Single-QCL-based absorption sensor for simultaneous trace-gas detection of CH4 and N2O

A quantum cascade laser (QCL)-based absorption sensor for the simultaneous dual-species monitoring of CH₄ and N₂O was developed using a novel compact multipass gas cell (MGC). This sensor uses a thermoelectrically cooled, continuous wave, distributed feedback QCL operating at ~7.8 µm. The QCL wavelength was scanned over two neighboring CH₄ (1275.04 cm^?1) and N₂O (1274.61 cm^?1) lines at a 1 Hz repetition rate. Wavelength modulation spectroscopy (f = 10 kHz) with second harmonic (2f) detection was performed to enhance the signal-to-noise ratio. An ultra-compact MGC (16.9 cm long and a 225 ml sampling volume) was utilized to achieve an effective optical path length of 57.6 m. With such a sensor configuration, a detection limit of 5.9 ppb for CH₄ and 2.6 ppb for N₂O was achieved, respectively, at 1-s averaging time.     

Improvement of two-photon laser induced fluorescence measurements of H- and O-atoms in premixed methane/air flames

3 photodissociation is shown to be an important photolytic source of H atoms in the reaction zone of the methane flames. At 226 nm, an efficient energy transfer between O(³P) and N₂ is established from the observation of O-resonant emissions from the second positive system of N₂. The subsequent rate of O(³P) depletion appears to be essentially “controlled” by the O(³P) concentration and is probably only minimally temperature dependent. Finally quenching rate coefficients for O(³P) by water and nitrogen are deduced from quenching rates measurements performed in CH₄/O₂/N₂ and CH₄/O₂/Ar flames. Received: 7 November 1996/Revised version: 28 January 1997     

Isovector deformation and its link to the neutron shell closure

DWBA analysis of the inelastic ^30-40S(p,p') and ^18-22O(p,p') scattering data measured in the inverse kinematics has been performed to determine the isoscalar (δ₀) and isovector (δ₁) deformation lengths of the 2⁺₁ excitations in the Sulfur and Oxygen isotopes using a compact folding approach. A systematic N-dependence of δ₀ and δ₁ has been established which shows a link between δ₁ and the neutron-shell closure. Strong isovector deformations were found in several cases, e.g., the 2⁺₁ state in ²⁰O where δ₁ is nearly three times larger than δ₀. These results confirm the relation δ₁>δ₀ anticipated from the core polarization by the valence neutrons in the open-shell (neutron rich) nuclei. The effect of neutron shell closure at N=14 or 16 has been discussed based on the folding model analysis of the inelastic ²²O+p scattering data at 46.6 MeV/u measured recently at GANIL.     

Optimization of a compact photoacoustic quantum cascade laser spectrometer for atmospheric flux measurements: application to the detection of methane and nitrous oxide

Room temperature (RT) quantum cascade lasers (QCL) are now available even in continuous wave (cw) mode, which is very promising for in situ gas detectors. Ambient air monitoring requires high sensitivity with robust and simple apparatus. For that purpose, a compact photoacoustic setup was combined with two cw QCLs to measure ambient methane and nitrous oxide in the 8 μm range. The first laser had already been used to calibrate the sensitivity of the photoacoustic cell and a detection limit of 3 ppb of CH₄ with a 1s integration time per point was demonstrated. In situ monitoring with this laser was difficult because of liquid nitrogen cooling. The second laser is a new RT cw QCL with lower power, which enabled one to reach a detection limit of 34 ppb of methane in flow. The loss in sensitivity is mainly due to the weaker power as photoacoustic signal is proportional to light power. The calibration for methane detection leads to an estimated detection limit of 14 ppb for N₂O flux measurements. Various ways of modulation have been tested. The possibility to monitor ambient air CH₄ and N₂O at ground level with this PA spectrometer was demonstrated in flux with these QCLs. PACS 07.88; 92.60.Sz     

A quantum cascade laser-based optical feedback cavity-enhanced absorption spectrometer for the simultaneous measurement of CH4 and N2O in air

Optical feedback cavity-enhanced absorption spectroscopy (OF CEAS) has been demonstrated with a thermoelectrically cooled continuous wave distributed feedback quantum cascade laser (QCL) operating at wavelengths around 7.84 μm. The QCL is coupled to an optical cavity which creates an absorption pathlength greater than 1000 m. The experimental design allows optical feedback of infra-red light, resonant within the cavity, to the QCL, which initiates self-locking at each TEM₀₀ cavity mode frequency excited. The QCL linewidth is narrowed to below the mode linewidth, greatly increasing the efficiency of injection of light into the cavity. At the frequency of each longitudinal cavity mode, the absorption coefficient of an intracavity sample is obtained from the transmission at the mode maximum, measured with a thermoelectrically cooled detector: spectral line profiles of CH₄ and N₂O in ambient air were recorded simultaneously and with a resolution of 0.01386 cm^?1. A minimum detectable absorption coefficient of 5.5×10^?8 cm^?1 was demonstrated after an averaging time of 1 s for this completely thermoelectrically cooled system. The bandwidth-normalised limit for a single cavity mode is 5.6×10^?9 cm^?1?Hz^?1/2 (1σ).     

Inelastic scattering on 12Be and disappearance of the N = 8 magic number

Experimental studies on in-beam γ-ray spectroscopy using a ¹²Be radioactive beam are presented. Inelastic scattering of the neutron-rich ¹²Be nucleus on ²⁰⁸Pb, ¹²C, and (CH₂)_n targets has been studied by measuring de-excitation γ-rays in coincidence with scattered particles. The level schemes and transition probabilities are determined for low-lying excited states in ¹²Be. The present paper presents a brief review of the spectroscopic results, which may be associated with the N = 8 shell quenching near the drip line. Received: 1 May 2001 / Accepted: 4 December 2001     

The “island of inversion" from a nuclear moments perspective and the g factor of 35Si

This paper reviews recent results from electromagnetic moment measurements on isotopes in the island of inversion around N=20. The obtained moments on neutron rich Na, Mg, Al and Si isotopes allow to draw conclusions on the amount of intruder components in their ground state wave function, demonstrating a gradual transition from the normal sd-shell region into the island of inversion, starting at N=18 for Na, N=19 for Mg and N=20 for Al isotopes. A measurement of the ground state g factor of ³⁵Si (N=21), using a polarized fragment beam at GANIL, is discussed in more detail. The magnetic moment μ(³⁵Si, I^π= 7/2^-) = (-)1.638(4) μ_N is consistent with a normal ground state structure, dominated by a νf_7/2 neutron.     

Systematics of related high-spin isomers in 144Sm and other N = 82 nuclei

An in-beam experiment with the reaction ¹²²Sn(²⁷Al,4np) at 127 MeV was performed at the Nordball multi-detector array in Roskilde. It provided evidence for a new high-spin isomer in ¹⁴⁴Sm. This isomer with T _1/2= (2.6 ± 0.5) ns at an excitation energy E _x= 9232 keV seems to belong to a family of isomers of similar configuration in neighbouring N= 82 nuclei. Received: 16 November 1997     

Investigations into the alpha-decay of <Superscript>195</Superscript>At

The low-energy nuclear structure and decay properties of the neutron-deficient isotopes ¹⁹⁵At and ¹⁹¹Bi have been studied. ¹⁹⁵At was produced in the reaction ¹⁴²Nd(⁵⁶Fe,p2n)¹⁹⁵At and ¹⁹¹Bi as the daughter activity of ¹⁹⁵At. The activities were implanted in a position-sensitive silicon detector after being separated from the primary beam by a gas-filled recoil separator. The 1/2⁺ intruder state was determined to be the ground state in ¹⁹⁵At with an alpha-decay energy of E _α = 6953(3) keV and a half-life T _1/2 = 328(20) ms. Another state with an alpha-decay energy E _α = 7075(4) keV and a half-life T _1/2 = 147(5) ms was found to decay to a 148.7(5) keV excited state in ¹⁹¹Bi for which a spin and parity of 7/2^- were deduced. Consequently, the same 7/2^- character was assigned to the initial state at 32(7) keV in ¹⁹⁵At on the basis of unhindered alpha-decay. The 9/2^- state, being the ground state in heavier odd-mass astatine isotopes, was not observed. Received: 16 September 2002 / Accepted: 19 December 2002 / Published online: 25 March 2003 RID="a" ID="a"e-mail: heikki.kettunen@phys.jyu.fi RID="b" ID="b"Present address: Laboratory of Radiochemistry, P.O. Box 55, FIN-00014, University of Helsinki, Finland. RID="c" ID="c"Present address: Radiation and Nuclear Safety Authority, P.O. Box 14, FIN-00881 Helsinki, Finland. Communicated by W. Henning     

16O-8Be break-up states and cluster structure of 24Mg

High-spin states of ²⁴Mg produced in the ¹⁶O + ¹²C interaction and decaying into the ¹⁶O_g.s. + ⁸Be_g.s. channel have been observed in the excitation region between 35 and 52 MeV. Spins have been assigned on the basis of the analysis of the measured angular correlations. Some of these states with positive parity correspond to the known resonances of the ¹²C( ¹²C, ⁸Be_g.s.) ¹⁶O reaction belonging to the ¹⁶O-2α rotational band of ²⁴Mg. Moreover other resonances show up at higher excitation energy with an energy-spin relationship again suggesting a ¹⁶O-2α cluster structure for the associated configuration. Received: 6 July 2001 / Accepted: 16 October 2001     

PreCon: A Fully Automated Interface for the Pre-Gc Concentration of Trace Gases on Air for Isotopic Analysis

Abstract

For the high precision isotope analysis of atmospheric trace gases a computer controlled concentration interface has been developed. From small air samples it collects either N₂O or CO₂ derived from CH₄ at their respective concentrations (0.3 ppm for N₂O, 1.7 ppm for CH₄) into a small diameter cold trap (?196°C) and interfaces via GC and open split to an isotope ratio mass spectrometer (Finnigan MAT 252) for on-line isotope evaluation. External reproducibilities for repeated measurements of 100 ml air samples from the same source of < 0.2° (δ-notation) have been achieved for ¹³C/¹²C from CH₄ and for ¹⁵N/¹⁴N and ¹⁸O/¹⁶O from N₂O. The precision is adequate to monitor the isotopic changes in these gases during a day's course.     

Spectroscopy of 13B, 14B, 15B and 16B using multi-nucleon transfer reactions

New information has been obtained on excited states of the neutron-rich boron isotopes ¹⁴B, ¹⁵B and ¹⁶B, using the reactions ¹²C(¹⁴C,¹²N)¹⁴B, ¹³C(¹⁴C,¹²N)¹⁵B and ¹⁴C(¹⁴C,¹²N)¹⁶B at about 24 MeV/A. The mass excess of ¹⁶B has been measured for the first time, it is 37.08(6) MeV. This means that ¹⁶B is unbound by only 0.04(6) MeV. Furthermore, the nucleus ¹³B has been investigated with the four reactions ¹⁶O(¹⁴C,¹⁷F), ¹²C(¹⁴C,¹³N), ¹²C(¹³C,¹²N) and ¹²C(¹⁵N,¹⁴O). Choosing different target-projectile combinations, it was possible to populate states with different selectivity. New states are observed in ¹³B at excitation energies above the threshold for two-neutron decay. Received: 27 December 1999 / Revised version: 11 February 2000     

Synergistic effects in mixed wormlike micelles of dimeric and single-chain cationic surfactants at high ionic strength

The mixed micellization between the cationic gemini surfactant [ C₁₂H₂₅( CH₃)₂N⁺( C₂H₄) N⁺( CH₃)₂ C₁₂H₂₅•2Br^-] and the cationic cetyltrimethylammonium bromide (CTAB) in 150 mM KBr solutions has been investigated. The variation of the cmc of the mixtures, measured by surface tension experiments, with composition revealed synergism in micelle formation. T-Jump and light scattering experiments performed in the vicinity of the crossover volume fraction showed the existence of two micellar populations, possibly linear and toroidal micelles. Rheological and dynamic light scattering experiments allowed to fully characterize the linear viscoelasticity of the mixtures. These measurements revealed synergistic gains in viscoelastic properties with a maximum of the stress-relaxation time around the equimolar composition. These effects are ascribed to a progressive intermicellar crosslinking resulting from a continuous increase of the end-cap energy with the 12-2-12 content in the mixture. Received: 18 November 2002 / Accepted: 8 April 2003 / Published online: 27 May 2003 RID="a" ID="a"e-mail: candau@fresnel.u-strasbg.fr     

Evolution of the N = 20 and N = 28 shell closures in neutron-rich nuclei

The isospin dependence of shell closure phenomena is studied for light neutron-rich nuclei within a microscopic self-consistent approach using the Gogny force. Introducing configuration mixing, ³²Mg is found to be dynamically deformed, although the N = 20 spherical shell closure persists at the mean-field level for all N = 20 isotones. In contrast, the N = 28 spherical shell closure is found to disappear for N - Z≥ 10 whereas deformed shell closures are preserved and lead to shape coexistence in ⁴⁴ S. Configuration mixing shows that the ground state of this nucleus is triaxially deformed. The first 2⁺ excitation energy E_x = 1.46 MeV and the reduced transition probability B(E2;0⁺ _gs→ 2⁺ ₁)= 420 e ² fm ⁴ obtained with our approach are in good agreement with experimental data. Received: 26 July 2000 / Accepted: 30 August 2000     

New states in heavy Cd isotopes and evidence for weakening of the N = 82 shell structure

A chemically selective laser ion source has been used in a β-decay study of heavy Ag isotopes into even-even Cd nuclides. Gamma-spectroscopic techniques in time-resolving event-by-event and multiscaling modes have permitted the identification of the first 2⁺ and 4⁺ levels in ¹²⁶Cd₇₈, ¹²⁸Cd₈₀, and tentatively the 2⁺ state in ¹³⁰Cd₈₂. From a comparison of these new states in ₄₈Cd with the E(2⁺) and E(4⁺)/E(2⁺) level systematics of ₄₆Pd and ₅₂Te isotopes and several recent model predictions, possible evidence for a weakening of the spherical N = 82 neutron-shell below double-magic ¹³²Sn is obtained. Received: 13 July 2000 / Accepted: 12 October 2000     

Laser-induced fluorescence study of the influence of N <Emphasis Type="Bold">2</Emphasis> and CH <Emphasis Type="Bold">4</Emphasis> on the <Emphasis Type="Bold">114</Emphasis>Cd intercombination line

Using a laser-induced fluorescence method a detailed analysis of profiles of the ¹¹⁴Cd 326.1 nm line perturbed by N₂ and CH₄ was performed which revealed deviations from the ordinary Voigt profile. These deviations are shown to be consistent with fits of experimental profiles to an asymmetric Voigt profile. Coefficients of the pressure broadening, shift and collision-time asymmetry are determined and compared with those calculated for van der Waals interaction potential. Received 29 November 2001 / Received in final form 12 July 2002 Published online 4 February 2003     

High quality CVD diamond: a Raman scattering and photoluminescence study

High quality synthetic diamonds were grown on single-crystal silicon by microwave plasma enhanced chemical vapour deposition (CVD). A careful optimisation of both the experimental setup and the growth parameters was necessary before that the achievement of the best results was made possible. The films were deposited using a CH₄-H₂ gas mixture at methane concentrations variable in the range 0.6-2.2%, while the substrate temperature was fixed at 750 ^°C. Raman spectroscopy and photoluminescence (PL) were utilised to monitor the quality of the deposited films and to study the spatial distribution of defects, respectively. Micro-Raman analysis shows that linewidths of the diamond peak lower than 2.4 cm^-1 can be easily measured at the growth surface, indicating that the crystalline quality of individual grains is comparable to that of the best natural diamonds. The excellent phase purity of the diamond microcrystals at the growth surface is witnessed by the complete absence of any non-diamond carbon feature and by a very weak luminescence background in the 1.6-2.4 eV spectral range. A worsening of the quality of the diamond particles is found moving from the growth surface towards the film-substrate interface. A photoluminescence feature at about 1.68 eV, commonly associated to Si impurities, is distinctly observed as the exciting laser beam is focused close to the interface. A progressive degradation of the global quality of the films is found with increasing methane concentration in the gas mixture, as witnessed by an increased PL background in the films grown at higher methane concentrations. Received 24 November 2000     

Decay modes of 24Mg excited at 46.4 MeV

⁸Be_gs coincidences with ¹²C, ⁸Be_gs and α-particles produced in the ¹²C +¹²C interaction at 65 MeV have been measured in a wide in-plane angular range. The 3 −⁸Be_gs final state is found to be produced, even if poor statistics prevent any identification of the ¹⁶O states involved in the first stage of the process. The ⁸Be_gs−α and ⁸Be_gs−¹²C coincidence yields are found to be due to ¹²C and ¹⁶O excited states, decaying into the ⁸Be_gs+α and ¹²C +α systems, respectively. Received: 15 June 1998 / Revised version: 4 December 1998     

Coulomb excitation of 72 30Zn42

The reduced transition probability B(E2: 0₁ ⁺→ 2⁺) of ⁷²Zn has been measured for the first time by Coulomb excitation at intermediate energy. The result B(E2: 0₁ ⁺→ 2⁺) = 1740±210 e²fm⁴, corresponds to the deformation parameter β₂ of 0.23, in close agreement with expectations derived from the neighboring nucleus ⁷³Zn. A discussion of the evolution of the N = 40 sub-shell closure as a function of Z is presented. Received: 19 December 2001 / Accepted: 14 March 2002     

Hyperfine splitting and isotope shift in the atomic D2 line of 22,23Na and the quadrupole moment of 22Na

The hyperfine structure of the D₂ optical line in ²²Na and ²³Na has been investigated using high resolution laser spectroscopy of a well-collimated atomic beam. The hyperfine splitting constants A and B for the excited 3p ²P_3/2 level for both investigated sodium isotopes have been obtained. They are as follows: A(22) = 7.31(4) MHz, B(22) = 4.71(28) MHz, A(23) = 18.572(24) MHz, B(23) = 2.723(55) MHz. With this data, using the high precision MCHF calculations for the electric field gradient at the nucleus, the electric quadrupole moment of ²²Na has been deduced: Q_s(22) =+0.185(11) b. The sign of Q_s(22), determined for the first time, indicates a prolate nuclear deformation. A precise value of the isotope shift ^22,23Na in the D₂ line has also been obtained. Received: 26 February 1998 / Revised version: 25 June 1998