Multiexciton quintet state populations in a rigid pyrene-bridged parallel tetracene dimer
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- Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309, USA
- Department of Chemistry & Center for Applied Energy Research, University of Kentucky, Lexington, Kentucky 40506-0055, USA
- National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, Colorado 80401, USA
- Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309, USA, Renewable and Sustainable Energy Institute (RASEI), University of Colorado Boulder, Boulder, CO, 80309, USA
- National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, Colorado 80401, USA, Renewable and Sustainable Energy Institute (RASEI), University of Colorado Boulder, Boulder, CO, 80309, USA
The multiexciton quintet state, 5TT, generated as a singlet fission intermediate in pairs of molecular chromophores, is a promising candidate as a qubit or qudit in future quantum information science schemes. In this work, we synthesize a pyrene-bridged parallel tetracene dimer, TPT, with an optimized interchromophore coupling strength to prevent the dissociation of 5TT to two decorrelated triplet (T1) states, which would contaminate the spin-state mixture. Long-lived and strongly spin-polarized pure 5TT state population is observed via transient absorption spectroscopy and transient/pulsed electron paramagnetic resonance spectroscopy, and its lifetime is estimated to be >35 µs, with the dephasing time ($$T_2$$) for the 5TT-based qubit measured to be 726 ns at 10 K. Direct relaxation from 1TT to the ground state does diminish the overall excited state population, but the exclusive 5TT population at large enough persistent density for pulsed echo determination of spin coherence time is consistent with recent theoretical models that predict such behavior for strict parallel chromophore alignment and large exchange coupling.
- Research Organization:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Organization:
- USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF)
- Grant/Contract Number:
- AC36-08GO28308; CHE-2102713; DMR 1627428
- OSTI ID:
- 2067640
- Alternate ID(s):
- OSTI ID: 2217126
- Report Number(s):
- NREL/JA-5900-86990; CSHCBM
- Journal Information:
- Chemical Science, Journal Name: Chemical Science Vol. 14 Journal Issue: 41; ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry (RSC)Copyright Statement
- Country of Publication:
- United Kingdom
- Language:
- English
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