CO2 capture is considered as one of the most ideal strategies for solving the environmental issues and against global warming.Recently,experimental evidence has suggested that aluminum double bond(dialumene) species can capture CO2 and further convert it into value-added products.However,the catalytic application of these species is still in its infancy.Both the dynamics mechanism of CO2 fixation and the detailed structures of catalytic intermediates are not well understood.In this work,we investigate the structure dependent resonance Raman (RR) signals for different reaction intermediates.Ab-initio simulations of spontaneous resonance Raman (spRR) and time-domain stimulated resonance Raman (stRR) give spectral signatures correlated to the existence of different intermediates during the CO2-dialumene binding process.The unique Raman vibronic features contain rich structural information with high temporal resolution,enabling to monitor the transient catalytic intermediates under reaction conditions.Our work shows that RR can be used to monitor intermediates during the dialumene based CO2 capture reaction.The spectral features not only provide insight into the structural information of intermediate species,but also allow a deeper understanding of the dynamical details of this kind of catalytic process.