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Physical Review Letters

Line Shapes in Coherent Ion Dip Spectroscopy of Polyatomic Molecules

R. Neuhäuser, Ralf Sussmann, Hans Jürgen Neusser

Published Apr 17, 1995• 14 citations
Publisher

Abstract

Using two narrow-band Fourier-transform limited, tunable ns laser pulses the observation of coherent adiabatic Raman processes becomes feasible for polyatomic molecules. Recent experiments reveal the possibility of an effective suppression of ionization in an ion dip experiment using a lambda-type resonant coherent optical-optical UV-double-resonance process and suggest its application in molecular spectroscopy. The experiments, including the observed ionization enhancement for off-resonance conditions, are quantitatively described using a few-level density matrix approach.

DOI
10.1103/physrevlett.74.3141

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Using two narrow-band Fourier-transform limited, tunable ns laser pulses the observation of coherent adiabatic Raman processes becomes feasible for polyatomic molecules. Recent experiments reveal the possibility of an effective suppression of ionization in an ion dip experiment using a lambda-type resonant coherent optical-optical UV-double-resonance process and suggest its application in molecular spectroscopy. The experiments, including the observed ionization enhancement for off-resonance conditions, are quantitatively described using a few-level density matrix approach.
The interaction of two narrow band (Δν<100 MHz) UV light pulses of different intensity with a molecular three-level system is investigated experimentally. The laser frequencies are tuned to an up (pump) and a down (dump) transition sharing a common excited rovibronic S1 level whose population is probed by a transition to the ionization continuum and ion detection. The time sequence of the two pulses results either in a lambda type coherent stimulated Raman adiabatic passage or a stimulated emission pumping (SEP) process. When the first case is realized by a 6.4 ns delay of the low intensity pump laser from the high intensity dump laser pulse, a fourfold increase of the depth of the ion dips compared to the SEP experiment is observed. This is in line with numerical calculations of the level populations using a density matrix formalism including coherent effects. Rotationally resolved ion dip spectra of the 62 state of benzene are presented and demonstrate the high sensitivity of the coherent excitation process of this work for ion dip spectroscopy.
Exact and asymptotic line shape expressions are derived from the semiclassical density matrix representation describing a set of closed three-level $\ensuremath{\Lambda}$ atomic or molecular states including decoherences, relaxation rates, and light shifts. An accurate analysis of the exact steady-state dark-resonance profile describing the Autler-Townes doublet, the electromagnetically induced transparency or coherent population trapping resonance, and the Fano-Feshbach line shape leads to the linewidth expression of the two-photon Raman transition and frequency shifts associated to the clock transition. From an adiabatic analysis of the dynamical optical Bloch equations in the weak field limit, a pumping time required to efficiently trap a large number of atoms into a coherent superposition of long-lived states is established. For a highly asymmetrical configuration with different decay channels, a strong two-photon resonance based on a lower states population inversion is established when the driving continuous-wave laser fields are greatly unbalanced. When time separated resonant two-photon pulses are applied in the adiabatic pulsed regime for atomic or molecular clock engineering, where the first pulse is long enough to reach a coherent steady-state preparation and the second pulse is very short to avoid repumping into a new dark state, dark-resonance fringes mixing continuous-wave line shape properties and coherent Ramsey oscillations are created. Those fringes allow interrogation schemes bypassing the power broadening effect. Frequency shifts affecting the central clock fringe computed from asymptotic profiles and related to the Raman decoherence process exhibit nonlinear shapes with the three-level observable used for quantum measurement. We point out that different observables experience different shifts on the lower-state clock transition.
We report on an investigation of simultaneous generation of several narrow-bandwidth laser-like coherent emissions from nitrogen molecular ions ( ) produced in intense mid-infrared laser fields. With systematic examinations on the dependences of coherent emissions on gas pressure as well as several laser parameters including laser intensity, polarization and wavelength of the pump laser pulses, we reveal that the multiple coherent emission lines generated in originate from a series of nonlinear processes beginning with four-wave mixing, followed with stimulated Raman scattering. Our analyses further show that the observed nonlinear processes are greatly enhanced at the resonant wavelengths, giving rise to high conversion efficiencies from the infrared pump laser pulses to the coherent emission lines near the transition wavelengths between the different vibrational energy levels of ground X and that of the excited B states.
A new method of molecular beam spectroscopy with the ultrahigh resolution is theoretically suggested. This method is based on the phenomenon of the coherent population trapping of molecular levels and allows the identification of the overlapping optical lines in complex spectra (typical for polyatomic molecules), even when frequency intervals between the centers of given lines are less than their natural line widths. The theoretical analysis is carried out on the basis of the Schrödinger equation for the three-level molecular A-system interacting with the two-frequency laser radiation. The conditions of the practical realization and possible applications of the suggested spectroscopy method are discussed.
We examine the suppression of 1+1 photodissociation or photoionization by laser fields. We find that atoms and molecules become more stable against photoionization or photodissociation when the intensity of the nonresonant laser field is increased above a limiting value for a two level plus continuum model system. We treat the ionization or dissociation dynamics analytically and discuss the conditions for optimum yields in a two-frequency square pulse laser field. We observe similar suppression against photodissociation for realistic sine-squared laser pulses. We demonstrate such a type of molecular suppression for 1+1 photodissociation of H2.
We present theoretical and experimental progress towards a new approach for the precision spectroscopy, coherent manipulation and state-to-state chemistry of single isolated molecular ions in the gas phase. Our method uses a molecular beam for creating packets of rotationally cold neutrals from which a single molecule is state-selectively ionized and trapped inside a radiofrequency ion trap. In addition to the molecular ion, a single co-trapped atomic ion is used to cool the molecular external degrees of freedom to the ground state of the trap and to detect the molecular state using state-selective coherent motional excitation from a modulated optical-dipole force acting on the molecule. We present a detailed discussion and theoretical characterization of the present approach. We simulate the molecular signal experimentally using a single atomic ion, indicating that different rovibronic molecular states can be resolved and individually detected with our method. The present approach for the coherent control and non-destructive detection of the quantum state of a single molecular ion opens up new perspectives for precision spectroscopies relevant for, e.g., tests of fundamental physical theories and the development of new types of clocks based on molecular vibrational transitions. It will also enable the observation and control of chemical reactions of single particles on the quantum level. While focusing on N2+ as a prototypical example in the present work, our method is applicable to a wide range of diatomic and polyatomic molecules.