摘要： An instrument combining laser-induced breakdown spectroscopy (LIBS) and Raman spectroscopy was developed for the in situ atomic and molecular composition analysis of minerals. The apparatus consists of an optical system, a sample chamber, a spectrometer for Raman and another for LIBS, as well as a control system equipped with laboratory-written software. Gypsum, calcite, prehnite, pearl, lazurite, and several mixtures of NaBr and CaCO3 were selected as samples for evaluation of the performance of the instrument. Sulfate, carbonate, silicate, and crystalline water were identified and different structures of CaCO3 were clearly distinguished by the use of a Gaussian fit. The limit of detection for CaCO3 in a NaBr mixture was 5.7 mg/g by Raman. LIBS was employed to determine calcium, magnesium, iron, sodium, aluminum, and carbon with the newly developed system. The limits of detection obtained for Ca, Na, and C were 90.2 lg/g, 84.6 lg/g, and 2.5 mg/g, respectively. The experimental results from commercial Raman spectroscopy instruments were used to verify and support the measurements from this novel instrument.