Publication date: 22nd July 2026
Lead halide perovskites (LHP) are promising materials for direct hard radiation detection, a field that requires high-quality crystals. Among them CsPbBr3, a stable material containing heavy Cs+ cation, shows the best electronic performance when grown from the melt by the Bridgman-Stockbarger technique. While phase purity of the crystalline CsPbBr3 ingots is often confirmed by X-ray diffraction, quality assessment relies on optical microscopy and eventually device performance – a costly, iterative and irreversible process that requires full device fabrication. Furthermore, the orthorhombic crystal structure of CsPbBr3 at room temperature, with distinct lattice parameters, makes reliable determination of crystallographic alignment in melt-grown crystals particularly important, yet remains challenging. To address these limitations, we establish nuclear quadrupole resonance (NQR) spectroscopy as a versatile, non-invasive technique for evaluating the quality of melt grown CsPbBr3 ingots prior to the first device fabrication step. We demonstrate that, beyond probing the local environment around a quadrupolar nucleus, NQR spectroscopy is inherently sensitive to crystallinity and crystal orientation. We correlate key spectroscopic descriptors, such as linewidth and integral, with macroscopic and microscopic structural features, to establish a robust evaluation of the crystal orientation and quality for a guided sample selection. Decreasing crystallite-domain size leads to the pronounced broadening of the observed NQR signal, with the full width half maximum differing by up to 70 kHz between pristine melt-grown crystals and polycrystalline powder. We further support the experimental results by ab initio calculations of bromine NQR frequency distributions, which capture the effect of structural disorder on the NQR signal. Customized resonators allowed us to accommodate large ingots directly within the quartz ampules used for growth and enabled semiautomated spatial mapping of the spectroscopic descriptors across the ingots. We show that the removal of the impurities collected near the top of the ingot and subsequent recrystallization improve the homogeneity and overall crystallinity of the samples, highlighting the need for multiple purification steps. We also observed reorientation in crystal-domain alignment along the ingot which is preserved after cutting and polishing. Our findings deepen the understanding of both applied NQR spectroscopy and melt-growth processes of lead halide perovskites, paving the way for integrated quality control and innovative in situ applications.
