実験報告書様式（一般利用課題・成果公開利用）

MLF Experimental Report

提出日 Date of Report
2010/7/23

課題番号 Project No.

装置責任者 Name of responsible person

2009B0011

Hideki Seto

実験課題名 Title of experiment

装置名 Name of Instrument/（BL No.）

Measurement of deuterium and hydrogen content o f DLC film by

ARISA-II / BL 16

neutron reflectivity.

実施日 Date of Experiment

実験責任者名 Name of principal investigator

2010/5/28-2010/5/31

Kazuhide Ozeki
所属 Affiliation
Ibaraki University
試料、実験方法、利用の結果得られた主なデータ、考察、結論等を、記述して下さい。（適宜、図表添付のこと）
Please report your samples, experimental method and results, discussion and conclusions. Please add figures andtables for better explanation.
1. 試料 Name of sample(s) and chemical formula, or compositions including physical form.
Following DLC samples were measured by BL16. (Chemical formula: resource gas ratio). Two samples at a
coating condition.
・Carbon hydrogen DLC film DLC (CxHy): (x=5, y=5: 50CH4, 50H2), (x=2, y=8: 20CH4, 80H2), (x=7, y=3:70CH4, 30H2), (x=10, y=10: 100CH4)
・Carbon deuterated DLC film (CxDy): (x=2, y=8: 20CD4, 80D2), (x=5, y=5: 50CD4, 50D2), (x=7, y=3: 70CD4,30D2), (x=10, y=10: 100CD4)
・Carbon hydrogen deuterated DLC film (CxHyDz): (x=2, y=2, z=8: 20CH4, 80D2), (x=5, y=5, z=5: 50CH4,50D2), (x=7, y=7, z=3: 70CH4, 30D2), (x=2, y=8, z=2: 20CD4, 80D2), (x=5, y=5, z=5: 50CD4, 50H2), (x=7, y=3,z=7: 70CD4, 30H2)

2. 実験方法及び結果 （実験がうまくいかなかった場合、その理由を記述してください。）
Experimental method and results.

If you failed to conduct experiment as planned, please describe reasons.

1. Experimental method
1.1 Sample preparation
DLC deposition on the Si substrate (30mm x 30mm) was performed using a PED-301 RF CVD system. In
this experiment, we focused on the contribution of H2 gas source to the H content in the DLC film inCH4+H2 gas flow system, which helps us for understanding the complex coating mechanism of DLC film.
We have chosen D2 gas instead of H2 gas or CD4 gas instead of CH4 gas for the DLC coating.
CH4, H2, CD4 and D2 gases were introduced into the chamber. The coating carried out at 13.3 Pa and adischarge power of 250W. Four types of flow gas combination were selected as CH4+H2, CD4+H2, CH4+D2
and CD4+D2. At each flow condition, the partial flow rate of H2 or D2 was varied from 20% to 80%. The
film thickness of all samples was around 200nm.

1

2. 実験方法及び結果（つづき） Experimental method and results (continued)
1.2 Measurement
The neutron reflectivity was performed using a BL16 reflectometer, and neutron reflectivities were takenfrom 0.007 to 0.18 in qz (Å-1). In addition to the reflectivity measurement, Rutherford backscattering
spectroscopy (RBS) and elastic recoil detection
1.0E+00

analysis (ERDA) were performed for analysis ofmeasured
1.0E-01

average H or D content of the DLC film.

1.0E-02

Reflectivity

Results
Figures 1 and 2 show an example of neutronreflectivity and the SLD of the DLC film (50CD4,

1.0E-03
1.0E-04

50H2) from fitting simulation, respectively. From

1.0E-05

fig.2, the SLD at the film surface reached 7.0E-6 /1.0E-06
02

0.05

0.1

Å . The layer thickness is around 50 Å, which can

0.15

0.2Qz/Å-1

Fig.1 Neutron reflectivity for DLC (50CD4,50H2)

be considered to be an oxide layer. The SLD2film.

gradually decreased from 6.8 E-6 / Å to 4.6 E-62/A at the range of 760 Å - 1390 Å. This indicatesthe decrease of the mass density or the increase of

8hydrogen. In addition, third layer (SLD = 3.0767.0E-6 / Å2) was also observed at the interface of
SLD /10-6Å-22.

fittedthe DLC/Si substrate. The layer thickness wasaround 20 Å, which can be an intermediate layer of

5432Si, or SiO. The layer has not observed yet in the1neutron reflectivity measurement. BL16 can00500

1000

1500

provide the reflectivity at high Q range, and thisDistance from film surface /Åhigh Q range measurement contributes to find thisFig.2 Scattering length density for the DLC

thin layer. The intermediate layer was observed in all(50CD4,50H2) film.

measured samples.

Table 1 SLD and H/ D content of the DLC film.

Table 1 shows SLD and D/H content of the DLC
ERDA

Averagefilms coated under various conditions. The averageNo.

SamplesSLD(10-6 /A2)

H (%)

120CD4 ,80H2

4.5

22172

50CD4 ,50H2

6.4

1135

370CD4 ,30H2

6.9

438

420CD4,80 D 2

6.1432550 CD 4,50 D2

7.1239670CD4,30 D 2

7.0

1125

7100CD4

7.4

2378

20CH4,80H2

3.3

380

950CH4,50H2

3.5

340

H and D contents widely changed from 6% to1070CH4,30H2

3.9

320

115.5

112126%. This might indicate that H from CH4 gas and

20CH4,80D2

1250CH4,50D2

6.5

15241370CH4,30D2

4.2

26614100CH44.1

310

SLD increased with increase of D/H ratio of thefilm. Even if the H2/(H2+CH4) ratio was changed
from 0 to 0.8 in the sample No.8-10 and 14, themeasured hydrogen content varied only from 31%
to 38%, which may impose the small contributionof H from H2 gas source. In the sample No.11-13,

H from H2 gas evenly contribute to H content inthe DLC film.
2D (%)