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The Infrared Absorption Band and Vibronic Structure of the Nitrogen-Vacancy Center in Diamond

Negatively-charged nitrogen-vacancy (NV$^-$) color centers in diamond have generated much interest for use in quantum technology. Despite the progress made in developing their applications, many questions about the basic properties of NV$^-$ centers remain unresolved. Understanding these properties can validate theoretical models of NV$^-$, improve their use in applications, and support their development into competitive quantum devices. In particular, knowledge of the phonon modes of the $^1A_1$ electronic state is key for understanding the optical pumping process. Using pump-probe spectroscopy, we measured the phonon sideband of the ${^1}E\rightarrow{^1}A_1$ electronic transition in the NV$^-$ center. From this we calculated the ${^1}E\rightarrow{^1}A_1$ one-phonon absorption spectrum and found it to differ from that of the ${^3}E\rightarrow{^3}A_2$ transition, a result which is not anticipated by previous group-theoretical models of the NV$^-$ electronic states. We identified a high-energy 169 meV localized phonon mode of the $^1A_1$ level.