Security Metrics for Nonlinear Optical Light Sources from Interferometric Field Reconstruction

Nonlinear optical light sources enable the generation of photons with quantum states that are intrinsically linked to underlying material dynamics, rather than imposed through external modulation. Here we investigate fundamental quantum communication metrics of four-wave-mixing signal fields generated by the two-dimensional perovskite (PEA)2PbI4. Using polarization-resolved interferometric measurements together with a microscopic nonlinear response model for the Bloch vector, we reconstruct effective single-photon polarization density matrices inferred from the experimental signal fields and evaluate the corresponding Holevo bound and effective secret-bit rates as a function of the coherence time, population time, and detection wavelength. We find that incorporating the coherence-time degree of freedom systematically lowers the Holevo bound by approximately 2.6-5.8% across the various excitonic resonances, indicating reduced distinguishability of the polarization states when the full multidimensional parameter space is sampled. To connect the polarization-state indistinguishability with experimentally achievable throughput, we further introduce an effective secret-bits-per-pulse metric that enables rapid evaluation of secure information throughput for candidate materials without requiring photon-number-resolved detection. For the present system, control of the population time via spin-dependent evolution yields substantially higher secret-bit rates than manipulation of the coherence time, while spectral regions associated with single-exciton and biexciton resonances define complementary operating regimes for secure communication. More broadly, this work positions nonlinear spectroscopy as a framework for exploring how emergent optical materials can generate and structure quantum states in ways that are advantageous for established quantum communication schemes.