Observation of Nuclear Transmutation Reactions induced by D2 Gas Permeation

through Pd Complexes

Yasuhiro Iwamura 1, Takehiko Itoh1, Mitsuru Sakano1, Noriko Yamazaki1, Shizuma Kuribayashi1, Yasuko Terada2 and Testuya Ishikawa3 and Jirohta Kasagi4

ICCF-11, Marseilles, France, October31-November5, 2004

1Advanced Technology Research Center, Mitsubishi Heavy Industries, Ltd.2Japan Synchrotron Radiation Research Institute

3Coherent X-ray Optics Laboratory, SPring-8/RIKEN4Laboratory for Nuclear Science, Tohoku University

Contents1. Introduction

3. Experimental Results and Discussion 3-1 Transmutation of 137Ba and138Ba into 149Sm and 150Sm : Mass distribution of Sm depending on the given mass distribution of Ba 3-2 Pr confirmation by XRF and experiments for in-situ measurement at SPring-8 3-3 Consideration on the role of CaO layer

2. Experimental method and Results so far

4. Concluding Remarks

Features of the Present Method

D2 gas permeation through the Pd complex

Pd

CaOPd

Pd

CaOPd

Pd

CaOPd

Pd substrate

CaOPd 40nm

2nm

D Flux

Vacuum

D2 gas

D Permeation Surface

Cross Section of Pd Complex

Cs,Ba, etc.

Fabrication of Pd Complex

Pd 400CaO/Pd1000

25mm×25mm

900 C 10H Annealing under Vacuum Condition (< 10 Torr)

°-7

Washing a Palladium Sample with Acetone

Washing the Sample with Aqua Regia (100sec)

5 times Alternatingly Sputtering of CaO (20 ) and Pd (180 )

Ion Beam Sputtering of Pd only (400 )

Pd 0.1mm

Schematic View of the Experimental Apparatus

X-ray GunPhotoelectron Energy Analyzer

D Evacuation

D2 Gas

Pd ComplexTest Piece

Q-Mass

Ge Detector

XPS

Evacuation

Chamber A

Chamber B

Photograph of the Experimental SetupPhotoelectronEnergy Analyzer

X-ray Gun

D2 Inlet

Ge Detector

Main Chamber

PhotoelectronEnergy Analyzer

X-ray Gun

D2 Inlet

Ge Detector

Main Chamber

Decrease of Cs and Emergence of Pr

0 20 40 60 80 100 12002468

10121416

Cs 1st Pr 1st Cs 2nd Pr 2nd

Num

ber o

f ato

ms (

/10

14/c

m2 )

Time (h)

D

Cs

PdCaOPd

Identification of Pr by TOF-SIMS

D2 Gas Permeation

D

Cs

PdCaOPd

D

Cs

PdCaOPd

Pr

TOF-SIMS device (TRIFTTM ;ULVAC-PHI)

Molecular Ions

0 100 200 300 40002468

101214

Sr 1st Mo 1st Sr 2nd Mo 2nd Sr 3rd Mo 3rd

Num

ber o

f ato

ms (

/10

14/c

m2 )

Time (h)

D

Sr

PdCaO

Pd

Decrease of Sr and Emergence of Mo

Relation of Isotopic Composition between Sr and Mo

020406080

100

92 94 95 96 97 98 100Mass number

Isot

ope

ratio

(%)

Detected Mo

84 86 87 88Mass number

Isot

ope

ratio

(%)

020406080

100

(Natural abundance of Sr)

Given Sr

MoSr 96428838 →

Mass N. +8

Atomic N. +4

Pr1415913355 →Cs

Mass N. +8

Atomic N. +4

Recent Results Part 1

Transmutation of 138Ba into 150Sm and 137Ba into 149Sm

Transmutation of Ba into Sm; Natural Ba

D

PdCaOPd

D

Natural Ba(138Ba major)

PdCaOPd

D

PdCaOPd

D

Natural Ba(138Ba major)

PdCaOPd

150Sm was detected after D permeationon the Pd complex

Schematic View of the Ex-situ Measurement Apparatus

D2 Gas

Chamber B

D2

B-A GaugeB-A Gauge

TMPRP

Chamber A

D

Pd Complex with an Element(Cs, Sr,Ba,etc) D2 Gas

Chamber B

D2

B-A GaugeB-A Gauge

TMPRP

Chamber A

D

Pd Complex with an Element(Cs, Sr,Ba,etc)

Ex-situ MeasurementXPS, SIMS, ICP-MS, etc.

XPS Spectra for detected Sm

4.2 10 4

4.4 10 4

4.6 10 4

4.8 10 4

5 10 4

5.2 10 4

5.4 10 4

5.6 10 4

1070 1080 1090 1100 1110 1120 1130 1140

Counts(Ba1st)Counts(Ba2nd)

Binding Energy (eV)

Cou

nts

Sm 3d 5/2

Sm 3d 3/2

Full Spectrum

0

1 105

2 105

3 105

4 105

5 105

6 105

0 200 400 600 800 1000 1200 1400

Cou

nts

Binding Energy (eV)

Pd

Sm 3dBaC

Sm 4d

0

1 105

2 105

3 105

4 105

5 105

6 105

0 200 400 600 800 1000 1200 1400

Cou

nts

Binding Energy (eV)

0

1 105

2 105

3 105

4 105

5 105

6 105

0 200 400 600 800 1000 1200 1400

Cou

nts

Binding Energy (eV)

Pd

Sm 3dBaC

Sm 4d

D

PdCaOPd

D

Natural Ba(138Ba major)

PdCaOPd

D

PdCaOPd

D

Natural Ba(138Ba major)

PdCaOPd

D

PdCaOPd

D

Natural Ba(138Ba major)

PdCaOPd

D

PdCaOPd

D

Natural Ba(138Ba major)

PdCaOPd

Sm Natural Abundance

22.5%

26.6%

7.5%13.8%

11.3%

15.1%

3.2%

154Sm152Sm150Sm149Sm148Sm147Sm144Sm

00.20.40.60.8

1

144 145 146 147 148 149 150 152 153 154151

Sm Natural Abundance

Mass Number

Rat

io to

152 S

m

SIMS Spectra for Given and Detected Elements

10

10

10

104

105

135 140 145 150 155

3

2

1

Cou

nts

Mass Number

150Sm

138Ba

FG.BG.

00.20.40.60.8

1

144 145 146 147 148 149 150 152 153 154151

Sm Natural Abundance

Mass Number

Rat

io to

152 S

m

00.20.40.60.8

1

144 145 146 147 148 149 150 152 153 154151

Sm Natural Abundance

Mass Number

Rat

io to

152 S

m

BaOPd40Ca

138BaO71.7%

6.6%

11.3%7.8%

2.4%

Examination of Molecular Ions

150110 (12%)148108 (26%)146106 (27%)145105 (22%)144104 (11%)142102(1%)

Pd40CaPd

154138(71.7%)153137

(11.3%)

152136(7.8%)151135(6.6%)150134(2.4%)148132(0.1%)146130(0.1%)

Ba16OBa

No Molecular Ions for 149.110Pd(12%)Ca and 134Ba(2.4%)O for mass150, however their effects should be lower than 106Pd(27%)Ca and 138Ba(71.7%)O

Transmutation of Natural Ba into Sm

• XPS analysis showed Sm signal.• SIMS analysis showed the increase of mass

150.• Natural Sm isotopic distribution did not

match with SIMS mass data.• These facts strongly suggests that 150Sm

exists on the Pd complex after D2 gas permeation.

Transmutation of Ba into Sm; mass 137 Enriched Ba

149Sm may have been detected after D permeationon the Pd complex

D

PdCaOPd

D

137Ba

PdCaOPd

D

PdCaOPd

D

PdCaOPd

(Enriched Ba)

SIMS Spectra for #1Experiment

1

10

100

135 140 145 150 155

149Sm

137Ba

Cou

nts

Mass Number

FG.BG.

00.20.40.60.8

1

144 145 146 147 148 149 150 152 153 154151

Sm Natural Abundance

Mass Number

Rat

io to

152 S

m

00.20.40.60.8

1

144 145 146 147 148 149 150 152 153 154151

Sm Natural Abundance

Mass Number

Rat

io to

152 S

m

BaO

Pd40Ca

SIMS Spectra for #2 Experiment

1

10

100

1000

135 140 145 150 155

Cou

nts

Mass Number

FG.BG.

149Sm

137Ba0

0.20.40.60.8

1

144 145 146 147 148 149 150 152 153 154151

Sm Natural Abundance

Mass Number

Rat

io to

152 S

m

00.20.40.60.8

1

144 145 146 147 148 149 150 152 153 154151

Sm Natural Abundance

Mass Number

Rat

io to

152 S

m

BaO

Pd40Ca

Transmutation of 137Ba into Sm

• SIMS analysis showed the increase of mass 149.

• Natural Sm isotopic distribution did not match with SIMS mass data.

• XPS analysis showed very weak Sm spectra. Now we are trying to obtain clear XPS signals.

• These facts suggests that 149Sm exists on the Pd complex if we consider that Sm spectra were obtained by XPS using natural Ba.

Mass Correlation between Given and Detected Elements

0

20

40

60

80

100

146 147 148 149 150 1510

20

40

60

80

100

146 147 148 149 150 151

0

500

1000

1500

146 147 148 149 150 1510

500

1000

1500

146 147 148 149 150 1510

5000

1 104

1.5 104

2 104

133 134 135 136 137 138 1390

5000

1 104

1.5 104

2 104

133 134 135 136 137 138 139

0

500

1000

1500

133 134 135 136 137 138 1390

500

1000

1500

133 134 135 136 137 138 139

FG.BG.FG.BG.

FG.BG.FG.BG.

138Ba

137Ba

150Sm

149Sm

GivenElement

Given Element

DetectedElement

DetectedElement

SmBad

15062

613856 →

SmBad

14962

613756 →

M +12Z +6

M +12Z +6

The Aim of Ba Transmutation Experiments

149Sm is a Mossbauer Isotope

If we measure the Mossbauer effect of 149Sm, we will obtain clear evidence of generation of 149Sm.And the information on the ultra fine structure relating to the electronic state and phonon of the generated 149Sm will be obtained.

Experimental Results

SmBad

14962

)3(613756

α

→

Excitation Energy: 22.5keV

Recent Results Part 2

Pr Confirmation by XRF

and Experiments for

in-situ Measurement at SPring-8

Identification of Pr by X-ray Fluorescence

Detection of Pr using SOR X-ray at Spring-8, Harima, Japan(FG1, FG2: Signals from Samples after D2 Permeation BG: Signals from the sample before Permeation)

Experimental Set-up for in-situ Measurement located at SPring-8

TMP

DP

Be Window

SOR X-ray

Cl Filter

Detector

Evacuation

D2 Gas Inlet

VacuumSystem

Evacuation

Pd Complex with Cs

D

Fluorescence X-ray

Photograph of the Experimental Set-up

DetectorSOR X-ray

Chamber

BL-37XU

An Example of Pr Detection by the Experiments at SPring-8

3 4 5 650

100

150

200

35 36

Co

un

ts

E ne r gy ( k e V)

Pr-Lα 1

Cs-Lα 1

Cs-Lβ 2

Cs-Lβ 1

3 4 5 650

100

150

200

35 36

Co

un

ts

E ne r gy ( k e V)

Pr-Lα 1

Cs-Lα 1

Cs-Lβ 2

Cs-Lβ 1 3536 3536

Recent Results Part 3

Measurement and Experiments

relating to the role of CaO

TEM Photograph of the Pd Complex

CaO

Pd Substrate

400Pd

CaO and Pd Layers :1000

Bulk Pd : 0.1mm25mm× 25mm

Thin Pd Film : 400

CaO and Pd Layers :1000

Bulk Pd : 0.1mm25mm× 25mm

Thin Pd Film : 400

Depth Profile of Cs and Pr by TOF-SIMS

0 200 400 600 80010000.0

2.0x105

4.0x105

6.0x105

8.0x105100

No D After DCsPr

Sputtering time(sec)

Coun

ts(a

rv.u

nit)

Pr

Cs

0 200 400 600 80010000.0

2.0x105

4.0x105

6.0x105

8.0x105100

No D After DCsPr

No D After DCsPr

Sputtering time(sec)

Coun

ts(a

rv.u

nit)

Pr

Cs

Depth Profile of Cs and Pr by XPS(1)

0 2 4 6 8 10 12 14 16 180.00.20.40.60.81.01.2

B.G Cs F.G Cs F.G Pr

Ato

mic

Rat

io to

Pd

(%)

Sputter Time (min)

10nm

D+ Ion Bombardment Experiment Performed at Tohoku Univ.

Metal

d

d

P

t

d

dd

d

d

d d

d

Experimental ApparatusD+ Ion beam bombardmenton metal target

Deuterium Density measured by D+ Ion Bombardment Experiment

Density of Pd complex(Pd/CaO) indicated one order larger than normal Pd

MgO cannot work instead of CaO

ICP-MS measurements show no Pr(

Consideration on the Role of CaO

• Increase of Deuterium Density?• Modify the Electronic State of Surface Pd?

Depth Profile Measurement of DBy a Resonance Nuclear Reaction

BedLi 9421

73 ),( γ

Concluding RemarksTransmutations of Ba into Sm were observed both when natural Ba was applied to the Pd complex samples, and when mass-137-enriched Ba (monoisotopic Ba) was applied. The mass distribution of Sm that we obtained depended on the starting isotopic distribution of Ba.

1.

According to a D+ ion beam bombardment experiment performed at Tohoku University, the deuterium density of our Pd complex indicated one order larger than normal Pd.

3.

One of our experimental apparatus was carried to SPring-8 to perform an in-situ measurement. We obtained some Pr signals by the X-ray Fluorescence method.

2.