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Acta Physica Sinica

Rovibrational population transfer controlled by two overlapping pulses

Niu Ying-Yu, Rong Wang, Jun-Ling Xiu

Published Jan 1, 2012• 4 citations
Publisher

Abstract

Rovibrational population transfer is controlled by a two-overlapping- pulse scheme in which the frequency ratio of the two pulses is 1:3. The calculated results show that nearly 100% of the population can be transferred from initial state |0,0to target state |3,1. The probability of population transfer can be controlled by pulse phase. When 1 =1.68 , the two pulses can be increased mutually and the probability of population transfer is also increased. When 1 =0.64 , the two pulses can be offset mutually and the probability of population transfer is reduced. The intensity of the second pulse has a significant effect on the population transfer.

DOI
10.7498/aps.61.093302

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Rovibrational population transfer is controlled by a two-overlapping- pulse scheme in which the frequency ratio of the two pulses is 1:3. The calculated results show that nearly 100% of the population can be transferred from initial state |0,0to target state |3,1. The probability of population transfer can be controlled by pulse phase. When 1 =1.68 , the two pulses can be increased mutually and the probability of population transfer is also increased. When 1 =0.64 , the two pulses can be offset mutually and the probability of population transfer is reduced. The intensity of the second pulse has a significant effect on the population transfer.
A time-dependent quantum wave-packet method is employed to investigate the rovibrational dynamics of population transfer in the ground electronic state controlled by two-color ($\ensuremath{\omega}+2\ensuremath{\omega}$) pulses analogous to coherently control the processes of ionization and dissociation. The population can be transferred to three target states, $|4,1\ensuremath{\rangle},\phantom{\rule{0.16em}{0ex}}|0,1\ensuremath{\rangle}$, and $|4,0\ensuremath{\rangle}$, at the same time through the ladder $\ensuremath{\Lambda}$ and multiphoton transitions. With the variation of the relative phase between $\ensuremath{\omega}$ and $2\ensuremath{\omega}$ pulses, the population distributions show oscillation behavior with a period of $\ensuremath{\pi}$. The population variation with relative phase depends on the size of the electric field asymmetry. The probabilities transferred to different target states can be controlled by varying the pulse amplitudes.
The processes of population transfer in the ground electronic state of HCl molecule through the three transition schemes are investigated by numerically solving the time-dependent Schrödinger equation. Two harmonic pulses are employed to induce population transfer and the relative phase of the two pulses can control the final population distributions. In the ladder transition scheme, the variation range of the target population with the relative phase is nearly 100% which is larger than that in the multi-photon transition scheme. It is more efficient for the mixed transition scheme to control population transfer between the initial and target states by using the relative phase. Comparing with the multi-photon and ladder schemes, the transition probability of the target population is more sensitive to the two pulse amplitudes in the mixed transition scheme.
The multiphoton transition is investigated theoretically by using wave packet method for the ground electronic state of HF molecule. A laser field composed of two overlapping infrared pulses is used in our model, and the ratio of their frequencies is 1:2. States |4,0> and |4,2> are chosen as target states. Calculated results show that the population can be transferred to different target states as the corresponding resonant frequency is chosen. The probability of the population transfer can be controlled by the initial phase difference of the two pulses. When the initial phase difference is of an odd number of π/2, the probability of population transfer reaches the maximal value. When the initial phase difference is of an even number of π/2, the probability of population transfer reaches the minimum value. In comparison with the state |4,2>, the initial phase difference has a stronger in fluence on the population of the state |4,0>.
The extended “ladder” transition controlled by two harmonic pulses is investigated by using a time-dependent quantum wave packet method. The molecular population transfers from the state|0, 0> angle to the states|5, 0> angle and|5, 2> angle induced by the fundamental and second-harmonic pulses, and to the states|5, 3> angle and |6, 2> angle induced by the fundamental and third-harmonic pulses. The calculated results show that the two harmonic pulses can induce a nearly 100% of population to transfer to the target state. The relative phase of two pulses can affect the population distribution. The variation of population has a period of π for the fundamental and second-harmonic pulses, and a period of 2π for the fundamental and third-harmonic pulses.
We have examined the sensitivity to the presence of background states of population transfer to a predissociating molecular state generated by coherent two-pulse excitation. The system studied is intended to model optical control of the formation of a product in a photofragmentation reaction. The model spectrum of states is a generalization of the three-state spectrum considered in the conventional STIRAP method in three respects: the target state is a resonance in the continuum, the spectrum includes both unoccupied background states that have finite lifetimes and some unoccupied pairs of background states that are in resonance with the excitation pulses, and nonadiabatic population transfer is allowed. We examine the variation of the population transfer to the target state with respect to its lifetime, as well as the robustness of the population transfer with respect to variation of the area of overlap of the two excitation pulses and with respect to the presence of background states (some of which have finite lifetimes). Our results show that there is a broad range of conditions under which it is possible to transfer population efficiently from an initial state to a target predissociating state using coherent two-pulse excitation, although that population transfer is not always adiabatic.
This work presents a method for achieving complete, robust, and efficient population transfer between the two ground states in a three-level loop quantum system. The approach utilizes composite pulse sequences by effectively mapping the three-state system onto an equivalent two-level system. This transformation allows the use of broadband composite pulses designed initially for conventional two-state quantum systems. Unlike traditional implementations, the composite pulses in the three-level system are not controlled through phase adjustments; instead, they are realized via the amplitude ratio of the Rabi frequencies.