We suggest that infrared stimulated Raman adiabatic passage, a coherent multiple excitation process, can be used to create a superposition of (2J+1) highly correlated M-state sublevels of a rigid rotor molecule with vibrational level v and rotational level J. This method employs the (v=0,J-2) to (v=2,J) S-branch transition, which is carried out in a counterintuitive manner in which the v=1 to v=2 transition is pumped prior to the v=0 to v=1 transition, causing nearly complete population transfer to the v=2 final level. We use perpendicular and parallel linearly polarized infrared excitation (biaxial excitation). Specifically, the perpendicular polarization connects the v=1 intermediate level to the final vibrational level v=2, and the parallel polarization connects the initial level v=0 to the intermediate level v=1. By this means we break the cylindrical symmetry for an ensemble of vibrationally excited molecules in a rovibrational eigenstate (v=2,J). The angular momentum polarization is determined by the relative phases rather than by the populations of the magnetic M-sublevels. For the phase correlated ensemble, the angular momentum polarization can be considered as a purely quantum mechanical effect. Using a fully general density matrix treatment, we illustrate this approach by considering a beam of carbon monoxide (CO) molecules. We find that significant polarization for J=2, 5, and 10 can be achieved with a cw infrared laser source having modest power (∼100 mW/mm(2)). We believe that this technique is a general one and may offer an experimentally accessible new platform for different applications, from scattering studies with M-state entangled ensembles of molecules to logic gate operations of a quantum computer.
We suggest that infrared stimulated Raman adiabatic passage, a coherent multiple excitation process, can be used to create a superposition of (2J+1) highly correlated M-state sublevels of a rigid rotor molecule with vibrational level v and rotational level J. This method employs the (v=0,J-2) to (v=2,J) S-branch transition, which is carried out in a counterintuitive manner in which the v=1 to v=2 transition is pumped prior to the v=0 to v=1 transition, causing nearly complete population transfer to the v=2 final level. We use perpendicular and parallel linearly polarized infrared excitation (biaxial excitation). Specifically, the perpendicular polarization connects the v=1 intermediate level to the final vibrational level v=2, and the parallel polarization connects the initial level v=0 to the intermediate level v=1. By this means we break the cylindrical symmetry for an ensemble of vibrationally excited molecules in a rovibrational eigenstate (v=2,J). The angular momentum polarization is determined by the relative phases rather than by the populations of the magnetic M-sublevels. For the phase correlated ensemble, the angular momentum polarization can be considered as a purely quantum mechanical effect. Using a fully general density matrix treatment, we illustrate this approach by considering a beam of carbon monoxide (CO) molecules. We find that significant polarization for J=2, 5, and 10 can be achieved with a cw infrared laser source having modest power (∼100 mW/mm(2)). We believe that this technique is a general one and may offer an experimentally accessible new platform for different applications, from scattering studies with M-state entangled ensembles of molecules to logic gate operations of a quantum computer.
A density matrix treatment is presented for a general process of preparing polarized molecules through their coherent interaction with two or more infrared photons of different frequencies, each tuned to cause a transition between real levels. This process, which might be called infrared stimulated Raman adiabatic passage, allows complete population transfer to selected rotational-vibrational levels and controls the direction of the rotational angular momentum vector J of the molecule with the possibility of preparing higher moments of the J spatial distribution. HCl molecules in a supersonic molecular beam are considered as a candidate system. Theory predicts that under collision-free conditions two infrared laser pulses of microsecond duration and milliwatt power are able to achieve complete population transfer and alignment of HCl (v=2, J=2, and M=0) for mutually parallel excitation and HCl (v=2, J=2, and M=+/-1) for mutually perpendicular excitation. Orientation of the HCl (v=2, J=2, and M=+/-2) can also be achieved using two circularly polarized pulses of the same helicity. For simplicity, our treatment ignores nuclear spin depolarization, which would be the case for molecules such as (12)C(16)O and (12)C(16)OO(2). Polarized molecules in higher vibrational levels can be prepared using additional infrared pulses.
Control of molecular angular momentum orientation enables state-resolved studies of molecular interactions and provides a basis for quantum information processing. Here we propose all-optical Autler-Townes state-selective adiabatic passage (ASAP) to prepare molecules in a single ∣J,M⟩ sublevel. An Autler-Townes branch created by a strong coupling field is selectively populated and adiabatically mapped onto the target vibrational state. We resolve detuning-dependent rovibrational Autler-Townes splitting in 13CO2, establishing the spectroscopic basis for the selective excitation of the target dressed branch. The density-matrix model calibrated by these spectra predicts transfer approaching 90\%. The scheme can exploit millisecond vibrational radiative lifetimes within the electronic ground state and extend to polar and nonpolar molecules with infrared-active vibrational modes.
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: 3P0?3P1?3P2 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 prepare an ensemble of isolated rovibrationally excited (v = 1, J = 2) H2 molecules in a phase-locked superposition of magnetic sublevels M using Stark-induced adiabatic Raman passage with linearly polarized single-mode pump (at 532 nm, ∼6 ns pulse duration, 200 mJ/pulse) and Stokes (699 nm, ∼4 ns pulse duration, 20 mJ/pulse) laser excitation. A biaxial superposition state, given by [line]ψ(t)⟩ = 1/√(2)[[line]ν = 1, J = 2, M = -2⟩ - [line]ν = 1, J = 2, M = +2⟩], is prepared with linearly but cross-polarized pump and Stokes laser pulses copropagating along the quantization z-axis. The degree of phase coherence is measured by using the O(2) line of the H2 E,F-X (0,1) band via 2 + 1 resonance enhanced multiphoton ionization (REMPI) at 210.8 nm by recording interference fringes in the REMPI signal in a time-of-flight mass spectrometer as the direction of the UV laser polarization is rotated using a half-wave plate. Nearly 60% population transfer from H2 (v = 0, J = 0) ground state to the superposition state in H2 (v = 1, J = 2) is measured from the depletion of the Q(0) line of the E,F-X (0,0) band as the Stokes frequency is tuned across the (v = 0, J = 0) → (v = 1, J = 2) Raman resonance.
We consider an adiabatic population transfer process that resembles the well-established stimulated Raman adiabatic passage. In our system, the states have nonzero angular momentums J , therefore, the coupling laser fields induce transitions between the magnetic sublevels of the states. In particular, we discuss the possibility of creating coherent superposition states in a system with coupling pattern J = 0 ⇔ 1 and 1 ⇔ 2. Initially, the system is in the J = 0 state. We show that by, applying two delayed overlapping laser pulses, it is possible to create any final superposition state of the magnetic sublevels |2, −2⟩, |2, 0⟩, |2, +2⟩. Moreover, we find that the relative phases of the applied pulses influence not only the phases of the final superposition state but also the probability amplitudes. We show that if we fix the shape and the time delay between the pulses, the final state space can be entirely covered by varying the polarizations and relative phases of the two pulses. Performing numerical simulations we find that our transfer process is nearly adiabatic for the whole parameter set.
A technique for creation of well-defined preselected coherent superpositions of multiple quantum states is proposed. It is based on an extension of the technique of stimulated Raman adiabatic passage (STIRAP) to degenerate levels. As an example, the nine-state system composed of the magnetic sublevels of three levels with angular momenta Jg=0, Je=1, and Jf=2 is studied in detail. Starting from the $\ensuremath{\mid}{J}_{g}=0,{M}_{g}=0⟩$ state, STIRAP can create an arbitrary preselected coherent superposition between the five Mf sublevels $({M}_{f}=\ensuremath{-}2,\ensuremath{-}1,0,+1,+2)$ of the Jf=2 level with 100% efficiency in the adiabatic limit. The populations and the phases of the Mf states in this superposition are determined entirely by the polarizations of the two laser fields. It is shown that this technique allows one to create any superposition of the five Mf states, that is, to reach any point in the Hilbert space of the Jf=2 manifold, and the corresponding recipes for choosing the laser polarizations are presented.