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Journal of the American Chemical Society

Using Molecular Design to Enhance the Coherence Time of Quintet Multiexcitons Generated by Singlet Fission in Single Crystals

Robert M. Jacobberger, Yunfan Qiu, Malik L. Williams, Matthew D. Krzyaniak, Michael R. Wasielewski

Published Jan 31, 2022• 84 citations
Publisher

Abstract

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 information science. However, the factors that determine the spin coherence of these states remain underexplored. Here, we engineer the packing of tetracene molecules within single crystals of 5,12-bis(tricyclohexylsilylethynyl)tetracene (TCHS–tetracene) to demonstrate a 5 (TT) state that exhibits promising spin qubit properties, including a coherence time, T 2, = 3 μs at 10 K, a population lifetime, T pop, = 130 μs at 5 K, and stability even at room temperature. The single-crystal platform also enables global alignment of the spins and, consequently, individual addressability of the spin-sublevel transitions. Decoherence mechanisms, including exciton diffusion, electronic dipolar coupling, and nuclear hyperfine interactions, are elucidated, providing design principles for increasing T 2 and the operational temperature of 5 (TT). By dynamically decoupling 5 (TT) from the surrounding spin bath, T 2 = 10 μs is achieved. These results demonstrate the viability of harnessing singlet fission to initiate multiple electron spins in a well-defined quantum state for next-generation molecular-based quantum technologies.

DOI
10.1021/jacs.1c12414

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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 information science. However, the factors that determine the spin coherence of these states remain underexplored. Here, we engineer the packing of tetracene molecules within single crystals of 5,12-bis(tricyclohexylsilylethynyl)tetracene (TCHS–tetracene) to demonstrate a 5 (TT) state that exhibits promising spin qubit properties, including a coherence time, T 2, = 3 μs at 10 K, a population lifetime, T pop, = 130 μs at 5 K, and stability even at room temperature. The single-crystal platform also enables global alignment of the spins and, consequently, individual addressability of the spin-sublevel transitions. Decoherence mechanisms, including exciton diffusion, electronic dipolar coupling, and nuclear hyperfine interactions, are elucidated, providing design principles for increasing T 2 and the operational temperature of 5 (TT). By dynamically decoupling 5 (TT) from the surrounding spin bath, T 2 = 10 μs is achieved. These results demonstrate the viability of harnessing singlet fission to initiate multiple electron spins in a well-defined quantum state for next-generation molecular-based quantum technologies.
Quantum-to-quantum transduction is the coherent exchange of information between quantum systems, which is an essential element of quantum information science (QIS). Molecular architectures provide unmatched flexibility for tailoring the properties that are critical to quantum transduction, and molecular synthesis affords the opportunity to build novel molecular materials from the bottom-up. Singlet fission (SF) in organic chromophore solids provides a potential means of executing photon-to-spin quantum transduction because absorption of a single photon results in formation of four entangled spins that constitute a triplet pair state (TT). We have demonstrated that SF in single crystals of 5,12-bis(tricyclohexylsilylethynyl)-tetracene (TCHS-tetracene) produces a long-lived quintet state 5 (TT) that provides a promising new route to multiqubit systems for QIS. Here, we investigate the interaction of classical and entangled photons with TCHS-tetracene as well as the related TIPS-tetracene and tetracene to assess the molecular properties required for quantum transduction. From the classical two-photon absorption (TPA) experiment, we observed that TCHS-tetracene and TIPS-tetracene have a higher TPA cross-section than tetracene. The entangled TPA cross-sections of TCHS-tetracene and TIPS-tetracene (6.914 × 10 –19 and 5.057 × 10 –19 cm 2 /molecule, respectively) are about an order of magnitude larger than that of tetracene (5.146 × 10 –20 cm 2 /molecule), making TCHS-tetracene and TIPS-tetracene excellent candidates for demonstrating photon-to-spin transduction using SF. We also observed a longer coherence time for the TCHS-tetracene in comparison to the tetracene molecular systems investigated, which suggests its suitability for possible QIS applications.
Abstract Organic high electron spin states, such as quintet state, can be used as multiple quantum bits for implementing quantum information. However, the practical quintet state via singlet fission is generally observed in strict conditions. Achieving long‐term quantum coherence of quintets at room temperature is still challenging. Here, quantum coherence in electron quintet states up to 505 ns at room temperature is observed, enabling quantum operations up to 54 times. Detailed investigations show that two Rabi oscillations from the multiple levels of the quintet are detectable at room temperature, with frequencies of 1.69 ± 0.01 and 1.39 ± 0.01 times of that of triplet states, respectively. More importantly, this quintet derived from singlet fission process can be realized via a simple co‐melting technology with amorphous form of 6,13‐bis(triisopropylsilylethynyl)pentacene dopped 1,3,5‐tri(1‐naphthyl)benzene (TIPS‐Pn:TNB). The organic TNB host with light elements is helpful for achieving long decoherence time. This study not only proves a simple method for preparing controllable quintet state at room temperature, but also emphasizes the opportunities of organic high electron spin states in quantum information science for working at low‐cost and friendly condition.
Optically addressable molecular triplet spins provide a chemically tunable platform for quantum application, but their coherence is often limited by interactions with surrounding spin baths. Here we demonstrate controlled suppression of nuclear-bath-induced decoherence in photoexcited triplet spins of pentacene co-crystallized in high-purity naphthalene single crystals. By hyperpolarizing the proton spin bath through triplet dynamic nuclear polarization (triplet-DNP), magnetic noise generated by the nuclear spins is suppressed, leading to an extension of the electron spin transverse coherence time. Experimentally, we observe a 25\% enhancement of the spin-echo decay time with 60%60\%60% polarization of the proton spin bath. The measured scaling of the spin-echo decay time (T2T_2T2​) with nuclear polarization quantitatively follows the predicted dependence derived from the polarization-controlled nuclear second moment. Both the enhancement and the absolute value of the coherence time are quantitatively reproduced by cluster correlation expansion (CCE) simulations. These results establish nuclear spin hyperpolarization as a general and actively tunable approach to engineering coherence in molecular qubits. This work provides a broadly applicable design framework for high-coherence molecular and solid-state spin systems.
The identification of molecules that combine long spin coherence times and efficient spin-optical interfaces, ideally at room temperature, is pivotal towards the development of molecular quantum technology. By means of advanced first-principles methods, we here unravel the electronic structure for triangulene (1), its aza-cation derivative (2), and the crystal of 2,6,10-tri-tert-butyl-4,8,12-trimesityl-triangulene (3), and show that these organic diradicals possess a triplet ground state well separated from the first singlet excited state approaching 0.5 eV, closely resembling solid-state defects like nitrogen vacancy centers. In addition, we compute spin decoherence times due to the interaction with phonons and surrounding nuclear spins, showing that a deuterated molecule of 3 in a nuclear spin-free environment would support T2=0.21T_2 = 0.21T2​=0.21 ms at 10 K. Importantly, we show that the engineering of specific low-energy vibrations could significantly improve T2T_2T2​ toward the limit imposed by the molecular core spin relaxation, here estimated to be as long as T1=27T_1=27T1​=27 ms at 300 K for 2. Finally, we compute two-phonon contributions to inter-system crossing at 300 K for2 as a luminescent prototype, and find that it is highly spin-selective, supporting the possibility to engineer optical read out and spin initialization. These results advance a unified first-principles theoretical foundation of spin decoherence and spin-selective excited-state processes and point to novel chemical design strategies for optically addressable, highly coherent molecular qubits.
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.
Excitonic quantum batteries, based on organic fluorescent molecules embedded in optical microcavities, offer a room-temperature platform for studying collective effects in energy storage and developing applications. Recent experiments have offered evidence of superabsorption, a collective enhancement to the light absorption rate of organic molecules which leads to a scalable power density. However, they have also highlighted the challenge posed by rapid radiative decay of fluorescent molecules, which limits the energy storage lifetime. Current strategies to overcome this trade-off focus on controlling the coupling between the absorbing manifold and that used for energy storage. In this chapter, we review three implementations of this design principle: transferring energy from optically excited states to long-lived dark triplet states, generating triplet pairs and higher-spin states through singlet exciton fission, and forming charge-separated states. We discuss each mechanism from both theoretical and experimental perspectives, with particular emphasis on recent device implementations that have extended storage times by several orders of magnitude. We conclude with a cross-platform outlook on the role of metastable states across coherent and room-temperature implementations, from neutral atom arrays to masers and colour centres.