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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

Polaritons are unique hybrid light-matter states that offer an alternative way to manipulate chemical processes and change material properties. In this work we theoretically demonstrate that singlet fission dynamics can be accelerated under…

Chemical Physics · Physics 2021-10-06 Clàudia Climent , David Casanova , Johannes Feist , Francisco J. García-Vidal

Excitons in organic crystalline semiconductors play a crucial role in the operation of optoelectronic devices such as organic solar cells, light-emitting diodes, and photodetectors. The excitonic properties of materials are dramatically…

Materials Science · Physics 2023-10-25 M. V. Klymenko , L. Z. Tan , S. P. Russo , J. H. Cole

The successful use of molecular dyes for solar energy conversion requires efficient charge injection, which in turn requires the formation of states with sufficiently long lifetimes (e.g. triplets). The molecular structure elements that…

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…

The coherent two-dimensional (2D) electronic spectra with respect to the singlet fission (SF) process in organic molecular aggregates are simulated by the Davydov ansatz combined with the Frenkel-Dirac time-dependent variational algorithm.…

Mesoscale and Nanoscale Physics · Physics 2018-01-17 Ke-Wei Sun , Yao Yao

We describe our dynamical simulations of the excited states of the carotenoid, neurosporene, following its photoexcitation into the 'bright' (nominally $1^1B_u^+$) state. We employ the adaptive tDMRG method on the UV model of…

Chemical Physics · Physics 2022-11-07 Dilhan Manawadu , Timothy N. Georges , William Barford

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…

We present an exciton/lattice model of the electronic dynamics of primary photoexcitations in a polymeric semiconductor heterojunction which includes both polymer pi-stacking, energetic disorder, and phonon relaxation. Results from our…

Materials Science · Physics 2013-09-26 Eric R. Bittner , Carlos Silva

The representation of information within the spins of electrons and nuclei has been powerful in the ongoing development of quantum computers. Although nuclear spins are advantageous as quantum bits (qubits) due to their long coherence…

Understanding and controlling exciton transport is a strategic way to enhance the optoelectronic properties of high-performance organic devices. In this article we study triplet exciton migration in crystalline poly($p$-phenylene vinylene)…

Materials Science · Physics 2019-11-13 Igor Lyskov , Egor Trushin , Ben Q. Baragiola , Timothy W. Schmidt , Jared H. Cole , Salvy P. Russo

We investigate the cascade decay mechanism for ultrafast intersystem crossing mediated by the spin-orbit coupling in transition-metal complexes. A quantum-mechanical description of the cascading process that occurs after photoexcitation is…

Strongly Correlated Electrons · Physics 2010-08-16 Jun Chang , A. J. Fedro , Michel van Veenendaal

Intersystem crossings between singlet and triplet states represent a crucial relaxation pathway in photochemical processes. Herein, we probe the intersystem crossing in hexafluoro-acetylacetone with ultrafast X-ray transient absorption…

We have evaluated hyperfine-induced electron spin dynamics for two electrons confined to a double quantum dot. Our quantum solution accounts for decay of a singlet-triplet correlator even in the presence of a fully static nuclear spin…

Mesoscale and Nanoscale Physics · Physics 2007-05-23 W. A. Coish , Daniel Loss

When considering the optimal molecular packing to realize charge multiplication in organic photovoltaic materials, subtle changes in intermolecular charge transfer (CT) coupling can strongly modulate singlet fission. To understand why…

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

Non-radiative exciton relaxation processes are critical for energy transduction efficiencies in optoelectronic materials, but how these processes are connected to the underlying crystal structure and its associated electron, exciton, and…

Materials Science · Physics 2023-05-09 Galit Cohen , Jonah B. Haber , Jeffrey B. Neaton , Diana Y. Qiu , Sivan Refaely-Abramson

A new mechanism for the primary photoinduced charge separation in photosynthesis is proposed. It involves as real intermediate between the excited special pair state P* and the primary charge separated state P+HL- a trip-trip-singlet PTBLT,…

Soft Condensed Matter · Physics 2008-02-03 S. F. Fischer , P. O. J. Scherer

Inclusion of heavy metal atoms in a polymer backbone allows transitions between the singlet and triplet manifolds. Interfacial dissociation of triplet excitons constitutes a viable mechanism for enhancing photovoltaic (PV) efficiencies in…

Materials Science · Physics 2009-08-10 K. Yang , U. Scherf , S. Guha

Organic solar cells (OSCs) have recently shown a rapid improvement in their performance, bringing power conversion efficiencies (PCEs) closer to the point where commercial applications of the technology become viable. However, the low…

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