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It appears to have been after they met Strax. In "A Good Man Goes to War", which is when they met him, they were definitely a couple but Vastra didn't refer to Jenny as her wife. By the time of "The Snowmen" (about 4 years later, in their timelines), Vastra did describe Jenny as her wife.

Note that it's never been made clear whether they took part in any kind of formal wedding ceremony or whether they just started referring to each other as if they were married, without any formalities -- something which unmarried heterosexual couples have also been known to do.