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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

Singlet fission, the molecular process through which photons are effectively converted into pairs of lower energy triplet excitons, holds promise as a means of boosting photovoltaic device efficiencies. In the preceding article of this…

Materials Science · Physics 2017-05-12 Roel Tempelaar , David R. Reichman

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

Several recent electron spin resonance studies have observed a quintet multiexciton state during the singlet fission process. Here we provide a general theoretical explanation for the generation of this state by invoking a time-varying…

Materials Science · Physics 2020-01-08 Miles I. Collins , Dane R. McCamey , Murad J. Y. Tayebjee

Singlet fission may boost photovoltaic efficiency [by transforming a singlet exciton into two triplet excitons and thereby doubling the number of excited charge carriers. The primary step of singlet fission is the ultrafast creation of the…

We investigate the physical mechanisms for spin-dependent recombination of a strongly bound pair of triplet excitons generated by singlet fission and forming a spin quintet (total spin of two) bi-exciton. For triplet excitons the…

Mesoscale and Nanoscale Physics · Physics 2024-02-16 Yan Sun , L. R. Weiss , V. Derkach , J. E. Anthony , M. Monteverde , A. D. Chepelianskii

Singlet fission is a form of multiple exciton generation which occurs in organic chromophores when a high energy singlet exciton separates into two lower energy triplet excitons, each with approximately half the singlet energy. Since this…

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

We present a generic theory of primary photoexcitations in low band gap donor-acceptor conjugated copolymers. Because of the combined effects of strong electron correlations and broken symmetry, there is considerable mixing between a…

Mesoscale and Nanoscale Physics · Physics 2016-01-01 Karan Aryanpour , Tirthankar Dutta , Uyen N. V. Huynh , Zeev Valy Vardeny , Sumit Mazumdar

Internal conversion from the photoexcited state to a correlated singlet triplet-pair state is believed to be the precursor of singlet fission in carotenoids. We present numerical simulations of this process using a pi-electron model that…

Chemical Physics · Physics 2021-11-23 Dilhan Manawadu , Darren Valentine , Max Marcus , William Barford

Two electrons in a quantum dot (QD) can form triplet states. We analyze the exchange coupling of the triplet states of the negatively charged exciton in a QD (X$^-$, two electrons and one hole) with the spin of a magnetic atom (Mn). Two…

Mesoscale and Nanoscale Physics · Physics 2023-07-12 L. Besombes , S. Ando , S. Kuroda , H. Boukari

Carrier multiplication by singlet exciton fission enhances photovoltaic conversion efficiencies in organic solids. This decay of one singlet exciton into two triplet states promises to overcome the Shockley-Queisser limit as up to two…

Materials Science · Physics 2016-12-16 K. Kolata , S. Marquardt , N. W. Rosemann , A. Mager , A. Hansmann , U. Höfer , R. Berger , T. Breuer , G. Witte , S. Chatterjee

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

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

Producing advanced quantum states of light is a priority in quantum information technologies. While remarkable progress has been made on single photons and photon pairs, multipartite correlated photon states are usually produced in purely…

The giant exciton binding energy and the richness of degrees of freedom make monolayer transition metal dichalcogenide an unprecedented playground for exploring exciton physics in 2D systems. Thanks to the well energetically separated…

Mesoscale and Nanoscale Physics · Physics 2023-07-26 Bairen Zhu , Ke Xiao , Siyuan Yang , Kenji Watanabe , Takashi Taniguchi , Xiaodong Cui

Recent time-resolved spectroscopic experiments have indicated that vibronic coupling plays a vital role in facilitating the process of singlet fission. In this work, which forms the first article of a series, we set out to unravel the…

Materials Science · Physics 2017-05-12 Roel Tempelaar , David R. Reichman

Singlet fission, a spin-allowed energy transfer process generating two triplet excitons from one singlet exciton, has the potential to dramatically increase the efficiency of organic solar cells. However, the dynamical mechanism of this…

Materials Science · Physics 2015-06-12 Timothy C. Berkelbach , Mark S. Hybertsen , David R. Reichman

Singlet fission is a process whereby two triplet excitons can be produced from one photon, potentially increasing the efficiency of photovoltaic devices. Endothermic singlet fission is desired for maximum energy conversion efficiency, and…

From organic electronics to biological systems, understanding the role of intermolecular interactions between spin pairs is a key challenge. Here we show how such pairs can be selectively addressed with combined spin and optical…

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