Ultrafast dynamics of photoinduced charge separation

Abstract

Phenomena involving electron transfer are ubiquitous in nature, photosynthesis and enzymes or protein activity being prominent examples. Their deep understanding thus represents a mandatory scientific goal. Moreover, controlling the separation of photogenerated charges is a crucial prerequisite in many applicative contexts, including quantum electronics, photo-electrochemical water splitting, photocatalytic dye degradation, and energy conversion. In particular, photoinduced charge separation is the pivotal step driving the storage of sun light into electrical or chemical energy. If properly mastered, these processes may also allow us to achieve a better command of information storage at the nanoscale, as required for the development of molecular electronics, optical switching, or quantum technologies, amongst others. In this Topical review we survey recent progress in the understanding of ultrafast charge separation from photoexcited states. We report the state-of-the-art of the observation and theoretical description of charge separation phenomena in the ultrafast regime mainly focusing on molecular- and nano-sized solar energy conversion systems. In particular, we examine different proposed mechanisms driving ultrafast charge dynamics, with particular regard to the role of quantum coherence and electron-nuclear coupling, and link experimental observations to theoretical approaches based either on model Hamiltonians or on first principles simulations.

arXiv comment65 pages, 9 figures

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Cited by in corpus (12)

• Understanding real-time time-dependent density-functional theory simulations of ultrafast laser-induced dynamics in organic molecules
• Charge separation in donor-C60 complexes with real-time Green's functions: The importance of nonlocal correlations
• Analytical nonadiabatic couplings and gradients within the state-averaged orbital-optimized variational quantum eigensolver
• Probing quantum coherence in ultrafast molecular processes: an ab initio approach to open quantum systems
• Ultrafast charge transfer and vibronic coupling in a laser-excited hybrid inorganic/organic interface
• Laser-Induced Electronic and Vibronic Dynamics in the Pyrene Molecule and its Cation
• Ab initio simulation of laser-induced electronic and vibrational coherence
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