Macrocyclic Parallel Dimer Showing Quantum Coherence of Quintet Multiexcitons at Room Temperature
Singlet fission (SF) is a promising approach in quantum information science because it can generate spin-entangled quintet triplet pairs by photoexcitation independent of temperature. However, it is still challenging to rationally achieve quantum coherence at room temperature, which requires precise control of the orientation and dynamics of triplet pairs. Here we show that the quantum coherence of quintet multiexcitons can be achieved at room temperature by arranging two pentacene chromophores in parallel and in close proximity within a macrocycle. By making dynamic covalent Schiff-base bonds between aldehyde-modified pentacene derivatives, macrocyclic parallel dimer-1 (<b>MPD-1</b>) can be selectively synthesized in a high yield. <b>MPD-1</b> exhibits fast subpicosecond SF in polystyrene film and generates spin-polarized quintet multiexcitons. Furthermore, the coherence time <i>T</i><sub>2</sub> of the <b>MPD-1</b> quintet is as long as 648 ns, even at room temperature. This macrocyclic parallel dimer strategy opens up new possibilities for future quantum applications using molecular multilevel qubits.
Authors
- Samara Medina Rivero (ORCID: https://orcid.org/0000-0003-4490-4813)
- Yasuhiro Kobori (ORCID: https://orcid.org/0000-0001-8370-9362)
- Akio Yamauchi (ORCID: https://orcid.org/0009-0006-2340-5790)
- Masaaki Fuki (ORCID: https://orcid.org/0000-0002-8779-5250)
- Masanori Uji (ORCID: https://orcid.org/0009-0001-6521-9236)
- Bhavesh Parmar (ORCID: https://orcid.org/0000-0003-4263-7635)
- Jenny Clark (ORCID: https://orcid.org/0000-0001-9664-967X)
- Go Watanabe (ORCID: https://orcid.org/0000-0001-6713-1249)
- Wataru Ishii (ORCID: https://orcid.org/0000-0002-4992-2255)
- Shunsuke Sato (ORCID: https://orcid.org/0000-0002-3915-7895)
- Nobuhiro Yanai (ORCID: https://orcid.org/0000-0003-0297-6544)
- Catherine Helenna Mulyadi (ORCID: https://orcid.org/0009-0000-1729-0356)
- Eman M. Bu Ali
Institutions
- Kyushu University (JP)
- Japan Science and Technology Agency (JP)
- Kanagawa Industrial Technology Center (JP)
- King Faisal University (SA)
- Kitasato University (JP)
- Kobe University (JP)
- The University of Tokyo (JP)
- Universidad de Málaga (ES)
- University of Sheffield (GB)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2024-09-09
- DOI
- https://doi.org/10.1021/jacs.4c05677
- Citations
- 13
- Primary Topic
- Spectroscopy and Quantum Chemical Studies
- Type
- article
- Field-Weighted Citation Impact
- 4.39
Funders
- Universidad de Málaga
- Saudi Arabian Cultural Bureau
- Kobe University
- European Commission
- Kyushu University
- King Faisal University
- Engineering and Physical Sciences Research Council
- Japan Society for the Promotion of Science
- Core Research for Evolutional Science and Technology