Syahrun Nur Abdulmadjid

Quantitative hydrogen analysis of zircaloy-4 in laser-induced breakdown spectroscopy with ambient helium gas

This experiment was carried out to address the need for overcoming the difficulties encountered in hydrogen analysis by means of plasma emission spectroscopy in atmospheric ambient gas. The result of this study on zircaloy-4 samples from a nuclear power plant demonstrates the possibility of attaining a very sharp emission line from impure hydrogen with a very low background and practical elimination of spectral contamination of hydrogen emission arising from surface water and water vapor in atmospheric ambient gas. This was achieved by employing ultrapure ambient helium gas as well as the proper defocusing of the laser irradiation and a large number of repeated precleaning laser shots at the same spot of the sample surface. Further adjustment of the gating time has led to significant reduction of spectral width and improvement of detection sensitivity to ~50 ppm. Finally, a linear calibration curve was also obtained for the zircaloy-4 samples with zero intercept. These results demonstrate the feasibility of this technique for practical in situ and quantitative analysis of hydrogen impurity in zircaloy-4 tubes used in a light water nuclear power plant.

The role of He in enhancing the intensity and lifetime of H and D emissions from laser-induced atmospheric-pressure plasma

A series of measurements have been performed on the time dependences of the intensities of helium, hydrogen, and deuterium emission lines from the corresponding laser-induced helium plasma at atmospheric pressure for two different He flow rates. The prolonged Hα and Hβ emissions along with their constant intensity ratio over a relatively extended period indicate the need to provide an alternative excitation mechanism other than the well-known thermal excitation process in a hot plasma. This additional excitation mechanism is also related to the metastable excited state of a He atom as indicated by the similar characteristics of the observed time dependence of the emission intensities. The enhanced intensity and lifetime of He emission at a high He flow rate was explained in terms of the collision-induced increase in the number of He atoms excited to above the 2 S10 metastable state, which was also responsible for the delayed excitation of H and D atoms via an energy transfer mechanism involving a Penning-...

Detection of deuterium and hydrogen using laser-induced helium gas plasma at atmospheric pressure

An experimental study on gas analysis by means of laser-induced breakdown spectroscopy was conducted using a Nd-yttrium aluminum garnet laser (1,064 nm, 120 mJ, 8 ns) and helium host gas at atmospheric pressure on a sample of mixed water (H2O) and heavy water (D2O) in vapor form. It was shown that completely resolved hydrogen (Hα) and deuterium (Dα) emission lines that are separated by only 0.179 nm could be obtained at a properly delayed detection time when the charged particles responsible for the strong Stark broadening effect in the plasma have mostly disappeared. It is argued that the helium metastable excited state plays an important role in the hydrogen excitation process.

Quenching of He-induced intensity enhancement effect in H and D emission produced by Nd-doped yttrium aluminum garnet laser irradiation on solid targets in low pressure helium gas

An experimental study was performed on the N2-induced quenching of He-induced intensity enhancement effect in reduced-pressure plasma emission produced by Nd-YAG irradiation on solid zircaloy and porous fossil samples. The spatial distributions and temporal variations in the emission intensities show pronounced intensity quenching effects on the He I 667.9 nm, H I 656.2 nm, and D I 656.1 nm emission lines in both samples when a tiny amount (5% by volume) of nitrogen was added to helium gas, while leaving the spatial and temporal intensity profiles of the heavier Zr and Ca atoms virtually unaffected. In both cases of different ambient gases, the spatial and temporal variations in the He, H, and D emission intensities exhibit distinct features and changes, which are clearly distinguishable from those observed on the Zr and Ca emission lines, which were mainly produced by the shock-wave induced thermal excitation process. The analysis of these data unambiguously revealed the presence of an additional and dis...

Intensity distributions of enhanced H emission from laser-induced low-pressure He plasma and a suggested He-assisted excitation mechanism

An experimental study was conducted on the spatial distributions of hydrogen emission intensities from low-pressure plasmas generated by laser ablation of zircaloy-4 and black stone targets in nitrogen and helium ambient gases. In addition to confirming the previously observed intensity enhancement effect in ambient helium gas, the hydrogen and helium emission intensities measured along the plasma expansion direction revealed remarkable extended spatial distributions featuring unexpected maxima near the far end of the plasma where the available shock-wave generated thermal excitation energy should have been significantly reduced. This “anomalous” feature necessarily implied the presence of an additional excitation process beside the well known shock-wave excitation process which is responsible for the plasma emission of heavy atoms in low-pressure ambient gas. Further analysis of the data led to a suggested physical mechanism explaining the possible contribution of a helium metastable excited state to the...

Spectral and Dynamic Characteristics of Helium Plasma Emission and its Effect on a Laser-Ablated Target Emission in a Double-Pulse Laser-Induced Breakdown Spectroscopy (LIBS) Experiment

A systematic study has been performed on the spectral characteristics of the full spectrum of He emission lines and their time-dependent behaviors measured from the He gas plasmas generated by a nanosecond neodymium-doped yttrium aluminum garnet laser. It is shown that among the major emission lines observed, the triplet He(I) 587.6 nm emission line stands out as the most prominent and long-lasting line, associated with de-excitation of the metastable triplet (S = 1) excited state (1s 1 3d 1 ). The role of this metastable excited state is manifested in the intensity enhancement and prolonged life time of the Cu emission with narrow full width half-maximum, as demonstrated in an orthogonal double-pulse experiment using a picosecond laser for the target ablation and a nanosecond laser for the prior generation of the ambient He gas plasma. These desirable emission features are in dire contrast to the characteristics of emission spectra observed with N2 ambient gas having no metastable excited state, which exhibit an initial Stark broadening effect and rapid intensity diminution typical to thermal shock wave-induced emission. The aforementioned He metastable excited state is therefore responsible for the demonstrated favorable features. The advantage of using He ambient gas in the double-pulse setup is further confirmed by the emission spectra measured from a variety of samples. The results of this study have thus shown the potential of extending the existing laser-induced breakdown spectroscopy application to high-sensitivity and high-resolution spectrochemical analysis of wide-ranging samples with minimal destructive effect on the sample surface.

Observation of exclusively He-induced H emission in cooled laser plasma

An experiment was performed for the observation of H emission induced in a cooled laser-induced atmospheric pressure gas plasma of He atoms in their metastable excited state. The strong H emission detected clearly established, to the exclusion of other well known major excitation processes, the exclusive contribution of the He-induced excitation (HIE) mechanism. The process is suggested to take place by means of energy transfer from the excited He atoms to the H atoms via Penning collision induced ionization involving electron exchange. The result further shows that this mechanism may also work for elements other than H and thereby strongly suggests the use of ambient He gas to broaden and complement the applications of standard laser-induced breakdown spectroscopy.

Direct evidence of mismatching effect on H emission in laser-induced atmospheric helium gas plasma

A time-resolved orthogonal double pulse laser-induced breakdown spectroscopy (LIBS) with helium surrounding gas is developed for the explicit demonstration of time mismatch between the passage of fast moving impurity hydrogen atoms and the formation of thermal shock wave plasma generated by the relatively slow moving major host atoms of much greater masses ablated from the same sample. Although this so-called “mismatching effect” has been consistently shown to be responsible for the gas pressure induced intensity diminution of hydrogen emission in a number of LIBS measurements using different ambient gases, its explicit demonstration has yet to be reported. The previously reported helium assisted excitation process has made possible the use of surrounding helium gas in our experimental set-up for showing that the ablated hydrogen atoms indeed move faster than the simultaneously ablated much heavier major host atoms as signaled by the earlier H emission in the helium plasma generated by a separate laser pr...

Deuterium analysis in zircaloy using ps laser-induced low pressure plasma

An experimental study on picosecond laser induced plasma spectroscopy of a zircaloy sample with low-pressure surrounding helium gas has been carried out to demonstrate its potential applicability to three-dimensional quantitative micro-analysis of deuterium impurities in zircaloy. This was achieved by adopting the optimal experimental condition ascertained in this study, which is specified as 7 mJ laser energy, 1.3 kPa helium pressure, and 50 μs measurement window, and which was found to result in consistent D emission enhancement. Employing these operational parameters, a linear calibration line exhibiting a zero intercept was obtained from zircaloy-4 samples doped with various concentrations of D impurity, regarded as surrogates for H impurity. An additional measurement also yielded a detection limit of about 10 μg/g for D impurity, well below the acceptable threshold of damaging H concentration in zircaloy. Each of these measurements was found to produce a crater size of only 25 μm in diameter, promisi...

Quantitative Deuterium Analysis of Titanium Samples in Ultraviolet Laser-Induced Low-Pressure Helium Plasma

An experimental study of ultraviolet (UV) laser-induced plasma spectroscopy (LIPS) on Ti samples with low-pressure surrounding He gas has been carried out to demonstrate its applicability to quantitative micro-analysis of deuterium impurities in titanium without the spectral interference from the ubiquitous surface water. This was achieved by adopting the optimal experimental condition ascertained in this study, which is specified by 5 mJ laser energy, 10 Torr helium pressure, and 1–50 μs measurement window, which resulted in consistent D emission enhancement and effective elimination of spectral interference from surface water. As a result, a linear calibration line exhibiting a zero intercept was obtained from Ti samples doped with various D impurity concentrations. An additional measurement also yielded a detection limit of about 40 ppm for D impurity, well below the acceptable threshold of damaging H concentration in Ti and its alloys. Each of these measurements was found to produce a crater size of only 25 μm in diameter, and they may therefore qualify as nondestructive measurements. The result of this study has therefore paved the way for conducting further experiments with hydrogen-doped Ti samples and the technical implementation of quantitative micro-analysis of detrimental hydrogen impurity in Ti metal and its alloys, which is the ultimate goal of this study.