Depending where you are in the world, I think the ones you have that fit your criteria of ‘unusual, uncommon, but easy to pronounce and spell’ are [name_u]Romy[/name_u] and [name_f]Astrid[/name_f]–they’re lovely with [name_f]Luna[/name_f]!
[name_f]Rainey[/name_f] and [name_f]Lainey[/name_f] will both have spelling and mis-hearing challenges ([name_u]Rainy[/name_u], [name_u]Reign[/name_u], [name_f]Reina[/name_f]; [name_f]Leni[/name_f], [name_u]Laney[/name_u], [name_u]Lanie[/name_u], [name_f]Alayna[/name_f], [name_f]Elaine[/name_f]), plus [name_f]Luna[/name_f] and [name_f]Lainey[/name_f] are very close for sisters!
[name_f]Aurora[/name_f] gives you an astronomical theme, and [name_f]Aurora[/name_f] is similar in popularity to [name_f]Luna[/name_f]. It’s a really good match, with a clear theme of Latin words for things in the night sky. Have you considered what you might call a third child in that case, though? Does that matter to you? If it were me, I’d feel like I’d absolutely have to call a third daughter [name_f]Stella[/name_f] so she didn’t feel left out!
[name_f]Asta[/name_f] fits your criteria for uncommon and unusual, though it’s so uncommon in English that you might have some trouble with it–misheard for [name_f]Aster[/name_f], or with her sister’s name, for [name_f]Astra[/name_f].
[name_m]How[/name_m] do you feel about the popularity of [name_f]Luna[/name_f]? It’s #37 in the USA and #78 in the UK–is it more popular than you’d like for her sister? [name_m]Just[/name_m] about right?
If you like where [name_f]Luna[/name_f] sits in terms of its popularity (assuming that you’re in the US!):
[name_f]Maya[/name_f], [name_f]Cora[/name_f], [name_f]Zoe[/name_f], [name_f]Nova[/name_f], [name_f]Daisy[/name_f], [name_f]Athena[/name_f], [name_f]Fiona[/name_f], [name_u]Eden[/name_u], [name_f]Amara[/name_f], [name_f]Iris[/name_f]
If you’d like the name to be rarer than [name_f]Luna[/name_f], and more like [name_f]Astrid[/name_f] (US numbers):
[name_f]Freya[/name_f], [name_f]Eve[/name_f], [name_u]Winter[/name_u], [name_f]Esme[/name_f], [name_f]Liv[/name_f], [name_f]Lyra[/name_f], [name_f]Poppy[/name_f], [name_f]Nola[/name_f], [name_f]Mavis[/name_f], [name_f]Opal[/name_f], [name_f]Etta[/name_f], [name_u]Zola[/name_u], [name_f]Flora[/name_f], [name_f]Elodie[/name_f],
If you’d like the name to be very rare, like [name_u]Romy[/name_u] and [name_f]Asta[/name_f] (US numbers):
[name_f]Cleo[/name_f], [name_u]Vida[/name_u], [name_f]Coral[/name_f], [name_f]Honor[/name_f], [name_f]Arwen[/name_f], [name_u]Ever[/name_u], [name_f]Fern[/name_f], [name_f]Amada[/name_f], [name_f]Saskia[/name_f], [name_f]Avis[/name_f], [name_f]Merrin[/name_f], [name_f]Finola[/name_f], [name_u]Seren[/name_u], [name_f]Nell[/name_f]