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1. Zombie S1
2. Nurse S1
3. Female Characters - pre-S11
4. Team GB
5. Costumed Characters - pre-S14
More recently, the assortments per case seem to be balanced - thus less price spike.
Bricklink is always a pretty good gauge for relative values when you cross-reference with the case assortments for each series. Lots of people sell the Hot Dog Guy at a higher price - even though there are more of him per case.
Althoufh Series 1 and Series 2 were particularly difficult to find in stores. I remember searching all over for them, but eventually found them all.
Glad I started collecting them from day one.
The simplest thing if you want to know demand / value is to look on bricklink at sold values and volumes.