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Molecular Physics

Computational study of cold ions trapped in a double-well potential

Dmytro Shyshlov, Dmitri Babikov

Published Dec 25, 2018• 0 citations
Publisher

Abstract

We report a rigorous computational treatment of quantum dynamics of cold ions in a double-well trap using the time-dependent Schrödinger equation. Our method employs a numerically accurate approach that avoids approximations, such as assumption of weak coupling between the wells; normal mode nature of vibrations; or harmonic approximation for energy spectrum of the double-well system. Our goal is to reproduce, from first principles, the process of energy swaps between the wells observed in the experiments at NIST [Nature 471, 196 (2011)] and Innsbruck [Nature 471, 200 (2011)]. The model parameters and the initial conditions are carefully chosen to mimic experimental conditions. We obtain accurate energies and wave functions of the system numerically, and study the evolution of motional wave packets to provide new insight. This model reproduces experimental results obtained by NIST and Innsbruck in detail. We explain the energy transfer in terms of wave packet dynamics in the asymmetric potential energy well. We also show that, for a localised initial wave packet, this phenomenon can be interpreted using the terms of classical dynamics, such as trajectory of motion governed by the well-known simple principle: the angle of reflection equals the angle of incidence.

DOI
10.1080/00268976.2018.1559956

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We report a rigorous computational treatment of quantum dynamics of cold ions in a double-well trap using the time-dependent Schrödinger equation. Our method employs a numerically accurate approach that avoids approximations, such as assumption of weak coupling between the wells; normal mode nature of vibrations; or harmonic approximation for energy spectrum of the double-well system. Our goal is to reproduce, from first principles, the process of energy swaps between the wells observed in the experiments at NIST [Nature 471, 196 (2011)] and Innsbruck [Nature 471, 200 (2011)]. The model parameters and the initial conditions are carefully chosen to mimic experimental conditions. We obtain accurate energies and wave functions of the system numerically, and study the evolution of motional wave packets to provide new insight. This model reproduces experimental results obtained by NIST and Innsbruck in detail. We explain the energy transfer in terms of wave packet dynamics in the asymmetric potential energy well. We also show that, for a localised initial wave packet, this phenomenon can be interpreted using the terms of classical dynamics, such as trajectory of motion governed by the well-known simple principle: the angle of reflection equals the angle of incidence.
A string of cold ions confined in a linear trap represents a man-made quantum object with a broad range of applications in atomic and molecular spectroscopy, such as high-precision measurement of atomic properties. An efficient isolation from the environment guarantees excellent coherent properties of such systems and makes them suitable for practical realization of the quantum information processing. The pioneering theoretical [Cirac and Zoller] and experimental [Wineland and Monroe] work in 1990s resulted in the explosive expansion of this field during the last decade. In this dissertation an alternative new method for controlling the quantized motional/vibrational states of ions in a trap is explored theoretically. It is proposed to create small anharmonicity in the trapping potential which would modify the spectrum of states and allow addressing the state-to-state transitions selectively. In this approach all ions remain in the ground electronic state and their motion is controlled adiabatically and coherently by applying the optimally shaped electric fields (RF). The optimal control theory, accurate numerical calculation of the energies and wavefunctions, and numerical propagation of wave packets are employed. Two sources of vibrational anharmonicity are studied: the intrinsic Coulomb anharmonicity due to the ion-ion interactions and the external anharmonicity of the trapping potential. It is shown that the magnitude of Coulomb anharmonicity is insufficient for the control. In contrast, anharmonicity of the trapping potential allows controlling the motion of ions very accurately. It is demonstrated that one ion in a slightly anharmonic trap can be easily controlled and used to represent one qubit. A multi-qubit system can be created by employing a long progression of states of a single ion, or by trapping multiple ions and controlling several normal vibration modes of the ion string. Up to four qubits are modeled in this work and accurate pulses are optimized for a set of universal quantum gates: NOT, conditional NOT (CNOT) and Hadamard transformation. The control field for Shor's algorithm (quantum algorithm for factorization onto prime numbers) is also obtained. It is demonstrated that a careful choice of system properties allows achieving very high accuracy of qubit transformations, up to 0.999.
Using numerical simulations of the time-dependent Schrödinger equation, we study the full quantum dynamics of the motion of an atomic ion in a linear Paul trap. Such a trap is based on a time-varying, periodic electric field and hence corresponds to a time-dependent potential for the ion, which we model exactly. We compare the center-of-mass motion with that obtained from classical equations of motion, as well as to results based on a time-independent effective potential. We also study the oscillations of the width of the ion’s wave packet, including close to the border between stable (bounded) and unstable (unbounded) trajectories. Our results confirm that the center-of-mass motion always follows the classical trajectory, that the width of the wave packet is bounded for trapping within the stability region, and therefore that the classical trapping criterion is fully applicable to quantum motion.
The thesis involves three different aspects of quantum dynamics in cold and isolated molecular systems that are investigated theoretically with methods ranging from wavepacket dynamics to density matrix propagation. In the first part the efficiency of cavity sideband cooling of trapped molecules is theoretically investigated for the case in which the infrared transition between two ro-vibrational states is used as a cycling transition. The molecules are assumed to be trapped either by a radio frequency or optical trapping potential, depending on whether they are charged or neutral, and confined inside a high-finesse optical resonator that enhances radiative emission into the cavity mode. Using realistic experimental parameters and Carbonyl sulfide as a molecular representative, we show that in this setup, cooling to the trap ground state is feasible. The second part investigates femtosecond pump-probe spectroscopy of single MgH+ ions confined in an ion trap. The molecular ions are embedded in a coulomb crystal of atomic magnesium ions which are laser cooled to a few millikelvin. Single molecules are addressed by femtosecond ultraviolet laserpulses and the induced molecular processes are investigated. The simulations of the wave packet motion and dissociation behavior were used to predict the experimental parameter regime and are compared directly to the laboratory results. For this purpose a multiscale model is developed which involves the wave packet motion as well as the problem of vibrational heating occurring on a millisecond time scale under laboratory conditions. The third part investigates the gas phase SN2 collision reaction of chloride and methyl iodine. Motivated by the experimental results of Roland Wester and co-workers [Mikosch et al., Science 319, 183 (2008)], remaining questions were addressed. The collision reaction is simulated by solving the time dependent Schrödinger equation on ab initio potential energy surfaces. With the chosen reactive coordinates it is possible to reproduce the basic features of the immediate collision reaction. The internal molecular coordinates are transformed into reaction path based model which allows for an efficient numerical description of the nuclear dynamics. The energy transfer in the system is investigated and compared to the experimental results. From the new insight into the process, an intuitive concept of a dynamical barrier can be derived. Moreover the role of the spectator mode can be clarified.
In some molecules such as ammonia, double vibrations are observed at small energies. These small vibrations are thought to arise from double well potentials. To explain these small energy gaps, double potential wells are investigated, and complex calculations are made. Until recently, since the exact solution of the Schrödinger equation was not known, approximate solutions were always obtained. The exact solution of the Schrödinger equation is now known. In previous studies, a simple procedure for the general solution of the radial Schrödinger Equation has been found for spherical symmetric potentials without making any approximation. In this article, the Schrodinger equation was solved with this new solution method. It has been applied to the oscillations through a barrier tunneling potential for a particle in a central quadratic deformed potential well (double potential well). It is seen that there is no need to look for complex potentials to explain the double wells observed in small vibrations in ammonia and similar molecules, they were compared with experimentally measured energies. The results were found to be fully compatible. It has been seen that there can always be double well potentials at small energies for all molecules, atomic nuclei, and similar particles with angular momentum other than zero.
Abstract We perform quantum trajectory simulations of the decay dynamics of initially localized resonant states. Quantum dynamics is represented by a swarm of interacting trajectories which maps the originally quantum problem into the motion of an equivalent (higher-dimensional) classical system. We address two model problems, in which the decay of the initial resonance leads to either spatially confined or asymptotically free wave-packet dynamics, specifically on a double well potential and on a potential plain. The traditional choice of fixed boundary conditions in the interacting trajectory representation (ITR), set at infinity, is found to have a moderate influence on the accuracy of the ITR of quantum trajectory dynamics, for the motion on a double well potential, i.e. the results of the trajectory-based scheme are in good correspondence with those obtained via quantum wave-packet propagation up to several fundamental vibrational periods. On the other hand, standard boundary conditions have negligible effect on the interacting trajectory dynamics of a decaying shape resonance, whose predictions reproduce quantum mechanical results at long times.
Many important chemical and biochemical processes in the condensed phase are notoriously difficult to simulate numerically.Often, this difficulty arises from the complexity of simulating dynamics resulting from coupling to structured, mesoscopic baths, for which no separation of time scales exists and statistical treatments fail.A prime example of such a process is vibrationally assisted charge or energy transfer.A quantum simulator, capable of implementing a realistic model of the system of interest, could provide insight into these processes in regimes where numerical treatments fail.We take a first step towards modeling such transfer processes using an ion-trap quantum simulator.By implementing a minimal model, we observe vibrationally assisted energy transport between the electronic states of a donor and an acceptor ion augmented by coupling the donor ion to its vibration.We tune our simulator into several parameter regimes and, in particular, investigate the transfer dynamics in the nonperturbative regime often found in biochemical situations.