Direct evidence of He-induced excitation process of H atoms in - - PowerPoint PPT Presentation

Direct evidence of He-induced excitation process of H atoms in cooled laser plasma

Koo Hendrik Kurniawan, Rinda Hedwig, Zener Sukra Lie, Kiichiro Kagawa

• Research Centre of Maju Makmur Mandiri Foundation,

Jakarta, Indonesia 11630 (http://www.mmmfoundation.org)

• Computer Engineering Laboratory, Bina Nusantara University,

Jakarta, Indonesia 11480 (http://binus.ac.id)

• Research Institute of Nuclear Engineering, University of Fukui,

Fukui, Japan 910-8507 (http://www.u-fukui.ac.jp/eng)

Laser I nduce Plasma Spectroscopy

targ arget et OMA LASER fibe iber

Time Controller

(Cremers & Radziemski’s Group, 1981)

Kagawa & Kurniawan’s Group 1 atm plasma Low pressure plasma He gas plasma Advantage

• Metal and non metal
• Without pre-treatment
• In-situ analysis
• Micro-area analysis

Mechanism

Practical Application of LI BS for Hydrogen Analysis I n Nuclear Power Station

Problem: Hydrogen accumulation in the pipe wall degrades the pipe’s strength Anticipation: Periodical Inspection Now in use Inspection Method: Gas Chromatography (sample and time consuming, hand touched radioactive and not in situ analysis) New Method: Laser Induced Plasma Spectroscopy (LIPS)

Water Zircaloy pipe Uranium Fuel

Zircaloy pipe is an important material used in a light water nuclear power station to contain uranium fuel

Hydrogen Analysis Using Laser Plasma Method has not been Carried Out Before



Stark broadening effect happens when plasma is produced at 1 atm

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Emission efficiency is very low for H atom at 1 atm due to the “mismatching effect”

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Disturbance of H2O

Why

H-656.3 Stone sample

• -- High pressure (1 atm)
• -- Low pressure (10 torr)

H is light mass “Mismatching effect”

No Mismatching Effect for Other Elements

• Red line – High Pressure (1 atm)
• Blue line – Low Pressure (10 torr)

Si line O line Stone sample Stone sample

Concept of Mismatching Effect

Ideal Shockwave Plasma Formation

Hydrogen Atom Case early later

Hydrogen atoms gush out faster Shock-wave generation

MH=1 MSi=28

Time difference between gushing

• ut of H atoms and

shock-wave generation

Mismatching Effect

Mismatching Effect will significant at higher pressure, or at low power density, because shockwave generation is somewhat delayed

Gas Plasma I nduced by Focusing Nd-YAG laser in the Gas

N2 Gas Plasma He Gas Plasma Nd-YAG 120mJ Lens f 100mm (in faint ethanol vapor) To OMA

Time Profile of Laser I nduced Gas Plasma Emission

5 10 15 20 25 30 5 10 15 time (μsecond) FWHM (A) helium nitrogen limit of the system

He as host gas: Long Life Emission Very narrow spectral width at later stage N2 as host gas: Short Life Emission Rather broad spectral width Later stage is cooled plasma

Spectral width of H-656.3nm

He 587.56nm

Double Excitation Scheme for H analysis under He 1 Atm

20 40 60 80 100 120 140 160 180 200 610 620 630 640 650 660 670 680 690 wavelength, nm intensity, counts Ca I 671.7 nm

H I 656.2 nm 20 40 60 80 100 120 140 160 610 620 630 640 650 660 670 680 690 wavelength, nm intensity, counts H I 656.2 nm Ca I 671.7 nm He I 667.8 nm

Hydrogen Emission can be detected with high efficiency and very narrow spectral width

Ordinary LIBS Double excitation Sample: Slide glass

Experiment Setup for Proving Excitation in Cooled Plasma

Stone Sample For gas Plasma: Nd-YAG (1064nm), 163mJ For ablate sample: Nd-YAG (532nm), 74mJ Delay Time between two laser: 10us In this experiment, He gas plasma was made at 5mm in front the sample. After the gas plasma formation, second laser was irradiated for ablation with 10us delay time. Atoms come out from the sample and excited in the cooled He gas plasma.

Time Profile of Emission of the Gas Plasma

Due to the thermal excitation Due to the He meta-stable excitation He-667 emission In helium gas Nitrogen emission In Nitrogen gas Life time is long Life time is short

He＊

He emission proceeds in

cooled plasma

 He meta - He meta collision  Thermal excitation from He

meta

* * ( ) ** He He He He e He e He He hv

+ − + −

+ → + + + → → +

*

** He thermal He He hv + → → +

Two possible mechanism

The evidence to prove He emission is not due to thermal excitation

0.5 1 1.5 2 2.5 3 500 1000 1500 2000 2500 3000 5 10 15 20 25 30 35 40 45 Intensity (a.u)

Time (uS)

3He*-471 3.8eV Ratio 1He*-501 2.5eV

2.5eV 3.8eV

not thermal excitation

Time correlation between He-501nm and He-471nm

The Excitation Mechanism through Helium Meta-stable

* ( ) ** He X He X e X e X X hv

+ − + −

+ → + + + → → +

Penning effect recombination

Electron recombines with X+ ion X atom collides with He metastable X atom is ionized and Releases free electron Spectral emission of X atom He*

Time Profile of H, O, Ca emission in the cooled He gas plasma

5000 10000 15000 20000 25000 30000 35000 500 1000 1500 2000 2500 3000 3500 4000 intensity, arb units OMA delay, ns

H I 656.2 nm O I 777.1 nm Ca I 422.6 nm

10000 20000 30000 40000 50000 60000 500 1000 1500 2000 2500 3000 3500 4000 4500 5000 intensity, counts time delay

H I 656.2 nm He I 667.8 nm Ca I 422.6 nm (x10) O I 777.4 nm

High energy Low energy Due to Helium meta-stable excitation Another mechanism (shock wave excitation) works for high energy pulse case

H atoms come out faster than

• ther atoms, which proves the

“mismatching effect”

Direction of Gushing Atoms

1000 2000 3000 4000 5000 6000 7000 8000 9000 10000

• 6
• 4
• 2

2 4 6 intensity, counts z position, mm

Ca-422.6nm Distribution of H atoms is more straight forwards compared to other atoms H-656nm

X Position, mm

I ntensity Calibration Curve of the Deuterium I mpurity in Zircaloy-4 Samples

Conclusion

 He emission takes place through the collision of two

Helium meta-stable atoms (He* ).

 In a cooled He plasma, Helium meta-stable atoms

(He* ) excites atoms including Hydrogen

 Hydrogen atoms gushed out faster than other atoms,

which proved our hypothesis, namely “mismatching effect”

* * ( ) ** * He He He He e He He hv

+ −

+ → + + → → +

**

* ( ) He X He X e He X hv

+ −

+ → + + → → +

Published work

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Z.S. Lie, H. Niki, K. Kagawa, M.O. Tjia, R. Hedwig, M. Pardede, E. Jobiliong, M.M. Suliyanti, S.N. Abdulmadjid, K.H. Kurniawan, Observation of Exclusively He-Induced H Emission in Cooled Laser Plasma, J. Appl. Phys., 109, 10 (2011) pp. 103305 1-4

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• R. Hedwig, Z.S. Lie, K.H. Kurniawan, A.N. Chumakov, K. Kagawa, M.O. Tjia, Toward

Quantitative Deuterium Analysis with Laser-Induced Breakdown Spectroscopy Using Atmospheric-Pressure Helium Gas, J. Appl. Phys. 107, 2 (2010) pp. 023301 1-5

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Z.S. Lie, M. Pardede, R. Hedwig, M.M. Suliyanti, E. Steven, Maliki, Koo H. Kurniawan,

• M. Ramli, S.N. Abdulmadjid, N. Idris, K. Lahna, K. Kagawa and M.O. Tjia, Intensity

Distributions of Enhanced H Emission from Laser-Induced Low-Pressure He Plasma and a Suggested He-Assisted Excitation Mechanism, J. Appl. Phys., 106, 3 (2009)

• pp. 043303 1-6

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Koo H. Kurniawan, T.J. Lie, M.M. Suliyanti, R. Hedwig, M. Pardede, M. Ramli, H. Niki, S.N. Abdulmadjid, N. Idris, K. Lahna, Y. Kusumoto, K. Kagawa, M.O. Tjia, The Role

• f He in Enhancing the Intensity and Lifetime of H and D Emissions from Laser-

Induced Atmospheric-Pressure Plasma, J. Appl. Phys. 105 (2009) pp. 103303-1-6

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K.H. Kurniawan, M. Pardede, R. Hedwig, Z.S. Lie, T.J. Lie, D.P. Kurniawan, M. Ramli,

• K. Fukumoto, H. Niki, S.N. Abdulmadjid, N. Idris, T. Maruyama, K. Kagawa, M.O.

Tjia, Quantitative Hydrogen Analysis of Zircaloy-4 Using Low-Pressure Laser Plasma Technique, Anal. Chem. 79,7 (2007) pp. 2703-2707

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• M. Pardede, R. Hedwig, M.M. Suliyanti, Z.S. Lie, T.J. Lie, D.P. Kurniawan, K.H.

Kurniawan, M. Ramli, K. Fukumoto, H. Niki, S.N. Abdulmadjid, N. Idris, T. Maruyama,

• K. Kagawa, M.O. Tjia, Comparative Study of Laser-Induced Plasma Emission of

Hydrogen from Zircaloy-2 Samples in Atmospheric and Low Pressure Ambient Helium Gas, Appl. Phys. B. 89, 2-3 (2007) pp. 291 - 298.