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Observation of Ultrafast Coherence Transfer and Degenerate States with Polarization-Controlled Two-Dimensional Electronic Spectroscopy

Sardjan, A. S., Westerman, F. P., Ogilvie, J. P. & Jansen, T. L. C., 22-Oct-2020, In : Journal of Physical Chemistry B. 124, 42, p. 9420-9427 8 p.

Research output: Contribution to journalArticleAcademicpeer-review

Optical spectroscopy is a powerful tool to interrogate quantum states of matter. We present simulation results for the cross-polarized two-dimensional electronic spectra of the light-harvesting system LH2 of purple bacteria. We identify a spectral feature on the diagonal, which we assign to ultrafast coherence transfer between degenerate states. The implication for the interpretation of previous experiments on different systems and the potential use of this feature are discussed. In particular, we foresee that this kind of feature will be useful for identifying mixed degenerate states and for identifying the origin of symmetry breaking disorder in systems like LH2. Furthermore, this may help identify both vibrational and electronic states in biological systems such as proteins and solid-state materials such as hybrid perovskites.

Original languageEnglish
Pages (from-to)9420-9427
Number of pages8
JournalJournal of Physical Chemistry B
Volume124
Issue number42
Publication statusPublished - 22-Oct-2020

    Keywords

  • VIBRATIONAL SPECTROSCOPY, EXCITON DELOCALIZATION, NONLINEAR SPECTROSCOPY, PHOTOSYNTHETIC ENERGY, IR-SPECTROSCOPY, RAMAN RESPONSE, LH2 COMPLEX, LIQUID CS2, DYNAMICS, SPECTRA

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