(a) Reaction paths for BO-MD and rt-TDDFT. Both simulations have proton bonding to ⋆CO to make the reaction successful (thus rt-TDDFT has a higher initial velocity than BO-MD). (b) Measured change of total charge counted above the plane. This horizontal plane has its z-value in the middle, between C and the top Cu layer. Here, simulation- “TDDFT reaction fail” has the same initial velocity to “BO-MD reaction successful,” while “TDDFT reaction successful” has higher initial velocity than “BO-MD reaction successful.” (c) Eigen-energy of the adiabatic states for “BO-MD reaction successful” and “TDDFT reaction successful.” The bottom isosurface is the state I charge density difference between BO-MD and rt-TDDFT at t = 20 fs (charge density at the “red” dot minus the “blue” dot). In the isosurface, yellow indicates positive and blue indicates negative.