実験報告書様式（一般利用課題・成果公開利用）（ ※本報告書は英語で記述してください。ただし、産業利用課題として採択されている方は日本語で記述していただいても結構です。 ）Experimental Report

承認日 Date of Approval 2017/03/28
承認者 Approver Kaoru SHIBATA
提出日 Date of Report 2017/03/28

課題番号 Project No.

装置責任者 Name of Instrument scientist

2015A0078

Kaoru Shibata

実験課題名 Title of experiment

装置名 Name of Instrument/（BL No.）

Systematic studies on hierarchic structure and dynamics in model

DNA /(BL-02)

rubber materials: global cooperative dynamics in rubbers

実施日 Date of Experiment

実験責任者名 Name of principal investigator

2016/3/14 ～ 2016/3/19

Toshiji Kanaya
所属 Affiliation
High Energy Accelerator Research Organization (KEK)
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.
Polybutadiene rubbers (-(C4H6)n-) including silica filler (SiO2) (volume fraction of 0, 0.05, 0.2) were used forsample and the thicknesses of prepared samples were at around 0.2mm.

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.

Neutron scattering studies are now looking towards realistic materials (or industrial materials) in addition to
traditional scientific researches on simple model materials. In soft matter, intensive studies are now performed on
industrial rubber materials such as mobile tire and rubber base-isolated structure. However, generally speaking,the realistic rubber materials have complicated structure and dynamics in wide spatial and time scales, which aredominated by many factors such as fillers, aggregations of fillers, crosslinks between polymers, coupling agents
between filler and polymer. Hence, it is not easy to interpret the complicated results or extract useful information
for industries from the results.
To understand the data on the realistic (industrial) complicated rubber materials and to fill up the gap ofstudies between the realistic (industrial) and ideal materials we propose systematic studies on some model rubbermaterials by means of various kinds of quantum beams. In this experiment, we focus on polybutadiene (PB)
including silica powder fillers with no crosslinks using BL02 at J-PARC to see the local heterogeneousdynamics.
Dynamic scattering laws S(Q, ) in the range Q = 1.8 Å−1 at 300 K are shown in Fig.1. The narrowing of S(Q,) with the increase in silica volume fraction can be observed with an energy resolution of 4.0 eV, suggestingthat the motion of PB is slowed down by an addition of silica. To understand this result in detail, we adopted theKohlrausch-Williams-Watts (KWW) function to describe the observed S(Q, ), and the following model2. 実験方法及び結果（つづき） Experimental method and results (continued)
function was proposed.

 S Q ,    A 1  EISF F exp  t  100

 EISF    R Q ,   (1)PB
PB/Silica(=0.05)
PB/Silica(=0.2)

65

where A, EISF,  and  are the amplitude of the relaxation

4function, the elastic incoherent structure factor, the relaxation
S(Q, ) [a.u.]

3time, and the distribution of the relaxation function,respectively. It should be noted that the KWW function isutilized in the time domain, necessitating that we adopt the210

Fourier-transformed KWW function (F(KWW)) in the

65frequency region. R(Q, ) indicates the instrumental resolution

43function. Fig. 1 shows the results of the fits to S(Q, ) with Eq.

2(1) at Q = 1.8 Å−1 and 300 K. The S(Q, ) from both samples

-0.02

0.00

0.02

0.04

0.06

Energy transfer [meV]

are fitted fairly well by Eq. (1), confirming the appropriate
model function selection.

Fig. 1 Dynamic scattering laws S(Q, )

The dependence values of the average relaxation time <>normalized at the peak top at 300 K in the range

and the relaxation time distribution  at 300 K in the range Q

Q = 1.8 Å−1. Solid lines are the results of fittings= 1.8 Å−1 on the volume fraction of silica are shown in Fig. 2.

with Eq. (1). The dashed line is the instrumental<> was calculated using Eq. (2)[1]: where  is a gamma

resolution function.
70function.

(2)

silica volume fraction were evaluated, suggesting that themotion of mobile component is slowed down and dynamical

0.43500.4240heterogeneity is increased with increases in the silica volume
fraction. The detailed analysis is still on progress.

The increase of <> and decrease of with increases in the0.4460<> [ps]   1        

0.45

0.41

<>

30
0.00

0.05

0.10

0.15

0.40
0.20

Volume fraction of silica

Reference[1] F. Alvarez et al., J. Phys. Rev. B 44, 7306 (1991).

Fig. 2 Volume fraction of silica dependence of<> and  at 300 K in the range Q = 1. 8 Å−1.