MPS/CHE-EPSRC: A New Framework for Exploring and Exploiting Quantum Correlations in Molecular Singlet Fission

University Of Texas At Austin, Austin TX

Investigators

Abstract

With support from the Division of Chemistry, Professors Sean Roberts of the University of Texas at Austin and Niels Damrauer of the University of Colorado Boulder, together with collaborators from the University of Sheffield in the United Kingdom, will investigate unique quantum states generated by singlet fission. During singlet fission, an excited molecule shares half of its energy with a neighbor, placing both molecules into an entangled quantum state wherein actions that impact one molecule also impact the other. However, developing materials that produce these states requires an improved understanding of the singlet fission process. To achieve this goal, Professors Roberts, Damrauer and their UK collaborators will develop rigid molecular dimers and oligomers that undergo singlet fission and use ultrafast optical and magnetic resonance spectroscopies, along with open quantum-systems theory, to characterize their ability to generate and sustain quantum mechanical entanglement. Their discoveries could further our fundamental understanding of the role that entanglement plays in excited state phenomena, as well as have implications for quantum-based technologies in sensing and chemical catalysis. The project will also create research opportunities for graduate students in advanced quantum information science, thereby contributing to the development of a quantum-enabled workforce. This award is made under the NSF-UKRI lead agency opportunity. Singlet fission converts a spin-singlet exciton into a pair of spin-triplet excitons in molecular systems. Due to their generation from a single excited species, triplet pairs created by singlet fission are spin-entangled upon their production. This entanglement offers potential to design systems for chemical catalysis and sensing that exhibit unique quantum advantages, where the actions that impact one member of a triplet pair can alter the behavior of its counterpart. To evaluate this potential, the team will develop molecular systems that undergo singlet fission and vet their ability to drive multielectron transfer reactions wherein each exciton within an entangled triplet pair simultaneously acts as a charge donor. These efforts will be guided by a theoretical framework developed for describing the creation of entangled states via singlet fission and their subsequent dynamics. In addition to facilitating gains in our fundamental understanding of singlet fission, this project will bring together physicists working on open quantum systems with synthetic and physical chemists to develop a common language and new research tools that will accelerate the exchange of ideas across these distinct disciplines. This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.