Charge transfer is the primary energy conversion step in photosynthesis and organic solar cells. Ultrafast spectroscopy, particularly two-dimensional electronic spectroscopy (2DES), has played an important role in characterizing its kinetics and mechanisms in the past decade1-4. Relatively recently, two-dimensional electronic-vibrational spectroscopy (2DEV) has been developed to provide complementary information about the interplay of electronic and vibrational states5-7. I will present our recent development8 of a multispectral multidimensional spectrometer (MMDS) capable of performing 2D spectroscopy over a wide spectral window from the ultraviolet to mid-infrared and a time window from femtoseconds to seconds—i.e. conferring a detailed structural and dynamical picture to reveal the kinetics and mechanisms of charge transfer. To illustrate its capabilities, I will discuss our recent applications to understanding charge transfer in the heliobacterial reaction centers (HbRC) and organic donor-acceptor heterojunction blends. The HbRC, a homodimeric reaction center, is believed to be the closest homolog of the common ancestor of all photosynthetic reaction centers9. In this example, MMDS from the visible to mid-IR provides insight into the excitonic structure and the kinetics and charge separation mechanism of the HbRC. In the second example, I present an MMDS study of an organic solar cell that is a promising candidate for addressing the global energy challenge10. I will describe how to take advantage of electronic and vibrational probes to uncover the charge generation pathway via hole transfer, a process that is often hidden underneath the congested absorption spectra of donor and acceptor in the visible and near-IR range.

Probing charge transfer in photosynthetic reaction centers and organic solar cells using multispectral multidimensional spectroscopy

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.