Two-photon excitation (TPE) of the photocycle of bacteriorhodopsin (BR
) with 1064 nm pulses was observed, and the subsequent transient absor
ption and linear dichroism changes measured at 568 nm. An anisotropy o
f 0.55 was induced in the ground-state transition of BR. A theoretical
formalism is described to treat the isotropic and anisotropic compone
nt of the two-photon absorptivity measured by a secondary transition d
ipole that is induced by TPE and probed by polarized fluorescence or t
ransient-absorption methods. The two-photon tensor for BR is found to
contain components that are not parallel to the one-photon transition
dipole.