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Molecular spin systems based on photoexcited triplet pairs formed via singlet fission (SF) are attractive as carriers of quantum information because of their potentially pure and controllable spin polarization, but developing systems that…

Mesoscale and Nanoscale Physics · Physics 2022-11-09 Gajadhar Joshi , Ryan D. Dill , Karl J. Thorley , John E. Anthony , Obadiah G. Reid , Justin C. Johnson

Singlet Fission (SF) into two triplets offers exciting avenues for high-efficiency photovoltaics and optically initializable qubits. While the chemical space of SF chromophores is ever-expanding, the mechanistic details of…

For the theoretical screening of Singlet Fission (SF) rates in molecular aggregates, commonly dimer model systems are employed. However, there is experimental evidence, that the SF process proceeds from the $^{1}$(TT) state via an…

Chemical Physics · Physics 2023-12-22 Anurag Singh , Merle I. S. Röhr

Singlet fission is a photoconversion process that generates a doubly excited, maximally spin entangled pair state. This state has applications to quantum information and computing that are only beginning to be realized. In this article, we…

Chemical Physics · Physics 2020-11-11 Kori Smyser , Joel Eaves

The photo-driven process of singlet fission generates coupled triplet pairs (TT) with fundamentally intriguing and potentially useful properties. The quintet 5TT0 sublevel is particularly interesting for quantum information because it is…

Molecular dimers are widely utilized as a tool to investigate the structure-property relationships behind the complex photophysical processes of condensed-phase systems, where structural tuning remains a challenge. This approach often…

Singlet fission (SF) is a photophysical process where a singlet excitation generates two triplet excited states, enhancing exciton multiplication potentially useful for solar energy conversion. Since SF typically outcompetes radiative…

Chemical Physics · Physics 2025-12-24 Sumanta Paul , Oleksandr Yampolskyy , Zehua Wu , Klaus Müllen , Thomas Basché

Singlet fission describes the spin-conserving production of two triplet excitons from one singlet exciton. The existence of a spin-2 (quintet) triplet-pair state as a product of singlet fission is well established in the literature, and…

Mesoscale and Nanoscale Physics · Physics 2022-06-03 Miles I. Collins , Francesco Campaioli , Murad J. Y. Tayebjee , Jared H. Cole , Dane R. McCamey

Molecular quantum sensors represent a promising frontier for the detection of nuclear magnetic resonance signals and alternating current magnetic fields at the nanoscale, potentially reaching single-proton sensitivity. Although the triplet…

Chemical Physics · Physics 2026-05-18 Maria Grazia Concilio , Yiwen Wang , Siyuan Wang , Xueqian Kong

Probing extended polyene systems with energy in excess of the bright state ($1^1B_u^+$/$S_2$) band edge generates triplets via singlet fission. This process is not thought to involve the $2^1A_g^-$/$S_1$ state, suggesting that other states…

Strongly Correlated Electrons · Physics 2021-11-25 Darren J Valentine , Dilhan Manawadu , William Barford

Spin triplet exciton formation sets limits on technologies using organic semiconductors that are confined to singlet-triplet photophysics. In contrast, excitations in the spin doublet manifold in organic radical semiconductors can show…

Chemical Physics · Physics 2023-12-19 Qinying Gu , Sebastian Gorgon , Alexander S. Romanov , Feng Li , Richard H. Frienda , Emrys Evansd

The photoinduced switching of Fe(II)-based spin-crossover complexes from singlet to quintet takes place at ultrafast time scales. This a priori spin-forbidden transition triggered numerous time-resolved experiments of solvated samples to…

Low-lying excited states for indeno[1,2-b]fluorene homo dimers with or without benzene spacers are calculated using the Density Matrix Renormalization group (DMRG) approach within Pariser-Parr-Pople (PPP) model Hamiltonian. DMRG…

Materials Science · Physics 2020-11-03 Sumit Naskar , Mousumi Das

Triplet formation and its regulation have always been of central interest in understanding the photophysical behavior of living systems. In organic systems, excessive triplet formation poses significant challenges, as it can promote…

Biological Physics · Physics 2026-05-12 Parul Raghuvanshi , Vishvendra Singh Poonia

The electronic interaction between an optically active singlet state ($S_1S_0$) and a dark state of singlet multiplicity, known as correlated triplet pair ($^1[TT]$), plays a crucial role in the effective transformation from $S_1S_0$ to…

A theory of singlet fission (SF) in carotenoid dimers is applied to explain the SF in lycopene H-aggregates observed after high energy photoexcitation. The explanation proposed here is that a high energy, delocalized bright $^1B_u^+$ state…

Chemical Physics · Physics 2023-08-31 William Barford

Experiments in several intramolecular singlet fission materials have indicated that the triplet-triplet spin biexciton has a much longer lifetime than believed until recently, opening up loss mechanisms that can annihilate the biexciton…

Materials Science · Physics 2021-01-27 Rafi Chesler , Souratosh Khan , Sumit Mazumdar

Singlet fission is commonly defined to involve a process by which an overall singlet state with local triplet structure spin-decoheres into two triplet states, thereby completing the fission process. This process, often defined in loose…

Chemical Physics · Physics 2020-07-29 Max Marcus , William Barford

Singlet fission (SF) is a multielectron process in which one singlet exciton S converts into a pair of triplet excitons T+T. SF is widely studied as it may help overcome the Shockley-Queisser efficiency limit for semiconductor photovoltaic…

The growing interest in harnessing singlet fission for photovoltaic applications stems from the possibility of generating two excitons from a single photon. Quantum efficiencies above unity have been reported, yet the correlation between…

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