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Showing papers on "Excited state published in 2020"


Journal ArticleDOI
TL;DR: In this paper, the authors review the techniques necessary for the manipulation of neutral atoms for the purpose of quantum simulation and explain how the different types of interactions between Rydberg atoms allow a natural mapping onto various quantum spin models.
Abstract: Recent decades have witnessed great developments in the field of quantum simulation—where synthetic systems are built and studied to gain insight into complicated, many-body real-world problems. Systems of individually controlled neutral atoms, interacting with each other when excited to Rydberg states, have emerged as a promising platform for this task, particularly for the simulation of spin systems. Here, we review the techniques necessary for the manipulation of neutral atoms for the purpose of quantum simulation—such as quantum gas microscopes and arrays of optical tweezers—and explain how the different types of interactions between Rydberg atoms allow a natural mapping onto various quantum spin models. We discuss recent achievements in the study of quantum many-body physics in this platform, and some current research directions beyond that. This Review Article outlines the techniques necessary for the manipulation of neutral atoms and making use of their interactions, when excited to Rydberg states, to achieve the goal of quantum simulation of many-body physics.

471 citations


Journal ArticleDOI
TL;DR: In this article, the authors designed an ideal thermally activated delayed fluorescence molecules with near-degenerate 1CT, 3CT and 3LE states by controlling the distance between the donor and acceptor segments in a molecule with tilted intersegment angles.
Abstract: Reverse intersystem crossing (RISC), originally considered forbidden in purely organic materials, has recently become possible by minimizing the energy gap between the lowest excited singlet state (S1) and lowest triplet state (T1) in thermally activated delayed fluorescence systems. However, direct spin-inversion from T1 to S1 is still inefficient when both states are of the same charge transfer (CT) nature (that is, 3CT and 1CT, respectively). Intervention of locally excited triplet states (3LE) between 3CT and 1CT is expected to trigger fast spin-flipping. Here, we report the systematic design of ideal thermally activated delayed fluorescence molecules with near-degenerate 1CT, 3CT and 3LE states by controlling the distance between the donor and acceptor segments in a molecule with tilted intersegment angles. This system realizes very fast RISC with a rate constant (kRISC) of 1.2 × 107 s−1, resulting in organic light-emitting diodes with excellent performance, particularly at high brightness. An organic molecule, TpAT-tFFO, which is designed to support rapid reverse intersystem crossing allows the fabrication of efficient organic light-emitting diodes.

262 citations


Journal ArticleDOI
TL;DR: In this article, the authors review the techniques underlying quantum gas microscopes and arrays of optical tweezers used in these experiments, explain how the different types of interactions between Rydberg atoms allow a natural mapping onto various quantum spin models, and describe recent results that were obtained with this platform to study quantum many-body physics.
Abstract: Over the last decade, systems of individually-controlled neutral atoms, interacting with each other when excited to Rydberg states, have emerged as a promising platform for quantum simulation of many-body problems, in particular spin systems. Here, we review the techniques underlying quantum gas microscopes and arrays of optical tweezers used in these experiments, explain how the different types of interactions between Rydberg atoms allow a natural mapping onto various quantum spin models, and describe recent results that were obtained with this platform to study quantum many-body physics.

261 citations


Journal ArticleDOI
TL;DR: It is reported that the hole transfer channel of photocharge generation is mediated by an intra-moiety excited state in a blend of donor polymer PM6 and NFA Y6 using broadband transient absorption (TA) spectroscopy, suggesting that manipulating the interplay between intra-Moiety and interfacial excited species can provide a promising route for further improving device performance.
Abstract: Bulk-heterojunction organic photovoltaic devices with nonfullerene acceptors (NFAs) exhibit efficient hole transfer with small interfacial energy offset, which results in power conversion efficiencies above 17% in single junction devices using the high-performance NFA of Y6. However, the underlying mechanism responsible for the hole transfer channel in the polymer/Y6 blends remains poorly understood. Herein, we report that the hole transfer channel of photocharge generation is mediated by an intra-moiety excited state in a blend of donor polymer PM6 and NFA Y6 using broadband transient absorption (TA) spectroscopy. By comparing the TA data recorded from the solution and film Y6 samples, we identify the ultrafast formation of an intra-moiety excimer state together with the conversion from the primary local excitation on a time scale of ∼0.2 ps in the Y6 film. The intra-moiety excimer state acts as the intermediate for the hole transfer channel, which dissociates into free polarons on a time scale of ∼15 ps in the PM6/Y6 blend at room temperature. The intra-moiety intermediate state, arising from the intermolecular coupling in Y6 domains, is markedly different from the interfacial charge transfer state, which is commonly accepted as the intermediate state for the electron transfer channel. These findings suggest that manipulating the interplay between intra-moiety and interfacial excited species can provide a promising route for further improving device performance.

174 citations


Journal ArticleDOI
TL;DR: Recently reported heavy-atom-free BODIPY donor-acceptor dyads and dimers which produce long-living triplet excited states and generate singlet oxygen are reviewed.
Abstract: Organic photosensitizers possessing efficient intersystem crossing (ISC) and forming long-living triplet excited states, play a crucial role in a number of applications. A common approach in the design of such dyes relies on the introduction of heavy atoms (e.g. transition metals or halogens) into the structure, which promote ISC via spin–orbit coupling interaction. In recent years, alternative methods to enhance ISC have been actively studied. Among those, the generation of triplet excited states through photoinduced electron transfer (PET) in heavy-atom-free molecules has attracted particular attention because it allows for the development of photosensitizers with programmed triplet state and fluorescence quantum yields. Due to their synthetic accessibility and tunability of optical properties, boron dipyrromethenes (BODIPYs) are so far the most perspective class of photosensitizers operating via this mechanism. This article reviews recently reported heavy-atom-free BODIPY donor–acceptor dyads and dimers which produce long-living triplet excited states and generate singlet oxygen. Structural factors which affect PET and concomitant triplet state formation in these molecules are discussed and the reported data on triplet state yields and singlet oxygen generation quantum yields in various solvents are summarized. Finally, examples of recent applications of these systems are highlighted.

147 citations


Journal ArticleDOI
TL;DR: In this article, the authors studied a layered compound, LaTe3, where a small lattice anisotropy in the a-c plane results in a unidirectional charge density wave (CDW) along the c axis1,2.
Abstract: When electrons in a solid are excited by light, they can alter the free energy landscape and access phases of matter that are out of reach in thermal equilibrium. This accessibility becomes important in the presence of phase competition, when one state of matter is preferred over another by only a small energy scale that, in principle, is surmountable by the excitation. Here, we study a layered compound, LaTe3, where a small lattice anisotropy in the a–c plane results in a unidirectional charge density wave (CDW) along the c axis1,2. Using ultrafast electron diffraction, we find that, after photoexcitation, the CDW along the c axis is weakened and a different competing CDW along the a axis subsequently emerges. The timescales characterizing the relaxation of this new CDW and the reestablishment of the original CDW are nearly identical, which points towards a strong competition between the two orders. The new density wave represents a transient non-equilibrium phase of matter with no equilibrium counterpart, and this study thus provides a framework for discovering similar states of matter that are ‘trapped’ under equilibrium conditions. Short pulses of light shift the balance between two competing charge density wave phases, allowing the weaker one to manifest transiently while suppressing the stronger one. This shows that competing phases can be tuned in a non-equilibrium setting.

146 citations


Journal ArticleDOI
TL;DR: A new concept in the piezochromic field is reported and a novel strategy to achieve luminescence from a high-lying excited state is provided and ascribed to the cooperative effect be-tween the aggregation-induced emission of TPE units and energy-transfer suppression from TPE to an AN excimer.
Abstract: Most organic piezochromic materials exhibit red-shifted and quenched emission as pressure increases. However, an abnormal phenomenon of pressure-induced blue-shifted and enhanced emission is observed in a 9-(3-(1,2,2-triphenylvinyl)phenyl)anthracene crystal, which is based on discrete π–π anthracene (AN) dimers stacking with tetraphenylethylene (TPE) as spacer. A blue-shifted emission appears and strengthens when the pressure is more than 1.23 GPa, and it reaches the maximum when the pressure is 4.28 GPa. This phenomenon is ascribed to the cooperative effect between the aggregation-induced emission of TPE units and energy-transfer suppression from TPE to an AN excimer. This work reports a new concept in the piezochromic field and provides a novel strategy to achieve luminescence from a high-lying excited state.

144 citations


Journal ArticleDOI
TL;DR: In this article, a quantum metasurface made of an atom array is proposed, providing the possibility to control both spatio-temporal and quantum properties of transmitted and reflected light.
Abstract: Metasurfaces mould the flow of classical light waves by engineering subwavelength patterns from dielectric or metallic thin films. We introduce and analyse a method in which quantum operator-valued reflectivity can be used to control both the spatiotemporal and quantum properties of transmitted and reflected light. Such quantum metasurfaces are realized by entangling the macroscopic response of atomically thin atom arrays to light. We show that such a system allows for parallel quantum operations between atoms and photons as well as for the generation of highly entangled photonic states such as photonic Greenberger–Horne–Zeilinger and three-dimensional cluster states suitable for quantum information processing. We analyse the influence of imperfections as well as specific implementations based on atom arrays excited into Rydberg states. A kind of quantum metasurface made of an atom array is proposed, providing the possibility to control both spatiotemporal and quantum properties of transmitted and reflected light.

126 citations


Journal ArticleDOI
TL;DR: In this paper, a metal-to-ligand charge transfer (MLCT) state with an energy of 1.6 eV (38 kcal/mol) was found for Ni(t-Bubpy)(o-Tol)Cl, which is representative of proposed intermediates in many Ni-photoredox reactions.
Abstract: Synthetic organic chemistry has seen major advances due to the merger of nickel and photoredox catalysis. A growing number of Ni-photoredox reactions are proposed to involve generation of excited nickel species, sometimes even in the absence of a photoredox catalyst. To gain insights about these excited states, two of our groups previously studied the photophysics of Ni(t-Bubpy)(o-Tol)Cl, which is representative of proposed intermediates in many Ni-photoredox reactions. This complex was found to have a long-lived excited state (τ = 4 ns), which was computationally assigned as a metal-to-ligand charge transfer (MLCT) state with an energy of 1.6 eV (38 kcal/mol). This work evaluates the computational assignment experimentally using a series of related complexes. Ultrafast UV-Vis and mid-IR transient absorption data suggest that a MLCT state is generated initially upon excitation but decays to a long-lived state that is 3d-d rather than 3MLCT in character. Dynamic cis,trans-isomerization of the square planar complexes was observed in the dark using 1H NMR techniques, supporting that this 3d-d state is tetrahedral and accessible at ambient temperature. Through a combination of transient absorption and NMR studies, the 3d-d state was determined to lie ∼0.5 eV (12 kcal/mol) above the ground state. Because the 3d-d state features a weak Ni-aryl bond, the excited Ni(II) complexes can undergo Ni homolysis to generate aryl radicals and Ni(I), both of which are supported experimentally. Thus, photoinduced Ni-aryl homolysis offers a novel mechanism of initiating catalysis by Ni(I).

126 citations


Journal ArticleDOI
TL;DR: To demonstrate the potential applicability of this new class of low energy emitters in future photonic applications, such as non-classical light sources for quantum communication or quantum cryptography, single-molecule photon-correlation experiments of 2 are successfully conducted, showing distinct anti-bunching as required for single photon emitters.
Abstract: A series of copper(I) complexes bearing a cyclic (amino)(aryl)carbene (CAArC) ligand with various complex geometries have been investigated in great detail with regard to their structural, electronic, and photophysical properties. Comparison of [CuX(CAArC)] (X = Br (1), Cbz (2), acac (3), Ph2acac (4), Cp (5), and Cp* (6)) with known CuI complexes bearing cyclic (amino)(alkyl), monoamido, or diamido carbenes (CAAC, MAC, or DAC, respectively) as chromophore ligands reveals that the expanded π-system of the CAArC leads to relatively low energy absorption maxima between 350 and 550 nm in THF with high absorption coefficients of 5-15 × 103 M-1 cm-1 for 1-6. Furthermore, 1-5 show intense deep red to near-IR emission involving their triplet excited states in the solid state and in PMMA films with λemmax = 621-784 nm. Linear [Cu(Cbz)(DippCAArC)] (2) has been found to be an exceptional deep red (λmax = 621 nm, ϕ = 0.32, τav = 366 ns) thermally activated delayed fluorescence (TADF) emitter with a radiative rate constant kr of ca. 9 × 105 s-1, exceeding those of commercially employed IrIII- or PtII-based emitters. Time-resolved transient absorption and fluorescence upconversion experiments complemented by quantum chemical calculations employing Kohn-Sham density functional theory and multireference configuration interaction methods as well as temperature-dependent steady-state and time-resolved luminescence studies provide a detailed picture of the excited-state dynamics of 2. To demonstrate the potential applicability of this new class of low-energy emitters in future photonic applications, such as nonclassical light sources for quantum communication or quantum cryptography, we have successfully conducted single-molecule photon-correlation experiments of 2, showing distinct antibunching as required for single-photon emitters.

123 citations


Journal ArticleDOI
TL;DR: The present contribution gathers a large, diverse and accurate set of more than 200 highly-accurate transition energies for states of various natures (valence, Rydberg, singlet, triplet, n-pi*, pi-pi*...) to benchmark a series of popular methods for excited state calculations.
Abstract: Following our previous work focussing on compounds containing up to 3 non-hydrogen atoms [\emph{J. Chem. Theory Comput.} {\bfseries 14} (2018) 4360--4379], we present here highly-accurate vertical transition energies obtained for 27 molecules encompassing 4, 5, and 6 non-hydrogen atoms. To obtain these energies, we use equation-of-motion coupled cluster theory up to the highest technically possible excitation order for these systems (CC3, EOM-CCSDT, and EOM-CCSDTQ), selected configuration interaction (SCI) calculations (with tens of millions of determinants in the reference space), as well as the multiconfigurational $n$-electron valence state perturbation theory (NEVPT2) method. All these approaches are applied in combination with diffuse-containing atomic basis sets. For all transitions, we report at least CC3/\emph{aug}-cc-pVQZ vertical excitation energies as well as CC3/\emph{aug}-cc-pVTZ oscillator strengths for each dipole-allowed transition. We show that CC3 almost systematically delivers transition energies in agreement with higher-level methods with a typical deviation of $\pm 0.04$ eV, except for transitions with a dominant double excitation character where the error is much larger. The present contribution gathers a large, diverse and accurate set of more than 200 highly-accurate transition energies for states of various natures (valence, Rydberg, singlet, triplet, $n \rightarrow \pi^*$, $\pi \rightarrow \pi^*$, \ldots). We use this series of theoretical best estimates to benchmark a series of popular methods for excited state calculations: CIS(D), ADC(2), CC2, STEOM-CCSD, EOM-CCSD, CCSDR(3), CCSDT-3, CC3, as well as NEVPT2. The results of these benchmarks are compared to the available literature data.

Journal ArticleDOI
TL;DR: The results suggest that orbital optimized excited state DFT methods can be used to push past the limitations of TDDFT to doubly excited, charge-transfer or Rydberg states, making them a useful tool for the practical quantum chemist's toolbox for studying excited states in large systems.
Abstract: We present a general approach to converge excited state solutions to any quantum chemistry orbital optimization process, without the risk of variational collapse. The resulting square gradient minimization (SGM) approach only requires analytic energy/Lagrangian orbital gradients and merely costs 3 times as much as ground state orbital optimization (per iteration), when implemented via a finite difference approach. SGM is applied to both single determinant ΔSCF and spin-purified restricted open-shell Kohn-Sham (ROKS) approaches to study the accuracy of orbital optimized DFT excited states. It is found that SGM can converge challenging states where the maximum overlap method (MOM) or analogues either collapse to the ground state or fail to converge. We also report that ΔSCF/ROKS predict highly accurate excitation energies for doubly excited states (which are inaccessible via TDDFT). Singly excited states obtained via ROKS are also found to be quite accurate, especially for Rydberg states that frustrate (semi)local TDDFT. Our results suggest that orbital optimized excited state DFT methods can be used to push past the limitations of TDDFT to doubly excited, charge-transfer, or Rydberg states, making them a useful tool for the practical quantum chemist's toolbox for studying excited states in large systems.

Journal ArticleDOI
TL;DR: Long-lived emission via thermally activated delayed fluorescence has been demonstrated from an air- and water-stable zirconium complex featuring excited states with significant ligand-to-metal charge transfer character.
Abstract: Advances in chemical control of the photophysical properties of transition-metal complexes are revolutionizing a wide range of technologies, particularly photocatalysis and light-emitting diodes, but they rely heavily on molecules containing precious metals such as ruthenium and iridium. Although the application of earth-abundant ‘early’ transition metals in photosensitizers is clearly advantageous, a detailed understanding of excited states with ligand-to-metal charge transfer (LMCT) character is paramount to account for their distinct electron configurations. Here we report an air- and moisture-stable, visible light-absorbing Zr(iv) photosensitizer, Zr(MesPDPPh)2, where [MesPDPPh]2− is the doubly deprotonated form of [2,6-bis(5-(2,4,6-trimethylphenyl)-3-phenyl-1H-pyrrol-2-yl)pyridine]. This molecule has an exceptionally long-lived triplet LMCT excited state (τ = 350 μs), featuring highly efficient photoluminescence emission (Ф = 0.45) due to thermally activated delayed fluorescence emanating from the higher-lying singlet configuration with significant LMCT contributions. Zr(MesPDPPh)2 engages in numerous photoredox catalytic processes and triplet energy transfer. Our investigation provides a blueprint for future photosensitizer development featuring early transition metals and excited states with significant LMCT contributions. Understanding the photophysical properties of transition-metal complexes is paramount to advances in photocatalysis, solar energy conversion and light-emitting diodes. Now, long-lived emission via thermally activated delayed fluorescence has been demonstrated from an air- and water-stable zirconium complex featuring excited states with significant ligand-to-metal charge transfer character.

Journal ArticleDOI
27 Oct 2020
TL;DR: In this paper, a quantum algorithm for the calculation of molecular excited states was proposed and applied to lithium hydride on a superconducting qubit device. But the algorithm is not suitable for the case of superconducted qubits.
Abstract: The authors introduce a quantum algorithm for the calculation of molecular excited states and apply it to lithium hydride on a superconducting qubit device.

Journal ArticleDOI
TL;DR: This work creates and isolate near-surface single vanadium dopants in silicon carbide (SiC) with stable and narrow emission in the O band, with brightness allowing cavity-free detection in a wafer-scale material.
Abstract: Solid-state quantum emitters with spin registers are promising platforms for quantum communication, yet few emit in the narrow telecom band necessary for low-loss fiber networks. Here, we create and isolate near-surface single vanadium dopants in silicon carbide (SiC) with stable and narrow emission in the O band, with brightness allowing cavity-free detection in a wafer-scale material. In vanadium ensembles, we characterize the complex d1 orbital physics in all five available sites in 4H-SiC and 6H-SiC. The optical transitions are sensitive to mass shifts from local silicon and carbon isotopes, enabling optically resolved nuclear spin registers. Optically detected magnetic resonance in the ground and excited orbital states reveals a variety of hyperfine interactions with the vanadium nuclear spin and clock transitions for quantum memories. Last, we demonstrate coherent quantum control of the spin state. These results provide a path for telecom emitters in the solid state for quantum applications.

Journal ArticleDOI
TL;DR: In the laboratory, covalent dimers are utilized to precisely arrange the chromophores in rigid, well-defined geometries to systematically study the factors that determine the degree of state mixing and its fate, and this framework is especially useful in demonstrating the connections between these different states.
Abstract: ConspectusChromophore aggregates are capable of a wide variety of excited-state dynamics that are potentially of great use in optoelectronic devices based on organic molecules. For example, singlet fission, the process by which a singlet exciton is down converted into two triplet excitons, holds promise for extending the efficiency of solar cells, while other processes, such as excimer formation, are commonly regarded as parasitic pathways or traps. Other processes, such as symmetry-breaking charge transfer, where the excited dimer charge separates into a radical ion pair, can be both a trap and potentially useful in devices, depending on the context. Thus, an understanding of the precise mechanisms of each of these processes is vital to designing tailor-made organic chromophores for molecular optoelectronics.These excited-state phenomena have each been well-studied in recent years and show tantalizing connections as the molecular systems and environments are subtly changed. These seemingly disparate phenomena can be described within the same unifying framework, where each case can be represented as one point in continuum of mixed states. The coherent mixed state is observed experimentally, and it collapses to each of the limiting cases under well-defined conditions. This framework is especially useful in demonstrating the connections between these different states so that we can determine the factors that control their evolution and may ultimately guide the state mixtures to the product state of choice. The emerging picture shows that tuning the electronic coupling through proper arrangement of the chromophores must accompany environmental tuning of the chromophore energies to produce a fully mixed state. Changes in either of these quantities leads to evolution of the admixture and ultimately collapsing the superposition onto a given state, producing one of the photophysical pathways discussed above.In our laboratory, we are utilizing covalent dimers to precisely arrange the chromophores in rigid, well-defined geometries to systematically study the factors that determine the degree of state mixing and its fate. We interrogate these dynamics with transient absorption spectroscopy from the UV continuously into the mid-infrared, along with time-resolved Raman and emission and magnetic resonance spectroscopies to build a complete and detailed molecular level picture of the dynamics of these dimers. The knowledge gained from dimer studies can also be applied to the understanding the dynamics in extended molecular solids. The insight afforded by these studies will help guide the creation of new designer chromophores with control over the fate of the excited state.

Journal ArticleDOI
TL;DR: MOMAP as mentioned in this paper is a MOlecular MAterial Property prediction package, wherein the key function is the thermal vibration correlation function (TVCF) formalism for excited state decay, allowing theoretical prediction of light-emitting quantum efficiency and carrier mobility.
Abstract: What is the most favorite and original chemistry developed in your research group? MOMAP, abbreviated for MOlecular MAterials Property prediction package, wherein the key function is the thermal vibration correlation function (TVCF) formalism for excited state decay, allowing theoretical prediction of light-emitting quantum efficiency and carrier mobility. MOMAP starts to be popular after its first launch in 2015.

Journal ArticleDOI
14 Dec 2020
TL;DR: In this paper, the ground state of a given Hamiltonian and its ground energy are estimated on a quantum computer, where the spectral gap between the ground energy and the first excited energy is bounded from below.
Abstract: Preparing the ground state of a given Hamiltonian and estimating its ground energy are important but computationally hard tasks. However, given some additional information, these problems can be solved efficiently on a quantum computer. We assume that an initial state with non-trivial overlap with the ground state can be efficiently prepared, and the spectral gap between the ground energy and the first excited energy is bounded from below. With these assumptions we design an algorithm that prepares the ground state when an upper bound of the ground energy is known, whose runtime has a logarithmic dependence on the inverse error. When such an upper bound is not known, we propose a hybrid quantum-classical algorithm to estimate the ground energy, where the dependence of the number of queries to the initial state on the desired precision is exponentially improved compared to the current state-of-the-art algorithm proposed in [Ge et al. 2019]. These two algorithms can then be combined to prepare a ground state without knowing an upper bound of the ground energy. We also prove that our algorithms reach the complexity lower bounds by applying it to the unstructured search problem and the quantum approximate counting problem.

Journal ArticleDOI
TL;DR: An overview of the Rydberg quantum toolbox is given in this paper, emphasizing the high degree of flexibility for encoding qubits, performing quantum operations and engineering quantum many-body Hamiltonians.
Abstract: Arrays of optically trapped atoms excited to Rydberg states have recently emerged as a competitive physical platform for quantum simulation and computing, where high-fidelity state preparation and readout, quantum logic gates and controlled quantum dynamics of more than 100 qubits have all been demonstrated. These systems are now approaching the point where reliable quantum computations with hundreds of qubits and realistically thousands of multiqubit gates with low error rates should be within reach for the first time. In this article we give an overview of the Rydberg quantum toolbox, emphasizing the high degree of flexibility for encoding qubits, performing quantum operations and engineering quantum many-body Hamiltonians. We then review the state-of-the-art concerning high-fidelity quantum operations and logic gates as well as quantum simulations in many-body regimes. Finally, we discuss computing schemes that are particularly suited to the Rydberg platform and some of the remaining challenges on the road to general purpose quantum simulators and quantum computers.

Journal ArticleDOI
TL;DR: The promising thermometric performance corroborates the potential of CaHfO3:Cr3+ as a Boltzmann cryothermometer, being characterized by a high relative sensitivity and exceptional thermal resolution.
Abstract: Luminescence Boltzmann thermometry is one of the most reliable techniques used to locally probe temperature in a contactless mode. However, to date, there is no report on cryogenic thermometers based on the highly sensitive and reliable Boltzmann-based 4T2 → 4A2/2E → 4A2 emission ratio of Cr3+. On the basis of structural information of the local HfO6 octahedral site we demonstrated the potential of the CaHfO3:Cr3+ system by combining deep theoretical and experimental investigation. The material exhibits simultaneous emission from both the 2E and 4T2 excited states, following the Boltzmann law in a cryogenic temperature range of 40-150 K. The promising thermometric performance corroborates the potential of CaHfO3:Cr3+ as a Boltzmann cryothermometer, being characterized by a high relative sensitivity (∼ 2%·K-1 at 40 K) and exceptional thermal resolution (0.045-0.77 K in the 40-150 K range). Moreover, by exploiting the flexibility of the 4T2-2E energy gap controlled by the crystal field of the local octahedral site, the design proposed herein could be expanded to develop new Cr3+-doped cryogenic thermometers.

Journal ArticleDOI
TL;DR: In this article, the two-valence electron structure of individual alkaline-earth Rydberg atoms has been exploited to achieve state detection, single-atom Rabi operations and two-atom entanglement.
Abstract: Trapped neutral atoms have become a prominent platform for quantum science, where entanglement fidelity records have been set using highly excited Rydberg states. However, controlled two-qubit entanglement generation has so far been limited to alkali species, leaving the exploitation of more complex electronic structures as an open frontier that could lead to improved fidelities and fundamentally different applications such as quantum-enhanced optical clocks. Here, we demonstrate a novel approach utilizing the two-valence electron structure of individual alkaline-earth Rydberg atoms. We find fidelities for Rydberg state detection, single-atom Rabi operations and two-atom entanglement that surpass previously published values. Our results pave the way for novel applications, including programmable quantum metrology and hybrid atom–ion systems, and set the stage for alkaline-earth based quantum computing architectures. High entanglement fidelity between neutral atoms is achieved using highly excited Rydberg states. The unique electron structure provided by alkaline-earth atoms makes it a promising platform for various quantum-technology-based applications.

Journal ArticleDOI
TL;DR: It is reported that the energy gap between the lowest localized triplet excited state and the lowest singlet charge-transfer excited state in the exciplex system significantly controls the LPL performance.
Abstract: Organic long-persistent luminescence (LPL) is an organic luminescence system that slowly releases stored exciton energy as light. Organic LPL materials have several advantages over inorganic LPL materials in terms of functionality, flexibility, transparency, and solution-processability. However, the molecular selection strategies for the organic LPL system still remain unclear. Here we report that the energy gap between the lowest localized triplet excited state and the lowest singlet charge-transfer excited state in the exciplex system significantly controls the LPL performance. Changes in the LPL duration and spectra properties are systematically investigated for three donor materials having a different energy gap. When the energy level of the lowest localized triplet excited state is much lower than that of the charge-transfer excited state, the system exhibits a short LPL duration and clear two distinct emission features originating from exciplex fluorescence and donor phosphorescence.

Journal ArticleDOI
TL;DR: In this paper, the authors demonstrate the practical application of these algorithms to challenging quantum computations of relevance for chemistry and nuclear physics, using the deuteron-binding energy and molecular hydrogen binding and excited state energies as examples.
Abstract: Various methods have been developed for the quantum computation of the ground and excited states of physical and chemical systems, but many of them require either large numbers of ancilla qubits or high-dimensional optimization in the presence of noise. The quantum imaginary-time evolution (QITE) and quantum Lanczos (QLanczos) methods proposed in Motta et al. (2020) eschew the aforementioned issues. In this study, we demonstrate the practical application of these algorithms to challenging quantum computations of relevance for chemistry and nuclear physics, using the deuteron-binding energy and molecular hydrogen binding and excited state energies as examples. With the correct choice of initial and final states, we show that the number of timesteps in QITE and QLanczos can be reduced significantly, which commensurately simplifies the required quantum circuit and improves compatibility with NISQ devices. We have performed these calculations on cloud-accessible IBM Q quantum computers. With the application of readout-error mitigation and Richardson error extrapolation, we have obtained ground and excited state energies that agree well with exact results obtained from diagonalization.


Journal ArticleDOI
TL;DR: A novel twisting D–π–A fluorescent molecule (triphenylamine–anthracene–phenanthroimidazole; TPAAnPI) is designed and synthesized and its excited state properties reveal that its fluorescence is due to the HLCT excited state.
Abstract: Designing a donor–acceptor (D–A) molecule with a hybridized local and charge transfer (HLCT) excited state is a very effective strategy for producing an organic light-emitting diode (OLED) with a high exciton utilization efficiency and external quantum efficiency. Herein, a novel twisting D–π–A fluorescent molecule (triphenylamine–anthracene–phenanthroimidazole; TPAAnPI) is designed and synthesized. The excited state properties of the TPAAnPI investigated through photophysical experiments and density functional theory (DFT) analysis reveal that its fluorescence is due to the HLCT excited state. The optimized non-doped blue OLED using TPAAnPI as a light-emitting layer exhibits a novel blue emission with an electroluminescence (EL) peak at 470 nm, corresponding to the Commission International de L'Eclairage (CIE) coordinates of (0.15, 0.22). A fabricated device termed Device II exhibits a maximum current efficiency of 18.09 cd A−1, power efficiency of 12.35 lm W−1, luminescence of ≈29 900 cd cm−2, and external quantum efficiency (EQE) of 11.47%, corresponding to a high exciton utilization efficiency of 91%. Its EQE remains as high as 9.70% at a luminescence of 1000 cd m−2 with a low efficiency roll-off of 15%. These results are among the best for HLCT blue-emitting materials involved in non-doped blue fluorescent OLEDs. The performance of Device II highlights a great industrial application potential for the TPAAnPI molecule.

Journal ArticleDOI
TL;DR: An approach to quantum computing with Rydberg atoms or superconducting qubits suggests using multiqubit gates, rather than one-and two-qubit gates to reduce the number of operations and errors as discussed by the authors.
Abstract: An approach to quantum computing with Rydberg atoms or superconducting qubits suggests using multiqubit gates, rather than one- and two-qubit gates, to reduce the number of operations and errors.

Journal ArticleDOI
TL;DR: In this article, the Fourier transform of the charged moments gives the desired symmetry resolved entropies for CFT with U(1) symmetry, as in the ground state, but with sub-leading terms that break it.
Abstract: We report a throughout analysis of the entanglement entropies related to different symmetry sectors in the low-lying primary excited states of a conformal field theory (CFT) with an internal U(1) symmetry. Our findings extend recent results for the ground state. We derive a general expression for the charged moments, i.e. the generalised cumulant generating function, which can be written in terms of correlation functions of the operator that define the state through the CFT operator-state correspondence. We provide explicit analytic computations for the compact boson CFT (aka Luttinger liquid) for the vertex and derivative excitations. The Fourier transform of the charged moments gives the desired symmetry resolved entropies. At the leading order, they satisfy entanglement equipartition, as in the ground state, but we find, within CFT, subleading terms that break it. Our analytical findings are checked against free fermions calculations on a lattice, finding excellent agreement. As a byproduct, we have exact results for the full counting statistics of the U(1) charge in the considered excited states.

Journal ArticleDOI
TL;DR: In this paper, a 1D bosonic lattice model with a soft constraint in the form of density-assisted hopping has been proposed to simulate the many-body scars on Rydberg atoms.
Abstract: Recent experiments on Rydberg atom arrays have found evidence of anomalously slow thermalization and persistent density oscillations, which have been interpreted as a many-body analog of the phenomenon of quantum scars. Periodic dynamics and atypical scarred eigenstates originate from a “hard” kinetic constraint: the neighboring Rydberg atoms cannot be simultaneously excited. Here we propose a realization of quantum many-body scars in a 1D bosonic lattice model with a “soft” constraint in the form of density-assisted hopping. We discuss the relation of this model to the standard Bose-Hubbard model and possible experimental realizations using ultracold atoms. We find that this model exhibits similar phenomenology to the Rydberg atom chain, including weakly entangled eigenstates at high energy densities and the presence of a large number of exact zero energy states, with distinct algebraic structure. Quantum many-body scarring, a peculiar phenomenon whereby a system thermalizes whilst it keeps returning to its initial state during the time evolution, has recently been observed in experiments on arrays of Rydberg atoms. The authors theoretically investigate the spectral properties of three Hamiltonians using a chain of bosons with density-dependent hopping, providing new insight in the phenomenon of many-body quantum scarring.

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TL;DR: Qualitative theory and quantum chemical calculations are used to develop explicit strategies on how to use Baird’s 4n rule on excited-state aromaticity, combined with Hückel's 4n + 2 rule for ground- state aromaticity to tailor new potential chromophores for singlet fission.
Abstract: Singlet exciton fission photovoltaic technology requires chromophores with their lowest excited states arranged so that 2E(T-1) LUMO configurations, providing a rational for the simultaneous tunin ...

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TL;DR: In the absolute ground state, the inelastic collisions between ultracold CaF molecules are measured by combining two optical tweezers to find a two-body loss rate which is below, but close to, the predicted universal loss rate.
Abstract: We measure inelastic collisions between ultracold CaF molecules by combining two optical tweezers, each containing a single molecule. We observe collisions between ^{2}Σ CaF molecules in the absolute ground state |X,v=0,N=0,F=0⟩, and in excited hyperfine and rotational states. In the absolute ground state, we find a two-body loss rate of 7(4)×10^{-11} cm^{3}/s, which is below, but close to, the predicted universal loss rate.