Metastable Excited State Research Articles

H-D Analysis Employing Energy Transfer from Metastable Excited-State He in Double-Pulse LIBS with Low-Pressure He Gas.

A laser-induced-breakdown-spectroscopy (LIBS) experiment with a unique double-pulse setup and operated in low-pressure (3 kPa) He ambient gas is performed to study the detection of light elements, such as hydrogen (H) and deuterium (D), as well as elements of high excitation energies, such as fluorine (F) and chlorine (Cl), which are usually difficult to detect using ordinary LIBS techniques. A nanosecond Nd:YAG laser operated in its fundamental wavelength with energy of 54 mJ is focused onto the Al target to generate the He plasma. Another picosecond Nd:YAG laser operated in its fundamental wavelength with energy of 2 mJ is focused onto the sample surface and activated 2 μs before the operation of the nanosecond laser. The application to polyvinyl chloride (PVC) and polytetrafluoroethylene (PTFE) samples produces sharp and high-intensity Cl- and F-emission lines. Meanwhile, the sharp and well-resolved H-D-emission lines with merely 0.18 nm wavelength separation are also clearly detected from a zircaloy sample. Further measurement of a set of zircaloy samples containing different concentrations of D yields a linear calibration curve with a zero intercept. The detection limit of D is found to be about 10 ppm.

Enhancement of carbon detection sensitivity in laser induced breakdown spectroscopy with low pressure ambient helium gas

Carbon detection is usually difficult to carry out with high sensitivity and minimally destructive effect. While the conventional laser induced breakdown spectroscopy (LIBS) method operated with atmospheric ambient air is well known as a powerful and versatile analytical tool, it suffers nevertheless from the low sensitivity of C detection when measured in both atmospheric and low pressure ambient air with the more adverse effect found in the former case. This was shown to have its origin in the serious time mismatching effect between the formation of the shock wave plasma by the ablated major host elements and the premature fast passage of the much lighter ablated C atom. However, this study shows the result of high sensitivity C analysis of stone samples using LIBS technique with relatively low laser pulse energy of 60 mJ and low pressure He ambient gas without showing visible surface damage. The helium gas provides the additional delayed excitation by the He metastable excited states through the Penning-like ionization process. The C emission intensities measured from the jasper and black stone in 2.6 kPa He ambient gas are in general significantly higher than those measured in 0.5 kPa ambient air. The enhancement is shown to increase reaching an 8 fold enhancement with increased laser energy up to 60 mJ before undesirable surface damage is created. A further measurement of C emission using pelletized KBr mixtures with various CaCO3 concentrations reveals a straight calibration line of rather large slope with extrapolated zero intercept and estimated detection limit of around 0.6 ppm, demonstrating its potential application for highly sensitive quantitative analysis of C with minimal destructive effect.

Characterization of a plasma source for biomedical applications by electrical, optical, and chemical measurements

This paper reports the characterization of a low‐power, atmospheric pressure plasma source developed for and successfully tested in applications of plasma medicine. The source produces plasma by ionizing a helium flow containing traces of air. The effluent gas is thus enriched in reactive oxygen and nitrogen species as well as helium metastable excited states. Electrical measurements, Schlieren imaging, OES and various chemical analyses and probes enabled us to fully characterize the plasma source and to determine some fundamental parameters for treating living samples such as the power feeding the discharge, the optimal source to target distance, the maximum exposure time, and to identify the major chemical species responsible for the biological action on exposed living matter.

Resonance State Method for Electron Injection in Dye Sensitized Solar Cells

Herein, the ab initio method is applied to examine metastable molecular excited states on a solid surface using resonance state theory and Green's function. A formula for the complex energy correction that determines the decay rate is presented; the configuration interaction effect together with major molecule-surface interactions are considered in more detail as compared to previous studies. Furthermore, the lifetimes of the excited states of Ru-terpyridine dyes adsorbed on an anatase surface are calculated, and the effects of the molecular structure and adsorption mode on the electron injection rate are studied. Also, the adsorption structures and relative stabilities of a series of Ru-terpyridine dyes-including the black dye-are reported. An implicit solvation model is necessary to reliably calculate the alignment between the photoabsorption spectrum and the conduction band density of states, governing the injection rate. Finally, some of the factors that limit the injection ability of dyes are discussed.

Luminescence of ND radicals during the destruction of molecular nitrogen nanoclusters

In this work we studied optical spectra of thermoluminescence accompanying the destruction of collections of molecular nitrogen nanoclusters containing stabilized nitrogen, oxygen, and deuterium atoms. These collections of nanoclusters were formed by the injection of products of a radio-frequency discharge in deuterium-nitrogen-helium gas mixtures into bulk superfluid 4He. In the range from 200 to 1650 nm, the bands at 336 nm, 473 nm along with a new band at 1170 nm as well as the known bands of atomic nitrogen and oxygen, and bands of molecular nitrogen, oxygen, and NO were observed. These three bands were assigned to the emission of the ND radicals formed due to recombinations of nitrogen atoms in excited metastable states and deuterium atoms in the ground state during the destruction of ensembles of molecular nitrogen nanoclusters.

Real and Imaginary Excitons: Making Sense of Resonance Wave Functions by Using Reduced State and Transition Density Matrices.

Within non-Hermitian quantum mechanics, metastable electronic states can be represented by isolated L2-integrable complex-valued wave functions with complex energies. An analysis scheme of the real and imaginary parts of resonance wave functions by using reduced transition density matrices and natural transition orbitals is presented. While the real parts of excitons describe changes in the electron density corresponding to the bound part of the resonance, the imaginary excitons can be interpreted as virtual states facilitating one-electron decay into the continuum. The different nature of real and imaginary excitons is revealed by exciton descriptors, in particular hole-particle separation and their correlation. Singular values and respective participation ratios quantify the extent of collectivity of the excitation and a number of distinct decay channels. The utility of the new tool is illustrated by the analysis of bound and metastable excited states of cyanopolyyne anions.

A volume-averaged model of nitrogen–hydrogen plasma chemistry to investigate ammonia production in a plasma-surface-interaction device

Nitrogen impurity seeding is a promising technique for increasing the radiative power dissipation rate in the edge plasma of a fusion device. It will be required in future fusion devices such as ITER to reduce the directed heat flux on the divertor strike-points to within erosion limits. However, chemical reactions between nitrogen and fuel isotopes may complicate tritium control measures by increasing in-vessel retention and impacting the gas-handling plant. To gain insight into the nitrogen–hydrogen plasma chemistry a volume-averaged (global) model is developed and compared with experimental measurements in the MAGnetised Plasma Interaction Experiment plasma device. A set of 702 reactions is compiled and used to model the population dynamics of 51 relevant neutral, ionic, electron, surface and metastable excited state species. Stable equilibrium values are compared to results from an experimental investigation in which a combination of mass spectrometry, Langmuir probe analysis and optical emission spectroscopy is used to determine neutral and positive-ionic trends under the same conditions. The dominant ammonia production mechanism is found to be the Langmuir–Hinshelwood reaction between adsorbed atomic hydrogen and above 25% hydrogen concentration. For lower hydrogen proportions the Eley–Rideal reaction between free atomic hydrogen and is found to dominate. The dominant loss mechanism (for all compositions) is found to be electron impact dissociation into neutral fragments.

Localized Magnetic Moments with Tunable Spin Exchange in a Gas of Ultracold Fermions.

We report on the experimental realization of a state-dependent lattice for a two-orbital fermionic quantum gas with strong interorbital spin exchange. In our state-dependent lattice, the ground and metastable excited electronic states of ^{173}Yb take the roles of itinerant and localized magnetic moments, respectively. Repulsive on-site interactions in conjunction with the tunnel mobility lead to spin exchange between mobile and localized particles, modeling the coupling term in the well-known Kondo Hamiltonian. In addition, we find that this exchange process can be tuned resonantly by varying the on-site confinement. We attribute this to a resonant coupling to center-of-mass excited bound states of one interorbital scattering channel.

A New Window into Escaping Exoplanet Atmospheres: 10830 Å Line of Helium

Observational evidence for escaping exoplanet atmospheres has been obtained for a few exoplanets to date. It comes from strong transit signals detected in the ultraviolet, most notably in the wings of the hydrogen Lyman-$\alpha$ (Ly$\alpha$) line. However, the core of the Ly$\alpha$ line is often heavily affected by interstellar absorption and geocoronal emission, limiting the information about the atmosphere that can be extracted from that part of the spectrum. Transit observations in atomic lines that are (a) sensitive enough to trace the rarefied gas in the planetary wind and (b) do not suffer from significant extinction by the interstellar medium could enable more detailed observations, and thus provide better constraints on theoretical models of escaping atmospheres. The absorption line of a metastable state of helium at 10830 \AA\ could satisfy both of these conditions for some exoplanets. We develop a simple 1D model of escaping planetary atmospheres containing hydrogen and helium. We use it to calculate the density profile of helium in the 2$^3$S metastable excited state and the expected in-transit absorption at 10830 \AA\ for two exoplanets known to have escaping atmospheres. Our results indicate that exoplanets similar to GJ 436b and HD 209458b should exhibit enhanced transit depths at 10830 \AA, with $\sim 8\%$ and $\sim 2\%$ excess absorption in the line core, respectively.

Anomalous diamagnetic response in multiband superconductors with broken time-reversal symmetry

Within a Ginzburg-Landau formalism we establish analytically the necessary and sufficient conditions to realize a doubly degenerate superconducting ground state with broken time-reversal symmetry (BTRS) in a multi-band superconductor. Using these results we analyze the ground state of a three-band superconductor in the cylindrical geometry in an external magnetic field. We show that depending on the interband coupling constants, a magnetic flux can induce current density jumps in such superconducting geometries that are related to adiabatic or non-adiabatic transitions from BTRS to time-reversal symmetric states and vice versa. This unusual current induced magnetic flux response can in principle be used experimentally to detect superconducting BTRS ground states as well as corresponding metastable excited states.

Properties of arrays of microplasmas: application to control of electromagnetic waves

Microplasma arrays (MAs) are being investigated as a method to control the propagation of electromagnetic waves. The use of MAs as an electromagnetic wave controlling material is attractive as the electrical properties of MAs can be rapidly changed through combinations of the choice of operating conditions (e.g. pressure, gas mixture), the spatial distribution of the plasma and applied voltage waveforms. In this paper, results from a computational investigation of the plasma properties of small arrays of microplasmas are discussed. The model systems are arrays of microplasmas sustained in rare gases at pressures of up to 100 Torr in a sealed chamber. Individual plasma cells are ≈100 μm in size. Pulsed dc voltage waveforms having widths of 30 ns are applied at repetition rates of up to 10 MHz. The cross-talk between plasma cells was investigated, as well as the consequences of gas heating and sequencing of the pulses. We found that even without physical barriers between the plasma cells to control cross-talk between cells, the individual character of each cell can be retained; however the plasma cells were not completely independent. The diffusion of metastable excited atomic states and small fluxes of ions did enable adjacent cells to operate at lower voltages. The ability to control microwave propagation through waveguides was computationally investigated by placing a MA inside a standard waveguide and examining the resulting transmission coefficients. We found that for frequencies of tens to 100 GHz, the transmitted power could be controlled by the spatial distribution of the MA cells with respect to the modal structure of the wave.

Escape of O(3P), O(1D), and O(1S) from the Martian atmosphere

We have computed here the escape probabilities, fluxes and rates for hot O atoms that are initially produced in the ground state and the first two excited metastable states, O(1D)and O(1S), in the Martian thermosphere by dissociative recombination of O2+. In order to compare our results with those of our previous calculations and with those of others, we have employed here the pre-MAVEN models that we have used previously. To compute the escape probabilities, we have employed the Monte Carlo escape code that has been described previously, but we here use for the first time energy-dependent elastic cross sections for collisions of the energetic O atoms with each of the twelve background species in our model. We also incorporate three mechanisms that interchange identities of the O(3P) and O(1D) atoms, including collisional excitation of O(3P) to O(1D), quenching of O(1D) to O(3P), and excitation exchange of O(1D) with O(3P). We find that the escape probabilities of O atoms that are produced initially as O(1D) are reduced compared to those in which these processes are not included, but the escape probabilities of O atoms that are initially produced as O(3P) are not significantly reduced. As a guide for our future research and those of other investigators, we review here what is known about the interactions of O atoms with other species in which the energies of the O atoms are altered, and several other sources of hot and escaping O, many of which have been suggested by other investigators. We will incorporate these data in a future MAVEN-like model.

Variational Monte Carlo method for fermionic models combined with tensor networks and applications to the hole-doped two-dimensional Hubbard model

The conventional tensor-network states employ real-space product states as reference wave functions. Here, we propose a many-variable variational Monte Carlo (mVMC) method combined with tensor networks by taking advantages of both to study fermionic models. The variational wave function is composed of a pair product wave function operated by real space correlation factors and tensor networks. Moreover, we can apply quantum number projections, such as spin, momentum and lattice symmetry projections, to recover the symmetry of the wave function to further improve the accuracy. We benchmark our method for one- and two-dimensional Hubbard models, which show significant improvement over the results obtained individually either by mVMC or by tensor network. We have applied the present method to hole doped Hubbard model on the square lattice, which indicates the stripe charge/spin order coexisting with a weak $d$-wave superconducting order in the ground state for the doping concentration less than 0.3, where the stripe oscillation period gets longer with increasing hole concentration. The charge homogeneous and highly superconducting state also exists as a metastable excited state for the doping concentration less than 0.25.

Adiabatically tuning quantized supercurrents in an annular Bose-Einstein condensate

The ability to generate and tune quantized persistent supercurrents is crucial for building superconducting or atomtronic devices with novel functionalities. In ultracold atoms, previous methods for generating quantized supercurrents are generally based on dynamical processes to prepare atoms in metastable excited states. Here we show that arbitrary quantized circulation states can be adiabatically prepared and tuned as the ground state of a ring-shaped Bose-Einstein condensate by utilizing spin-orbital-angular-momentum (SOAM) coupling and an external potential. There exists superfluid hysteresis for tuning supercurrents between different quantization values with nonlinear atomic interactions, which is explained by developing a nonlinear Landau-Zener theory. Our work will provide a powerful platform for studying SOAM coupled ultracold atomic gases and building novel atomtronic circuits.

Non-Hermitian matter-wave mixing in Bose-Einstein condensates: Dissipation-induced amplification

We investigate the nonlinear scattering dynamics in interacting atomic Bose-Einstein condensates under non-Hermitian dissipative conditions. We show that by carefully engineering a momentum-dependent atomic loss profile one can achieve matter-wave amplification through four wave mixing in a one-dimensional quasi free-space setup - a process that is forbidden in the counterpart Hermitian systems due to energy mismatch. Additionally, we show that similar effects lead to rich nonlinear dynamics in higher dimensions. Finally, we propose a physical realization for selectively tailoring the momentum-dependent atomic dissipation. Our strategy is based on a two step process: (i) exciting atoms to narrow Rydberg- or metastable excited states, and (ii) introducing loss through recoil; all while leaving the bulk condensate intact due to protection by quantum interference.

Development of a hybrid model to quantify the single and double strand breaks following the iron 57 de-excitation

The therapeutic utility of certain Auger emitters such as iodine-125 depends on their position within the cell nucleus. Or diagnostically, and to maintain as low as possible cell damage, it is preferable to have radionuclide localized outside the cell or at least the core. One solution to this problem is to consider markers capable of conveying anticancer drugs to the tumor site regardless of their location within the human body. The objective of this study is to simulate the impact of a complex such as bleomycin on single and double strand breaks in the DNA molecule. Indeed, this simulation consists of the following transactions: Construction of BLM -Fe- DNA complex, simulation of the electron’s transport from the metastable state excitation of Fe 57 by the Monte Carlo method, treatment of chemical reactions in the considered environment by the diffusion equation. For physical, physico-chemical and finally chemical steps, the geometry of the complex is considered as a sphere of 50 nm centered on the binding site , and the mathematical method used is called step by step based on Monte Carlo codes.

Interaction between the exchanged Mn2+ and Yb3+ ions confined in zeolite-Y and their luminescence behaviours

Luminescent zeolites exchanged with two distinct and interacted emissive ions are vital but less-studied for the potential applications in white light emitting diodes, solar cells, optical codes, biomedicine and so on. Typical transition metal ion Mn2+ and lanthanide ion Yb3+ are adopted as a case study via their characteristic transitions and the interaction between them. The option is considered with that the former with d-d transition has a large gap between the first excited state 4T1 and the ground state 6A1 (normally >17,000 cm−1) while the latter with f-f transition has no metastable excited state above 10,000 cm−1, which requires the vicinity of these two ions for energy transfer. The results of various characterizations, including BET measurement, photoluminescence spectroscopy, solid-state NMR, and X-ray absorption spectroscopy, etc., show that Yb3+ would preferably enter into the zeolite-Y pores and introduction of Mn2+ would cause aggregation of each other. Herein, cation-cation repulsion may play a significant role for the high valence of Mn2+ and Yb3+ when exchanging the original cations with +1 valence. Energy transfer phenomena between Mn2+ and Yb3+ occur only at elevated contents in the confined pores of zeolite. The research would benefit the design of zeolite composite opto-functional materials.

Long-range interactions of hydrogen atoms in excited states. I.2S−1Sinteractions and Dirac-δperturbations

The theory of the long-range interaction of metastable excited atomic states with ground-state atoms is analyzed. We show that the long-range interaction is essentially modified when quasi-degenerate states are available for virtual transitions. A discrepancy in the literature regarding the van der Waals coefficient C_6(2S;1S) describing the interaction of metastable atomic hydrogen (2S state) with a ground-state hydrogen atom is resolved. In the the van der Waals range a_0 << R << a_0/alpha, where a_0= hbar/(alpha m c) is the Bohr radius and alpha is the fine structure constant, one finds the symmetry-dependent result E_{2S;1S}(R) ~ (-176.75 +/- 27.98) E_h (a_0/R)^6 (E_h denotes the Hartree energy). In the Casimir-Polder range a_0/alpha << R << hbar c/L, where L = E(2S_{1/2})-E(2P_{1/2}) is the Lamb shift energy, one finds E_{2S;1S}(R) ~ (-121.50 +/- 46.61) E_h (a_0/R)^6. In the the Lamb shift range R >> hbar c/L, we find an oscillatory tail with a negligible interaction energy below 10^(-36) Hz. Dirac-delta perturbations to the interaction are also evaluated and results are given for all asymptotic distance ranges; these effects describe the hyperfine modification of the interaction, or, expressed differently, the shift of the hydrogen 2S hyperfine frequency due to interactions with neighboring 1S atoms. The 2S hyperfine frequency has recently been measured very accurately in atomic beam experiments.

Magnetic-field control of subradiance states of a system of two atoms

A method is proposed for the creation of an entangled metastable (subradiance) excited state in a system of two closely spaced identical atoms. The system of unexcited atoms is first placed in a magnetic field that is directed at a magic angle of $${\alpha _0} = {\text{arccos}}\left( {1/\sqrt 3 } \right) \approx 54.7^\circ $$ to the line connecting the atoms and has a transverse gradient. The gradient of the field results in the detuning of frequencies of an optical transition of the atoms. Then, the resonant laser excitation of an atom with a higher transition frequency is performed with the subsequent adiabatic switching-off of the gradient of the magnetic field. It is shown that the excited atomic system in this case transits with overwhelming probability to an entangled subradiance state. Requirements on the spectroscopic parameters of the transitions and on the rate of varying the gradient of the magnetic field necessary for the implementation of this effect are analyzed.

A summary of results obtained with the cryogenic electrostatic storage ring DESIREE

This paper highlights results from recent studies of cryogenically cooled atomic and molecular anions carried out at the DESIREE storage ring facility at Stockholm University in Stockholm, Sweden. These results include measurements of lifetimes of excited metastable states in atomic anions (S−, Se−, Te−, Ni−, and Pt−), pilot studies of rotational cooling of OH−, and cooling and decay of cluster anions exemplified by results for Ag5−.