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Spectroscopic signatures of bond-breaking internal rotation. II. Rotation-vibration level structure and quantum monodromy in HCP
The rotation-vibration level structure of ground electronic state HCP is investigated at vibrational energies approaching and exceeding that of the linear CPH saddle point. With respect to energies ab...
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Ab initio study of silver bromide AgnBr<sub>p</sub><sup>(+)</sup> clusters (n<=6,p = n,n–1)
Ab initio calculations in the framework of the density functional theory (DFT) with 19-electron pseudopotential on silver atoms are performed to study the lowest-energy isomers of silver bromide clust...

Theory of sub-Doppler Autler–Townes splitting in molecules: Alignment and orientation of the angular momentum in nonpolar molecules

J. Chem. Phys. 114, 276 (2001); doi:10.1063/1.1328381

Issue Date: 1 January 2001

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Frank C. Spano
Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122
Within a density matrix framework, an analytical expression for the optical–optical double resonance (OODR) line shape for a molecule in the presence of a strong coupling laser is derived. The coupling laser is tuned to a transition between the upper level in the OODR sequence and another excited level which is not part of the OODR sequence. The pump and probe lasers are treated perturbatively, while the coupling laser is treated exactly. The line shape reveals sub-Doppler Autler–Townes (AT) splitting of the states |J,m> within the highest excited level. The splitting depends on |m|(m) for linearly (circularly) polarized coupling fields. m-state selectivity and therefore alignment and orientation of the angular momentum can be achieved by tuning the probe laser in the presence of a coupling field which is sufficiently strong to resolve the m-dependent AT splittings. m selectivity is analyzed for e and f parity 1Pig levels in diatomic molecules. A method to orient nonpolar diatomics using circularly polarized lasers is proposed. ©2001 American Institute of Physics.
History: Received 31 July 2000; accepted 4 October 2000
Permalink: http://link.aip.org/link/?JCPSA6/114/276/1
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KEYWORDS and PACS

Keywords
PACS
  • 33.55.Be
    Molecular properties and interactions with photons Optical activity and dichroism; magnetooptical and electrooptical spectra Zeeman and Stark effects
  • 33.40.+f
    Molecular properties and interactions with photons Multiple resonances (including double and higher-order resonance processes, such as double nuclear magnetic resonance, electron double resonance, and microwave optical double resonance)
  • 33.70.Jg
    Molecular properties and interactions with photons Intensities and shapes of molecular spectral lines and bands Line and band widths, shapes, and shifts
  • YEAR: 2001

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ISSN:
0021-9606 (print)   1089-7690 (online)
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