Electron-vibration coupling induced renormalization in the photoemission spectrum of diamondoids

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The development of theories and methods devoted to the accurate calculation of the electronic quasi-particle states and levels of molecules, clusters and solids is of prime importance to interpret the experimental data. These quantum systems are often modelled by using the Born-Oppenheimer approximation where the coupling between the electrons and vibrational modes is not fully taken into account, and the electrons are treated as pure quasi-particles. Here, we show that in small diamond cages, called diamondoids, the electron-vibration coupling leads to the breakdown of the electron quasi-particle picture. More importantly, we demonstrate that the strong electron-vibration coupling is essential to properly describe the overall lineshape of the experimental photoemission spectrum. This cannot be obtained by methods within Born-Oppenheimer approximation. Moreover, we deduce a link between the vibronic states found by our many-body perturbation theory approach and the well-known Jahn-Teller effect.




Gali, A., Demján, T., Vörös, M., Thiering, G., Cannuccia, E., & Marini, A. (2016). Electron-vibration coupling induced renormalization in the photoemission spectrum of diamondoids. Nature Communications, 7. https://doi.org/10.1038/ncomms11327

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