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The Journal of Chemical Physics

Molecular population transfer, alignment, and orientation using chirped pulse absorption

Y. B. Band, Paul S. Julienne

Published Dec 15, 1992• 40 citations
Publisher

Abstract

We describe a technique for totally transferring the population of a molecular vibronic level to another optically accessible level by chirped pulse absorption. The method can be applied even for nonvanishing angular momentum states where the Rabi frequencies for the transitions depend on the magnetic quantum number M of the states. The population of a large J initial state can be totally transferred to a J′=J+1 state by R branch transitions with linearly or circularly polarized light pulses with negative or positive frequency chirp if the bandwidth of the chirped pulse is sufficiently small. For an initial state with small J, having P(Q) and R transitions that are closely spaced in energy and within the chirped pulse bandwidth, the situation is complicated by the presence of transitions involving additional nearby J states which can participate in transitions induced by the chirped pulse. For positive frequency chirp, population can be totally transferred to the excited electronic state, whereas for the negative frequency chirp case the population distribution depends on the details of the energy levels and laser pulse. The technique can be employed to align and orient states in which not all the M states of the initial level are transferred to the same branch, but each M state is totally transferred from the initial state. Criteria for this type of population transfer and alignment and orientation are described and the conditions under which adiabatic passage is maintained are discussed.

DOI
10.1063/1.463338

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We describe a technique for totally transferring the population of a molecular vibronic level to another optically accessible level by chirped pulse absorption. The method can be applied even for nonvanishing angular momentum states where the Rabi frequencies for the transitions depend on the magnetic quantum number M of the states. The population of a large J initial state can be totally transferred to a J′=J+1 state by R branch transitions with linearly or circularly polarized light pulses with negative or positive frequency chirp if the bandwidth of the chirped pulse is sufficiently small. For an initial state with small J, having P(Q) and R transitions that are closely spaced in energy and within the chirped pulse bandwidth, the situation is complicated by the presence of transitions involving additional nearby J states which can participate in transitions induced by the chirped pulse. For positive frequency chirp, population can be totally transferred to the excited electronic state, whereas for the negative frequency chirp case the population distribution depends on the details of the energy levels and laser pulse. The technique can be employed to align and orient states in which not all the M states of the initial level are transferred to the same branch, but each M state is totally transferred from the initial state. Criteria for this type of population transfer and alignment and orientation are described and the conditions under which adiabatic passage is maintained are discussed.
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 have theoretically investigated the population transfer from the initial ground rovibrational level v(g)=0, J(g)=0 to the final rovibrational levels v(f)=1,2, J(f)=0 of the ground electronic state X (1)Sigma(g) (+) via the resonant intermediate level v(i)=6, J(i)=0 of the excited electronic state EF (1)Sigma(g) (+) of H(2) molecule by (2+2)-photon stimulated hyper-Raman passage (STIHRP). The density matrix technique has been employed to evaluate the population transfer to the final target levels using linearly chirped pump and Stokes laser pulses with different chirp rates. Both the pulses are considered to have the same temporal shape, pulse width, and linear parallel polarizations. We have studied in detail the dependence of the population transfer on the set of laser parameters for pulse (peak) intensities in the ranges of 1.5 x 10(11)-1.0 x 10(12) and 1.0 x 10(12)-7.0 x 10(12) W/cm(2). The corresponding pulse widths (full width at half maximum) are of the order of 115-200 and 15-30 ps. We have found that the chirp rate parameters can be optimized to achieve almost complete population transfer from the ground (g) to the final (f) target levels. This, to our knowledge, is the first application of a (2+2)-photon STIHRP process with chirpings to a model molecular system (H(2)). The study demonstrates the suitability of the chirped (2+2)-photon STIHRP technique for selective and almost total inversion of vibrational population in a diatomic molecule.
The technique of stimulated Raman adiabatic passage (STIRAP) has become an established procedure for producing complete population inversion in atoms or molecules via application of Stokes and pump pulses in a counterintuitive sequence. Previously we reported on numerical and analytical investigations showing some of the additional and important phenomena that arise when some of the levels involved have nonzero angular momentum, the field polarization directions have no simplifying symmetries, and Zeeman splitting lifts the magnetic sublevel degeneracy. Here we verify our theoretical findings using the metastable neon system: 3^{3}3P0{\mathit{P}}_{0}P0​?3{\mathrm{?}}^{3}?3P1{\mathit{P}}_{1}P1​?3{\mathrm{?}}^{3}?3P2{\mathit{P}}_{2}P2​ with the corresponding angular momentum sequence J=0?J=1?J=2. In particular, we demonstrate that it is possible to transfer all population from the single initial state to any single selectable final magnetic sublevel M. Selectivity can be achieved either by choosing special laser polarization angles or, for fixed polarizations, by tuning the two lasers into two-photon resonance between the initial and desired final state. The complete control of magnetic sublevel population enabled by this procedure extends the customary experimental methods for producing oriented or aligned beams of atoms. In addition, we demonstrate very clearly the previous prediction that population transfer may fail for certain sets of parameters (detunings, Rabi frequencies, and polarization angles). \textcopyright{} 1996 The American Physical Society.
We have numerically explored the feasibility and the mechanism of population transfer to the excited E (1)Σ(g) electronic state of Li(2) from the v=0 level of the ground electronic state X (1)Σ(g) using the A (1)Σ(u) state as an intermediate. In this system, the use of transform limited pulses with a frequency difference greater than the maximum Rabi frequency does not produce population transfer when all possible radiative couplings are taken into account. We have employed two synchronous pulses far detuned from the allowed transition frequencies, mainly with the lower frequency pulse positively chirped, and both pulses coupling the successive pair of states, X-A and A-E. The adiabaticity of the process has been investigated by a generalized Floquet calculation in the basis of 12 field dressed molecular states, and the results have been compared with those obtained from the full solution of time dependent Schrödinger equation. The conventional representation of the process in terms of three (or four) adiabatic potentials is not valid. It has been found that for cases of almost complete population transfer in full calculations with the conservation of the vibrational quantum number, adiabatic passage is attained with the 12 state Floquet model but not with the six state model. The agreement between the full calculations and the 12 state Floquet calculations is generally good when the transfer is adiabatic. Another characteristic feature of this work is the gaining of control over the vibrational state preparation in the final electronic state by careful tuning of the laser parameters as well as the chirp rate sign. This causes time dependent changes in the adiabatic potentials and nonadiabatic transfers can be made to occur between them.
Using the concept of light-induced potentials introduced by Garraway and Suominen [Phys. Rev. Lett. 80, 932 (1998)], we study alternative schemes of adiabatic population transfer in a diatomic molecule from the lowest vibrational level of the ground electronic state to the lowest vibrational level of a third electronic state via allowed optical transitions from the ground and third electronic states to a second electronic state. Our chirped-pulse rapid adiabatic passage scheme is implemented with short-duration optical pulses, and can be understood in terms of ``road design engineering'' of the light-induced time-dependent adiabatic potential upon which the dynamics occurs. We explicitly show that complete adiabatic vibronic population transfer occurs using chirped picosecond-duration pulses in the sodium dimer example.
We propose a scheme for coherent control of population transfer and arbitrary superpositions of quantum states by a single-chirped laser pulse in a Λ-type excited-doublet four-level system. It is shown that selective, efficient, and robust population transfer from the initial state to the target states (excited or ground) can be achieved via chirped adiabatic passage when the pulse bandwidth is smaller than about 1/10 of the energy separations between the excited-doublet levels and between the ground states. Moreover, arbitrary coherent superpositions between the excited-doublet states, or between the higher ground state and either of the excited-doublet states, can be created by appropriately tuning the chirp rate and detuning the laser field. The proposed flexible method of coherent control of population transfer and arbitrary superpositions between the initially unpopulated states requires only a single pulse, and is robust against variations in the laser parameters, which has potential applications in quantum information processing.