New Science from new New Science from new Technology:Technology:
NanoSIMS and RIMS NanoSIMS and RIMS
Peter HoppePeter Hoppe
Max-Planck-Institute for ChemistryMax-Planck-Institute for Chemistry
IAU Meeting 2006IAU Meeting 2006
PraguePrague
August 21, 2006August 21, 2006
OutlineOutline1. 1. IntroductionIntroduction2.2. NanoSIMS 50 Ion MicroprobeNanoSIMS 50 Ion Microprobe3.3. RIMS - CharismaRIMS - Charisma4.4. NanoSIMS StudiesNanoSIMS Studies
4.1. Submicrometer-sized Presolar Grains4.1. Submicrometer-sized Presolar Grains4.2. Isotopic Homogeneity within Presolar 4.2. Isotopic Homogeneity within Presolar GrainsGrains4.3. Presolar Silicates4.3. Presolar Silicates4.4. Coordinated NanoSIMS-TEM Studies4.4. Coordinated NanoSIMS-TEM Studies
5.5. RIMS StudiesRIMS Studies5.1. SiC Mainstream Grains5.1. SiC Mainstream Grains5.2. SiC X Grains5.2. SiC X Grains
6.6. SummarySummary
Introduction (I)Introduction (I)
A b u n d a n c e ( p p m )
S i C
D i a m o n d
C o r u n d u m
S i 3 N 4
1 0 - 3 1 0 - 2 1 0 - 1 1 0 0 1 0 1 0 2 1 0 3 1 0 4
S p i n e l
S i l i c a t e s i n M e t e o r i t e s
S i l i c a t e s i n I D P s
G r a p h i t e
Presolar MineralsPresolar Minerals
Introduction (II)Introduction (II)
1 0
1 0 2
1 0 3
1 0 4
1 0 5
1 0 0Novae
1 0 0 1 0 41 0 1 0 2 1 0 31 0 - 1 1 0 5
MainstreamType A&BType XType Y&Z
12C/13C
14N
/15N
C-rich zonein SN II
CNO cycle
C stars
Presolar SiC PopulationsPresolar SiC Populations
Introduction (III)Introduction (III)
Noble gas mass spectrometry of bulk Noble gas mass spectrometry of bulk samples (late 1980s, early 1990s)samples (late 1980s, early 1990s)
Conventional SIMS (late 1980s, Conventional SIMS (late 1980s, 1990s, early 2000s)1990s, early 2000s)
RIMS (late 1990s)RIMS (late 1990s) NanoSIMS (2000s)NanoSIMS (2000s)
Isotope Analyses of Presolar GrainsIsotope Analyses of Presolar Grains
Introduction (IV)Introduction (IV)
NanoSIMS:NanoSIMS: Analysis of submicrometer-sized presolar dustAnalysis of submicrometer-sized presolar dust In-situ search for presolar dustIn-situ search for presolar dust Investigation of isotopic heterogeneity within Investigation of isotopic heterogeneity within
grainsgrains
RIMS:RIMS: Isotopic compositions of heavy elements in Isotopic compositions of heavy elements in
individual grainsindividual grains
The Role of NanoSIMS and RIMSThe Role of NanoSIMS and RIMS
NanoSIMS 50 (I)NanoSIMS 50 (I) Commercial ion microprobe from CamecaCommercial ion microprobe from Cameca Introduction to field of cosmochemistry in 2001 Introduction to field of cosmochemistry in 2001
(Washington University, St. Louis and MPI for (Washington University, St. Louis and MPI for Chemistry, Mainz)Chemistry, Mainz)
Three fundamental features:Three fundamental features:1. Small beam size (down to 50 nm for Cs1. Small beam size (down to 50 nm for Cs++--ions)ions)2. High transmission at high mass resolution2. High transmission at high mass resolution (30x higher than in the IMS3f for conditions (30x higher than in the IMS3f for conditions used for O-isotopic measurements) used for O-isotopic measurements)3. Simultaneous detection of up to five isotopes3. Simultaneous detection of up to five isotopes (minimum mass separation is M/30, i.e., (minimum mass separation is M/30, i.e., isotopes up to mass 30 (Si) can be measured isotopes up to mass 30 (Si) can be measured simultaneously simultaneously
RIMS - CharismaRIMS - Charisma Most advanced (in the field): CHARISMAMost advanced (in the field): CHARISMA
(Chicago-Argonne Resonant Ionization(Chicago-Argonne Resonant IonizationSpectrometer for Mass Analysis)Spectrometer for Mass Analysis)
Laser ablation + laser ionization + TOF-MSLaser ablation + laser ionization + TOF-MS Superior to SIMS for trace elements , Superior to SIMS for trace elements ,
especially such with small ion yields in SIMS especially such with small ion yields in SIMS Basically a single-element-methodBasically a single-element-method First applications: Fe, Sr, Zr, Mo, Ru, and Ba First applications: Fe, Sr, Zr, Mo, Ru, and Ba
in single presolar SiC & graphite grainsin single presolar SiC & graphite grains Prospects:Prospects:
““Useful yield” of current setup ~ 1 %Useful yield” of current setup ~ 1 % Planned modification: aiming at ~ 30%Planned modification: aiming at ~ 30%
CHARISMA – Schematics (I)CHARISMA – Schematics (I)
atoms & molecules
ions
Mo Ba
Ti2
Ti
Si
Ti+ Si+
Neutral species drift up; ions are
suppressed
Gold mount
Mo
Ba+
Ti2
Ti
Si
Ba ions are accel- erated and mass- analyzed with a
time-of-flight mass spectrometer
Mo Ba+
Ti2
Ti
Si
Two lasers tuned to resonantly ionize
Ba are fired just above surface
Ablationlaser fires
SiC grainfocus to 1 µm
Most presolar grains are submicrometer Most presolar grains are submicrometer in sizein size Previous characterization was biasedPrevious characterization was biased
NanoSIMS made it possible to obtain NanoSIMS made it possible to obtain information on previously largely information on previously largely unexplored presolar grain types:unexplored presolar grain types: Sub-population of presolar SiC with specific Sub-population of presolar SiC with specific
Si-isotopic signatureSi-isotopic signature Presolar spinel (MgAlPresolar spinel (MgAl22OO44))
NanoSIMS Studies (I)NanoSIMS Studies (I)Submicrometer-sized Presolar GrainsSubmicrometer-sized Presolar Grains
NanoSIMS Studies (II)NanoSIMS Studies (II)
Group 2 Group 1
Group 3
Group 4
Figure 1
1.0E-4
1.0E-3
17O
/16O
1.0E-4 1.0E-3
18O/16O
Semarkona
OCs
Orgueil
Murray
solar
sola
r
OC2M12
OR1
M8OR4
OC1
M16M20
M18
M17
OC3OR2
M13
M10
S-S21
Zin
ner et al., 2005
O in Presolar SpinelO in Presolar Spinel
NanoSIMS Studies (III)NanoSIMS Studies (III)
Isotopic homogeneity can be Isotopic homogeneity can be studied within micrometer-sized studied within micrometer-sized presolar grainspresolar grains
In most cases isotopic compositions In most cases isotopic compositions turned out to be homogeneousturned out to be homogeneous
Isotopic heterogeneities:Isotopic heterogeneities: TiC within graphiteTiC within graphite SiC from supernovaeSiC from supernovae
Isotopic Homogeneity within Presolar Isotopic Homogeneity within Presolar GrainsGrains
NanoSIMS Studies (IV)NanoSIMS Studies (IV)
28Si48Ti
min max
18O/16O17O/16O16O
16O 17O/16O 18O/16O
1 m
Sah-602-4
Standard grain
Mostefaoui et al., 2002
O in Presolar CorundumO in Presolar Corundum
NanoSIMS Studies (V)NanoSIMS Studies (V)
MurchisonSiC X grains
MainstreamGrains
-1000 -800 -600 -400 -200 0 200 400
d30Si/28Si (‰ )
-1000
-800
-600
-400
-200
0
200
400
d29S
i/28S
i (‰
)
NanoSIMSNanoSIMS, 44TiIMS3f
Besm
ehn
and
Hop
pe, 2003
Presolar SiC-XPresolar SiC-X
NanoSIMS Studies (VI)NanoSIMS Studies (VI)B
esmeh
n an
d H
opp
e, 2003
30Si/28Si28Si
min max
1 m
28Si 29Si/28Si 30Si/28Si
Presolar SiC-XPresolar SiC-X
NanoSIMS Studies (VII)NanoSIMS Studies (VII)
Most presolar minerals can be separated by Most presolar minerals can be separated by harsh chemical treatments from meteoritesharsh chemical treatments from meteorites
Does not hold for silicatesDoes not hold for silicates Silicates are the major constituent of O-rich Silicates are the major constituent of O-rich
dust around starsdust around stars First silicates discovered in an IDP in 2002 First silicates discovered in an IDP in 2002
(Messenger et al.); use of NanoSIMS was (Messenger et al.); use of NanoSIMS was essentialessential
O-isotopic mapping of slices of meteorites or O-isotopic mapping of slices of meteorites or IDPs with 100 nm lateral resolutionIDPs with 100 nm lateral resolution
Presolar SilicatesPresolar Silicates
NanoSIMS Studies (VIII)NanoSIMS Studies (VIII)
16O 17O 17O/16O
Acfer 094 Meteorite (Mostefaoui and Hoppe, 2004)
Presolar SilicatesPresolar Silicates
NanoSIMS Studies (IX)NanoSIMS Studies (IX)
Simultaneous information on Simultaneous information on mineralogy, structure, isotopic mineralogy, structure, isotopic compositions, and petrological compositions, and petrological context of presolar materialscontext of presolar materials
Preparation of thin sections of Preparation of thin sections of individual particles by ultra-individual particles by ultra-microtomy or FIB lift-outmicrotomy or FIB lift-out
Coordinated NanoSIMS-TEM StudiesCoordinated NanoSIMS-TEM Studies
NanoSIMS Studies (X)NanoSIMS Studies (X)
1
2
3
NRL, Carnegie Institution, and MPI Mainz, 2004, unpublished
Presolar SiC-XPresolar SiC-X
RIMS Studies (I)RIMS Studies (I)Zr in SiC mainstream grainsZr in SiC mainstream grains
Nicolu
ssi et al., 1997
90 92 94 96Zr isotope
-1000
-800
-600
-400
-200
0
200di Z
r/92
Zr
(‰)
91
Grain KJH-151
s-process path
RIMS Studies (II)RIMS Studies (II)
-400
-200
0
d90Z
r (ä
)
-400
-200
0
d91Z
r (ä
)
-200
0
d92Z
r (ä
)
-1000 -800 -600 -400 -200 0
d(96
Zr/94
Zr) (ä)
D12D6D3D2D1.5STU1.3U2
SiC grains
[Fe/H]=0solar
metallicity
1.5 M
Lessons from Zr:Lessons from Zr: Mainstream SiC grains Mainstream SiC grains
come from low-mass come from low-mass AGB stars, probably AGB stars, probably mostly 1.5–3 Mmostly 1.5–3 M; 5 M; 5 M can be excludedcan be excluded
A variety of conditions A variety of conditions are required to explain are required to explain the array of grain the array of grain compositionscompositions
Models do a good job of Models do a good job of explaining most of the explaining most of the data, but low data, but low 9696Zr grains Zr grains remain a difficultyremain a difficulty
Zr in SiC mainstream grainsZr in SiC mainstream grains
RIMS Studies (III)RIMS Studies (III)9999Tc in SiC mainstream grainsTc in SiC mainstream grains
Savina et al., 2004
RIMS Studies (IV)RIMS Studies (IV)Mo in SiC X grainsMo in SiC X grains
Pel
lin
et
al.,
1999
Although previously Although previously postulated, a new type postulated, a new type of nucleosynthesis was of nucleosynthesis was recognized in naturerecognized in nature
The neutron burst The neutron burst required is a natural required is a natural consequence of Type II consequence of Type II supernova explosionssupernova explosions
X-grains must come X-grains must come from Type II, not Type Ia from Type II, not Type Ia supernovae, as such a supernovae, as such a burst does not occur in burst does not occur in SN IaSN Ia
SummarySummary
NanoSIMS and RIMS have become well-NanoSIMS and RIMS have become well-established tools in presolar grain researchestablished tools in presolar grain research
Important breakthroughs:Important breakthroughs: Extension of isotope analyses to Extension of isotope analyses to
submicrometer-sized grainssubmicrometer-sized grains Study of isotopic homogeneity within Study of isotopic homogeneity within
micrometer-sized grainsmicrometer-sized grains Discovery of presolar silicate grainsDiscovery of presolar silicate grains Isotope analyses of the heavy elements by Isotope analyses of the heavy elements by
RIMS provided important input for a better RIMS provided important input for a better understanding of neutron-capture reactions in understanding of neutron-capture reactions in the grain’s parent starsthe grain’s parent stars
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