Spectrum of the two-photon emission from the metastable state of singly ionized helium.
Spectral distribution of two photon emission from metastable state of singly ionized He by broadband spectroscopic coincidence counting technique
Artura, C. J.↗
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Results for “METASTABLE STATES”
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Direct detection of two-photon emission from the metastable state of singly ionized helium.
Detection by coincidence counting techniques of two-photon decay of metastable state of singly ionized helium
PHOTON BEAM↗
Unravelling photoisomerization dynamics in a metastable-state photoacid
Direct access to the trans – cis photoisomerization dynamics in a complex photoreaction cycle of an indazole metastable state photoacid is realized.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Multi-metastable states induced by the optical pump-probe process in terahertz quantum cascade lasers
The optical pump-probe process in terahertz quantum cascade lasers is studied theoretically by using the open system simulation method. The emitter injection is considered and the charge neutrality in the active region is broken. We find that nonequilibrium oscillations may appear in the recovery processes. In particular, the formation of different equilibrium values of the population change after the periodic pulse pumping is observed clearly. Here, the phenomenon of multi-metastable states stems from the electron regulation by the emitter injection. Finally, we discuss the important impacts of the equilibrium stabilization time and obtain an in-depth understanding of the emitter injection.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Metastable states and mass loss in Be stars
Three strong asymmetric absorption features with short-wavelength wings extending 350 km/s from their respective line centers at 2061.6, 2068.2, and 2079.0 A appear in high-resolution UV spectral data (0.1 A) for the Be star Phi Per (B2 Ve4) obtained with the Balloon-borne Ultraviolet Stellar Spectrometer (BUSS) on the evening of September 16, 1976. These transitions are not resonance lines and have been identified as transitions of Fe III (UV 48) originating from a metastable state with an excitation of 5.01 eV. The relative populations of the metastable and ground states are independent of the dilution factor, allowing calculation of the mass-outflow rate for a generalized model. Thus, a mass-outflow rate of 5 hundred-billionths of a solar mass per year is obtained. These transitions are observable with IUE and represent an important tool for studying mass outflow in Be and shell stars.
Bruhweiler, F. C.↗
Metastable states of highly excited heavy ions
Description of the method used and results obtained in an experimental study of the metastable states of highly stripped heavy ions, aimed at determining the lifetimes of such states by the rates of autoionization and radiation. The significance and limitations of the results presented are discussed.
Pegg, D. J.↗
The quenching effect of hydrogen on the nitrogen in metastable state in atmospheric-pressure N{sub 2}-H{sub 2} microwave plasma torch
The atmospheric-pressure microwave N{sub 2}-H{sub 2} plasma torch is generated and diagnosed by optical emission spectroscopy. It is found that a large amount of N atoms and NH radicals are generated in the plasma torch and the emission intensity of N{sub 2}{sup +} first negative band is the strongest over the spectra. The mixture of hydrogen in nitrogen plasma torch causes the morphology of the plasma discharge to change with appearance that the afterglow shrinks greatly and the emission intensity of N{sub 2}{sup +} first negative band decreases with more hydrogen mixed into nitrogen plasma. In atmospheric-pressure microwave-induced plasma torch, the hydrogen imposes a great influence on the characteristics of nitrogen plasma through the quenching effect of the hydrogen on the metastable state of N{sub 2}.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Solid-State Interconversions: Unique 100 % Reversible Transformations between the Ground and Metastable States in Single-Crystals of a Series of Nickel(II) Nitro Complexes
The solid-state, low-temperature linkage isomerism in a series of five square planar group 10 phosphino nitro complexes have been investigated by a combination of photocrystallographic experiments, Raman spectroscopy and computer modelling. The factors influencing the reversible solid-state interconversion between the nitro and nitrito structural isomers have also been investigated, providing insight into the dynamics of this process. The cis-[Ni(dcpe)- (NO 2 ) 2 ] (1) and cis-[Ni(dppe)(NO 2 ) 2 ] (2) complexes show reversible 100% interconversion between the h 1 -NO 2 nitro isomer and the h 1 -ONO nitrito form when single-crystals are irradiated with 400 nm light at 100 K. Variable temperature photocrystallographic studies for these complexes established that the metastable nitrito isomer reverted to the ground-state nitro isomer at temperatures above 180 K. By comparison, the related trans complex [Ni(PCy 3 ) 2 (NO 2 ) 2 ] (3) showed 82% conversion under the same experimental conditions at 100 K. The level of conversion to the metastable nitrito isomers is further reduced when the nickel centre is replaced by palladium or platinum. Prolonged irradiation of the trans-[Pd(PCy 3 ) 2 (NO 2 ) 2 ] (4) and trans-[Pt(PCy 3 ) 2 (NO 2 ) 2 ] (5) with 400 nm light gives reversible conversions of 44 and 27%, respectively, consistent with the slower kinetics associated with the heavier members of group 10. The mechanism of the interconversion has been investigated by theoretical calculations based on the model complex [Ni(dmpe)Cl(NO 2 )].
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Structural Evolution of Photoexcited Methylcobalamin toward a CarH-like Metastable State: Evidence from Time-Resolved X-ray Absorption and X-ray Emission
CarH is a protein photoreceptor that uses a form of B 12 , adenosylcobalamin (AdoCbl), to sense light via formation of a metastable excited state. Aside from AdoCbl bound to CarH, methylcobalamin (MeCbl) is the only other example – to date – of photoexcited cobalamins forming metastable excited states with lifetimes of nanoseconds or longer. The UV-visible spectra of the excited states of MeCbl and AdoCbl bound to CarH are similar. We have used transient Co K-edge X-ray absorption and X-ray emission spectroscopies in conjunction with transient absorption spectroscopy in the UV–visible region to characterize the excited states of MeCbl. These data show that the metastable excited state of MeCbl has a slightly expanded corrin ring and increased electron density on the cobalt, but only small changes in the axial bond lengths. Finally, this is similar to changes seen previously for CarH, suggesting that MeCbl may be a good model for AdoCbl in CarH.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Theory of Metastable State Relaxation for Non-Critical Binary Systems with Non-Conserved Order Parameter
A new mathematical ansatz for a solution of the time-dependent Ginzburg-Landau non-linear partial differential equation is developed for non-critical systems such as non-critical binary solutions (solute + solvent) described by the non-conserved scalar order parameter. It is demonstrated that in such systems metastability initiates heterogeneous solute redistribution which results in formation of the non-equilibrium singly-periodic spatial solute structure. It is found how the time-dependent period of this structure evolves in time. In addition, the critical radius r(sub c) for solute embryo of the new solute rich phase together with the metastable state lifetime t(sub c) are determined analytically and analyzed.
Izmailov, Alexander↗
Observation of multiple metastable states induced by electric pulses in the hysteresis temperature range of 1 T - TaS 2
The electric pulses induced responses of 1T - TaS 2 in the commensurate charge-density-wave phase in the hysteresis temperature region (160 ~ 210 K) have been investigated. We observed an abrupt jump of the resistance excited by pulse, followed by a slow relaxation process in a time scale of ~ 100 s. At a fixed temperature, the various electric pulses can drive the system to multi metastable states. Here, we propose that the spontaneous evolution or slow relaxation of the system by pulse excitations corresponds to the rearrangements of the textures of CCDW domains.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Photochemically-Driven CO 2 Release Using a Metastable-State Photoacid for Energy Efficient Direct Air Capture
One of the grand challenges underlying current direct air capture (DAC) technologies relates to the intensive energy cost for sorbent regeneration and CO 2 release, making the massive scale (GtCO 2 /year) deployment required to have a positive impact on climate change economically unfeasible. This challenge underscores the critical need to develop new DAC processes with substantially reduced regeneration energies. Here, in this work, we report a photochemically-driven approach for CO 2 release by exploiting the unique properties of an indazole metastable-state photoacid (mPAH). Our measurements on simulated and amino acid-based DAC systems revealed the potential of mPAH to be used for CO 2 release cycles by regulating pH changes and associated isomers driven by light. Upon irradiating with moderate intensity light, a ≈55 % and ≈68 % to ≈78 % conversion of total inorganic carbon to CO 2 was found for the simulated and amino acid-based DAC systems, respectively. Our results confirm the feasibility of on-demand CO 2 release under ambient conditions using light instead of heat, thereby providing an energy efficient pathway for the regeneration of DAC sorbents.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Photochemically‐Driven CO 2 Release Using a Metastable‐State Photoacid for Energy Efficient Direct Air Capture
Abstract One of the grand challenges underlying current direct air capture (DAC) technologies relates to the intensive energy cost for sorbent regeneration and CO 2 release, making the massive scale (GtCO 2 /year) deployment required to have a positive impact on climate change economically unfeasible. This challenge underscores the critical need to develop new DAC processes with substantially reduced regeneration energies. Here, we report a photochemically‐driven approach for CO 2 release by exploiting the unique properties of an indazole metastable‐state photoacid (mPAH). Our measurements on simulated and amino acid‐based DAC systems revealed the potential of mPAH to be used for CO 2 release cycles by regulating pH changes and associated isomers driven by light. Upon irradiating with moderate intensity light, a ≈55 % and ≈68 % to ≈78 % conversion of total inorganic carbon to CO 2 was found for the simulated and amino acid‐based DAC systems, respectively. Our results confirm the feasibility of on‐demand CO 2 release under ambient conditions using light instead of heat, thereby providing an energy efficient pathway for the regeneration of DAC sorbents.
Premadasa, Uvinduni I.↗
Tuning the Properties of Nanocomposites by Trapping Them in Deep Metastable States
We report the interfacial region formed in a polymer matrix around nanoparticles (NPs) controls many macroscopic properties of polymer nanocomposites (PNCs). However, understanding the factors controlling structure and properties of interfacial region remains a challenge. We demonstrated that the initial trapping of polymer chains at surfaces of NPs in solution strongly affects the macroscopic properties of PNCs. The most surprising result is that the differences in properties of PNCs persist even after an extremely long thermal annealing time. We ascribe the observed changes to the formation of interfacial layer that is trapped in a deep metastable state already in solution. Furthermore, presented analysis suggests that PNC equilibration time is defined by the chain desorption time that can be extremely long and, in some cases, even not accessible on a reasonable experimental time scale. These results highlight the importance of polymer solution concentrations on the formation of interfacial layer and the macroscopic properties of PNCs.
36 MATERIALS SCIENCE↗
Magnesium ions mitigate metastable states in the regulatory landscape of mRNA elements
Residing in the 5' untranslated region of the mRNA, the 2'-deoxyguanosine (2'-dG) riboswitch mRNA element adopts an alternative structure upon binding of the 2'-dG molecule, which terminates transcription. RNA conformations are generally strongly affected by positively charged metal ions (especially Mg 2+ ). We have quantitatively explored the combined effect of ligand (2'-dG) and Mg 2+ binding on the energy landscape of the aptamer domain of the 2'-dG riboswitch with both explicit solvent all-atom molecular dynamics simulations (99 μsec aggregate sampling for the study) and selective 2'-hydroxyl acylation analyzed by primer extension (SHAPE) experiments. We show that both ligand and Mg 2+ are required for the stabilization of the aptamer domain; however, the two factors act with different modalities. The addition of Mg 2+ remodels the energy landscape and reduces its frustration by the formation of additional contacts. In contrast, the binding of 2'-dG eliminates the metastable states by nucleating a compact core for the aptamer domain. Mg 2+ ions and ligand binding are required to stabilize the least stable helix, P1 (which needs to unfold to activate the transcription platform), and the riboswitch core formed by the backbone of the P2 and P3 helices. Mg 2+ and ligand also facilitate a more compact structure in the three-way junction region.
59 BASIC BIOLOGICAL SCIENCES↗
First-principles calculations of solute transport in zirconium: Vacancy-mediated diffusion with metastable states and interstitial diffusion
Zirconium alloys are the most widely used nuclear fuel cladding materials for light water power reactors where irradiation damage causes solute redistribution, leading to degradation of alloy properties such as corrosion resistance. Designing radiation-tolerant zirconium alloys requires a thorough understanding of the atomic-scale transport behavior of the alloying elements in Zr. In this work, we perform density function theory calculations to investigate the diffusion of Sn, Cr, Fe, Be, Al, and Ni in the hexagonal close-packed (HCP) Zr matrix. We develop a methodology to accurately model the metastable vacancy states along the basal migration path, known to occur in group IV metals. We compute the vacancy-mediated solute diffusion coefficients and drag ratios using the kinetic Monte Carlo method and an analytic Green's function method—the agreement between the two validates our methodology. The computed diffusion coefficients of Sn and Al show good agreement with the experimental data and we expect these solutes to diffuse via the vacancy-mediated mechanism. We use a Green's function approach, parameterized with data from density functional theory calculations, to compute the interstitial diffusion coefficients of Cr, Fe, Be, and Ni in the HCP Zr lattice. The computed diffusion coefficients of Cr, Ni, and Be agree with the experimental measurements within one order of magnitude, while those of Fe are within two orders of magnitude of the experimental measurements. The drag ratios for Cr, Fe, Be, and Ni are positive up to 1235 K, which suggests that nonequilibrium vacancy fluxes could drag these solutes toward sinks such as dislocation loops and grain boundaries. We also compute the transport coefficients without including the metastable states, and using the eight- and thirteen-frequency model. Our results show significant differences in drag ratio for the eight- and thirteen-frequency model predictions compared with the Green's function methodology, but smaller errors in the solute diffusivity. Combining interstitial and vacancy-mediated diffusivities, we predict the unusual result that increased vacancy concentration slows down solute diffusivity, while a sufficiently high vacancy concentration can change the dominant mechanism to an accelerated vacancy-mediated diffusion.
36 MATERIALS SCIENCE↗
Surface-supported cluster catalysis: Ensembles of metastable states run the show
It has recently been demonstrated that the dynamic behaviour of surface-supported nanocluster catalysts in realistic reaction conditions defies conventional models used in catalysis. This opens new doors in catalysis by giving more leverage in catalyst design, but also requires a major revision of the understanding of how dynamic heterogeneous catalytic interfaces operate, as well as of the computational approaches of catalyst modelling, and experimental methods of catalyst characterization. Key aspects of the new paradigm include the collective action of many catalyst states that form a statistical ensemble in reacting conditions, the catalytic activity and selectivity being driven by rare and metastable catalyst states, reaction thermodynamics and kinetics being controlled by different states of the catalyst, broken scaling relationships, non-Arrhenius behaviours, and catalyst dynamic restructuring being an essential part of the reaction mechanism. For computation, this complexity means the departure from the standard DFT calculations of reaction mechanisms on a single catalyst structure. For experiment, it calls for the development of operando characterization tools with the per-site resolution and the ability to find the minority sites that govern the catalytic activity. For catalyst design, the goal becomes the creation of the catalyst state (geometric and electronic) that might not be present in the as-prepared catalyst, but would develop in the reaction conditions and would have the desired activity then. While cluster catalysts are the most dramatic in their dynamic fluxionality, other amorphous interfaces also exhibit some of it, and thus are also subject to similar paradigm revision.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Time-of-flight measurements of metastable state lifetimes.
A time-of-flight method for measurement of the lifetime of metastable molecules is described. The method is applicable to a molecular beam that has molecules in several different metastable excited states. As compared to methods used previously, the method has the advantages that it does not require selective excitation or quenching of the different states; moreover, it does not require a determination of the relative populations or velocity distributions of molecules in the excited states.
Kaslow, D. E.↗