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292 records · Page 17

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NASA NTRS2002

Photodissociation of Peroxynitric Acid in the Near-IR

Temperature-dependent near-IR photodissociation spectra were obtained for several vibrational overtone transitions of peroxynitric acid (HNO4) with a tunable OPO photolysis/OH laser-induced-fluorescence system. Band-integrated photodissociation cross-sections (definity integral of sigma(sub diss)), determined relative to that for the 3nu(sub 1), OH stretching overtone, were measured for three dissociative bands. Assuming unit quantum efficiency for photodissociation of 3nu(sub 1), we find 2nu(sub 1) + nu(sub 3)(8242/cm) = (1.21 x 10(exp -20) (independent of temperature), 2nu(sub 1) (6900/cm) = 4.09 x 10(exp 18) * e(sup (-826,5/T)) (295 K greater than T greater than 224 K), and nu(sub 1) + 2nu(sub 3) (6252/cm) = 1.87 x 10(exp -19) * e(sup (- 1410.7/T)) (278 K greater than T greater than 240 K) sq cm/molecule cm. The photodissociation cross-sections are independent of pressure over the range 2 to 40 Torr. Temperature-dependent quantum yields (phi) for these transitions were obtained using integrated absorption cross-sections (definity integral of sigma(sub abs)) of HNO4 overtone vibrations measured with a FTIR spectrometer. In the atmosphere, photodissociation in the infrared is dominated by excitation of the first overtone of the OH stretching vibration (2nu((sub 1)). Inclusion of all dissociative HNO4 overtone and combination transitions yields a daytime IR photolysis rate of approximately 1 x 10(esp -1)/s. This process significantly shortens the estimated lifetime of HNO4 in the upper troposphere and lower stratosphere.

Roehl, Coleen M.↗

DOE OSTI2021

Photoluminescence Dynamics Defined by Exciton Trapping Potential of Coupled Defect States in DNA-Functionalized Carbon Nanotubes

Chemical reactions between semiconducting single-wall carbon nanotubes (SWCNTs) and single-stranded DNA (ssDNA) achieve spatially patterned covalent functionalization sites and create coupled fluorescent quantum defects on the nanotube surface, tailoring SWCNT photophysics for applications such as single-photon emitters in quantum information technologies. The evaluation of relaxation dynamics of photoluminescence (PL) from those coupled quantum defects is essential for understanding the nanotube electronic structure and beneficial to the design of quantum light emitters. Here, we measured the PL decay for ssDNA-functionalized SWCNTs as a function of the guanine content of the ssDNA oligo that dictates the red-shifting of their PL emission peaks relative to the band-edge exciton. We then correlate the observed dependence of PL decay dynamics on energy red-shifts to the exciton potential energy landscape, which is modeled using first-principles approaches based upon the morphology of ssDNA-altered SWCNTs obtained by atomic force microscopy (AFM) imaging. In this work, our simulations illustrate that the multiple guanine defects introduced within a single ssDNA strand strongly interact to create a deep exciton trapping well, acting as a single hybrid trap. The emission decay from the distinctive trapping potential landscape is found to be biexponential for ssDNA-modified SWCNTs. We attributed the fast time component of the biexponential PL decay to the redistribution of exciton population among the lowest energy bright states and a manifold of dark states emerging from the coupling of multiple guanine defects. The long lifetime component in the biexponential decay, on the other hand, is attributed to the redistribution of exciton population among different exciton trapping sites that arise from the binding of multiple ssDNA strands along the nanotube axis. AFM measurements indicate that those trapping sites are separated on average by ~8 nm along the nanotube axis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Influence of Water, Vacuum, and Temperature on Surface Conditions of a Zeolite‐based Molecular Sieve

Molecular sieves such as zeolite-based materials are ubiquitous in industrial separation processes. However, there is a significant gap in understanding the surface properties and adsorption mechanisms for commercial zeolites, as most research focuses on pure zeolite powders rather than industrially relevant forms. Here, this work addresses this gap in understanding by employing advanced characterization techniques, including positron annihilation spectroscopy, X-ray diffraction, scanning electron microscopy, X-ray fluorescence spectroscopy, X-ray photoelectron spectroscopy, liquid nitrogen sorption, and Fourier-transform infrared spectroscopy, to investigate the adsorption and desorption behavior of water in commercial zeolite 13X. Our research reveals insights into the pore-filling mechanisms, the impact of material binders on adsorption properties, and the dynamics of hydration and drying processes for zeolites. Monitoring changes on a minute scale allowed the distinction between fast and slow processes leading to sample drying. The identification of positronium bound to Na + ions indicated that water molecules remain in the vicinity of Na + ions after air-drying zeolite 13X. These findings highlight the importance of various environmental conditions in restoring zeolite properties to baseline after hydration, with significant implications for optimizing industrial processes. This work sets the direction for further research aimed at developing more efficient and robust separation techniques.

Beads Binder↗

DOE OSTI2025

Deviations from the Porter-Thomas Distribution due to Nonstatistical 𝛾 Decay below the 150 Nd Neutron Separation Threshold

We introduce a new method for the study of fluctuations of partial transition widths based on nuclear resonance fluorescence experiments with quasimonochromatic linearly polarized photon beams below particle separation thresholds. It is based on the average branching of decays of 𝐽=1 states of an even-even nucleus to the 2$^{+}_{1}$ state in comparison to the ground state. Between 5 and 7 MeV, a constant average branching ratio for 𝛾 decays from 1 − states of 0.490(16) is observed for the nuclide 150 Nd. Assuming 𝜒 2 -distributed partial transition widths, this average branching ratio is related to a degree of freedom of 𝜈 = 1.93⁢(12), rejecting the validity of the Porter-Thomas distribution, requiring 𝜈 = 1. The observed deviation can be explained by nonstatistical effects in the 𝛾-decay behavior with contributions in the range of 9.4(10)% up to 94(10)%.

150 ≤ A ≤ 189↗