A general technique for solving a system of rate equations describing the interaction of an electromagnetic field and a molecular system is presented. The method is used to obtain approximate time-dependent solutions for the upper-level populations of fluorescent dyes in the presence of a pump field.

Applied OpticsJan 15, 19793 citations

physica status solidi (b)

Fluorescence of molecular crystals at high levels of optical pumping

V. Kh. Brikenshteǐn, Viktor A. Benderskii, P. G. Filippov

Published May 1, 1983• 12 citations

Publisher

DOI: 10.1002/pssb.2221170102

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{\mathrm{H}}_{2}

gas. We obtained optical pumping efficiencies of about 96% into the first vibrational level of ${\mathrm{C}}_{2}^{\ensuremath{-}}$ and determined the absolute inelastic rate coefficient from

v=1

to 0 to be ${k}_{\mathrm{q}}=(3.2\ifmmode\pm\else\textpm\fi{}{0.2}_{\mathrm{stat}}\ifmmode\pm\else\textpm\fi{}{1.3}_{\mathrm{sys}})\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}13}\text{ }\text{ }{\mathrm{cm}}^{3}/\mathrm{s}$ at 20(3) K, over 3 orders of magnitude smaller than the capture limit. Reduced-dimensional quantum scattering calculations yield a small rate coefficient as well, but significantly larger than the experimental value. Using optical pumping and inelastic collisions, we also realized fluorescence imaging of negative molecular ions. Our work demonstrates high control of a cold ensemble of ${\mathrm{C}}_{2}^{\ensuremath{-}}$, providing a solid foundation for future work on laser cooling of molecular ions.