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

Smyser, Kori E.; Eaves, Joel D.

doi:10.1038/s41598-020-75459-x

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

Journal Article · 27 October 2020 · Scientific Reports

DOI: https://doi.org/10.1038/s41598-020-75459-x · OSTI ID:1690308

Smyser, Kori E.; Eaves, Joel D.

Abstract 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 for the transition into formally independent triplets. For adjacent dimers that are oriented and immobilized in an inert host, singlet fission can be strongly state-selective. We make predictions for electron paramagnetic resonance experiments and analyze experimental data from recent literature. Our results give conditions for which magnetic resonance pulses can drive transitions between optically polarized magnetic sublevels of the two-exciton states, making it possible to realize quantum gates at room temperature in these systems.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1690308

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 10; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

References (40)

The Physical Implementation of Quantum Computation DiVincenzo, David P. Fortschritte der Physik, Vol. 48, Issue 9-11 https://doi.org/10.1002/1521-3978(200009)48:9/11<771::Aid-prop771>3.0.Co;2-e	journal	September 2000
Electron Paramagnetic Resonance of Exchange Coupled Systems Bencini, Alessandro; Gatteschi, Dante https://doi.org/10.1007/978-3-642-74599-7	book	December 1989
EPR of triplet excitions in tetracene crystals: spin polarization and the role of singlet exciton fission Yarmus, L.; Rosenthal, J.; Chopp, M. Chemical Physics Letters, Vol. 16, Issue 3 https://doi.org/10.1016/0009-2614(72)80404-4	journal	October 1972
An EPR study of the triplet state of pentacene by electron spin-echo techniques and laser flash excitation Van Strien, A. J.; Schmidt, J. Chemical Physics Letters, Vol. 70, Issue 3 https://doi.org/10.1016/0009-2614(80)80115-1	journal	March 1980
On the rotation operators in quantum mechanics Bouten, M. Physica, Vol. 42, Issue 4 https://doi.org/10.1016/0031-8914(69)90162-1	journal	June 1969
Evidence for Charge-Transfer Mediation in the Primary Events of Singlet Fission in a Weakly Coupled Pentacene Dimer Basel, Bettina S.; Zirzlmeier, Johannes; Hetzer, Constantin Chem, Vol. 4, Issue 5 https://doi.org/10.1016/j.chempr.2018.04.006	journal	May 2018
Spin–orbit coupling and luminescence characteristics of conjugated organic molecules. I. Polyacenes Pedash, Yu. F.; Prezhdo, O. V.; Kotelevskiy, S. I. Journal of Molecular Structure: THEOCHEM, Vol. 585, Issue 1-3 https://doi.org/10.1016/s0166-1280(02)00035-0	journal	May 2002
Quantum computers and quantum coherence DiVincenzo, David P.; Loss, Daniel Journal of Magnetism and Magnetic Materials, Vol. 200, Issue 1-3 https://doi.org/10.1016/s0304-8853(99)00315-7	journal	October 1999
Triplet Pair States in Singlet Fission Miyata, Kiyoshi; Conrad-Burton, Felisa S.; Geyer, Florian L. Chemical Reviews, Vol. 119, Issue 6 https://doi.org/10.1021/acs.chemrev.8b00572	journal	January 2019
Correlated Pair States Formed by Singlet Fission and Exciton–Exciton Annihilation Scholes, Gregory D. The Journal of Physical Chemistry A, Vol. 119, Issue 51 https://doi.org/10.1021/acs.jpca.5b09725	journal	December 2015
What Can Be Learned from Magnetic Field Effects on Singlet Fission: Role of Exchange Interaction in Excited Triplet Pairs Wakasa, Masanobu; Kaise, Mana; Yago, Tomoaki The Journal of Physical Chemistry C, Vol. 119, Issue 46 https://doi.org/10.1021/acs.jpcc.5b10176	journal	November 2015
Exergonic Intramolecular Singlet Fission of an Adamantane-Linked Tetracene Dyad via Twin Quintet Multiexcitons Matsui, Yasunori; Kawaoka, Shuhei; Nagashima, Hiroki The Journal of Physical Chemistry C, Vol. 123, Issue 31 https://doi.org/10.1021/acs.jpcc.9b04503	journal	July 2019
Multiexciton Dynamics Depending on Intramolecular Orientations in Pentacene Dimers: Recombination and Dissociation of Correlated Triplet Pairs Sakai, Hayato; Inaya, Ryutaro; Nagashima, Hiroki The Journal of Physical Chemistry Letters, Vol. 9, Issue 12 https://doi.org/10.1021/acs.jpclett.8b01184	journal	May 2018
Singlet-Fission-Born Quintet State: Sublevel Selections and Trapping by Multiexciton Thermodynamics Nagashima, Hiroki; Kawaoka, Shuhei; Akimoto, Seiji The Journal of Physical Chemistry Letters, Vol. 9, Issue 19 https://doi.org/10.1021/acs.jpclett.8b02396	journal	September 2018
Singlet Fission Smith, Millicent B.; Michl, Josef Chemical Reviews, Vol. 110, Issue 11 https://doi.org/10.1021/cr1002613	journal	November 2010
Singlet Fission for Dye-Sensitized Solar Cells: Can a Suitable Sensitizer Be Found? Paci, Irina; Johnson, Justin C.; Chen, Xudong Journal of the American Chemical Society, Vol. 128, Issue 51 https://doi.org/10.1021/ja063980h	journal	December 2006
Quantum Beats in Crystalline Tetracene Delayed Fluorescence Due to Triplet Pair Coherences Produced by Direct Singlet Fission Burdett, Jonathan J.; Bardeen, Christopher J. Journal of the American Chemical Society, Vol. 134, Issue 20 https://doi.org/10.1021/ja301683w	journal	May 2012
Using Structurally Well-Defined Norbornyl-Bridged Acene Dimers to Map a Mechanistic Landscape for Correlated Triplet Formation in Singlet Fission Gilligan, Alexander T.; Miller, Ethan G.; Sammakia, Tarek Journal of the American Chemical Society, Vol. 141, Issue 14 https://doi.org/10.1021/jacs.9b00904	journal	March 2019
Experimental realization of Shor's quantum factoring algorithm using nuclear magnetic resonance Vandersypen, Lieven M. K.; Steffen, Matthias; Breyta, Gregory Nature, Vol. 414, Issue 6866 https://doi.org/10.1038/414883a	journal	December 2001
Unified model for singlet fission within a non-conjugated covalent pentacene dimer Basel, Bettina S.; Zirzlmeier, Johannes; Hetzer, Constantin Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15171	journal	May 2017
Strongly exchange-coupled triplet pairs in an organic semiconductor Weiss, Leah R.; Bayliss, Sam L.; Kraffert, Felix Nature Physics, Vol. 13, Issue 2 https://doi.org/10.1038/nphys3908	journal	October 2016
Quintet multiexciton dynamics in singlet fission Tayebjee, Murad J. Y.; Sanders, Samuel N.; Kumarasamy, Elango Nature Physics, Vol. 13, Issue 2 https://doi.org/10.1038/nphys3909	journal	October 2016
Identifying triplet pathways in dilute pentacene films Lubert-Perquel, Daphné; Salvadori, Enrico; Dyson, Matthew Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-06330-x	journal	October 2018
Molecular spins for quantum computation Gaita-Ariño, A.; Luis, F.; Hill, S. Nature Chemistry, Vol. 11, Issue 4 https://doi.org/10.1038/s41557-019-0232-y	journal	March 2019
Progress towards creating optically addressable molecular qubits Fataftah, Majed S.; Freedman, Danna E. Chemical Communications, Vol. 54, Issue 98 https://doi.org/10.1039/c8cc07939k	journal	January 2018
Electron spin polarization generated by transport of singlet and quintet multiexcitons to spin-correlated triplet pairs during singlet fissions Matsuda, Saki; Oyama, Shinya; Kobori, Yasuhiro Chemical Science, Vol. 11, Issue 11 https://doi.org/10.1039/c9sc04949e	journal	January 2020
Paramagnetic Excitons in Molecular Crystals Sternlicht, Himan; McConnell, Harden M. The Journal of Chemical Physics, Vol. 35, Issue 5 https://doi.org/10.1063/1.1732146	journal	November 1961
Solar conversion efficiency of photovoltaic and photoelectrolysis cells with carrier multiplication absorbers Hanna, M. C.; Nozik, A. J. Journal of Applied Physics, Vol. 100, Issue 7 https://doi.org/10.1063/1.2356795	journal	October 2006
Fluctuating exchange interactions enable quintet multiexciton formation in singlet fission Collins, Miles I.; McCamey, Dane R.; Tayebjee, Murad J. Y. The Journal of Chemical Physics, Vol. 151, Issue 16 https://doi.org/10.1063/1.5115816	journal	October 2019
Time dependent correlations of entangled states with nondegenerate branches and possible experimental realization using singlet fission Bardeen, Christopher J. The Journal of Chemical Physics, Vol. 151, Issue 12 https://doi.org/10.1063/1.5117155	journal	September 2019
Quintet-triplet mixing determines the fate of the multiexciton state produced by singlet fission in a terrylenediimide dimer at room temperature Chen, Michelle; Krzyaniak, Matthew D.; Nelson, Jordan N. Proceedings of the National Academy of Sciences, Vol. 116, Issue 17 https://doi.org/10.1073/pnas.1820932116	journal	April 2019
Theory of two coupled triplet states: Application to bicarbene structures Benk, H.; Sixl, H. Molecular Physics, Vol. 42, Issue 4 https://doi.org/10.1080/00268978100100631	journal	March 1981
Singlet Exciton Fission and Tri plet-Tri plet Exciton Fusion in Crystalline Tet racene Pope, Martin; Geacintov, Nicholas E.; Vogel, Frank Molecular Crystals, Vol. 6, Issue 1 https://doi.org/10.1080/15421406908082953	journal	August 1969
Criteria for exact qudit universality Brennen, Gavin; O’Leary, Dianne; Bullock, Stephen Physical Review A, Vol. 71, Issue 5 https://doi.org/10.1103/PhysRevA.71.052318	journal	May 2005
Effects of Magnetic Fields on the Mutual Annihilation of Triplet Excitons in Anthracene Crystals Johnson, R. C.; Merrifield, R. E. Physical Review B, Vol. 1, Issue 2 https://doi.org/10.1103/PhysRevB.1.896	journal	January 1970
Excitons in molecular crystals from first-principles many-body perturbation theory: Picene versus pentacene Cudazzo, Pierluigi; Gatti, Matteo; Rubio, Angel Physical Review B, Vol. 86, Issue 19 https://doi.org/10.1103/PhysRevB.86.195307	journal	November 2012
The Usefulness of NMR Quantum Computing Warren;, W. S. Science, Vol. 277, Issue 5332 https://doi.org/10.1126/science.277.5332.1688	journal	September 1997
Polynomial-Time Algorithms for Prime Factorization and Discrete Logarithms on a Quantum Computer Shor, Peter W. SIAM Review, Vol. 41, Issue 2 https://doi.org/10.1137/S0036144598347011	journal	January 1999
Recent Advances in Singlet Fission Smith, Millicent B.; Michl, Josef Annual Review of Physical Chemistry, Vol. 64, Issue 1 https://doi.org/10.1146/annurev-physchem-040412-110130	journal	April 2013
Magnetic effects on triplet exciton interactions Merrifield, R. E. Pure and Applied Chemistry, Vol. 27, Issue 3 https://doi.org/10.1351/pac197127030481	journal	January 1971

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
chemical physics
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Title: Singlet fission for quantum information and quantum computing: the parallel JDE model

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