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

J. Chem. Phys. 97, 9107 (1992); doi:10.1063/1.463338

Issue Date: 15 December 1992

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Y. B. Band
Department of Chemistry, Ben-Gurion University, Beer Sheva, Israel 84105
Institute for Theoretical Atomic and Molecular Physics, Harvard-Smithsonian Center for Astrophysics, 60 Garden Street, Cambridge, Massachusetts 02138


P. S. Julienne
Molecular Physics Division, National Institute of Standards and Technology, Gaithersburg, Maryland 20899
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[script ']=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. The Journal of Chemical Physics is copyrighted by The American Institute of Physics.
History: Received 8 July 1992; accepted 10 September 1992
Permalink: http://link.aip.org/link/?JCPSA6/97/9107/1
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KEYWORDS and PACS

Keywords
PACS
  • 33.80.Be
    Molecular spectra and interactions of molecules with photons Photon interactions with molecules Level crossing and optical pumping
  • 42.50.Hz
    Optics Quantum optics Strong-field excitation of optical transitions in quantum systems; multi-photon processes
  • YEAR: 1992

PUBLICATION DATA

ISSN:
0021-9606 (print)   1089-7690 (online)
Publisher:
AIP is a member of CrossRef AIP

REFERENCES (16)

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  21. Alternatively, the dressed state basis, |a,N(t)−1>, |g,N)t(> and |b,N(t)−1> can be used to express the Hamiltonian in tridiagonal form. The dressed-state Hamiltonian in this basis is given by

    [dformula H(t)[sub 3dress]  =   - [h-bar](( Delta[sub 1], ,  Omega[sub 1](t), , 0;  Omega[sub 1](t)*, , 0, ,  Omega[sub 2](t); 0, ,  Omega[sub 2](t)*, ,  Delta[sub 2])).]

    Making the transformation psi2(t) = psi2(t)exp[−(i/2)(dw/dt)t2], yields

    [dformula H(t)[sub 3dress]  =   - [h-bar](( Delta[sub 1], ,  Omega[sub 1](t), , 0;  Omega[sub 1](t), , ((d omega)/dt)t, ,  Omega[sub 2](t); 0, ,  Omega[sub 2](t), ,  Delta[sub 2])).]


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