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BACKGROUND: Photoablation in the infrared (IR) is an option for future refractive and corneal surgery; its basic principles have not yet been investigated systematically. For the first time, the free electron laser allows the dynamic study of photoablation over a wide range of wavelengths with variable combinations of pulselength and energy. The goal of this study is to use the free electron laser as a tool to describe photoablation in the IR quantitatively. We studied the function of wavelength as it is related to target material spectroscopy and the effects of corneal hydration and the pulse repetition rate. METHODS: Surface absorption spectroscopy of the human cornea and of gelatin as a proven model of the cornea was performed between 2.7 and 6.7 microns. Gelatin probes of well-defined thickness (140 +/- 5 microns) and controlled hydration (wet/dry weight 1 to 4.5) served as target material. Photoablation was performed with the Vanderbilt University free electron laser (Nashville, Tenn) in September 1992 at a fluence of 1.27 J/cm2, and a macropulse of 4 microseconds, composed of 2 ps micropulses at a 2.9 GHz pulse repetition rate. Wavelength was tunable between 2.7 and 6.7 microns at stable beam profiles. Ablation experiments were performed as a function of energy, hydration, and pulse repetition rate. Ablation rates were assessed by a) perforation experiments, and b) direct measurements using confocal laser topometry (UBM, Ettlingen, FRG). RESULTS: Ablation rate, assessed by perforation experiments and topometry, correlated well with the corresponding measured absorbencies of the target material: maximal ablation rate at maximal target absorption, around the 3- and 6-micrometer water absorption bands. The ablation threshold at 6.2 microns was 0.7 +/- 0.05 J/cm2 (perforation) and 0.55 +/- 0.08 J/cm2 for depth measurements. Ablation rate as a function of hydration increased to 2.3 (wet/dry weight) with a decrease for higher hydrations. Ablation rate as a function of the pulse repetition rate showed an increase of up to 20 Hz, where it was found to be 60% higher. CONCLUSION: The first systematic use of free electron laser technology positively correlated ablation efficiency with target material absorption, thus identifying a "new" promising wavelength at around 6.2 microns for materials with a high water content such as corneal tissue.