We have demonstrated that single crystals of a thiophene/phenylene co-oligomer ͓␣ , -bis-biphenyl-4-yl-terthiophene ͑BP3T͔͒ show interesting photonic aspects: ͑1͒ the self-waveguided amplified spontaneous light emissions with a comparable low threshold of 8 J/cm 2 to other optimized organic solid-state laser systems, and ͑2͒ the laser oscillation based on the optical self-confinement effect in the crystals. We have also presented electroluminescence from the crystals based on bipolar injection and the crystals' tolerance for intense current driving. These achievements strongly imply that BP3T crystals are a promising candidate for organic laser diodes. © 2005 American Institute of Physics. ͓DOI: 10.1063/1.2138361͔The achievement of long-lasting, bright electroluminescence with high efficiency in both polymeric 1 and lowmolecular-weight organic materials 2 has inspired the development of a new class of laser diodes ͑LDs͒. Within this development, optically induced solid-state organic lasers have been proposed and fabricated based on thin films by methods such as solution casting and vacuum deposition with a wide range of related organic semiconductors. [3][4][5][6][7] As a counterpart of these research streams, crystalline molecular materials also get much attention as promising candidates for organic LDs demanding high-density electric pumping for population inversion. Organic molecular single crystals exhibit superior charge-carrier transport properties to amorphous and polymeric organic semiconductors.8 This advantage is due to the inherent long-range structural ordering of these single crystals. Furthermore, there are several examples of stimulated emission, including amplified spontaneous emission 9-14 ͑ASE͒, from molecular single crystals. These excellent photonic and electronic features imply the possibility of current-injection lasing. However, chargeinjected luminescence from organic single crystals with high stimulated emission properties has not yet been reported. We have achieved optically induced laser oscillation and chargeinjected luminescence from a molecular single crystal. This breakthrough opens up a new research path toward developing organic LDs.The synthesis of a thiophene/phenylene co-oligomer, ␣ , -bis-biphenyl-terthiophene ͑BP3T͒ used can be seen in our previous work. 15 The procedures of the crystal growth were also described in detail elsewhere. 16 The charged pressure of the N 2 +H 2 ͑10 mol %͒ growth gas was −18.6 kPa ͑a differential pressure from the atmosphere͒ at room temperature. The temperature of the growth cylinder was maintained at 360°C at the material-loaded position ͑bottom͒ and 300°C at the growth position ͑top͒ during crystal growth ͑about 150 h͒. The melting temperature of BP3T is 388°C. The source materials of the crystals were highly purified by sublimation in advance. A N 2 -gas laser that generated a light pulse of 500 ps duration at 337 nm was used as an excitation light source for the gain-narrowing experiment. The detailed experimental setup was described in our p...