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The field of vibrational polariton chemistry was firmly established in 2016when a chemical reaction rate at room temperature was modified within aresonantly tuned infrared cavity without externally driving the system. Despiteintense efforts by scientists around the world to understand why the reactionrate changes, no convincing theoretical explanation exists. In thisperspective, first, we briefly review this seminal experiment, as well asrelevant experiments that have since followed that have hinted at the roles ofreactant concentration, cavity frequency, and symmetry. Then, we analyze therelevance of leading theories, such as quantum electrodynamics-modifiedtransition rate theories, the photonic solvent cage effect, the impact ofdissipation from dark states, bond strengthening via intramolecular vibrationalenergy redistribution, and collectively enhanced local molecular properties.Finally, we construct a roadmap toward the theory of vibrational polaritonchemistry by suggesting experiments to test theories and new paths fortheorists. We believe that understanding the importance of the onset of thestrong coupling regime, designing experiments to capture changes in reactionpathways, and further developing the theories of cavity-modified intramolecularvibrational energy redistribution and collectively enhanced local molecularproperties are crucial next steps. We hope this perspective will be a valuableresource for guiding research in the field of vibrational polariton chemistry.

A roadmap toward the theory of vibrational polariton chemistry