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The Journal of Chemical Physics

On the consistency, extremal, and global properties of counterdiabatic fields

Mustafa Demirplak, Stuart A. Rice

Published Oct 20, 2008• 260 citations
Publisher

Abstract

The control of population transfer can be affected by the adiabatic evolution of a system under the influence of an applied field. If the field is too rapidly varying or too weak, the conditions for adiabatic transfer are not satisfactorily met. We report the results of an analysis of properties of counterdiabatic fields (CDFs) that restore the adiabatic dynamics of a system by suppressing diabatic effects as they are generated. We observe that a CDF is not unique and find the one that has minimum intensity, and we provide natural upper and lower bounds to the integrated intensity of a CDF in terms of integrals of the eigenvalues of the system Hamiltonian. For Hamiltonians that are separable with respect to their parameters, we prove that the time integral of an associated CDF is path independent. Finally we explain why and when, in the neighborhood of an avoided crossing, a CDF can be approximated by Lorentzian pulses.

DOI
10.1063/1.2992152

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The control of population transfer can be affected by the adiabatic evolution of a system under the influence of an applied field. If the field is too rapidly varying or too weak, the conditions for adiabatic transfer are not satisfactorily met. We report the results of an analysis of properties of counterdiabatic fields (CDFs) that restore the adiabatic dynamics of a system by suppressing diabatic effects as they are generated. We observe that a CDF is not unique and find the one that has minimum intensity, and we provide natural upper and lower bounds to the integrated intensity of a CDF in terms of integrals of the eigenvalues of the system Hamiltonian. For Hamiltonians that are separable with respect to their parameters, we prove that the time integral of an associated CDF is path independent. Finally we explain why and when, in the neighborhood of an avoided crossing, a CDF can be approximated by Lorentzian pulses.
We propose a method to produce fast transitionless dynamics for finite-dimensional quantum systems without requiring additional Hamiltonian components not included in the initial control setup, remaining close to the true adiabatic path at all times. The strategy is based on the introduction of an effective counterdiabatic scheme: a correcting Hamiltonian is constructed which approximatively cancels nonadiabatic effects, inducing an evolution tracking the adiabatic states closely. This can be absorbed into the initial Hamiltonian by adding a fast oscillation in the control parameters. We show that a consistent speedup can be achieved without requiring strong control Hamiltonians, using it both as a stand-alone shortcut to adiabaticity and as a weak correcting field. A number of examples are treated, dealing with quantum state transfer in avoided-crossing problems and entanglement creation.
Previous studies have demonstrated that when experimental conditions generate non-adiabatic dynamics that prevents highly efficient population transfer between states of an isolated system by stimulated Raman adiabatic passage (STIRAP), the addition of an auxiliary counter-diabatic field (CDF) can restore most or all of that efficiency. This paper examines whether that strategy is also successful in a non-isolated system in which the energies of the states fluctuate, e.g., when a solute is subject to collisions with solvent. We study population transfer in two model systems: (i) the three-state system used by Demirplak and Rice [J. Chem. Phys. 116, 8028 (2002)] and (ii) a four-state system, derived from the simulation studies of Demirplak and Rice [J. Chem. Phys. 125, 194517 (2006)], that mimics HCl in liquid Ar. Simulation studies of the vibrational manifold of HCl in dense fluid Ar show that the collision induced vibrational energy level fluctuations have asymmetric distributions. Representations of these asymmetric energy level fluctuation distributions are used in both models (i) and (ii). We identify three sources of degradation of the efficiency of STIRAP generated selective population transfer in model (ii): too small pulse areas of the laser fields, unwanted interference arising from use of strong fields, and the vibrational detuning. For both models (i) and (ii), our examination of the efficiency of STIRAP + CDF population transfer under the influence of the asymmetric distribution of the vibrational energy fluctuations shows that there is a range of field strengths and pulse durations under which STIRAP + CDF control of population transfer has greater efficiency than does STIRAP generated population transfer.
In the past two decades many schemes to actively control the dynamical evolution of a quantum system have been proposed and established. We focus attention on the use of assisted adiabatic processes to generate selected target states with high efficiency. Specific control protocols that fall in this category are sometimes called shortcuts to adiabaticity. We review two assisted adiabatic population transfer schemes, the counter-diabatic and fast-forward protocols, with the intent of calling attention to their conceptual basis and applications to real systems, specifically vibrational energy transfer in polyatomic molecules and manipulation of Bose-Einstein (BEC) condensates. The particular applications of the counter-diabatic and fast-forward protocols to improving the efficiency of population transfer between vibrational states of a polyatomic molecule that we have studied are (i) selective vibrational energy transfer in the nonrotating thiophosgene (SCCl2) molecule and (ii) enhancing the yield of HNC in the driven rotation free isomerization reaction HCN→CNH. A major component of our considerations concerns reduction of the degradation of population transfer efficiency within a subset of states that is generated by coupling of the subset of states to a manifold of background states. We have examined the influence of a manifold of background vibrational states on population transfer within a subset of embedded vibrational states, and on how that influence can be suppressed. We emphasize that any control protocol must be designed to minimize interference between the background states and excitations within the selected subset of states that are used to define initial and target states. We have also examined the application of the fast-forward protocol to the transport of population between sites of a BEC in an optical lattice. Through the applications we illustrate how the theoretical framework of an assisted adiabatic process depends on the character of the system studied, on the available control parameters, on the constraints imposed by the experimental setting, on the efficiency of population transfer (fidelity) to be achieved, and on the stability of the control process with respect to the variation of the external control fields.
The task of controlling a quantum system under time and bandwidth limitations is made difficult by unwanted excitations of spectrally neighboring energy levels. In this article we review the Derivative Removal by Adiabatic Gate (DRAG) framework. DRAG is a multi-transition variant of counterdiabatic driving, where multiple low-lying gapped states in an adiabatic evolution can be avoided simultaneously, greatly reducing operation times compared to the adiabatic limit. In its essence, the method corresponds to a convergent version of the superadiabatic expansion where multiple counterdiabaticity conditions can be met simultaneously. When transitions are strongly crowded, the system of equations can instead be favorably solved by an average Hamiltonian (Magnus) expansion, suggesting the use of additional sideband control. We give some examples of common systems where DRAG and variants thereof can be applied to improve performance.
We theoretically study the interaction of two time delayed, phase-locked, and nonresonant pulses with a two-level system in the strong field regime. The population transfer is shown to be extremely sensitive to the phase shift $\ensuremath{\phi}$ between the pulses, with efficient population transfer taking place only for $\ensuremath{\phi}$ close to $\ensuremath{\pi}$. This effect is explained in terms of nonadiabatic jump and rapid adiabatic passage phenomena.
We report studies of state-to-state vibrational energy transfer in an isolated polyatomic molecule driven by combined stimulated Raman adiabatic passage (STIRAP) and counter-diabatic fields (CDFs). The goal of these studies is development of a method for improving the efficiency of level-to-level population transfer under conditions that degrade the efficiency of conventional STIRAP-generated population transfer. The vehicles for our studies are selective population of one of a pair of near-degenerate states in nonrotating SCCl 2 and enhancing the yield of nonrotating HNC in the HCN → HNC isomerization reaction. The efficiency of the population transfer within a subset of states embedded in a manifold of states is examined for the cases in which the transition dipole moments between the initial and target states are much smaller than and comparable to the transition dipole moments between background states and for the case in which the subset states have large transition dipole moments with the background states. We show that, in a subset of states that is coupled to background states, a combination of STIRAP fields and CDFs that do not individually generate processes that are competitive with the desired population transfer can generate population transfer efficiency greater than can ordinary STIRAP with field strength and/or pulse duration similarly restricted and that the exact CDF for an isolated three-level system is a useful approximation to the exact CDF for three- and five-state systems embedded in background states. We report a study of the stability of the STIRAP and approximate CDF control protocol to variation of the CDF intensity, the relative phase between the STIRAP and CDFs, and the pulse duration.