decoupling to produce desired effective Hamiltonians. In this paper, we demonstrate that significant time can be saved in producing an effective Hamiltonian if spin decoupling is avoided. We provide time-optimal pulse sequences for producing an important class of effective Hamiltonians in three-spin networks. These effective Hamiltonians are useful for coherence-transfer experiments in three-spin systems and implementation of indirect swap and ${\ensuremath{\Lambda}}_{2}(U)$ gates in the context of NMR quantum computing. It is shown that computing these time-optimal pulses can be reduced to geometric problems that involve computing sub-Riemannian geodesics. Using these geometric ideas, explicit expressions for the minimum time required for producing these effective Hamiltonians, transfer of coherence, and implementation of indirect swap gates, in a three-spin network are derived (Theorems 1 and 2). It is demonstrated that geometric control techniques provide a systematic way of finding time-optimal pulse sequences for transferring coherence and synthesizing unitary transformations in quantum networks, with considerable time savings (e.g., 42.3% for constructing indirect swap gates).