Cs2 HfCl6 Crystal for Rare Alpha Decay Search

Introduction
Measurements and results

Future work
Cs2 HfCl6 crystal scintillator for searches of rare

alpha decay in hafnium isotopes
C. Cardenas1,2 A. Burger1,2 B. Goodwin1 M. Groza1

M. Laubenstein3 S.Nisi3 S. Nagorny3,4 E. Rowe1
1
Department of Life and Physical Sciences,
Fisk University, Nashville, TN, USA
2
Department of Physics and Astronomy,
Vanderbilt University, Nashville, TN, USA
3
INFN Laboratori Nazionali del Gran Sasso, I-67100 Assergi, Italy
4
Gran Sasso Science Institute, I-67100 LAquila, Italy
MSAG Meeting, June 18, 2017

1/34
Crystal Cardenas Cs2 HfCl6 for rare alpha decay search
Introduction
Alpha decay of 174 Hf
Review of rare decay searches
Future work
Alpha decay today ... Neutrinoless double-beta decay

tomorrow
2/34
Introduction
Future work
Outline
1 Introduction
2 Measurements and results

Preparation of Cs2 HfCl6 crystal
Study of radioactive contamination
Characterization of Cs2 HfCl6
Pulse-shape analysis of scintillation signals
3 Future work
Summary
3/34
Introduction
Future work
174
Alpha decay of Hf scheme
174
R.D. Macfarlanes 1959 observation of Hf [1]

Surface Lab Passive Shield
Active Shield No PSD
40 d of data taking
100 mg sample mass
Enriched 174 Hf to 56%
FWHM = 4% at 2.3 MeV

Background (1 - 3 MeV) = 9
counts/hr
4/34
Introduction
Future work
Experimental Sensitivity
q
S = ln2 N t/Bg E (1)
High experimental sensitivity requires

Large # of active isotopes (N )
High registration efficiency ()
Low internal background (Bg)
Good energy resolution ( E)
Long term measurement (t)
5/34
Introduction
Future work
Requirements for developing a highly sensitive low

background detector
Desired properties
Radiopurity (internal
background)
Light yield
FWHM
PSD
High content of isotope of
interest
Non-hygroscopic
Easily produced
6/34
Introduction
Future work
Cesium hafnium chloride (CHC)

Possible detector for rare alpha decay in Hf isotopes
Table: Properties of Cs2 HfCl6 crystal scintillator.

Property Value Reference
Effective atomic number 58 -
Hf mass fraction 26% -
Density (g/cm3 ) 3.86 [2]
Melting point 820C [2]
Crystal structure cubic [3]
Wavelength of emission 400 - 430 nm [4, 2, 5, 6]
Energy resolution 3.3% at 662 keV of 137 Cs [2]
Average decay time 4 - 5 s [2, 5, 6]
Light yield relative to NaI(Tl) 135% [2]
* For -quanta, at room temperature.
7/34
Introduction
Future work
Cs2 HfCl6 crystal growth by vertical Bridgman
Bridgeman technique
Quartz ampule
CHC melts congruently at
820C
Pulling rate of 0.5 - 1.0 cm/day
Temperature gradient 5C/cm
at solid/liquid interface
Mass of sample 12.154 g
Top face diameter 20.8 - 21.5 mm
Bottom face diameter 23.5 - 24.0 mm
Height 7.90 - 7.97 mm
Volume 3.2 cm3
8/34
Introduction
Future work
HfCl4 3-fold static sublimation purification
9/34
Introduction
Future work
Chemical analysis
HR ICP-MS results
Table: Chemical purity of CsCl and HfCl4 (initial and after 3-fold static sublimation purification) starting
materials and sample CHC crystal measured by HR-ICP-MS, expressed in ppb unless stated otherwise. (For
complete list of measured chemical impurities please see paper )
Element CsCl HfCl4 (initial) HfCl4 (after ) CHC crystal

K 2.4 1.4 <0.5 <2
Co <5 <10 <5 <5
Cu <100 <200 <200 <100
Zr <0.5 918 966 78
La 8.7 2627 555 132
Sm <15 <15 <15 <15
Eu <3 33 25 130
Gd <5 <15 <5 <35
Pt <0.04 <100 <100 <40
Tl <5.5 <4 <4 <15
Bi <3 <2000 <2000 <1000
Th <0.5 <1 <1 <0.5
U <0.5 3200 267 <0.5

ppm 10/34
Introduction
Future work
Gran Sasso National Laboratory - Assergi, Italy
m.w.e. - meter water equivalent, the height of water equivalent to that of shielding material
11/34
Introduction
Future work
STELLA- SubTErranean Low Level Assay

facilities for ultra low background and spectroscopy
Details in: M.Laubenstein et al., Appl. Radiat. Isotopes 61 (2004) 167 12/34
Introduction
Future work
LNGS background
13/34
Introduction
Future work
Schematic view of HPGe "Ge-Cris" detector
14/34
Introduction
Future work
HPGe detector
3
measurements
measured with 3 cm CHC crystal for 494 h
15/34
Introduction
Future work
Estimation of radioactive activities
Sa Sb
A=( )/y m (2)
ta tb
High experimental sensitivity requires

Sa , Sb - Area of a peak in the sample(background)
ta , tb - time of sample (background) measurement
y - is the yield of corresponding -line [7]
- efficiency of full peak registration [8, 9]
m - mass of sample
16/34
Introduction
Future work
Radioactive activities
Table: Internal radioactive contamination of CsCl and HfCl4 (initial and after 3-fold static sublimation
purification) starting materials and as-grown CHC crystal measured by ULB-HPGe detector (see text).
Chain Nuclide Activities

CsCl HfCl4 (initial) HfCl4 (after ) CHC crystal
(Bq/kg) (Bq/kg) (Bq/kg) (mBq/kg)
232 Th 228 Ra <0.98 <1.1 <6.3 <12
228 Th <0.82 (0.8 0.4) <4.5 <6.3
238 U 226 Ra <0.54 <0.86 <4.5 <12
234 Th <22 <58 (130 30) <8.6
234m Pa <19 (50 20) <140 <3.7
235 U 235 U <0.53 (1.4 0.8) <2.7 <26
40 K <1.6 <2 <8 <0.18

60 Co - - - <19
132 Cs <0.45 - - 258
134 Cs (0.13 0.08) - - 526
137 Cs (1.2 0.2) <0.38 <1.5 83090
181 Hf - <3.1 <1.1 140.7
17/34
Introduction
Future work
Summary 1
Some measurements are affected by isobaric inference of Hf

and oxides
detection limits are then high: Yb, Lu, Ta, W, Ir, Pt and Bi
minor inferences from samples containing Cs
La reduced 5x
U reduced one order of magnitude (1.2x)
Growing helps to reduce the amount of Zr - to below 100 ppm
Free of nuclides of U/Th natural decay chains (few mBq/kg)
Artificial radionuclides: 134 Cs (52 6 mBq/kg), 137 Cs (0.8
Bq/kg)
Cosmic activated radionuclides = 132 Cs (25 8 mBq/kg),
181 Hf
(14 0.7 mBq/kg)
18/34
Introduction
Future work
Characterization set-up at Fisk University
19/34
Introduction
Future work
137
Calibration measurements with Cs source
Activity of source 10Ci (370 kBq)

Distance to crystal 11 cm
Time data acquisition 5 min
Energy resolution 4.3%
20/34
Introduction
Future work
241
Measurements with Am source
Activity of source 1Ci (370 kBq)

Distance to crystal 3 mm
Time data acquisition 5 min
E (starting) 4 MeV
E (- 3 mm) 3.7 MeV
E ( scale) 1475 keVee
Quenching factor 40%
Energy resolution 21%
21/34
Introduction
Future work
Quenching factor for external source
Typically in scintillating crystals

have different responses to
different types of irradiation
Alpha energy scale given in
electron-equivalent-energies
(MeVee) 1 MeV ray
produces 1 MeVee of electron
induced scintillation light
QF is important experimental
parameter, allowing one to
understand where peak
should appear in the
calibrated energy spectrum
22/34
Introduction
Future work
Scintillation timing characteristics
23/34
Introduction
Future work
Pulse-shape analysis on Cs2 HfCl6 by three methods

Figure of merit (FOM) determination
24/34
Introduction
Future work
Optimum filter
137
method
241
Average signal of Cs and Am
Fit Function
t
f (t) = (3)
X
Ai e i
Ai Amplitude
i Exp. decay
constant
25/34
Introduction
Future work
Optimum filter method
Weight Function
f f
P(t) = (4)
f + f
Shape-indicator formula
f (ti )P(ti )
P
SI = (5)
f (ti )
P
Sum over all time

steps
26/34
Introduction
Future work
Optimum filter method

Shape-indication distribution
Mean Sigma
-0.00894 0.00575
0.00126 0.00094
27/34
Introduction
Future work
Mean time analysis
Formula
f (tk )tk
P
< t >= P (6)
f (tk )
Sum over time steps
28/34
Introduction
Future work
Mean time analysis

Mean time distribution
Mean Sigma
4976 ns 90 ns
4225 ns 57 ns
29/34
Introduction
Future work
Charge integration analysis
Head
PSD ratio = (7)
Total
Each pulse is integrated

over two intervals t1
and t2 with charge
corresponding to Qt1
and Qt2
Max pt. 1.123 s

Crossing pt. 3.2 s
End pt. 25 s
30/34
Introduction
Future work
Charge integration analysis

Head / Total ratio distribution
31/34
Introduction
Future work
Summary 2
Differences between slow/fast components of scintillation

signal that allows one to differentiate between -quanta and
-particles.
We are able to fully separate signals originating from -quanta
and -particles.
OF (FOM = 9.3), MT (FOM = 7.4), CI (FOM = 7.45)
32/34
Introduction
Measurements and results Summary
Future work
For the future
Growth a bigger crystal out of starting material sent to us

from LNGS
higher purity, larger mass = more 174 Hf atoms
For decay measurements of other Hf isotopes would require
somewhere around 20 cm3 sample ( 77 g)
ground state to ground state, ground to excited + ray
For 02 decay of 174 Hf requires 100 cm3
33/34
Introduction
Future work
2cm3 sent to Cryogenic detector team - CRESST group

Max Planck Institute for Physics - Mnchen, Germany
7.55 g CHC = 1.075 1019 174 Hf atoms. Theor. 9 events. Exp.

143 events.
Experimental data coming soon! 34/34
Introduction
Future work
References
Ronald D Macfarlane and Truman P Kohman.
Natural alpha radioactivity in medium-heavy elements.
Physical Review, 121(6):1758, 1961.
Arnold Burger, Emmanuel Rowe, Michael Groza, Kristle
Morales Figueroa, Nerine J Cherepy, Patrick R Beck, Steven
Hunter, and Stephen Payne.
Cesium hafnium chloride: A high light yield, non-hygroscopic
cubic crystal scintillator for gamma spectroscopy.
Applied Physics Letters, 107(14):143505, 2015.
John F Ackerman.
Preparation and luminescence of some [k2ptcl6] materials.
Materials research bulletin, 19(6):783791, 1984.
By. Kang and Koushik Biswas.
34/34
Introduction
Future work
Carrier self-trapping and luminescence in intrinsically activated

scintillator: Cesium hafnium chloride (cs2hfcl6).
The Journal of Physical Chemistry C, 120(22):1218712195,
2016.
Keiichiro Saeki, Yutaka Fujimoto, Masanori Koshimizu,
Takayuki Yanagida, and Keisuke Asai.
Comparative study of scintillation properties of cs2hfcl6 and
cs2zrcl6.
Applied Physics Express, 9(4):042602, 2016.
S Kurosawa, S Kodama, Y Yokota, T Horiai, A Yamaji,
Y Shoji, R Krl, J Pejchal, Y Ohashi, K Kamada, et al.
Cesium hafnium chloride scintillator coupled with an avalanche
photodiode photodetector.
Journal of Instrumentation, 12(02):C02042, 2017.
C Arpesella.
34/34
Introduction
Future work
A low background counting facility at laboratori nazionali del

gran sasso.
Applied Radiation and Isotopes, 47(9-10):991996, 1996.
M Heisel, F Kaether, and H Simgen.
Statistical analysis of low-level material screening
measurements via gamma-spectroscopy.
Applied Radiation and Isotopes, 67(5):741745, 2009.
Melissa Boswell, Yuen-Dat Chan, Jason A Detwiler, Padraic
Finnerty, Reyco Henning, Victor M Gehman, Rob A Johnson,
David V Jordan, Kareem Kazkaz, Markus Knapp, et al.
Mage-a geant4-based monte carlo application framework for
low-background germanium experiments.
IEEE Transactions on Nuclear Science, 58(3):12121220, 2011.
34/34

Cs2 HfCl6 Crystal for Rare Alpha Decay Search

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Introduction

Measurements and results

Cs2 HfCl6 crystal scintillator for searches of rare

C. Cardenas1,2 A. Burger1,2 B. Goodwin1 M. Groza1

MSAG Meeting, June 18, 2017

Alpha decay today ... Neutrinoless double-beta decay

2 Measurements and results

Active Shield No PSD

Enriched 174 Hf to 56%

FWHM = 4% at 2.3 MeV

High experimental sensitivity requires

Requirements for developing a highly sensitive low

Cesium hafnium chloride (CHC)

Table: Properties of Cs2 HfCl6 crystal scintillator.

Cs2 HfCl6 crystal growth by vertical Bridgman

HfCl4 3-fold static sublimation purification

Element CsCl HfCl4 (initial) HfCl4 (after ) CHC crystal

Gran Sasso National Laboratory - Assergi, Italy

STELLA- SubTErranean Low Level Assay

Schematic view of HPGe "Ge-Cris" detector

Estimation of radioactive activities

High experimental sensitivity requires

Chain Nuclide Activities

40 K <1.6 <2 <8 <0.18

Some measurements are affected by isobaric inference of Hf

Characterization set-up at Fisk University

Activity of source 10Ci (370 kBq)

Activity of source 1Ci (370 kBq)

Quenching factor for external source

Typically in scintillating crystals

Scintillation timing characteristics

Pulse-shape analysis on Cs2 HfCl6 by three methods

Optimum filter method

Sum over all time

Optimum filter method

Mean time analysis

Sum over time steps

Mean time analysis

Charge integration analysis

Each pulse is integrated

Max pt. 1.123 s

Charge integration analysis

Differences between slow/fast components of scintillation

For the future

Growth a bigger crystal out of starting material sent to us

2cm3 sent to Cryogenic detector team - CRESST group

7.55 g CHC = 1.075 1019 174 Hf atoms. Theor. 9 events. Exp.

Carrier self-trapping and luminescence in intrinsically activated

A low background counting facility at laboratori nazionali del

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