Abstract
High-throughput experimentation can evaluate many reaction conditions, yet combinatorial condition spaces still exceed the available experiment budget. This makes experiment selection a sequential decision problem: each new condition must be chosen from limited observations before its outcome is known. LLMs can express task-specific selection logic. A direct recommendation, however, is neither a persistent executable object that can be validated and revised nor an independently auditable decision rule. We introduce CARE, a reference-conditioned controller that separates program synthesis from experiment selection. An LLM writes an executable scoring program that ranks the remaining conditions, while a non-LLM reference policy supplies a numerical candidate and support summary. CARE forms an optional alternative from the program, applies a reference-conditioned intervention gate to compare it with the reference, and records the decision before the selected outcome is revealed. Each new outcome updates controller state and can trigger retention, revision, or regeneration of the active program. This outcome-guided program evolution changes the scoring logic without updating the LLM parameters. In matched offline replay with 30 seeds on eight reaction-optimization tasks, CARE attains the lowest normalized regret, the highest normalized best-so-far AUC, and the highest Top-1% Success@15 among the evaluated methods. These results support using a scoring program written by an LLM as one component of a reference-conditioned optimizer rather than as a standalone experiment selector.