Abstract
The probability of direct excitation of excitonic molecule in the two-pho- ton absorption process is calculated with an Hylleraas-Ore type biexciton envelope, which is variationally optimized. In the second order of perturba- tion, because of the resonance effect, only the exciton .r5 intermediate state is taken into account. The band structure at band extrema due to spin—orbit interaction is assumed. The transition probability of two-photon absorption is expressed by matrix element between the free exciton and the biexciton envelopes. The obtained probability of two-photon absorption in CuCl is about three orders of magnitude smaller when compared to that obtained by Hauamura.
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