“…1, when the triplet excitons are separated from each other to result in a negligible magnitude of exchange coupling (J z 0), spin correlations in the triplet-triplet pair may occur to induce diagonalized nine spin-states as the quantum superpositions of the singlet-triplet-quintet character through the spin-spin dipolar couplings of individual triplet species. This is quite similar to the spin-correlated radical pair (SCRP) model 33,34,[36][37][38][39][40][41][42] in the photoinduced long-range chargeseparation system generated by singlet or triplet precursors, causing the superpositions of the singlet-triplet characters when the J-coupling is small in the radical pairs. We herein demonstrate that the transportations of the SF-induced 5 (TT) and 1 (TT) characters can be distinguished on the T + T dissociation using the ESP of the correlated T-T state by applying TREPR spectroscopy to thin lms of 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-Pn).…”
Section: Introductionsupporting
confidence: 57%
“…25 Interestingly, transport of spin-entangled multiexcitons 20,[29][30][31] by the dissociative exciton diffusion has been observed using ultrafast transient absorption imaging of pentacene crystals 32 and by the magnetic eld effect on the uorescence time-proles. Although such transportation of spin-entanglements is key to elucidate the dissociation mechanism and to apply in quantum information science, [33][34][35] no direct evidence for the transportation of spin-entanglements has been found in the separated T + T state with the singlet and quintet characters.…”
“…1, when the triplet excitons are separated from each other to result in a negligible magnitude of exchange coupling (J z 0), spin correlations in the triplet-triplet pair may occur to induce diagonalized nine spin-states as the quantum superpositions of the singlet-triplet-quintet character through the spin-spin dipolar couplings of individual triplet species. This is quite similar to the spin-correlated radical pair (SCRP) model 33,34,[36][37][38][39][40][41][42] in the photoinduced long-range chargeseparation system generated by singlet or triplet precursors, causing the superpositions of the singlet-triplet characters when the J-coupling is small in the radical pairs. We herein demonstrate that the transportations of the SF-induced 5 (TT) and 1 (TT) characters can be distinguished on the T + T dissociation using the ESP of the correlated T-T state by applying TREPR spectroscopy to thin lms of 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-Pn).…”
Section: Introductionsupporting
confidence: 57%
“…25 Interestingly, transport of spin-entangled multiexcitons 20,[29][30][31] by the dissociative exciton diffusion has been observed using ultrafast transient absorption imaging of pentacene crystals 32 and by the magnetic eld effect on the uorescence time-proles. Although such transportation of spin-entanglements is key to elucidate the dissociation mechanism and to apply in quantum information science, [33][34][35] no direct evidence for the transportation of spin-entanglements has been found in the separated T + T state with the singlet and quintet characters.…”
“…[125][126] The role of the third spin in the initial state preparation (information input) was discussed in relationt oq uantum teleportation.T he studies about the spin qubits and the quantum teleportation,w hich are strongly related to quantum informations cience, were carried out on photogenerated radical pair systems by Wasielewski and co-workers. [127][128][129] Initially entangled radicalp airs constituted D-C-A triad systems (cf. Figure 7), which could serve as coupled spin qubits in quantum information science applications,p rovided that the spin coherencel ifetimes of these systems are long.…”
Section: Possibleapplications To Information Technologymentioning
confidence: 99%
“…[128] The experiment of the quantum teleportation using ac ovalent donor-acceptor-radical (D-A-RC)m olecular system has been also carried out. [129] In this experiment, as pecific electron spin state on RC in amagnetic field was prepared by microwave pulse (information input), an entangled charge-separated radical pair (DC + -AC À )w as generatedb yaphotoexcitation (Bell-statef ormation). Ultrafast electron transfer from AC À to RC carriedo ut spin-state teleportation, that is, the input information on RC moved to DC + by the spin-selectivec hemical reaction DC + -AC À -RC!DC + -A-R À throught he agency of quantum entanglement.…”
Section: Possibleapplications To Information Technologymentioning
Recently,t he potentialu se of organic p-radicals and relateds pin systems has been expanded to modern technological applications. The unique excited-state dynamics of organic p-radicals can be useful to improvet he stability of photochemically unstable organic compounds, make the polarization transfer applicable to information technology,a nd achieve effective up-conversion of interest for luminescence bioimaging, amongo thers. Furthermore, highly luminescent stable p-radicalsh ave been recently reported, which are especially interesting fora pplication in organic light-emitting devices owing to their potentialt op rovide an internal quantum efficiency of 100 %. Thus,t he excited-state nature of stable p-radicalsa sw ell as the control of their excited-state spin dynamics are emerging topics both in terms of fundamental science and related technological applications. In this minireview,w ef ocus on the excited-state dynamics of both photostable non(weakly)-luminescent and luminescent p-radicals, which are opposites of each other.I n particular, we cover the following topics:1 )effective generation of high-spin photoexcited states and control of the excited-state dynamics by using non-luminescent p-radicals, 2) unique excited-state dynamics of luminescent p-radicals and radical excimers, and 3) applicationsu tilizing excitedstate dynamics of p-radicals.[a] Prof.
“…Moreover, the superparamagnetic nano-surfaces of FeNP, can maintain the spin correlations after electron hopping to a second donor, particularly in the presence of MF; hence we observe such long lifetimes for FeNPs. Several reports of electron hopping between adjacent donors and elongation of the spin decoherence time for the entangled spin correlated radicals in the bridged donor–acceptor system have been reported 86 – 89 . Figure 5 Transient absorption spectra of ( a ) ADN, ( b ) Au MQ-ADN and, ( c ) Fe MQ-ADN, respectively, between the pump and probe pulse at 1 μs time delay and all the red spectra represent the presence of the magnetic field for their corresponding spectra.…”
In this article, we highlight the alterations in the photoinduced electron transfer (ET) and hydrogen atom transfer (HAT) pathways between an anti-tumor drug vitamin-K3 (MQ) and a nucleobase adenine (ADN) in the presence of gold (Au) and iron (Fe) nanoparticles (NPs). Inside the confined micellar media, with laser flash photolysis corroborated with an external magnetic field (MF), we have detected the transient geminate radicals of MQ and ADN, photo-generated through ET and HAT. We observe that the presence of AuNP on the MQ-ADN complex (AuMQ-ADN) assists HAT by limiting the ET channel, on the other hand, FeNP on the MQ-ADN complex (FeMQ-ADN) mostly favors a facile PET. We hypothesize that through selective interactions of the ADN molecules with AuNP and MQ molecules with FeNP, a preferential HAT and PET process is eased. The enhanced HAT and PET have been confirmed by the escape yields of radical intermediates by time-resolved transient absorption spectroscopy in the presence of MF.
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