Visible room-temperature photoluminescence (PL) was observed from hydrogen-free nanostructured amorphous carbon films deposited by pulsed laser ablation in different background pressures of argon ͑P Ar ͒. By varying P Ar from 5 to 340 mTorr, the film morphology changed from smooth to rough and at the highest pressures, low-density filamentary growth was observed. Over the same pressure regime an increase in the ordering of sp 2 bonded C content was observed using visible Raman spectroscopy. The pulsed laser ablation (PLA) of graphite, in vacuum, has typically been used to produce smooth, hard, high density amorphous carbon (a-C) films with high sp 3 content (up to 90%) 2,3 due to the local densification, on the impact of high energy C atoms/ions, favoring the formation of the sp 3 phase. The optical properties of carbon films are largely governed by the sp 2 phase, with the tribological properties determined by the sp 3 phase. However, in these nanocomposite materials, some care must be exercised in extracting and interpretation of the Tauc band gap and the Urbach energy.Photoluminescence (PL) in amorphous carbon, is thought to occur due to the radiative recombination of electrons and holes in the band-tail states created by sp 2 rich clusters.4,5 PL has been extensively studied for polymeric a-C:H films, 4,6,7 where an increase in the PL intensity has been observed for increasing H content.7 In this letter we investigate the PL properties of hydrogen-free a-C films deposited by PLA of graphite in background pressures of argon. Unlike in vacuum, these conditions have been shown to produce low density nanostructured amorphous carbon (NAC) films. 8,9 Such films have been shown to have useful properties including low thresholds for electron emission 10 and high porosities. Films were deposited by PLA of a 99.999% pure pyrolytic graphite target (Kurt J. Lesker) using a Lambda-Physik LPX 210i excimer laser operating at 248 nm. The laser pulse was focused onto the rotating target, producing a fluence of ϳ6 J/cm 2 . The growth chamber was evacuated using a turbomolecular pump to 9 ϫ 10 −8 Torr, then backfilled with argon to the required pressure. Films were deposited onto Si substrates at a range of different background pressures of argon ͑P Ar ͒ from 5 to 340 mTorr. The target to substrate distance was fixed at 6 cm. Between 2000 and 5000 laser shots were used, depending on the background pressure in order to keep the film thickness constant as it was affected by P Ar .The morphology of the films was investigated in a Hitachi S4000 field emission gun scanning electron microscope (SEM). The structure and bonding configuration in the films was investigated by visible Raman spectroscopy (Renishaw Ramanscope) using two different laser wavelengths 488 and 514 nm. The PL measurements were also performed using the system with the 488 nm laser, which was also equipped with a cryostat (Oxford Instruments) that allowed measurements at substrate temperatures down to 6 K.After deposition the surface morphology of the films was ex...