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arXiv:1603.00777 · Physical Chemistry Chemical Physics

Protecting and accelerating adiabatic passage with time-delayed pulse sequences

Pablo Sampedro, Bo Y. Chang, Ignacio R. Solá

Published Jan 1, 2016• 6 citations
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Abstract

Using numerical simulations of two-photon electronic absorption with femtosecond pulses in Na2 we show that: (i) it is possible to avoid the characteristic saturation or dumped Rabi oscillations in the yield of absorption by time-delaying the laser pulses; (ii) it is possible to accelerate the onset of adiabatic passage by using the vibrational coherence starting in a wave packet; and (iii) it is possible to prepare the initial wave packet in order to achieve full state-selective transitions with broadband pulses. The findings can be used, for instance, to achieve ultrafast adiabatic passage by light-induced potentials and understand its intrinsic robustness.

DOI
10.1039/c6cp01680d

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Using numerical simulations of two-photon electronic absorption with femtosecond pulses in Na2 we show that: (i) it is possible to avoid the characteristic saturation or dumped Rabi oscillations in the yield of absorption by time-delaying the laser pulses; (ii) it is possible to accelerate the onset of adiabatic passage by using the vibrational coherence starting in a wave packet; and (iii) it is possible to prepare the initial wave packet in order to achieve full state-selective transitions with broadband pulses. The findings can be used, for instance, to achieve ultrafast adiabatic passage by light-induced potentials and understand its intrinsic robustness.
We present the process of adiabatic passage by light-induced potentials for transferring a wave packet from one molecular potential to the displaced ground vibrational state of another. The process uses a counterintuitive sequence of light pulses to couple three molecular states. It shares many features with the process of stimulated Raman adiabatic passage, such as high efficiency and insensitivity to pulse parameters. However, in the former there is no two-photon resonance, and the main mechanism for the transport of the wave packet is a light-induced potential.
We demonstrate numerically the conditions where a wave packet adiabatic passage method yields optimal results for selective excitation of a vibrational level on excited electronic states in molecules. In a recent contribution Garraway and Suominen [Phys. Rev. Lett. 80, 932 (1998)] introduced the method of adiabatic passage by light-induced potentials (APLIP). Here we test and analyze the robustness of the APLIP process under realistic conditions for exciting the ground vibrational state of the Na2{\mathrm{Na}}_{2}Na2​ molecule to the ground vibrational level of the excited ${}^{1}{\ensuremath{\Sigma}}_{g}(4s)$ state. The spatial and temporal adiabaticity of the process assures the conservation of the vibrational quantum number during the passage and leads to the remarkable robustness of the method, which at some extent prevents the usual rotating-wave approximation to be employed.
In this paper we propose to control the bond length of a diatomic molecule and its vibrational coherent motion over arbitrary distances. The method requires (a) mixing a dissociative potential with bound electronic configurations in order to stabilize the continuum, and (b) manipulating the wave-packet transfer below the threshold of adiabatic passage. Using asymmetric pulses it is possible to implement sudden-adiabatic transitions to stop or induce the motion in the light-induced potential, controlling the nonadiabatic dynamics in a most efficient way.
We study the dynamics of chirped adiabatic passage (CHIRAP) with temporally delayed pulses to selectively and fully transfer population in atoms and molecules. We show that the transfer of population via stimulated Raman adiabatic passage (STIRAP) and stimulated two-photon adiabatic absorption with temporally delayed laser pulses is not adversely affected by applying a chirp to the pulses, provided the intensity of the laser is sufficiently large to allow adiabatic passage. We then proceed to consider systems in which a near degeneracy of terminal state levels results in nonselective population of the terminal levels using nonchirped STIRAP or two-photon absorption stimulated passage, because the dynamics within the nearly degenerate pair of levels is not adiabatic. However, the CHIRAP process selectively populates only one of the terminal levels.
This thesis is based upon the work published in the following two articles entitled: Robust Operation of a Universal Set of Logic Gates for Quantum Computation using Adiabatic Population Transfer between Molecular Levels [37], and Piecewise Adiabatic Passage with a Series of Femtosecond Pulses [54]. Both papers involve using the concept of a quantum control phenomenon, known as adiabatic passage in different manners, in order to achieve particular goals. In the first paper we present a robust construction of a set of logic gates operating on a system of qubits encoded in the ro-vibrational eigenstates of an Na₂ molecule using the optical Adiabatic Population Transfer (APT) method. We demonstrate the operation of a complete universal gate-set for quantum computation on a two-qubit system with gate fidelities approaching 99.99%. Like other APT-based processes, the method is robust against substantial fluctuations in the intensity of the laser pulse. Our construction is easily scalable to dealing with a larger number of qubits. The second line of research developed from the desire to merge the robustness of an adiabatic process, as presented in the previous paper, with the speed and additional level of control available by using pulse shaping techniques of broadband pulses. Therein we develop a method of executing complete population transfers between quantum states in a piecewise manner using a series of femtosecond laser pulses. The method can be applied to a large class of problems as it benefits from the high peak powers and large spectral bandwidths afforded by femtosecond pulses. The degree of population transfer is found to be robust to a wide variation in the absolute and relative intensities, durations, and time ordering of the pulses. The method is studied in detail for atomic sodium where piecewise adiabatic population transfer, as well as the induction of Ramsey-type interferences, is demonstrated.
Recent techniques in x-ray free electron lasers allow the generation of highly coherent, intense x-ray pulses with time lengths on the order of femtoseconds. Here we explore the possibilities of using such x-ray pulses to control matter based on coherence. In particular we propose a theoretical scheme to perform stimulated Raman adiabatic passage in the x-ray regime by using inner-hole excited states. Numerical results in two well-known systems, the neon atom and the carbon monoxide molecule, show a robust control of population transfer. In the molecule, vibrational selectivity is achieved with femtosecond x-ray pulses. This work supports the possibility of using two-color x-ray pulses for coherent control.