A 532 nm‐excited resonance hyper‐Raman (HR) spectrum of deoxythymidine is reported. The 532 nm excitation satisfies the two‐photon resonance condition to the ππ* absorption band of the pyrimidine ring at 250–280 nm, and hence we recorded the resonance HR spectrum with high signal‐to‐noise ratio. The resonance HR spectrum of deoxythymidine is compared with its 266 nm‐excited resonance Raman spectrum. The remarkable similarity between these spectra indicates that the single electronic structure contributes to the resonance effect in each case. The peak assignment is given for the RHR bands by analogy with that for the resonance Raman spectrum. This study offers the fundamental information to study DNA using the HR spectroscopy.
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