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Creators/Authors contains: "Cai, Kang"

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  1. One of the key questions in quantum information is the preparation of desired multipartite quantum states with high fidelity. Adiabatic evolution has been widely explored to achieve state preparation in quantum many-body systems. However, in noisy quantum systems, the adiabatic approach faces a dilemma: either extending the evolution timescales to reduce diabatic transitions or shortening the timescales to mitigate decoherence effects. Various quantum control approaches have been studied to resolve this dilemma. In a few recent works, we utilized Jaynes-Cummings (JC) lattices as a platform to investigate the potential of several quantum control techniques in preparing quantum many-body states, including the optimized adiabatic evolution approach, the quantum optimal control technique, and quantum shortcuts to adiabaticity. Here we first give an overview of our previous results on utilizing quantum optimal control in JC lattices with unit filling and utilizing local counterdiabatic driving in JC lattices with a single excitation. Then we present our results on the energy costs and energy fluctuations in these approaches. Our studies give insights into the implementation of different approaches in practical quantum devices and the connection between the energy costs and the quantum speed limit in preparing desired quantum many-body states for quantum simulation and quantum computation. 
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    Free, publicly-accessible full text available December 1, 2025
  2. Abstract Strongly correlated polaritons in Jaynes–Cummings (JC) lattices can exhibit quantum phase transitions between the Mott-insulating and superfluid phases at integer fillings. The prerequisite to observe such phase transitions is to pump polariton excitations into a JC lattice and prepare them into appropriate ground states. Despite previous efforts, it is still challenging to generate many-body states with high accuracy. Here, we present an approach for the robust preparation of many-body ground states of polaritons in finite-sized JC lattices by optimized nonlinear ramping. We apply a Landau–Zener type of estimation to this finite-sized system and derive the optimal ramping index for selected ramping trajectories, which can greatly improve the fidelity of the prepared states. With numerical simulation, we show that by choosing an appropriate ramping trajectory, the fidelity in this approach can remain close to unity in almost the entire parameter space. This approach can shed light on high-fidelity state preparation in quantum simulators and advance the implementation of quantum simulation with practical devices. 
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  3. Abstract Two-photon excited near-infrared fluorescence materials have garnered considerable attention because of their superior optical penetration, higher spatial resolution, and lower optical scattering compared with other optical materials. Herein, a convenient and efficient supramolecular approach is used to synthesize a two-photon excited near-infrared emissive co-crystalline material. A naphthalenediimide-based triangular macrocycle and coronene form selectively two co-crystals. The triangle-shaped co-crystal emits deep-red fluorescence, while the quadrangle-shaped co-crystal displays deep-red and near-infrared emission centered on 668 nm, which represents a 162 nm red-shift compared with its precursors. Benefiting from intermolecular charge transfer interactions, the two co-crystals possess higher calculated two-photon absorption cross-sections than those of their individual constituents. Their two-photon absorption bands reach into the NIR-II region of the electromagnetic spectrum. The quadrangle-shaped co-crystal constitutes a unique material that exhibits two-photon absorption and near-infrared emission simultaneously. This co-crystallization strategy holds considerable promise for the future design and synthesis of more advanced optical materials. 
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  4. Abstract Complexation between a viologen radical cation (V.+) and cyclobis(paraquat‐p‐phenylene) diradical dication (CBPQT2(.+)) has been investigated and utilized extensively in the construction of mechanically interlocked molecules (MIMs) and artificial molecular machines (AMMs). The selective recognition of a pair ofV.+using radical‐pairing interactions, however, remains a formidable challenge. Herein, we report the efficient encapsulation of two methyl viologen radical cations (MV.+) in a size‐matched bisradical dicationic host — namely, cyclobis(paraquat‐2,6‐naphthalene)2(.+), i.e.,CBPQN2(.+). Central to this dual recognition process was the choice of 2,6‐bismethylenenaphthalene linkers for incorporation into the bisradical dicationic host. They provide the space between the two bipyridinium radical cations inCBPQN2(.+)suitable for binding twoMV.+with relatively short (3.05–3.25 Å) radical‐pairing distances. The size‐matched bisradical dicationic host was found to exhibit highly selective and cooperative association with the twoMV.+in MeCN at room temperature. The formation of the tetrakisradical tetracationic inclusion complex — namely, [(MV)2⊂CBPQN]4(.+)– in MeCN was confirmed by VT1H NMR, as well as by EPR spectroscopy. The solid‐state superstructure of [(MV)2⊂CBPQN]4(.+)reveals an uneven distribution of the binding distances (3.05, 3.24, 3.05 Å) between the three differentV.+, suggesting that localization of the radical‐pairing interactions has a strong influence on the packing of the twoMV.+inside the bisradical dicationic host. Our findings constitute a rare example of binding two radical guests with high affinity and cooperativity using host‐guest radical‐pairing interactions. Moreover, they open up possibilities of harnessing the tetrakisradical tetracationic inclusion complex as a new, orthogonal and redox‐switchable recognition motif for the construction of MIMs and AMMs. 
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