Related papers: Strong-Coupling Modification of Singlet-Fission Dy…
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…
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…
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…
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…
In computational chemistry of molecular materials, strong static correlation effects appear when electronic states, often involving the ground state, become quasi-degenerate, as occurs, for example, in bond-breaking processes. Such…
We develop a theory of singlet fission in carotenoid dimers. Following photoexcitation of the 'bright' state (i.e., a singlet electron-hole pair) in a single carotenoid, the first step in the singlet fission process is ultrafast…
We study the thermodynamic properties of a system of two-level dipoles that are coupled ultrastrongly to a single cavity mode. By using exact numerical and approximate analytical methods, we evaluate the free energy of this system at…
When the light interacts with matters in a lossy cavity, in the standard cavity quantum electrodynamics, the dissipation of cavity fields is characterized simply by the strengths of the two couplings: the light-matter interaction and the…
We present a new methodology to calculate the strong light-matter coupling between photonic modes in microcavities and large molecular aggregates that consist of hundreds of molecular fragments. To this end, we combine our fragment…
In organic microcavities, hybrid light-matter states can form with energies that differ from the bare molecular excitation energies by nearly 1 eV. A timely question, given recent advances in the development of thermally activated delayed…
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…
Singlet fission is a spin-allowed exciton multiplication process in organic semiconductors that converts one spin-singlet exciton to two triplet excitons. It offers the potential to enhance solar energy conversion by circumventing the…
The concept of modifying molecular dynamics in strongly coupled exciton-polariton systems is an emerging topic in photonics due to its potential to produce customized chemical systems with tailored photophysical properties. However, before…
Singlet fission (SF) is a very significant photophysical phenomenon and possesses potential applications. In this work, we try to give the rather detailed theoretical investigation of the SF process in the stacked polyacene dimer by…
We discuss the basic properties of a recently proposed hybrid light-matter system of strongly interacting photons in an array of coupled cavities each doped with a single two level system. Using the non-linearity generated from the photon…
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…
In the preceding paper, we assembled the theoretical components necessary for a unified framework of singlet fission, a type of multiexciton generation producing two triplet excitons from one singlet exciton. In this paper, we apply our…
Cavity-mediated light-matter coupling can dramatically alter opto-electronic and physico-chemical properties of a molecule. Ab initio theoretical predictions of these systems need to combine non-perturbative, many-body electronic structure…
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…
We demonstrate a new type of transition within the strong coupling regime, which alters the coupling mechanism in multimode cavities. We show that this transition drastically modifies the Hamiltonian describing the polaritons, such that…