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Physical Review A

State-selective chirped adiabatic passage on dynamically laser-aligned molecules

S. Thomas, S. Guérin, Hans Rudolf Jauslin

Published Jan 3, 2005• 23 citations
Publisher

Abstract

We show that rovibrational state selectivity can be achieved by chirped adiabatic passage of molecules that are adiabatically aligned by a nonresonant laser field. We develop the tools to design the appropriate frequency and amplitude modulations that allow us to select a given route in the Hilbert space that leads to a final complete excitation of the chosen state, by infrared or by Raman processes. This method allows us to select a given vibrational state in a well-defined rotational $J$ state.

DOI
10.1103/physreva.71.013402

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We show that rovibrational state selectivity can be achieved by chirped adiabatic passage of molecules that are adiabatically aligned by a nonresonant laser field. We develop the tools to design the appropriate frequency and amplitude modulations that allow us to select a given route in the Hilbert space that leads to a final complete excitation of the chosen state, by infrared or by Raman processes. This method allows us to select a given vibrational state in a well-defined rotational JJJ state.
Calculations indicate that high vibrational states of oxygen and chlorine can be excited using a series of nonresonant Raman pulses, where both the pump and the Stokes pulses are chirped with linear frequency sweeps. Most of the previously reported coherent processes (such as simple adiabatic passage) are seriously degraded when rotational effects are included. However, we find that the laser pulse parameters (intensity and bandwidth) required to invert population into high vibrational states via Raman chirped adiabatic passage are achievable using technology that is currently available. Applications to homonuclear diatomic molecules are discussed in detail.
Abstract We have theoretically investigated the population transfer and the selective excitation of vibrational states of the target state in a three-state Na 2 molecule using the chirped adiabatic passage. The population transfer among electronic states is studied. Compared with the single negative chirped pulse, complete population transfer can be achieved by using a positive chirped pulse. The effects of laser parameters on vibrational population distribution are discussed, and the selective excitation of vibrational states can be achieved by adjusting the central frequency. Finally, we give the method of selective excitation of specific vibrational states.
Chirped pulses allow for non-adiabatic passage between dressed states of Raman processes. It is shown that using an appropriately chirped pulse, one can control the interference between resonant and non-resonant pathways in stimulated Raman processes. A three-level system is studied in detail and application to complete ro-vibrational level inversion to high vibration quantum numbers (v > 10) in H2 via RCNAP (Raman chirped non-adiabatic passage) is presented. Copyright © 2000 John Wiley & Sons, Ltd.
We explore theoretically the rovibrational dynamics of stimulated Raman adiabatic passage (STIRAP) in molecular electronic states including both the rotational and the vibrational degrees of freedom, with the LiH molecule as an example. By using a pure rovibrational state as initial state, we find that, under the condition of two-photon resonance, an efficient rovibrational population transfer can be achieved via STIRAP in molecular electronic states and the desired target state can be selected by adjusting laser-pulse parameters. Besides the interested rovibrational states, however, some unwanted rovibrational states may affect population transfer process, especially while the two-photon detuning is taken into account. By inspecting the evolution process of wave packet, we can easily search these unwanted rovibrational states and study their influences. Moreover, the effect of rotational temperature on the population transfer process is discussed using thermal mixed state as initial state.
We review and compare recent experiments and theoretical models demonstrating complete population transfer to selected states in atoms and molecules using (1) Stimulated Raman Adiabatic Rapid Passage (STIRAP) with temporally delayed but partially overlapping time dependent fundamental and Stokes fields and (2) Chirped Adiabatic Passage (CHIRAP) using frequency chirped field with the frequency swept through the resonance frequency of transitions. The transfer efficiency in these processes is unity when the adiabatic criteria are satisfied. Alignment and orientation of the initial and terminals levels of the transitions can be obtained using these methods. The dynamics involve the atomic or molecular internal angular momentum states because the Rabi frequencies for the transitions depend on the magnetic quantum numbers of the states. Full wavefunction and density matrix (necessary when spontaneous emission of the excited states plays a role) calculations are presented and adiabatic-following wavefunction and density matrix descriptions are advanced to explain unexpected experimental results.
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.