GPT4All is fine-tuned on synthetic instruction data extracted from OpenAI's GPT-3.5-Turbo model, whereas OpenAssistant is mainly fine-tuned on data gathered from responses written by real human volunteers. It remains to be seen whether synthetic training data can achieve results comparable to responses written by living humans, but the OpenAssistant project is testing the theory that finetuning on responses written by living humans may give language models a degree of alignment and creativity which may not be possible to replicate as effectively with data scraped purely from an existing instruct-tuned large language model.
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