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 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    1
nn
Nonproportionality Studies in Single Crystal 
Scintillators: 
Towards Improved Energy Resolution for Nuclear 
and Radiological Detectors
M. Gascón, S. Lam, R. Gaume,  R. Feigelson
 Dept. of Material Science & Engineering, Stanford University
Sept. 26Th
,  2011  
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    2
Overview
Comments
  Motivation & background
  Modeling
  Temperature and Pressure studies
  Conclusions
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    3
Motivation: Scintillator applications
Comments
Petroleum Engineering
Medical Imaging
Scintillators
High­Energy Physics
Nuclear Radiation 
Detection
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    4
Motivation: scintillators history
M. J. Weber, J. Lumin. 100 (2002) 35
SrI2:Eu 1968/2008
LSO:Ce,Ca 2007
LuI3:Ce 2003
LaBr3:Ce 2001
LYSO:Ce 2001
LuYAP:Ce 2001
LaCl3:Ce 2000
LuAP:Ce 1994
LSO:Ce 1982
Invention 
of the PMT
CWE van Eijk, SCINT 2011
Robert Hofstadter
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    5
Motivation: Energy resolution
CWE van Eijk, SCINT 2011
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    6
Motivation: Nonproportionality in light yield
Light yield
 (relative to 662 keV)
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    7
Motivation: Nonproportionality in light yield
Light yield
 (relative to 662 keV)
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    8
Motivation: Temperature studies
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    9
Modeling: Pressure
DSSSD
Large Nonproportionality
LuAlO
3
conduction band
valence band
Small Nonproportionality
K2LaCl5
valence band
conduction band
dip: ↑ NPno dip: ↓ NP
Difference in charge carrier mobilities.
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    10
Light Yield Nonproportionality: Modeling
DSSSD
Observation of band structure 
of YAlO3 (YAP) and LuAlO3 
(LuAP). YAP and LuAP have the 
same crystal structure, but 
exhibit very different 
nonproportionality.
good proportionality poor proportionality
Similar band dispersion except for the presence of “dip” in conduction band 
minimum (CBM) of LuAP as indicated with the arrow
valence
band
X Y
Z
U R
T
S
1st
Brillouin
Zone
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    11
Motivation: Pressure experiment
Mobilities of charge carriers better matched
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    12
Isostatic pressure
http://harwoodeng.com/
Specifications:
Pressure range: 0<Piso<1 GPa
Large sample volume: >5 cm3
Operated at ambient temperature
Compatible with hygroscopic materials
Good pressure stability
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    13
Facilities
High pressure studies:  Eu:SrI2, BGO, Tl: CsI,  LSO
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    14
Isostatic pressure
Recall assumptions:
Pressure stability
Pressure dependence 
of optical coupling scintillator with 
window & reflector
Light output correction neededGood pressure stability 
|DP/P| < 1% after 1 hr
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    15
Isostatic pressure
  There is an increase in Light Output up to 
50%
 The optical coupling contribution was 
subtracted
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    16
 Conclusions
 Adequate detection and identification of radioactive material require 
scintillators with good light yield proportionality and energy resolution
 Light yield proportionality requires an effective mass ratio of 1 (well 
matched charge carrier mobilities)
 Nonproportionality and carrier mobility can be probed through 
application of high pressure and low temperature
This program is funded by the USA Domestic Nuclear
Detection Office (DNDO) and Dept. of Homeland
Security (DHS).
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    17
Recall assumptions:
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    18
Decay time
 Pulse were inverted  
 N Pulses were added after rise time correction
 Pulses with amplitudes bigger 0.4 (normalized) 
before ­0.5 us and after 2.5 us were discarded to avoid 
pile up. 
  Pulses with amplitudes below 1 mV were discarded.
Comments
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    19
Non Proportionality
Radioactive sources  and energies
 Cs­137..... 32 keV and 662 keV
 Ba­133..... 31 keV, 81 keV, 302 keV, 356 keV 
 Am­241.... 26 keV and 59.5 keV
 Cd­109..... 22 keV and 88 keV
 Co­57 …...122 keV
 Na­22........511 keV and 1274 keV
 Mn­54.......835 keV
 Eu­152......41 keV, 121 keV and 1408 keV
Cs-137
Ba-133
Am-241 Cd-109
Comments
 Fitting an extra peak can displace 
the peaks  5­10 channels  which 
means a huge change in NP at low 
energies
 M. Gascón, S. Lam, R. Gaumé, R. Feigelson   AOCL                      Stanford University                                    Sept. 26th, 2011    20
Non Proportionality
Radioactive sources  and energies
 Cs­137..... 32 keV and 662 keV
 Ba­133..... 31 keV, 81 keV, 302 keV, 356 keV 
 Am­241.... 26 keV and 59.5 keV
 Cd­109..... 22 keV and 88 keV
 Co­57 …...122 keV
 Na­22........511 keV and 1274 keV
 Mn­54.......835 keV
 Eu­152......41 keV, 121 keV and 1408 keV
Co-57
Na-22
Mn-54 Eu-152
Comments
  Co­57 has an additional peak below 122 
keV which is not in the tables
 Na and Mn are easily fit­able
 Eu has 41, 121 and 1408 are easily fit­able

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