The infiltration of three-dimensional opal structures has been investigated by atomic layer deposition. Demonstrations using ZnS:Mn show that filling fractions Ͼ95% can be achieved and that the infiltrated material is of high-quality crystalline material as assessed by photoluminescence measurements. These results demonstrate a flexible and practical pathway to attaining high-performance photonic crystal structures and optical microcavities. © 2003 American Institute of Physics. ͓DOI: 10.1063/1.1609240͔The work of John 1 and Yablonovitch 2 in the late 1980's has resulted in an extensive interest in the fabrication of photonic crystals. Numerous methods have been employed to make such structures 3-6 and a complete photonic band gap has been demonstrated in millimeter 3 and infrared 4,6 wavelengths. The requirements for a complete photonic band gap include: high refractive index contrast (Ͼ2.8), long-range three-dimensional periodicity, and a high filling fraction. Many groups have shown that the infiltration of opals is a suitable route for obtaining the desired periodic structure. [6][7][8][9][10] Most of these studies have involved variations of chemical bath deposition and report low filling fractions. The exceptions have been ZnS, 11 which has been incorporated with approximately 50% filling of the interstitial volume and CdS, 12 with filling fractions as high as 96%. However, this technique tends to produce many nanocrystallites such that the luminescent properties are very poor and usually the resulting structures exhibit low filling fractions due to high porosity. Also, chemical vapor deposition has been used for infiltration exhibiting filling fractions ranging from 1% to 100%, with the highest numbers being for silicon which is not a luminescent material. [6][7][8][9] In this letter, we report a method of fabricating inverse opal films that utilizes atomic layer deposition ͑ALD͒ for the infiltration step. ALD is a growth technique that utilizes the sequential application of reactants coupled with substrate temperature optimization to achieve monolayer-bymonolayer growth. 13 As a result, growth is surface controlled instead of source controlled, enabling highly controllable deposition of conformal films on substrates with complex geometries, 14 such as opals.For this study colloidal silica solutions containing monodispersed spheres, 145-500 nm in diameter, were formed by the Stober method. 15 Self-assembled face centered cubic silica opal templates were then formed on silica or silicon substrates by the sedimentation of monodispersed colloidal silica in confinement cells as pioneered by Park et al., 16 and then dried and sintered (700-800°C for 2 h͒ to enhance structural stability, and to provide interconnectivity between the spheres. The interstitial volume of the opal was next filled with ZnS:Mn using conventional ALD precursors. Etching the infiltrated films in a 2% HF solution resulted in the removal of the silica spheres, and the formation of structurally stable inverse opals. The films were characte...