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Well, the harpsichord, but I'm not sure you are lumping keyboard instruments together. (Love those smaller keys! Maybe like Chopin's Pleyel.) To me Les Barricades Mysterieuses sounds mushy on a piano. But if I were choosing a completely different instrument, the Renaissance lute would win hands down.
UPDATE: When Magdalena Stern-Baczewska plays Les Barricades on the piano, it does not sound mushy.
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I think I would choose voice. I grew up in a family of wonderful singers, and while my voice is not great, I am moved by beautiful a cappella singing more often than by any other "instrument." Indeed, I have had trouble connecting to the piano. The instruments I played previously (trombone and double bass) were quite physical in what you have to do to play them. I miss that, and sometimes when I play the piano it somehow feels like I'm not really 'making music.' Just a few weeks ago, though, I finally found a musical/physical connection to the piano, and it was through voice. Learning a new piece with my teacher, he asked that I sing one line in solfege while playing the other line, Practicing this, I suddenly found myself "feeling" the music. So, I'd really love to learn how to sing better both because singers impress me with their abilities and so that I can continue to feel a connection to the music I am playing.
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I have two instruments I would like to learn. I played the flute in high school though I never had a teacher. Now I would like to actually have a teacher.
The other instrument I would like to learn is violin. I had a semester of violin in college, but would really like to expand my ability to play the instrument. Though I don't currently have either instrument, it's a desire I have, and will pursue it when I have the opportunity.
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I play a few instruments (piano, cello, guitar, started singing in the past year), and I wish I could learn more, but at some point I've had to cut myself off from picking up new ones so I can get things done with the ones I have.
That said, if time and resources were infinite, I would love to learn both the oboe and english horn (which as I understand are fairly similar, so most oboists can easily pick up the other). I just love the expressive, lyrical, somber quality of those instruments.
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I would love to play the Uillian Pipes. I love the music of the Chieftains and other Gaelic groups. The pipes are crucial instruments for the expression of Gaelic music. They are much softer than the Scottish bagpipes, which give me tinnitus, and not an instrument of war. The sound is ancient, and can quickly change from a rhythmic jig to a mournful farewell. It can be played without ear damage in small areas, such as the gatherings of ‘kitchen parties’ in Nova Scotia or the Ceilidh get-together in Ireland and Celtic areas of Brittany, etc.