Xiaorui Ma, Xu Huang, Ying Guo, Zhili Jia, Shuo Jia
Lapis lazuli is a valued gemstone that displays a wide spectrum of blue hues, yet the quantitative link between its color and internal sulfur speciation remains unresolved. This study integrates colorimetry with electron probe microanalysis and UV-Vis, Raman, and X-ray photoelectron spectroscopy to establish this relationship and build a robust grading framework within the CIE 1976 L*a*b* color space. X-ray diffraction was employed to determine the mineral composition and confirm that the chromogenic elements originated from lazurite. K-means clustering with Fisher’s discriminant validation classifies samples into four grades: Fancy Blue, Fancy Intense Blue, Fancy Deep Blue, and Fancy Dark Blue. Multimodal analyses identify three sulfur species—[S3]·−, S2−, and SO42−—and show that higher sulfur content correlates with lower lightness, reduced chroma, and a violetish-blue shift. [S3]·− is confirmed as the dominant chromophore, producing the strong 600 nm absorption that defines the blue hue. A weak absorption band observed near 400 nm in some samples can be attributed to S2− and SO42− species, but no visually perceptible effect of this band on the overall color was detected.