the requirements listed above, is two-line atomic fluorescence (TLAF) [4][5][6]. TLAF is a laser-based ratiometric technique, in which the temperature-dependent population of two lower lying electronic states, of a seeded atom, is probed by laser excitation and the ratio of the resulting fluorescence is correlated with the temperature of the gas. TLAF offers several beneficial features for temperature measurements in reactive flows. Firstly, no a priori knowledge of the combustion environment is necessary as the technique is independent of quenching due to the excitation to a common upper state [7]. Secondly, the use of an atomic species as temperature marker offers advantages such as providing high transition probabilities yielding strong fluorescence signals as well as being free from errors related to vibrational and rotational energy transfer existing in molecules [8,9]. Thirdly, TLAF also has the possibility for thermometry measurements in sooting and particulate-laden flames as the detection wavelength can be shifted from the excitation wavelength [10,11]. The disadvantage of TLAF is that an atomic species, not normally present in the flame, has to be introduced which may add complexities to the experimental set-up.Two-line atomic fluorescence has been developed in steps where the first theoretical ground work was conducted by Alkemade [7] and experimentally demonstrated shortly thereafter using atomic lamps [12,13]. With the advent of suitable lasers, TLAF became a tool for temperature measurements with imaging capabilities in non-steady environments [4,10,11,[14][15][16]. Recently, TLAF measurement has been extended from the linear regime to non-linear regime by Medwell et al. [4] and to the saturation regime by Manteghi et al. [14] in an attempt to maximize the fluorescence signal for instantaneous temperature measurements. With the improvement in regards to available power and wavelengths of diode lasers, TLAF measurements using diode lasers have been shown to give accurate temperatures in both low-pressure and atmospheric Abstract A robust and relatively compact calibration-free thermometric technique using diode lasers two-line atomic fluorescence (TLAF) for reactive flows at atmospheric pressures is investigated. TLAF temperature measurements were conducted using indium and, for the first time, gallium atoms as temperature markers. The temperature was measured in a multi-jet burner running methane/air flames providing variable temperatures ranging from 1600 to 2000 K. Indium and gallium were found to provide a similar accuracy of ~ 2.7% and precision of ~ 1% over the measured temperature range. The reliability of the TLAF thermometry was further tested by performing simultaneous rotational CARS measurements in the same experiments.