harmonium UK /hɑːˈməʊ̯.niː.əm/US /hɑɹˈmoʊ̯.ni.əm/ noun2 •A small keyboard instrument that consists of a series of reed pipes, which sound when one of the keys is pressed to open a valve that allows air to pass through.The only other man was a little grey-headed fellow with a pleasant face and quick, twinkling eyes, who sat at a harmonium in the corner. — 1925 •Synonym of Hooke's atom. formsharmoniums