Sim, em ambos os casos. (Spoilers for post-GoF)
Maldição Cruciatus
A maldição Cruciatus é usada por Harry em Bellatrix Lestrange, enquanto ela foge do Departamento de Mistérios em Ordem da Fênix :
Hatred rose in Harry such as he had never known before; he flung himself out from behind the fountain and bellowed, “Crucio!”
Bellatrix screamed: the spell had knocked her off her feet, but she did not writhe and shriek with pain as Neville had - she was already back on her feet, breathless, no longer laughing. Harry dodged behind the golden fountain again. Her counter-spell hit the head of the handsome wizard, which was blown off and landed twenty feet away, gouging long scratches into the wooden floor.
“Never used an Unforgivable Curse before, have you, boy?” she yelled. She had abandoned her baby voice now. “You need to mean them, Potter! You need to really want to cause pain – to enjoy it – righteous anger won’t hurt me for long – I’ll show you how it is done, shall I? I’ll give you a lesson—”
Isso é depois que Bellatrix matou Sirius, o único membro restante da família de Harry, então ele está compreensivelmente zangado.
Se isso não conta, então o Bellatrix também o usa no Neville na mesma luta:
Bellatrix raised her wand. “Crucio!”
Neville screamed, his legs drawn up to his chest so that the Death Eater holding him was momentarily holding him off the ground. The Death Eater dropped him and he fell to the floor, twitching and screaming in agony.
Maldição Imperius
A maldição Imperius é usada (também por Harry) quando o trio invade o banco Gringotts. Na época, um dos goblins está prestes a explodir sua capa, então Harry precisa impedi-lo de fazer isso. (Neste ponto, o trio foi marcado criminosos, e disfarçado.)
Harry raised the hawthorn wand beneath the cloak, pointed it at the old goblin, and whispered, for the first time in his life, “Imperio!”
A curious sensation shot down Harry’s arm, a feeling of tingling warmth that seemed to flow from his mind, down the sinews and veins connecting him to the wand and the curse it had just cast.
Existem muitos outros casos em que as maldições são usadas ao longo dos livros (e filmes), mas esperamos que os dois exemplos acima sejam suficientes para mostrar que sim, todas as três maldições foram usadas.