The ultrafast photocarrier dynamics in polysilane alloys, amorphous (SiH2)n, has been studied using the picosecond photoinduced absorption (PA) technique. For excitation below the optical gap, the PA response decays exponentially and is faster at low temperatures. This is interpreted in terms ofe‐hgeminate recombination in the small clusters (∼10 A˚) ofa‐Si:H embedded in the polysilane matrix. The PA response with above‐gap excitation is similar to that of conventionala‐Si:H; it decays much slower in the form of a power lawt−&bgr;(&bgr;<1), independent of spectral range between 1.4 and 2.2 eV. This shows that thee‐hdistance after above‐gap photogeneration is larger than the size of thea‐Si:H clusters.