Direct air capture of CO\(_2\) remains bottlenecked by the thermal energy required to regenerate conventional sorbents, with regeneration heat accounting for a substantial share of operating costs in commercial systems. Stimulus-responsive materials that adsorb and release CO\(_2\) in response to light or an applied electric field offer a route to lower energy capture cycles by replacing continuous thermal swing with targeted, switchable surface chemistry. In this talk, I will present our computational and experimental program to identify and validate transition-metal materials that exhibit this switchable behavior. Using charge and field-controlled density functional theory (DFT), we screen pure metals and intermetallic alloys for surfaces that bind CO\(_2\) strongly in one electronic or field state and release it readily in another, identifying candidates such as Cu, Zn, and Fe-Co and Fe-Ni alloys with reversible, field-tunable adsorption-desorption behavior. On the experimental side, we built a custom photothermal reactor and benchmarked light-driven desorption against conventional thermal regeneration, demonstrating that solar-selective coatings and direct illumination can drive comparable CO\(_2\) release without continuous heating. We also report complementary results on metal foams as a platform for stimulus-responsive capture. Together, these results outline a materials design pathway toward reproducible, lower-energy CO\(_2\) capture and regeneration.