Two-photon absorption measurement has been carried out in a single 80 nmϫ 10 m ZnO nanowire using femtosecond laser pulses in the wavelength range of 700-800 nm. In addition to the deep-level green emission around 530 nm due to surface defects and the near band-edge ultraviolet emission around 360 nm due to the exciton, a second harmonic peak has been observed. The strength of the frequency-doubled component is found to enhance while the two-photon absorption wavelength is tuned towards the exciton wavelength of the nanowire. This behavior can be ascribed to the resonant exciton absorption in ZnO nanowires. © 2006 American Institute of Physics. ͓DOI: 10.1063/1.2200230͔Semiconductor nanocrystals have attracted much interest due to their fundamental importance in bridging the gap between bulk matter and molecular species. Zinc oxide is a remarkable II-VI semiconductor with potential applications owing to its diverse properties. 1 The combination of high excitonic and biexcitonic oscillator strength and good high temperature characteristics make ZnO a promising material for optical applications. 2 It has been used as a visible and ultraviolet photoconductor and as fluorescent material, apart from its usefulness in optical waveguides, acousto-optic devices, thin film transistors, etc. 3,4 Its wide band gap of 3.37 eV at room temperature makes ZnO suitable for shortwavelength optoelectronic devices, including light-emitting diodes ͑LEDs͒ and laser diodes ͑LDs͒. ZnO has a high exciton binding energy of 60 meV, which renders it more applicable for making room-temperature UV laser devices. 5 Small-diameter ZnO nanowires are expected to further lower the lasing threshold because quantum effects result in enhancement of density of states near the band edges and radiative recombination due to carrier confinement. The high exciton binding energy of ZnO at room temperature makes it a promising material for polariton lasers. 6-8 Among nanomaterials, a nanowire has the additional advantage of propagating these photon-exciton pairs due to better optical and carrier confinement. 9,10 However, the possibility of generating exciton-photon pairs by two-photon absorption process is not yet reported in ZnO nanowire. The goal of our research is to investigate the prospect to generate polariton modes that has huge importance for quantum optics and optical information transfer in photonic circuits. High optical nonlinearity due to the unequal atomic size of Zn and O is reported by Levine. 11 The acentrically located bond charge contributes a homopolar energy gap. Since nonlinear susceptibility is more sensitive to the crystal potentials, ZnO is found to be highly nonlinear. This high optical nonlinearity produces second harmonic photon, while the two-photon absorption creates excitons in ZnO nanowire. By tuning the second harmonic photon energy towards the exciton resonance, an enhancement in second harmonic generation ͑SHG͒ is revealed in the present investigation.The II-VI semiconductors are efficient second harmonic generators sin...