A nozzle configuration for technically premixed gas turbine flames was operated with CH₄ and air at atmospheric pressure. The flames were confined by a combustion chamber with large quartz windows, allowing the application of optical and laser diagnostics. In a distinct range of operating conditions the flames exhibited strong self-excited thermoacoustic pulsations at a frequency around 290 Hz. A flame with P=25 kW thermal power and an equivalence ratio of Φ=0.7 was chosen as a target flame in order to analyze the dynamics and the feedback mechanism of the periodic instability in detail. The velocity field was measured by three-component laser Doppler velocimetry, the flame structures were measured by chemiluminescence imaging and planar laser-induced fluorescence of OH, and the joint probability density functions of major species concentrations, mixture fraction, and temperature were measured by laser Raman scattering. All measuring techniques were applied in a phase-locked mode with respect to the phase angle of the periodic pulsation. In addition to the pulsating flame, a nonpulsating flame with increased fuel flow rate (P=30 kW, Φ=0.83) was studied for comparison. The measurements revealed significant differences between the structures of the pulsating and the nonpulsating (or “quiet”) flame. Effects of finite-rate chemistry and unmixedness were observed in both flames but were more pronounced in the pulsating flame. The phase-locked measurements revealed large variations of all measured quantities during an oscillation cycle. This yielded a clear picture of the sequence of events and allowed the feedback mechanism of the instability to be identified and described quantitatively. The data set presents a very good basis for the verification of numerical combustion simulations because the boundary conditions of the experiment were well-defined and the most important quantities were measured with a high accuracy.