Triton-fractionated photosystem-I particles poised at -625 mV, where the two bound iron-sulfur proteins are reduced, have been studied by optical and electron paramagnetic resonance spectroscopies from 293 to 5 K. At 5-9 K, these particles exhibit two decay components with lifetimes of 1.3 and 130 msec in the laser pulse-induced absorption and electron paramagnetic resonance signal changes. Spectral properties of the 130-msec decay component reflect the charge separation between P-700 and some iron-sulfur center having a broad optical absorbance in the 400- to 550-nm region and a previously reported electron paramagnetic resonance signal with g = 1.78, 1.88, and 2.08. Spectral properties of the 1-msec decay component indicate photoinduced charge separation between P-700 and a chlorophyll a dimer having absorption bands at 420, 450, and 700 nm. It is assumed that these two acceptors participate in the electron transfer from P-700(*) to the bound iron-sulfur proteins.