Large language models (LLMs) hold potential for innovative HCI research, including the creation of synthetic personae. However, their black-box nature and propensity for hallucinations pose challenges. To address these limitations, this position paper advocates for using LLMs as data augmentation systems rather than zero-shot generators. We further propose the development of robust cognitive and memory frameworks to guide LLM responses. Initial explorations suggest that data enrichment, episodic memory, and self-reflection techniques can improve the reliability of synthetic personae and open up new avenues for HCI research.