Single Excitation Research Articles

New rotational rate coefficients computation of MgC3N(X2Σ+) by collision with He(1S)

ABSTRACT Determining physical conditions in interstellar environments requires reliable estimation of collisional data for molecules detected in space. In this work, we report a rate coefficients calculation of MgC3N(X2Σ+) induced by collision with He. This study is based on a new 2D potential energy surface (2D-PES), obtained from the explicitly correlated restricted open-shell coupled cluster approach with single, double, and perturbative triple excitation (rccsd(t)-f12) and the aug-cc-pVTZ basis sets. The MgC3N–He PES presents a global minimum with a well depth of −45.6 cm−1. Based on this interaction potential, we derived the excitation cross-sections using the close-coupling quantum time-independent formalism for total energies ≤500 cm−1 and N ≤ 40. These cross-sections were then integrated on a Maxwell–Boltzmann distribution of kinetic energies to obtain the collisional (de)-excitation rate coefficients for thermal temperature below 100 K. A non-LTE radiative transfer calculation was performed using the present collisional rates in order to estimate their impact on the abundance of MgC3N. These collisional data can help astronomers for the detection and an accurate determination of MgC3N abundance in the investigated interstellar clouds.

Extreme single-excitation subradiance from two-band Bloch oscillations in atomic arrays

Atomic arrays provide an important quantum optical platform with photon-mediated dipole–dipole interactions that can be engineered to realize key applications in quantum information processing. A major obstacle for such applications is the fast decay of the excited states. By controlling two-band Bloch oscillations of single excitation in an atomic array under an external magnetic field, here we show that exotic subradiance can be realized and maintained with orders of magnitude longer than the spontaneous decay time in atomic arrays with the finite size. The key finding is to show a way for preventing the wavepacket of excited states scattering into the dissipative zone inside the free space light cone, which therefore leads to the excitation staying at a subradiant state for an extremely long decay time. We show that such operation can be achieved by introducing a spatially linear potential from the external magnetic field in the atomic arrays and then manipulating interconnected two-band Bloch oscillations along opposite directions. Our results also point out the possibility of controllable switching between superradiant and subradiant states, which leads to potential applications in quantum storage.

Structural damage identification with output-only strain measurements and swarm intelligence algorithms: a comparative study

The identification of structural damage with the unavailability of input excitations is highly desired but challenging since structural dynamic responses are affected by the coupling effect of structural parameters and external excitations. To deal with this issue, in this paper, an output-only damage identification strategy based on swarm intelligence algorithms and correlation functions of strain responses is proposed to identify structures subjected to single or multiple unknown white noise excitations. In the proposed strategy, four different population-based optimization algorithms—particle swarm optimization, the butterfly optimization algorithm, the tree seed algorithm, and a micro search Jaya (MS-Jaya)—are employed and compared. The micro search mechanism is integrated into a basic Jaya algorithm to improve its computational efficiency and accuracy by eliminating some damage variables with small values for the identified best solution after several iterations. The objective function is established based on the proposed auto/cross-correlation function of strain responses and a penalty function. The effectiveness of the proposed method is verified with numerical studies on a simply supported beam structure and a steel grid benchmark structure under ambient excitation. In addition, the effect of the reference point, number of sensors, and arrangement of strain gauges on the performance of the proposed method are discussed in detail. The investigated results demonstrate that the proposed approach can accurately detect, locate, and quantify structural damage with limited sensors and 20% noise-polluted strain responses. In particular, the proposed MS-Jaya algorithm presents a more superior capacity in solving the optimization-based damage identification problem than the other three algorithms.

Phonon-mediated temperature dependence of Er3+ optical transitions in Er2O3

Characterization of the atomic level processes that determine optical transitions in emerging materials is critical to the development of new platforms for classical and quantum networking. Such understanding often emerges from studies of the temperature dependence of the transitions. We report measurements of the temperature dependent Er3+ photoluminescence in single crystal Er2O3 thin films epitaxially grown on Si(111) focused on transitions that involve the closely spaced Stark-split levels. Radiative intensities are compared to a model that includes relevant Stark-split states, single phonon-assisted excitations, and the well-established level population redistribution due to thermalization. This approach, applied to the individual Stark-split states and employing Er2O3 specific single-phonon-assisted excitations, gives good agreement with experiment. This model allows us to demonstrate the difference in the electron-phonon coupling of the 4S3/2 and 2H11/2 states of Er3+ in E2O3 and suggests that the temperature dependence of Er3+ emission intensity may vary significantly with small shifts in the wavelength (~0.1 nm) of the excitation source.

Long-lived nitric oxide molecular tagging velocimetry with 1 + 1 REMPI.

The successful demonstration of long-lived nitric oxide (NO) fluorescence for molecular tagging velocimetry (MTV) measurements is described in this Letter. Using 1 + 1 resonance-enhanced multiphoton ionization (REMPI) of NO at a wavelength near 226 nm, targeting the overlapping Q1(7) and Q21(7) lines of the A-X (0, 0) electronic system, the lifetime of the NO MTV signal was observed to be approximately 8.6 µs within a 100-Torr cell containing 2% NO in nitrogen. This is in stark contrast to the commonly reported single photon NO fluorescence, which has a much shorter calculated lifetime of approximately 43 ns at this pressure and NO volume fraction. While the shorter lifetime fluorescence can be useful for molecular tagging velocimetry with single laser excitation within very high-speed flows at some thermodynamic conditions, the longer lived fluorescence shows the potential for an order of magnitude more accurate and precise velocimetry, particularly within lower speed regions of hypersonic flow fields such as wakes and boundary layers. The physical mechanism responsible for the generation of this long-lived signal is detailed. Furthermore, the effectiveness of this technique is showcased in a high-speed jet flow, where it is employed for precise flow velocity measurements.

Tuning Excitation Transport in a Dissipative Rydberg Ring

We demonstrate the flexible tunability of excitation transport in Rydberg atoms, under the interplay of controlled dissipation and interaction-induced synthetic flux. Considering a minimum four-site setup, i.e., a triangular configuration with an additional output site, we study the transport of a single excitation, injected into a vertex of the triangle, through the structure. While the long-range dipole-dipole interactions between the Rydberg atoms lead to geometry-dependent Peierls phases in the hopping amplitudes of excitations, we further introduce on-site dissipation to a vertex of the triangle. As a result, both the chirality and destination of the transport can be manipulated through the flux and dissipation. In particular, we illustrate a parameter regime where our Rydberg-ring structure may serve as a switch for transporting the injected excitation through to the output site. The underlying mechanism is then analyzed by studying the chiral trajectory of the excitation and the time-dependent dissipation. The switchable excitation transport reported here offers a flexible tool for quantum control in Rydberg atoms, and holds interesting potentials for applications in quantum simulation and quantum information.

Realization of an Extremely Anisotropic Heisenberg Magnet in Rydberg Atom Arrays

Strong mutual interaction which correlates elementary excitations of quantum matter plays a key role in a range of emergent phenomena, from binding and condensation to quantum thermalization and many-body localization. Here, we employ a Rydberg quantum simulator to experimentally demonstrate strongly correlated spin transport in anisotropic Heisenberg magnets, where the magnon-magnon interaction can be tuned 2 orders of magnitude larger than the magnon hopping strength. In our approach, the motion of magnons is controlled by an induced spin-exchange interaction through far off-resonant driving, which enables coherent transport of a single Rydberg excitation across a chain of ground-state atoms. As the most prominent signature of a giant anisotropy, we show that nearby Rydberg excitations form distinct types of magnon-bound states, where a tightly bound pair exhibits frozen dynamics in a fragmented Hilbert space, while a loosely bound pair propagates and establishes correlations beyond a single lattice site. Our scheme complements studies using resonant dipole-dipole interactions between Rydberg states and opens the door to exploring quantum thermodynamics with ultrastrong interactions and kinetic constraints. Published by the American Physical Society 2024

Electromagnetic response analysis of high temperature superconducting coated conductor tape with local debonding: Case of transporting current in an external magnetic field

In this article, the electromagnetic mechanical behavior of a long superconducting coating tape within a local internal cracking was analyzed when it transport current in a perpendicular magnetic field. Based on the superconducting critical state model, the distribution of current and magnetic field within the structure were calculated. Then, the control equation for the correlation between the flux pinning force inside the superconducting thin film and the shear force at the substrate interface was given using the plane strain method of linear elasticity theory. Combined with the Chebyshev polynomial solution, the distribution patterns of normal stress inside the superconducting thin film and shear stress at the substrate interface were finally obtained. The results indicate that, unlike the phenomenon observed under a single field excitation, the stress distribution in the structure exhibits an asymmetric distribution when both transport current and external magnetic field are applied. The normal stress inside the superconducting thin film is significantly larger on the right side of the structure than that on the left side, and the same distribution law is found in the shear stress at the substrate interface. The stress concentration occurs at the separation point between the film and the substrate. When the Young's modulus of the substrate material is high, the normal stress inside the superconducting film is low, while the shear stress at the interface is high, and vice versa. All these results provide theoretical guidance for the application of superconducting tapes.

Cy5 Dye Cassettes Exhibit Through-Bond Energy Transfer and Enable Ratiometric Fluorescence Sensing.

The chemosensor literature contains many reports of fluorescence sensing using polyaromatic hydrocarbon fluorophores such as pyrene, tetraphenylethylene, or polyaryl(ethynylene), where the fluorophore is excited with ultraviolet light (<400 nm) and emits in the visible region of 400-500 nm. There is a need for general methods that convert these "turn-on" hydrocarbon fluorescent sensors into ratiometric sensing paradigms. One simple strategy is to mix the responsive hydrocarbon sensor with a second non-responsive dye that is excited by ultraviolet light but emits at a distinctly longer wavelength and thus acts as a reference signal. Five new cyanine dye cassettes were created by covalently attaching a pyrene, tetraphenylethylene, or biphenyl(ethynylene) component as the ultraviolet-absorbing energy donor directly to the pentamethine chain of a deep-red cyanine (Cy5) energy acceptor. Fluorescence emission studies showed that these Cy5-cassettes exhibited large pseudo-Stokes shifts and high through-bond energy transfer efficiencies upon excitation with ultraviolet light. Practical potential was demonstrated with two examples of ratiometric fluorescence sensing using a single ultraviolet excitation wavelength. One example mixed a Cy5-cassette with a pyrene-based fluorescent indicator that responded to changes in Cu2+ concentration, and the other example mixed a Cy5-cassette with the fluorescent pH sensing dye, pyranine.

Influence of donor or acceptor presence on excitation states in molecular chains: Nonadiabatic polaron approach.

In this paper, we considered a molecular structure that consists of a molecular chain and an additional molecule (donor or acceptor) that can inject (or remove) single excitation (vibron, electron, etc.) onto the molecular chain. We assumed that the excitation forms a self-trapped state due to the interaction with mechanical oscillations of the chain structure elements. We analyzed the energy spectra of the excitation and showed that its state (when it migrates to the molecular chain) has the properties of the nonadiabatic polaron state. The conditions under which the excitation can migrate from one subsystem to another one were considered. It was shown that the presence of a "donor" molecule cannot significantly change the properties of the excitation located on the molecular chain. At the same time, the molecular chain can affect the position of the energy level of the excitation localized on the donor subsystem. Indirectly, this can influence the process of excitation migration from one subsystem to another one. The influence of the basic energy parameters of the system and the environment temperature on this process are discussed. The entire system was assumed to be in thermal equilibrium with the environment.

A Tubular Variable Reluctance Resolver With Single Coil Excitation Winding

A Tubular Variable Reluctance Resolver With Single Coil Excitation Winding

Use of bacterial photosynthetic vesicles to evaluate the effect of ionic liquids on the permeability of biological membranes

Ionic liquids (ILs) are salts composed of a combination of organic or inorganic cations and anions characterized by a low melting point, often below 100 °C. This property, together with an extremely low vapor pressure, low flammability and high thermal stability, makes them suitable for replacing canonical organic solvents, with a reduction of industrial activities impact on the environment. Although in the last decades the eco-compatibility of ILs has been extensively verified through toxicological tests performed on model organisms, a detailed understanding of the interaction of these compounds with biological membranes is far from being exhaustive. In this context, we have chosen to evaluate the effect of some ILs on native membranes by using chromatophores, photosynthetic vesicles that can be isolated from Rhodobacter capsulatus, a member of the purple non‑sulfur bacteria. Here, carotenoids associated with the light-harvesting complex II, act as endogenous spectral probes of the transmembrane electrical potential (ΔΨ). By measuring through time-resolved absorption spectroscopy the evolution of the carotenoid band shift induced by a single excitation of the photosynthetic reaction center, information on the ΔΨ dissipation due to ionic currents across the membrane can be obtained. We found that some ILs cause a rather fast dissipation of the transmembrane ΔΨ even at low concentrations, and that this behavior is dose-dependent. By using two different models to analyze the decay of the carotenoid signals, we attempted to interpret at a mechanistic level the marked increase of ionic permeability caused by specific ILs.

BINGO: a blind unmixing algorithm for ultra-multiplexing fluorescence images.

Spectral imaging is often used to observe different objects with multiple fluorescent labels to reveal the development of the biological event. As the number of observed objects increases, the spectral overlap between fluorophores becomes more serious, and obtaining a "pure" picture of each fluorophore becomes a major challenge. Here, we propose a blind spectral unmixing algorithm called BINGO (Blind unmixing via SVD-based Initialization Nmf with project Gradient descent and spare cOnstrain), which can extract all kinds of fluorophores more accurately from highly overlapping multichannel data, even if the spectra of the fluorophores are extremely similar or their fluorescence intensity varies greatly. BINGO can isolate up to 10 fluorophores from spectral imaging data for a single excitation. nine-color living HeLa cells were visualized distinctly with BINGO. It provides an important algorithmic tool for multiplex imaging studies, especially in intravital imaging. BINGO shows great potential in multicolor imaging for biomedical sciences. The source code used for this paper is available with the test data at https://github.com/Xinyuan555/BINGO_unmixing.

Blinking characteristics of organic fluorophores for blink-based multiplexing

Single-molecule fluorescence experiments have transformed our understanding of complex materials and biological systems. Whether single molecules are used to report on their nano-environment or provide for localization, understanding their blinking dynamics (i.e., stochastic fluctuations in emission intensity under continuous illumination) is paramount. We recently demonstrated another use for blinking dynamics called blink-based multiplexing (BBM), where individual emitters are classified using a single excitation laser based on blinking dynamics, rather than color. This study elucidates the structure-activity relationships governing BBM performance in a series of model rhodamine, BODIPY, and anthraquinone fluorophores that undergo different photo-physical and-chemical processes during blinking. Change point detection and multinomial logistic regression analyses show that BBM can leverage spectral fluctuations, electron and proton transfer kinetics, as well as photostability for molecular classification—even within the context of a shared blinking mechanism. In doing so, we demonstrate two- and three-color BBM with ≥ 93% accuracy using spectrally-overlapped fluorophores.

Rapid Atmospheric Reactions between Criegee Intermediates and Hypochlorous Acid.

Hypochlorous acid (HOCl) is a paramount compound in the atmosphere due to its significant contribution to both tropospheric oxidation capacity and ozone depletion. The main removal routes for HOCl are photolysis and the reaction with OH during the daytime, while these processes are unimportant during the nighttime. Here, we report the rapid reactions of Criegee intermediates (CH2OO and anti/syn-CH3CHOO) with HOCl by using high-level quantum chemical methods as the benchmark; their accuracy is close to coupled cluster theory with single, double, and triple excitations and quasiperturbative connected quadruple excitations with a complete basis limit by extrapolation [CCSDT(Q)/CBS]. Their rate constants have been calculated by using a dual-level strategy; this combines conventional transition state theory calculated at the benchmark level with variational transition state theory with small-curvature tunneling by a validated density functional method. We find that the introduction of the methyl group into Criegee intermediates not only affects their reactivities but also exerts a remarkable influence on anharmonicity. The calculated results uncover that anharmonicity increases the rate constants of CH2OO + HOCl by a factor of 18-5, while it is of minor importance in the anti/syn-CH3CHOO + HOCl reaction at 190-350 K. The present findings reveal that the loose transition state for anti-CH3CHOO and HOCl is a rate-determining step at 190-350 K. We also find that the reaction of Criegee intermediates with HOCl contributes significantly to the sink of HOCl during the nighttime in the atmosphere.

Performance of periodic EOM-CCSD for bandgaps of inorganic semiconductors and insulators.

We calculate bandgaps of 12 inorganic semiconductors and insulators composed of atoms from the first three rows of the Periodic Table using periodic equation-of-motion coupled-cluster theory with single and double excitations (EOM-CCSD). Our calculations are performed with atom-centered triple-zeta basis sets and up to 64 k-points in the Brillouin zone. We analyze the convergence behavior with respect to the number of orbitals and number of k-points sampled using composite corrections and extrapolations to produce our final values. When accounting for electron-phonon corrections to experimental bandgaps, we find that EOM-CCSD has a mean signed error of -0.12eV and a mean absolute error of 0.42eV; the largest outliers are C (error of -0.93eV), BP (-1.00eV), and LiH (+0.78eV). Surprisingly, we find that the more affordable partitioned EOM-MP2 theory performs as well as EOM-CCSD.

Coupled-cluster theory for trapped bosonic mixtures.

We develop a coupled-cluster theory for bosonic mixtures of binary species in external traps, providing a promising theoretical approach to demonstrate highly accurately the many-body physics of mixtures of Bose-Einstein condensates. The coupled-cluster wavefunction for the binary species is obtained when an exponential cluster operator eT, where T = T(1) + T(2) + T(12) and T(1) accounts for excitations in species-1, T(2) for excitations in species-2, and T(12) for combined excitations in both species, acts on the ground state configuration prepared by accumulating all bosons in a single orbital for each species. We have explicitly derived the working equations for bosonic mixtures by truncating the cluster operator up to the single and double excitations and using arbitrary sets of orthonormal orbitals for each of the species. Furthermore, the comparatively simplified version of the working equations are formulated using the Fock-like operators. Finally, using an exactly solvable many-body model for bosonic mixtures that exists in the literature allows us to implement and test the performance and accuracy of the coupled-cluster theory for situations with balanced as well as imbalanced boson numbers and for weak to moderately strong intra- and interspecies interaction strengths. The comparison between our computed results using coupled-cluster theory with the respective analytical exact results displays remarkable agreement exhibiting excellent success of the coupled-cluster theory for bosonic mixtures. All in all, the correlation exhaustive coupled-cluster theory shows encouraging results and could be a promising approach in paving the way for high-accuracy modeling of various bosonic mixture systems.

Pb2H2 +: convergent quantum mechanical study of seven lead hydride cation structures. Toward laboratory identification

ABSTRACT Lead is heavily utilised in industry, but it bears potential harm due to its toxic nature. Identifying lead is important in diagnosing and preventing lead poisoning. Hydride generation via inductively-coupled plasma mass spectrometer (HG-ICP-MS) can detect small amounts of lead with high accuracy. Here we investigate seven structures of Pb 2 H 2 + . The geometries of each structure were optimised using coupled cluster with single, double, and perturbative triple excitations [CCSD(T)] method with the cc-pwCVQZ-PP basis set for lead and the cc-pVQZ basis set for hydrogen. Likewise, harmonic vibrational frequencies were obtained using the same method. Anharmonic frequencies were determined using CCSD(T) with cc-pwCVTZ-PP and cc-pVTZ basis sets for lead and hydrogen, respectively. The focal point approach (FPA), including CCSDT and CCSDT(Q) computations, was applied to the seven structures to find the relative energies with respect to the global minimum butterfly structure. Relative to the global minimum butterfly structure, the energies for the planar transition state, monobridged, vinylidene-like, trans, cis, and linear structures are: 1.1, 18.3, 26.5, 27.8, 28.8, and 93.7 kcal mol − 1 , respectively. Natural bond orders and dipole moments are reported as well. The predicted vibrational frequencies should be helpful in guiding the laboratory observation of Pb 2 H 2 + .

Daily and annual modulation rate of low mass dark matter in silicon detectors

Low-threshold solid-state detectors with single electron excitation sensitivity can probe nuclear recoil energies in the sub-100 eV range, coinciding with the typical threshold displacement energies in the detector material. We investigate the daily and annual modulation of the observable event rate for dark matter mass ranging from 0.2 to 5 GeV/c2 in a silicon detector, considering the energy threshold and the direction of the nuclear recoil. The data for the energy threshold is obtained from a molecular dynamics simulation. It is shown that the directional dependence of the threshold energy and the motion of the laboratory result in the modulation of the interaction event rate. We demonstrate silicon’s average annual interaction rate is more considerable than germanium for low-mass dark matter. However, their event rates take a similar trend in large dark matter masses. Thus, silicon can be a reliable target to discriminate low-mass dark matter from backgrounds. We also find 8 h and 12h periodicities in the time series of event rates for silicon detectors due to the 45-degree symmetry in the silicon crystal structure.

Multicolor Tunable Upconversion Luminescence via Near‐Infrared Manipulation of Population Pathways of Er3+ Ions Excited‐State Levels for Volumetric Color Displays

AbstractPrecise control over multicolor luminescence of upconversion nanoparticles (UCNPs) is of significant importance for their applications in widespread fields of research. However, realizing the tunable emissions in single UCNPs with a single lanthanide element remains a great challenge. Herein, without multiple lanthanide elements, a new strategy for the regulation of the excited‐state level population pathways of the same lanthanide activator Er3+ ion to obtain multicolor‐tunable upconversion luminescence is proposed through utilizing 980 nm coupled 1973 nm synergistic excitation. Unlike typical single wavelength excitation, the synergistic excitation may affect population pathways of the excited‐state level of Er3+ ion by adjusting excitation wavelength and power density, resulting in a dynamically adjustable change in luminescence color output. Notably, multicolor luminescence involving green, chartreuse, yellow, orange, and red can be tuned dynamically in the NaYF4:Er3+ single UCNPs by using the tunable 980/1973 nm synergistic excitation. This dynamic luminescence color variation from these UCNPs has demonstrated promising potential applications in volumetric color display. The results provide a new approach to achieve multicolor‐tunable upconversion luminescence at single nanoparticles level and open up the possibility of developing true three‐dimensional volumetric color display technologies with resolution at the nanometer range.