Out of their earlier (pre-Soft Bulletin) material, I'd recommend:
Clouds Taste Metallic
Basically where the 'modern' Flaming Lips sound begins. Still traces of their Garage/Indie sound of earlier albums, but much more melodic, varied and 'widescreen' than before. Basically a more lo-fi Soft Bulletin, and my personal favourite of theirs.
Zaireeka
A real bitch to listen to properly (comes in 4 discs that need to be played simultaneously) - or you can do what I did and use a music program to merge the 4 discs together. This came out before Soft Bulletin, but in terms of sound it fits more accurately between SB and Yoshimi. Another excellent album.
In terms of pre-Clouds Taste Metallic material, there isn't a massive difference between many of the albums (although they're still all decent). They sound very much like Pixies on these albums, though never as brilliant as Pixies. Of these albums, I'd say feel free to choose between:
Hit To Death In The Future Head
Transmissions From The Satellite Heart
In A Priest Driven Ambulance
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