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Physical Review A

Rovibrational population transfer in the ground state controlled by two coherent laser pulses

Rong Wang, Ying‐Yu Niu, Ming‐Hui Qiu, Yong‐Chang Han

Published Jan 5, 2015• 10 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.91.013401

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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 (\ensuremathω+2\ensuremathω\ensuremath{\omega}+2\ensuremath{\omega}\ensuremathω+2\ensuremathω) pulses analogous to coherently control the processes of ionization and dissociation. The population can be transferred to three target states, ∣4,1\ensuremath⟩,∣0,1\ensuremath⟩|4,1\ensuremath{\rangle},\phantom{\rule{0.16em}{0ex}}|0,1\ensuremath{\rangle}∣4,1\ensuremath⟩,∣0,1\ensuremath⟩, and ∣4,0\ensuremath⟩|4,0\ensuremath{\rangle}∣4,0\ensuremath⟩, at the same time through the ladder \ensuremathΛ\ensuremath{\Lambda}\ensuremathΛ and multiphoton transitions. With the variation of the relative phase between \ensuremathω\ensuremath{\omega}\ensuremathω and 2\ensuremathω2\ensuremath{\omega}2\ensuremathω pulses, the population distributions show oscillation behavior with a period of \ensuremathπ\ensuremath{\pi}\ensuremathπ. 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.
The population transfer of stimulated Raman adiabatic passage (STIRAP) is investigated using a time-dependent quantum wave packet method. The population is transferred from an initial state to a target state through the interaction of the external laser field with the permanent dipole moment and the transition dipole moment. The laser field is composed of an infrared pulse and a near ultraviolet pulse. The two pulses with small detunings are more efficient to achieve the STIRAP transition. The process of STIRAP is sensitive to the detunings of the two pulses. When the two detunings are the same in a Λ transition or the positive detuning of the pump pulse is equal to the negative detuning of the Stokes pulse in a ladder transition, the final population in the intermediate state can be eliminated and the target population is increased.
Abstract The population transfer controlled by fundamental, 2nd-harmonic and 3rd-harmonic pulses is investigated by using the time-dependent quantum wave packet method. By varying the phase ϕ 1 of the fundamental pulse, it can be coherent with the 2nd-harmonic and 3rd-harmonic pulses. Compared with two harmonic pulses, the phase ϕ 1 in three harmonic pulses is more efficient in controlling population transfer. Molecular orientation can be controlled by the phases of the three pulses. The value of molecular orientation mainly depends on the phase coherence between the fundamental and 2nd-harmonic pulses.
Ultrafast pulse shapes are used to control simultaneously the optimal population transfer coefficients and rotational wave-packet quantum interferences in the $E{}^{1}{\ensuremath{\Sigma}}_{g}^{+}$ state of Li2{\mathrm{Li}}_{2}Li2​ $({\ensuremath{\nu}}_{E}=9,$ JE=27{J}_{E}=27JE​=27 and 29). By dividing the spectral bandwidth of the ultrafast pulses into multiple ``control domains'' centered on each resonant wavelength, the population transfer coefficients can be manipulated independently of the wave-packet interferences to maximize the Li2{\mathrm{Li}}_{2}Li2​ photoionization yield at arbitrary short pump-probe time delays. To investigate the population transfer coefficients with and without wave-packet interferences, respectively, the pump polarization is set to be either parallel to or at the magic angle (\ensuremath{\sim}55\ifmmode^\circ\else\textdegree\fi{}) relative to the probe polarization. A comparison is made between phases that are symmetric and antisymmetric about the resonances. The effects of resonant and nonresonant frequencies are separately established and quantified. It is estimated that up to 90% of the possible nonresonant Rabi oscillations can be brought into phase simultaneously for each rovibrational state in the wave packet, while at the same time a constant phase offset added to one of the control domains establishes the phase of the wave-packet interference.