Spin dynamics on photoexcited state of functionality π-radical via quantum-mixed state: Theoretical study of the spin polarized state generation using the mechanism via quantum-mixed state

Wave Function Control of Charge-Separated Excited-State Lifetimes

“…The same magnetic exchange interactions that determine variable excited-state spin polarizations also promote magnetic exchange dependent excited-state wave function mixing, and this provides a novel way to control and manipulate excited-state lifetimes via the radical–chromophore exchange interaction. Understanding these exchange interactions is important, as they figure prominently in the exciton–polaron interaction present in trion quasiparticles. − The dynamics of these trions have recently been studied in carefully charge-doped single-walled carbon nanotubes following photoexcitation and exciton formation, and excited-state exchange interactions are expected to affect the lifetimes of trion and higher-order multipartite quasiparticles.…”

“…While several studies have demonstrated how electron spin affects photophysical properties, ,− the evaluation of multiple pairwise exchange interactions and their effect on photoexcited states remain relatively unexplored. Our prior work has focused on using a combination of spectroscopy and magnetometry to determine the nature of exchange-dependent wave function mixing between the spin doublet donor–acceptor charge-transfer excited states of these radical-elaborated molecules .…”

Excited State Exchange Control of Photoinduced Electron Spin Polarization in Electronic Ground States

“…One approach to generating ESP in an organic radical system is to covalently attach the radical to a chromophore. − Following light excitation, the spin selective relaxation of the excited chromophore–radical system can lead to ESP in the radical. Such systems have been used to provide high-resolution information regarding the nature of their low-energy excited states, ,− illustrate how multiple, pairwise, excited state magnetic exchange interactions influence photophysical processes, and highlight how the excited state chromophore triplet–radical magnetic exchange interaction and associated excited state dynamics can affect ESP. ,,,,− ,− In liquid solution, modulations of the exchange interaction between species during intermolecular collisions lead to polarization of the radical via the radical–triplet pair or radical–quartet pair mechanism. In the glass phase, the generation of ESP in the radical is more challenging and the spin–spin coupling between the unpaired electrons of the chromophore and the radical plays a crucial role in determining whether ESP can be generated.…”

Metal Ion Control of Photoinduced Electron Spin Polarization in Electronic Ground States

“…Electron spins are an example of a two-level quantum system that can be put into a superposition state and can be used to create an entangled spin system. We, − and others, ,− are using radical-elaborated chromophores that allow for the S = 1/2 radical qubit to be exchange coupled with open-shell spins generated by photoexcitation. Photoexcitation of persistent radical-elaborated donor–acceptor (D–A) chromophores leads to the generation of three spatially distinct entangled electron spin qubits. − These radical-elaborated molecules may be used to probe photophysical processes at high resolution and develop a better understanding of how molecular and molecule-based systems can be fully exploited to prepare electron spin polarized statescharacterized by a non-Boltzmann population of m s levelsthat may be useful for quantum information science applications.…”