Radiative-dressed molecules:Ab initiotheory and single/multiphoton dissociation with electronic transitions

Molecules irradiated by intense laser fields become "dressed molecules" that possess significantly different properties due to changes in the electronic energy structures and wave functions. These new branches of distorted electron-field potential surfaces support different or new vibrational spectra. In this sense, a class of molecules is created with diagonal and off-diagonal properties that can be controlled by varying the laser intensity, frequency, and polarization. An ab initio theory that analyzes the dressed molecule with the field and their interaction treated as one dynamic system (rather than perturbatively) is formulated and summarized. The theory is applied to the study of single/multiphoton dissociation of molecules by intense lasers. Numerical results for the rate of $\mathrm{LiH}(X{}_{}{}^1{}_{}{}^{}\Sigma _{}^{+}{}_{}{}^{}, v=3)+4\mathrm{}\hslash \omega (\lambda =1.0648\mathrm{} \mu \mathrm{m}, \mathrm{YAlG}:{\mathrm{Nd}}^{3+})\to \mathrm{Li}\mathrm{}\left(2p\right)+\mathrm{H}\mathrm{}\left(1s\right)\mathrm{}$ via the repulsive state LiH(${\mathrm{B}}^1$II) are given. Subsequent fluorescence from $\mathrm{Li}\mathrm{}\left(2p\right)\mathrm{}$ can be detected experimentally.