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The NAND chips are accessed in a page/block/sector fashion like a hard drive, their physical memory foot print is consequently very small. The size limitation would be the software you have to access the device. The biggest problem is the constant obsolescence of parts, so have a clear strategy for parts/footprints.
I can't speak to the SAM9X25 directly, but most of the 9xxx family have chip select windows of 256MB
If you need a lot of flash, consider using an SD/MMC device. With that 2GB (16Gb) should be no problem.
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