Terahertz Time-Domain Spectroscopy as a Universal Defect Fingerprinting Tool for Organic Halide Perovskite Solar Cells

Abstract

Organic-inorganic hybrid perovskites (OHPs) deliver certified single-junction power conversion efficiencies (PCEs) exceeding 26% and perovskite-silicon tandem values surpassing 34%, yet a substantial gap with the Shockley-Queisser (S-Q) limit persists-primarily due to grain-boundary (GB) defects that drive non-radiative recombination, ion migration, and degradation. Rational passivation demands a non-contact tool capable of identifying and quantifying specific defect species in device-relevant thin films, a capability absent from conventional probes. This short review demonstrates that terahertz time-domain spectroscopy (THz-TDS, 0.3-3.0 THz) fulfills this role. Across four OHP compositions fabricated by sequential vacuum evaporation (SVE)-MAPbI3, MAPbBr3, FAPbI3, and CsPbI3-the THz spectral window captures both intrinsic phonon modes and GB-localized molecular defect vibrations, enabling species-specific, quantitative characterization at room temperature. Notably, the oscillator strength of the SVE-specific 1.58 THz absorption in MAPbI3 scales linearly with XPS-quantified CH3NH2 defect concentration, establishing THz-TDS as a direct, non-destructive defect meter. Building on these findings, we propose a three-pillar framework for THz-guided defect engineering: (I) quantitative defect measurement via oscillator-strength analysis, (II) material-specific fingerprint identification from a systematically constructed THz library, and (III) fingerprint-guided defect elimination with real-time feedback-together defining a closed-loop quality-control cycle that connects spectroscopic diagnosis to passivation strategy and, ultimately, to enhanced solar-cell efficiency.