We microstructured silicon surfaces with femtosecond laser irradiation in the presence of SF6. These surfaces display strong absorption of infrared radiation at energies below the band gap of crystalline silicon. We report the dependence of this below-band gap absorption on microstructuring conditions (laser fluence, number of laser pulses, and background pressure of SF6) along with structural and chemical characterization of the material. Significant amounts of sulfur are incorporated into the silicon over a wide range of microstructuring conditions; the sulfur is embedded in a disordered nanocrystalline layer less than 1 mm thick that covers the microstructures. The most likely mechanism for the below-band gap absorption is the formation of a band of sulfur impurity states overlapping the silicon band edge, reducing the band gap from 1.1 eV to approximately 0.4 eV.