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Singlet fission, a phenomenon in which a singlet exciton is converted to two triplet excitons, is sensitive to vibrations that perturb couplings between electronic states (i.e., Peierls vibrations). In singlet fission models larger than…

Chemical Physics · Physics 2025-06-24 Jacob K. Lynd , Doran I. G. B. Raccah

We develop a powerful tree tensor network states method that is capable of simulating exciton-phonon quantum dynamics of larger molecular complexes and open quantum systems with multiple bosonic environments. We interface this method with…

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…

One way for solar cell efficiencies to overcome the Shockley-Queisser limit is downconversion of high-energy photons using singlet fission (SF) in polyacenes like tetracene (Tc). SF enables generation of multiple excitons from the…

Applied Physics · Physics 2018-01-31 S. W. Tabernig , B. Daiber , T. Wang , B. Ehrler

Experimental investigations of magnetic field dependent kinetics of singlet fission (SF)processes in some organic semiconductors [i.e. splitting of excited singlet (S_1) state into a triplet exciton pair] have revealed the important…

Materials Science · Physics 2018-09-05 A. I. Shushin

A method for improving the efficiency of solar cells is combining a low-bandgap semiconductor with a singlet fission material (which converts one high energy singlet into two low energy triplets following photoexcitation). Here we present a…

Materials Science · Physics 2021-12-07 Alan R. Bowman , Samuel D. Stranks , Bartomeu Monserrat

We probe the dynamics of dissociating CS$_2$ molecules across the entire reaction pathway upon excitation. Photoelectron spectroscopy measurements using laboratory-generated femtosecond extreme ultraviolet pulses monitor the competing…

We present a comparative study of ultrafast photo-conversion dynamics in tetracene (Tc) and pentacene (Pc) single crystals and Pc films using optical pump-probe spectroscopy. Photo-induced absorption in Tc and Pc crystals is activated and…

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

Organic molecular crystals are appealing for next-generation optoelectronic applications, most notably due to their multiexciton generation process that can increase the efficiency of photovoltaic devices. However, a general understanding…

Materials Science · Physics 2021-11-01 Aaron R. Altman , Sivan Refaely-Abramson , Felipe H. da Jornada

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

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 (SF) is a potential pathway for significant enhancement of efficiency in organic solar cells (OSC). In this paper, we study singlet fission in a pair of polyene molecules in two different stacking arrangements employing…

Chemical Physics · Physics 2017-08-23 Suryoday Prodhan , S. Ramasesha

Singlet fission in tetracene generates two triplet excitons per absorbed photon. If these triplet excitons can be effectively transferred into silicon (Si) then additional photocurrent can be generated from photons above the bandgap of Si.…

Identifying multi-exciton states generated from singlet fission is key to understanding the carrier multiplication process, which presents a strategy for improving the efficiency of photovoltaics and bio-imaging. Broadband optically…

Mesoscale and Nanoscale Physics · Physics 2024-06-14 Yan Sun , M. Monteverde , V. Derkach , J. E. Anthony , A. D. Chepelianskii

High-spin states in molecular systems hold significant interest for a wide range of applications ranging from optoelectronics to quantum information and singlet fission (SF). Quintet and triplet states play crucial roles, particularly in SF…

A theory of singlet fission in carotenoid dimers is presented which aims to explain the mechanism behind the creation of two uncorrelated triplets. Following the initial photoexcitation of a carotenoid chain to a "bright" $n^1B_u^+$ state,…

Chemical Physics · Physics 2024-11-22 Alexandru G. Ichert , William Barford

Intramolecular singlet fission (iSF) materials provide remarkable advantages in terms of tunable electronic structures, and quantum chemistry studies have indicated strong electronic coupling modulation by high frequency phonon modes. In…

Chemical Physics · Physics 2018-01-03 Zhongkai Huang , Yuta Fujihashi , Yang Zhao

The economic value of a photovoltaic installation depends upon both its lifetime and power conversion efficiency. Progress towards the latter includes mechanisms to circumvent the Shockley- Queisser limit, such as tandem designs and…

Coupled pairs of nuclear spins-1/2 support one singlet state and three triplet states. Transitions between the singlet state and one of the triplet states may be driven by an oscillating low-frequency magnetic field, in the presence of…

Quantum Physics · Physics 2021-10-27 Laurynas Dagys , Christian Bengs , Malcolm H. Levitt