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The Journal of Physical Chemistry C

Understanding the Correlation of the Quantum Dephasing Time and Entangled Photon Interaction in Crystalline Tetracene Derivatives

Olusayo J. Ogunyemi, Chanchal Rani, Oleg P. Varnavski, Rumaisa Wajahath, Michael Norscia, Brock Malaikal, Yunfan Qiu, Shichao Sun, Yonghao Gu, Shaul Mukamel, Michael R. Wasielewski, Theodore G. Goodson III

Published Nov 14, 2024• 5 citations
Publisher

Abstract

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.

DOI
10.1021/acs.jpcc.4c05907

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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.
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.
Molecular quantum sensors represent a promising frontier for the detection of nuclear magnetic resonance signals and alternating current magnetic fields at the nanoscale, potentially reaching single-proton sensitivity. Although the triplet states T̂ of molecular pentacene provide a viable sensing architecture, the triplet pair states T̂T̂ produced by singlet fission of pentacene dimers could enable more flexible quantum manipulations through entanglement. In this work, we model the quantum sensing efficacy of a spin-polarized quintet manifold 5T̂T̂0,±1 in a photoexcited pentacene dimer generated via intramolecular singlet fission. Using a Lindblad master equation approach, we simulate the evolution of the triplet-pair state under standard dynamical decoupling sequences-including spin echo, XY4, and XY8-and provide a direct performance comparison to the traditional pentacene monomer benchmark. While both architectures exhibit comparable sensitivity for isolated single-spin detection, our findings indicate that the dimer architecture provides a superior interaction cross section for detecting small ensembles of nuclear spins. Analytical expressions derived for fluorescence modulation demonstrate that sensitivity is optimized in the low-magnetic field regime (≤0.01 T) and scales with the number of pulses in the sensing protocol. This study establishes a theoretical baseline for utilizing high-spin multi-excitonic states as chemically tunable, high-sensitivity quantum probes.
Molecular quantum sensors represent a promising frontier for the detection of nuclear magnetic resonance signals and alternating current magnetic fields at the nanoscale, potentially reaching single-proton sensitivity. Although the triplet states of molecular pentacene provide a viable sensing architecture, the triplet pair states produced by singlet fission of pentacene dimers could enable more flexible quantum manipulations through entanglement. In this work, we model the quantum sensing efficacy of a spin-polarized quintet manifold in a photoexcited pentacene dimer generated via intramolecular singlet fission. Using a Lindblad master equation approach, we simulate the evolution of the triplet pair state under standard dynamical decoupling sequences, including spin echo, XY4, and XY8 and provide a direct performance comparison to the traditional pentacene monomer benchmark. While both architectures exhibit comparable sensitivity for isolated single-spin detection, our findings indicate that the dimer architecture provides a superior interaction cross-section for detecting small ensembles of nuclear spins. Analytical expressions derived for fluorescence modulation demonstrate that sensitivity is optimized in the low-magnetic field regime and scales with the number of pulses in the sensing protocol. This study establishes a theoretical baseline for utilizing high-spin multi-excitonic states as chemically tunable, high-sensitivity quantum probes.
By utilizing entanglement property of photons the entangled two-photon absorption (ETPA) effect of an organic material, porphyrin dendrimer, is demonstrated through the comparison of the property of entangled photons to the property of quantum-correlated photons. The ETPA showed a cross-section 31 orders of magnitude higher than the cross-section of the classical two-photon absorption (TPA). This high cross-section is comparable to the cross-section of the resonant single-photon absorption. The entangled absorption effect is compared to the correlated TPA effect to determine the degree of correlation between the entangled and quantum correlated photon pairs. The experimental data describe the different degree of correlation of the non-entangled and entangled photon pairs by demonstrating linear and nonlinear relationship of the absorbed photon flux to the input photon flux. The linearity of the ETPA is an interesting quantum effect because the two-photon absorption is an inherently nonlinear process. Virtual state spectroscopy is also demonstrated as a novel spectroscopic method to investigate the properties of the virtual state from non-monotonic behavior of the cross-section which is represented by controlling temporal property of the entanglement. These results from the quantum spectroscopy methods show a unique quantum property which is not feasible to detect using classical methods.
Two-photon absorption (TPA) and other nonlinear interactions of molecules with time-frequency-entangled photon pairs have been predicted to display a variety of fascinating effects. Therefore, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This Tutorial presents a detailed theoretical study of one- and two-photon absorption by molecules, focusing on how to treat the quantum nature of light. We review some basic quantum optics theory and then we review the density-matrix (Liouville) derivation of molecular optical response, emphasizing how to incorporate quantum states of light into the treatment. For illustration, we treat in detail the TPA of photon pairs created by spontaneous parametric down conversion, with an emphasis on how quantum light TPA differs from that with classical light. In particular, we treat the question of how much enhancement of the TPA rate can be achieved using entangled states. This Tutorial includes a review of known theoretical methods and results as well as some extensions, especially the comparison of TPA processes that occur via far-off-resonant intermediate states only and those that involve off-resonant intermediate states by virtue of dephasing processes. A brief discussion of the main challenges facing experimental studies of entangled two-photon absorption is also given.