I develop a theory that predicts a two-photon-induced molecular polar order in solid polymers at a temperature far below the glass transition temperature of the polymer. Phenomenologically, the rotational mobility of the chromophores is enhanced during a two-photon isomerization process, allowing for polar order to build up in the presence of a dc field that is applied across the solid polymer. No (or negligible) poling is possible in the absence of two-photon isomerization. Using the formalism of Legendre polynomials solves the general equations of the theory, and analytical solutions are derived for the early time evolution and the steady state of this two-photon poling process. The effects of the poling parameters are discussed, and it is shown that the twophoton poling efficiency can be as high as that achieved by dc field poling at elevated temperatures.
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