Pair Of States Research Articles

Morphology- and crystal packing-dependent singlet fission and photodegradation in functionalized tetracene crystals and films.

Singlet fission (SF) is a charge carrier multiplication process that has potential for improving the performance of (opto)electronic devices from the conversion of one singlet exciton S1 into two triplet excitons T1 via a spin-entangled triplet pair state 1(TT). This process depends highly on molecular packing and morphology, both for the generation and dissociation of 1(TT) states. Many benchmark SF materials, such as acenes, are also prone to photodegradation reactions, such as endoperoxide (EPO) formation and photodimerization, which inhibit realization of SF devices. In this paper, we compare functionalized tetracenes R-Tc with two packing motifs: "slip-stack" packing in R = TES, TMS, and tBu and "gamma" packing in R = TBDMS to determine the effects of morphology on SF as well as on photodegradation using a combination of temperature and magnetic field dependent spectroscopy, kinetic modeling, and time-dependent density functional theory. We find that both "slip-stack" and "gamma" packing support SF with high T1 yield at room temperature (up to 191% and 181%, respectively), but "slip-stack" is considerably more advantageous at low temperatures (<150K). In addition, each packing structure has a distinct emissive relaxation pathway competitive to SF, while the states involved in the SF itself are dark. The "gamma" packing has superior photostability, both in regards to EPO formation and photodimerization. The results indicate that the trade-off between SF efficiency and photostability can be overcome with material design, emphasize the importance of considering both photophysical and photochemical properties, and inform efforts to develop optimal SF materials for (opto)electronic applications.

Dual-Isometric Projected Entangled Pair States.

Efficient characterization of higher dimensional many-body physical states presents significant challenges. In this Letter, we propose a new class of projected entangled pair states (PEPS) that incorporates two isometric conditions. This new class facilitates the efficient calculation of general local observables and certain two-point correlation functions, which have been previously shown to be intractable for general PEPS, or PEPS with only a single isometric constraint. Despite incorporating two isometric conditions, our class preserves the rich physical structure while enhancing the analytical capabilities. It features a large set of tunable parameters, with only a subleading correction compared to that of general PEPS. Furthermore, we analytically demonstrate that this class can encode universal quantum computation and can represent a transition from topological to trivial order.

Singlet, triplet, and mixed all-to-all pairing states emerging from incoherent fermions

The electron-electron and electron-phonon coupling in complex materials can be more complicated than simple density-density interactions, involving intertwined dynamics of spin, charge, and spatial symmetries. This motivates studying universal models with complex interactions and whether BCS-type singlet pairing is still the “natural” fate of the system. To this end, we construct a Yukawa-SYK model with nonlocal couplings in both spin and charge channels. Furthermore, we provide for time-reversal-symmetry breaking dynamics by averaging over the Gaussian unitary ensemble rather than the orthogonal ensemble. We find that the ground state of the system can be an orbitally nonlocal superconducting state arising from incoherent fermions with no BCS-like analog. The superconductivity has an equal tendency to triplet and singlet pairing states separated by a non-Fermi liquid phase. We further study the fate of the system within the superconducting phase and find that the expected ground state, away from the critical point, is a mixed singlet/triplet state. Finally, we find that, while at Tc the triplet and singlet transitions are dual to one another, below Tc the duality is broken, with the triplet state more susceptible to orbital fluctuations just by its symmetry. Our results indicate that such fluctuation-induced mixed states may be an inherent feature of strongly correlated materials. Published by the American Physical Society 2024

A generalization of quantum pair state transfer

A generalization of quantum pair state transfer

Ab Initio Molecular Dynamics Studies of Stacked Adenine–Thymine and Guanine–Cytosine Nucleic Acid Base Pairs in Aqueous Solution

Ab initio MD studies have been performed on stacked adenine–thymine (A–T) and guanine–cytosine (G–C) nucleobase pairs solvated in water using Born–Oppenheimer molecular dynamics. These two systems have been analyzed using RDF, SDF, angle–distance CDF (combined distribution functions), plane projection analysis, hydrogen bond analysis, and non–covalent interaction (NCI) plots. The stacking property studies have shown that the molecular orientation of the A–T pair is completely opposite to that of the G–C pair though the center of mass distance between the two molecules is similar. The G–C pair shows significantly more stability in water than the A–T system does. RDF analyses show that the –NH– group and carbonyl groups show predominant interaction with water molecules. Water molecules are found to be most in numbers around the cytosine molecule and least around the adenine molecule. Hydrogen bonding studies show that the guanine molecule forms the highest number of hydrogen bonds with water molecules. On the other hand, the hydrogen atom attached to the –NH– group of adenine molecule shows the longest mean H–bond lifetime with water oxygen atoms. NCI interactions calculated through the ab initio method help us to visualize the [Formula: see text]-electron stacking and H–bonding between aromatic nucleobases and water molecules. A great shift in bond polarity and interaction intensity in different functional groups is observed for the nucleobases going from individually solvated molecules to paired states.

Molecule‐level Design to Form Pocket Structures for Improving Amine Efficiency in CO2 Capture

AbstractSolid amine adsorbents represent a promising class of CO2 sorbents, but their amine efficiency is limited by the inaccessibility of peripheral amines. The surface of mesocellular silica foam (MCF) is functionalized with the mixture of short‐chain 3‐Glycidyloxypropyl) triethoxysilane (GPTES) and long‐chain Octadecyltrimethoxysilane (OTMS), forming pocket structures on the support surface, thereby exposing more amine sites and enhancing the amine efficiency of polyethylenimine (PEI). The resulting adsorbent demonstrates a high CO2 adsorption capacity (5.02 mmol g−1 at 50 °C, 10 vol.% CO2, and 50%RH), high amine efficiency (0.43 at the dry condition), outstanding cyclic stability (0.5% performance decline per cycle under the conditions of dry CO2 regeneration), and fast adsorption kinetics (15 min for adsorption saturation at 50 °C). First‐principles calculations and CO2 temperature‐programmed desorption (TPD) experiments demonstrate that the introduction of GPTES and OTMS is beneficial to decreasing adsorption energy and forming paired carbamic acid states and ammonium carbamate states.

Exact Thermal Eigenstates of Nonintegrable Spin Chains at Infinite Temperature.

The eigenstate thermalization hypothesis (ETH) plays a major role in explaining thermalization of isolated quantum many-body systems. However, there has been no proof of the ETH in realistic systems due to the difficulty in the theoretical treatment of thermal energy eigenstates of nonintegrable systems. Here, we write down analytically thermal eigenstates of nonintegrable spin chains. We consider a class of theoretically tractable volume-law states, which we call entangled antipodal pair (EAP) states. These states are thermal, in the most fundamental sense that they are indistinguishable from the Gibbs state with respect to all local observables, with infinite temperature. We then identify Hamiltonians having the EAP state as an eigenstate and rigorously show that some of these Hamiltonians are nonintegrable. Furthermore, a thermal pure state at an arbitrary temperature is obtained by the imaginary time evolution of an EAP state. Our results offer a potential avenue for providing a provable example of the ETH.

Multiqubit quantum state preparation enabled by topology optimization

Using topology optimization, we inverse-design nanophotonic cavities enabling the preparation of pure states of pairs and triples of quantum emitters. Our devices involve moderate values of the dielectric constant, operate under continuous laser driving, and yield fidelities to the target (Bell and W) states approaching unity for distant qubits (several natural wavelengths apart). In the fidelity optimization procedure, our algorithm generates entanglement by maximizing the dissipative coupling between the emitters, which allows the formation of multipartite pure steady states in the driven-dissipative dynamics of the system. Our findings open the way toward the efficient and fast preparation of multiqubit quantum states with engineered features, with potential applications for nonclassical light generation, and quantum sensing and metrology.

Engineering Rydberg-pair interactions in divalent atoms with hyperfine-split ionization thresholds

Quantum information processing with neutral atoms relies on Rydberg excitation for entanglement generation. While the use of heavy divalent or open-shell elements, such as strontium or ytterbium, has benefits due to their optically active core and a variety of possible qubit encodings, their Rydberg structure is generally complex. For some isotopes in particular, hyperfine interactions are relevant even for highly excited electronic states. We employ multichannel quantum defect theory to infer the Rydberg structure of isotopes with nonzero nuclear spin and perform nonperturbative Rydberg-pair interaction calculations. We find that due to the high level density and sensitivities to external fields, experimental parameters must be precisely controlled. Specifically in Sr87, we study an intrinsic Förster resonance, unique to divalent atoms with hyperfine-split thresholds, which simultaneously provides line stability with respect to external field fluctuations and enhanced long-range interactions. Additionally, we provide parameters for pair states that can be effectively described by single-channel Rydberg series. The explored pair states provide exciting opportunities for applications in the blockade regime, as well as for more exotic long-range interactions such as largely flat, distance-independent potentials. Published by the American Physical Society 2024

A hybrid method integrating Green’s function Monte Carlo and projected entangled pair states

Abstract This paper introduces a hybrid approach combining Green’s function Monte Carlo (GFMC) method with projected entangled pair state (PEPS) ansatz. This hybrid method regards PEPS as a trial state and a guiding wave function in GFMC. By leveraging PEPS’s proficiency in capturing quantum state entanglement and GFMC’s efficient parallel architecture, the hybrid method is well-suited for the accurate and efficient treatment of frustrated quantum spin systems. As a benchmark, we applied this approach to study the frustrated J 1–J 2 Heisenberg model on a square lattice with periodic boundary conditions (PBCs). Compared with other numerical methods, our approach integrating PEPS and GFMC shows competitive accuracy in the performance of ground-state energy. This paper provides systematic and comprehensive discussion of the approach of our previous work [Phys. Rev. B 109 235133 (2024)].

Strong-Coupling Modification of Singlet-Fission Dynamical Pathways.

We investigate theoretically the influence of strong light-matter coupling on the initial steps of the phototriggered singlet-fission process. In particular we focus on intramolecular singlet fission in a TIPS-pentacene dimer derivative described by a vibronic Hamiltonian including the optically active singlet excited states, doubly excited and charge transfer states, as well as the final triplet-triplet pair state. Quantum dynamics simulations of up to four dimers in the cavity indicate that the modified resonance condition imposed by the cavity strongly quenches the passage through the intermediate charge transfer and double-excitation states, thus largely reducing the triplet-triplet yield in the bare system. Subsequently, we modify the system parameters and construct a model Hamiltonian where the optically active singlet excitation lies below the final triplet-triplet state such that the yield of the bare system becomes insignificant. In this case we find that using the upper polariton as the doorway state for photoexcitation can lead to a much enhanced yield. This pathway is operative provided that the system is sufficiently rigid to prevent vibronic losses from the upper polariton to the dark-states manifold.

Cultural heritage and modernization: the evolution of Lifen neighborhoods in Wuhan

ABSTRACT The paper probes into the modernization and conservation of Hankou old Lifen which is a typical residential building with high historical value in Wuhan, China. This research emphasizes the range of government and community structures, using analysis on three different modernization models: Xian’an Fang, Changnian Li, and Tongxing Li. This includes qualitative analysis using a mixed method approach; on-site observation with photography to capture the spatial features as well as narratives from residents within these areas; and semi-structured interviews. The findings highlight the importance of conserving Lifen neighborhoods in view of its historical knowledge, cultural legacy and other urban development experience. In the end, maintaining and evolving them can be sustainable only through a hybrid that pairs state support with community involvement. This research provides key insights for policymakers, urban planners and conservationists working to balance heritage preservation with the contemporary needs of cities.

Real Topological Phonons in 3D Carbon Allotropes.

There has been a significant focus on real topological systems that enjoy space-time inversion symmetry and lack spin-orbit coupling. While the theoretical classification of the real topology has been established, more progress has yet to be made in the materials realization of real topological phononic states in 3D. To address this crucial issue, high-throughput computing is performed to inspect the real topology in the phonon spectrums of the 3D carbon allotropes. Among 1661 carbon allotropes listed in the Samara Carbon Allotrope Database (SACADA), 79 candidates host a phononic real Chern insulating (PRCI) state, 2 candidates host a phononic real nodal line (PRNL) state, 12 candidates host a phononic real Dirac point (PRDP) state, and 10 candidates host a phononic real triple-point pair (PRTPP) state. The PRCI, PRNL, PRTPP, and PRDP states of 27-SG. 166-pcu-h, 1081-SG. 194-42T13-CA, 52-SG. 141-gis, and 132-SG. 191-3,4T157 are exhibited as illustrative examples, and the second-order phononic hinge modes are explored. This study broadens the understanding of 3D topological phonons and expands the material candidates with phononic hinge modes and phononic realtopology.

Gauged Gaussian projected entangled pair states: A high dimensional tensor network formulation for lattice gauge theories

Gauge theories form the basis of our understanding of modern physics—ranging from the description of quarks and gluons to effective models in condensed matter physics. In the nonperturbative regime, gauge theories are conventionally treated discretely as lattice gauge theories. The resulting systems are evaluated with path-integral based Monte Carlo methods. These methods, however, can suffer from the sign problem and do not allow for a direct evaluation of real-time dynamics. In this work, we present a unified and comprehensive framework for gauged Gaussian projected entangled pair states (PEPS), a variational ansatz based on tensor networks. We review the construction of Hamiltonian lattice gauge theories, explain their similarities to PEPS, and detail the construction of the ansatz state. The estimation of ground states is based on a variational Monte Carlo procedure with the PEPS as an ansatz state. This sign-problem-free ansatz can be efficiently evaluated in any dimension with arbitrary gauge groups, and can include dynamical fermionic matter, suggesting new options for the simulation of nonperturbative regimes of gauge theories, including quantum chromodynamics. Published by the American Physical Society 2024

Configuration Interaction in Frontier Molecular Orbital Basis for Screening the Spin-Correlated, Spatially Separated Triplet Pair State 1(T···T) Formation.

In the theoretical screening of Singlet Fission rates in molecular aggregates, often the frontier molecular orbital model for dimers is employed. However, the dimer approach fails to account for recent experimental findings that suggest singlet fission progresses through a further intermediate state featuring two spatially separated, spin-correlated triplets, specifically a 1(T···T) state. We address this limitation by generalizing the often used frontier molecular orbital model for singlet fission by incorporation of both separated Charge Transfer (C···T) and 1(T···T) states as well as mixed triplet-charge transfer states, delivering analytic expressions for the diabatic matrix elements. Applying the methodology to the perylene diimide trimer, we examine the packing dependence of competing formation pathways of the 1(T···T) state by evaluation of diabatic matrix elements.

An introduction to infinite projected entangled-pair state methods for variational ground state simulations using automatic differentiation

Tensor networks capture large classes of ground states of phases of quantum matter faithfully and efficiently. Their manipulation and contraction has remained a challenge over the years, however. For most of the history, ground state simulations of two-dimensional quantum lattice systems using (infinite) projected entangled pair states have relied on what is called a time-evolving block decimation. In recent years, multiple proposals for the variational optimization of the quantum state have been put forward, overcoming accuracy and convergence problems of previously known methods. The incorporation of automatic differentiation in tensor networks algorithms has ultimately enabled a new, flexible way for variational simulation of ground states and excited states. In this work we review the state-of-the-art of the variational iPEPS framework, providing a detailed introduction to automatic differentiation, a description of a general foundation into which various two-dimensional lattices can be conveniently incorporated, and demonstrative benchmarking results.

Multiexperience-Assisted Efficient Multiagent Reinforcement Learning.

Recently, multiagent reinforcement learning (MARL) has shown great potential for learning cooperative policies in multiagent systems (MASs). However, a noticeable drawback of current MARL is the low sample efficiency, which causes a huge amount of interactions with environment. Such amount of interactions greatly hinders the real-world application of MARL. Fortunately, effectively incorporating experience knowledge can assist MARL to quickly find effective solutions, which can significantly alleviate the drawback. In this article, a novel multiexperience-assisted reinforcement learning (MEARL) method is proposed to improve the learning efficiency of MASs. Specifically, monotonicity-constrained reward shaping is innovatively designed using expert experience to provide additional individual rewards to guide multiagent learning efficiently, with the invariance guarantee of the team optimization objective. Furthermore, a reward distribution estimator is specially developed to model an implicated reward distribution of environment by using transition experience from environment, containing collected samples (state-action pair, reward, and next state). This estimator can predict the expectation reward of each agent for the taken action to accurately estimate the state value function and accelerate its convergence. Besides, the performance of MEARL is evaluated on two multiagent environment platforms: our designed unmanned aerial vehicle combat (UAV-C) and StarCraft II Micromanagement (SCII-M). Simulation results demonstrate that the proposed MEARL can greatly improve the learning efficiency and performance of MASs and is superior to the state-of-the-art methods in multiagent tasks.

Polarization-entangled photon-pair source with van der Waals 3R-WS2 crystal

Ultracompact entangled photon sources are pivotal to miniaturized quantum photonic devices. Van der Waals (vdW) nonlinear crystals promise efficient photon-pair generation and on-chip monolithic integration with nanophotonic circuitry. However, it remains challenging to generate maximally entangled Bell states of photon pairs with high purity, generation rate, and fidelity required for practical applications. Here, we realize a polarization-entangled photon-pair source based on spontaneous parametric down conversion in an ultrathin rhombohedral tungsten disulfide (3R-WS2) crystal. This vdW entangled photonic source exhibits a high photon-pair purity with a coincidence-to-accidental ratio of above 800, a generation rate of 31 Hz, and two maximally polarization-entangled Bell states with fidelities exceeding 0.93 and entanglement degree over 0.97. These results stem from scalable optical nonlinearity, enhanced second-order susceptibility by electronic transitions, and a well-defined symmetry-enabled selection rule inherent in 3R-WS2. Our polarization entangled photon source can be integrated with photonic structures for generating more complex entangled states, thus paving an avenue for advanced quantum photonic systems toward computation and metrology.

Single-layer tensor network approach for three-dimensional quantum systems

Calculation of observables with three-dimensional projected entangled pair states is generally hard, as it requires a contraction of complex multi-layer tensor networks. We utilize the multi-layer structure of these tensor networks to largely simplify the contraction. The proposed approach involves the usage of the layer structure both to simplify the search for the boundary projected entangled pair states and the single-layer mapping of the final corner transfer matrix renormalization group contraction. We benchmark our results on the cubic lattice Heisenberg model, reaching the bond dimension D=7, and find a good agreement with the previous results. Published by the American Physical Society 2024

Simulating chiral spin liquids with fermionic projected entangled pair states

Simulating chiral spin liquids with fermionic projected entangled pair states