Não, não é possível criar um instantâneo ao excluir arquivos ou diretórios. Veja o que o wiki do BTRFS diz:
A subvolume is like a directory - it has a name, there's nothing on it when it is created, and it can hold files and other directories. There's at least one subvolume in every Btrfs filesystem, the top-level subvolume.
As well as being like directories, subvolumes can be mounted independently of the rest of the filesystem. They are also the unit of snapshotting: you can make an atomic snapshot of a single subvolume, but not a whole tree of them; you can't make an atomic snapshot of anything smaller than a subvolume (like, say, a single directory). - https://btrfs.wiki.kernel.org/index.php/FAQ#Subvolumes