Singlet fission for quantum information and quantum computing: the parallel JDE model

@article{Smyser2020SingletFF,
  title={Singlet fission for quantum information and quantum computing: the parallel JDE model},
  author={Kori E. Smyser and Joel D. Eaves},
  journal={Scientific Reports},
  year={2020},
  volume={10}
}
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 construct and analyze a spin-exciton hamiltonian to describe the dynamics of the two-triplet state. We find the selection rules that connect the doubly excited, spin-singlet state to the manifold of quintet states and comment on the mechanism and conditions… 
Excited State Exchange Control of Photoinduced Electron Spin Polarization in Electronic Ground States.
TLDR
Ground state ESP is dependent on the magnitude of JSQ-NN, and it is postulate that this results from differences in 2T1 and 4T1 state mixing, which determines the 2T 1-4T1 energy gap.
Triplet-Pair Spin Signatures from Macroscopically Aligned Heteroacenes in an Oriented Single Crystal
The photo-driven process of singlet fission generates coupled triplet pairs (TT) with fundamentally intriguing and potentially useful properties. The quintet TT0 sublevel is particularly interesting
Using Molecular Design to Enhance the Coherence Time of Quintet Multiexcitons Generated by Singlet Fission in Single Crystals.
Multiexciton quintet states, 5(TT), photogenerated in organic semiconductors using singlet fission (SF), consist of four quantum entangled spins, promising to enable new applications in quantum
Biexciton Hamiltonian for the correlated triplet pair states in singlet fission: Revealing the contest between triplet-triplet exchange and triplet-triplet energy transfer coupling
The correlated triplet pair state 1(TT) is a key intermediate in the singlet fission process, and understanding the mechanism by which it separates into two independent triplet states is critical for
Clock transitions guard against spin decoherence in singlet fission
Short coherence times present a primary obstacle in quantum computing and sensing applications. In atomic systems, clock transitions (CTs), formed from avoided crossings in an applied Zeeman field,
Enthalpy-Entropy Compensation Effect for Triplet Pair Dissociation of Intramolecular Singlet Fission in Phenylene Spacer-Bridged Hexacene Dimers.
TLDR
The first observation of the quantitative TT generation together with the orientation-dependent photophysical discussions for TT dissociation using para- and meta-phenyl-bridged Hc dimers implies that "enthalpy-entropy compensation" has a large impact on the rate constants and quantum yields.
Open questions on the photophysics of ultrafast singlet fission
Ultrafast singlet fission has the potential to facilitate highly efficient photovoltaics through the multiplication of excitons in organic molecular architectures. Here, we consider the interplay of
Quantifying Ultrafast Three-Dimensional Transport Using Interferometrically Enhanced Pump-Probe Microscopy
We present a novel microscopic technique to access local transient optical constants and carrier motion in thin-film materials in three dimensions, with sub-10 nm spatial precision and sub-15 fs
...
1
2
...

References

SHOWING 1-10 OF 57 REFERENCES
Electron spin polarization generated by transport of singlet and quintet multiexcitons to spin-correlated triplet pairs during singlet fissions†
TLDR
The present interpretation of the spin correlation of the separated T + T exciton pair may pave new avenues not only for elucidating the vibronic role in the de-coupling between two excitons but also for scalable quantum information processing using quick T +T dissociation via one-photon excitation.
Time dependent correlations of entangled states with nondegenerate branches and possible experimental realization using singlet fission.
  • C. Bardeen
  • Physics
    The Journal of chemical physics
  • 2019
TLDR
It is argued that spin-entangled triplet exciton states produced by singlet fission could provide a new way to probe entangled state detection and collapse, complementing schemes based on polarization-entangling photon states.
Unified model for singlet fission within a non-conjugated covalent pentacene dimer
TLDR
The use of time-resolved optical and electron paramagnetic resonance spectroscopy is used to probe singlet fission in a pentacene dimer linked by a non-conjugated spacer and a single kinetic model is developed that describes the data over seven temporal orders of magnitude both at room and cryogenic temperatures.
Quintet-triplet mixing determines the fate of the multiexciton state produced by singlet fission in a terrylenediimide dimer at room temperature
TLDR
It is discovered that triplet–quintet-state mixing at room temperature can open a pathway that annihilates triplet states, potentially diminishing the performance of solar cells using singlet fission.
Correlated Pair States Formed by Singlet Fission and Exciton-Exciton Annihilation.
  • G. Scholes
  • Chemistry, Physics
    The journal of physical chemistry. A
  • 2015
TLDR
The eigenstates constituting the manifold of 16 bimolecular pair excitations and their relative energies in the weak-coupling regime are reported and it is shown that triplet pair states can be separated by a triplet-triplet energy-transfer mechanism to give a separated, yet entangled triplet Pair (1)[T···T].
Quantum beats in crystalline tetracene delayed fluorescence due to triplet pair coherences produced by direct singlet fission.
TLDR
The model provides good overall agreement with the data, supporting the conclusion that singlet fission in tetracene proceeds through the "direct" mechanism without strong electronic coupling between the singlet and triplet pair states.
Triplet Pair States in Singlet Fission.
TLDR
The challenges in treating singlet fission beyond the dimer approximation, in understanding the often neglected roles of delocalization on singlets fission rates, and in realizing the much lauded goal of increasing solar energy conversion efficiencies with singlet Fission chromophores are discussed.
Molecular spins for quantum computation
TLDR
Chemistry can contribute to designing robust spin systems based, in particular, on mononuclear lanthanoid complexes, the elementary unit of future quantum computers.
...
1
2
3
4
5
...