Two-dimensional correlation analysis for x-ray photoelectron spectroscopy

X-ray photoelectron spectroscopy (XPS) measures the binding energy of core-level electrons, which are well-localised to specific atomic sites in a molecular system, providing valuable information on the local chemical environment. The technique relies on measuring the photoelectron spectrum upon x-ray photoionisation, and the resolution is often limited by the bandwidth of the ionising x-ray pulse. This is particularly problematic for time-resolved XPS, where the desired time resolution enforces a fundamental lower limit on the bandwidth of the x-ray source. In this work, we report a novel correlation analysis which exploits the correlation between the x-ray and photoelectron spectra to improve the resolution of XPS measurements. We show that with this correlation-based spectral-domain ghost imaging method we can achieve sub-bandwidth resolution in XPS measurements. This analysis method enables XPS for sources with large bandwidth or spectral jitter, previously considered unfeasible for XPS measurements.

Automated summary

X-ray photoelectron spectroscopy (XPS) measures the binding energy of core-level electrons, providing information on the local chemical environment in a molecular system. The technique's resolution is often limited by the bandwidth of the ionising x-ray pulse, problematic for time-resolved XPS. A novel correlation analysis method is presented in this work, exploiting the correlation between x-ray and photoelectron spectra to improve resolution in XPS measurements.