We meet her in The Enterprise Incident. She whispers her name to Spock, but we never learn what it is, so let your imaginations run wild.
She is particularly significant because she was the first Romulan woman we ever met, and she just happened to be a starship Captain AND apparently also the leader of a group of three Romulan ships, because the other Romulans who were commanding the other ships deferred to her.
Long story short: Kirk and Spock perpetrate a big fraud for espionage purposes, and this lady is pranked by them, big time! Kirk pretends to be crazy, and Spock pretends to be a traitor who actually thinks this lady is sexy. She tries to seduce him, he tries to seduce her back, and we really have no way of knowing how sincere either one of them is until the end, when we learn that OF COURSE Spock was not sincere, but she was, kinda.
She didn't just tempt Spock with her womanly wiles, she offered him power, freedom and prestige as a Captain/commander of a Romulan ship of his own. Apparently it was within her power to grant such things, which is saying a lot.
While Spock was keeping her distracted, Kirk steals the Romulan cloaking device. Just as Spock is beaming back to the ship, she grabs onto him and is beamed back with him.
She is OF COURSE taken into custody, but not before ordering her guys to destroy the Enterprise, which shows she was willing to die if need be to keep the Federation from getting the device. BTW, that means she was willing to order her men to kill Spock and everybody else aboard the Enterprise, too, so don't harbor too many romantic ideas about her feelings about Spock the spy.
Once taken, she was treated with great respect by Kirk. She was not secured in the brig like a criminal, but was offered quarters of her own, as if she were an ambassador.
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