Control of excitation selectivity in pulse EPR on spin-correlated radical pairs with shaped pulses
Literature Information
Daniele Panariti, Sarah M. Conron, Jinyuan Zhang, Michael R. Wasielewski, Marilena Di Valentin, Claudia E. Tait
Spin-correlated radical pairs generated by photoinduced electron transfer are characterised by a distinctive spin polarisation and a unique behaviour in pulse electron paramagnetic resonance (EPR) spectroscopy. Under non-selective excitation, an out-of-phase echo signal modulated by the dipolar and exchange coupling interactions characterising the radical pair is observed and allows extraction of geometric information in the two-pulse out-of-phase electron spin echo envelope modulation (ESEEM) experiment. The investigation of the role of spin-correlated radical pairs in a variety of biological processes and in the fundamental mechanisms underlying device function in optoelectronics, as well as their potential use in quantum information science, relies on the ability to precisely address and manipulate the spins using microwave pulses. Here, we explore the use of shaped pulses for controlled narrowband selective and broadband non-selective excitation of spin-correlated radical pairs in two model donor–bridge–acceptor triads, characterised by different spectral widths, at X- and Q-band frequencies. We demonstrate selective excitation with close to rectangular excitation profiles using BURP (band-selective, uniform response, pure-phase) pulses and complete non-selective excitation of both spins of the radical pair using frequency-swept chirp pulses. The use of frequency-swept pulses in out-of-phase ESEEM experiments enables increased modulation depths and, combined with echo transient detection and Fourier transformation, correlation of the dipolar frequencies with the EPR spectrum and therefore the potential to extract additional information on the donor–acceptor pair geometry.
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.











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