In this lecture, I have covered basic introduction to presolar grains and its scope in understanding nucleosynthesis using multi-isotopic analyses NanoSIMS.
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Understanding Stellar Nucleosynthesis via Multi-isotopic NanoSIMS analyses of Presolar Grains
1. Understanding Stellar Nucleosynthesis via Multi-isotopic
NanoSIMS analyses of Presolar Grains
Lalit K Shukla
Assistant Professor
Faculty of Physical Sciences
4. Plan of the talk
• An introduction to Presolar Grains
• Approaches to laboratory studies
• Analysis tool: NanoSIMS
• Stellar nucleosynthesis: neutron capture processes
• Multi-isotopic analyses of heavy elements in single Presolar Grains
Understanding Stellar Nucleosynthesis via Multi-isotopic
NanoSIMS analyses of Presolar Grains
5. Presolar Grains: An introduction
Tiny grains (few µm or less) condensed in outer
envelop of stars during their mass ejection phase
and survived in all energetic processes in the
interstellar medium & collapse of molecular cloud
(that formed our solar system) and remained almost
intact.
Presolar Grains are found in the matrix of least
metamorphosed chondrites ( a class of stony
meteorites that have not been modified due to
melting or differentiation of the parent body) and
interplanetary dust particle (IDPs).
Presolar grains are identified from their isotopic
anomalies which can not be explained by any
process occurring within solar system
8. 8
Data is taken from Washington University
Presolar Grain Database
Presolar Grains: An introduction
❖ Varies from meteorite to meteorite (Amari et al. 1994, Huss et al. 1997),
❖ Variations in isotopic properties are seen with grain size (Lewis et al. 1994)
9. Chemical Separation: Separated
from meteorites by progressively
harsher acid dissolution.
In situ Search: Identified by
multi-detection raster ion imaging
by NanoSIMS.
❖ Some presolar phases get dissolve (silicates,
amorphous grains, less refractory coating
around grains etc.).
❖ May alter surfaces of grains chemically and/
or isotopically.
❖ Not great sampling issue (Abundance
calculation?)
❖ Time taking sample preparation. But once
over, thousands grains are ready for analysis.
❖ No dilution effect.
❖ All phases can be recovered (no
chemistry).
❖ Grain morphologies remain unchanged.
❖ S a m p l i n g m a t t e r s ( A b u n d a n c e
calculation?)
❖ Finding grains take quite time.
❖ Dilution effect (?)
Provide a glimpse into
dust population that
accumulated in the
presolar molecular
cloud.
Chemical and isotopic
signatures record
grain formation and
n u c l e o s y n t h e t i c
processes of various
stars.
Presolar Grains: Approaches to Study
Morphologies and
compositions may
reflect grain formation
conditions in stellar
environments.
10. In situ search for Presolar Grains
Isheyevo Clast 2 BSE Image
Total area analyzed: 13400 µm2
(10x10 µm2 raster)
Total presolar grains found: 2
(size:~240 nm and ~280nm)
Abundance: 8 ppm
SE Image
(overview of analyses)
Supernova(?) Grain
Isheyevo Meteorite
Work done with PRL NanoSIMS-50
Isheyevo Meteorite
Find, 2003, Russia, 16Kg
12. Decanted & added 30ml of 30% H2O2 slowly 1ml/min
(temp < 20oC)
Ultrasonic added DD water twice and
ultrasonic, centrifuge, decant
Colloid Extraction
Residue:
Wash with 0.1M NH3 (pH~9) (4 times)
Wash with DD water (2 times)
50 ml (0.5 N Na2Cr4O7+ 2 N H2SO4)
85oC , 24 hrs., centrifuge
Murray PM
(17.8 g)
PM +
HF (10M) + HCl (1M) (5 Changes)
HCl(6M) (5 Changes)
To dissolve silicates & metals (at room temp.)
PM +
HF (10M) + HCl (1M) (7 Changes)
HCl(6M) (7 Changes)
To dissolve silicates & metals (at 60oC)
PM +
H3BO3 (0.6M) + HCl (6M) (7 Changes)
HF(2M) + HCl(6M) (7 Changes)
To dissolve fluorides & silicates (at 55oC)
Wash with 0.1 M HCl
SEM: No Silicates
47ml 6M KOH to make soln. 4M (70oC, 24hrs)
To remove sulfur & reactive kerogen
After another colloid extraction
Residue + HClO4(200oC, 2 hrs.) (2 times)
To destroy remaining organic C & graphite
Residue + H2SO4(180oC, 4 hrs.)
Wash with DD water
(6 times alternatively)
To destroy oxides
Wash with 0.1M NaOH
SiC
Chemical Separation of Presolar Grains
13. Chemical Separation of Presolar Grains
NanoSIMS Study of Presolar Corundum grain, Mostefaoui et al., 2002
28Si
48Ti
min max
18O/16O17O/16O16O
16O 17O/16O 18O/16O
1 µm
Sah-602-4
Standard grain
14. Sputtering of a small localized area of solid
sample by an energetic primary ion beam under
high vacuum conditions to generate energetic
secondary ions from sample surface that are
mass analyzed.
Basic Principle:
❖ Non-destructive technique
❖ Less sample preparation is needed
❖ Element H to U may be detected
❖ Isotopic ratios can be measured precisely in
very localised area
Advantages:
❖ Matrix Dependent
❖ Sample must be vacuum Compatible
Limitations:
Ion Probe Technique: Secondary Ion Mass Spectrometer (SIMS)
15. Nano – Secondary Ion Mass Spectrometer (NanoSIMS)
High spatial resolution: ( ~ 50 nm for Cs+ and ~200
nm for O-)
Capable of analyzing sub micrometer-sized presolar
grains.
High mass resolution: Interferences can be resolved
with MRP
(m/Δm) = 10,000 to 15,000.
High Transmission: ~ 30 x IMS-4f
Multi isotope (5) detection facility: Made in-situ
search for presolar grains possible.
Less destructive technique: Few Å. Really needed for
such precious grains!
16. Nano – Secondary Ion Mass Spectrometer (NanoSIMS)
https://www.cameca.com/products/sims/nanosims
PRL NanoSIMS 50
PRL SIMS
17. Solar Value (270)
Solar Value (92)
Data is taken from Washington University Presolar Grain Database
Carbon and Nitrogen isotopic data:
Why Isotopic Abundances?
Formation of 12C:
α +α → 8Be + α → 12C
Formation of 13C:
12C(p, γ)13N(β+)13C
Completely different process!!
Formation of 14N:
13C(p,γ)14N
Formation of 15N:
14N(p,γ)15O(β+)15N
18O(p,α)15N
Oxygen Isotopic Data
Formation of 16O:
12C(α,γ)16O
Formation of 17O:
16O(p, γ)17F(β+)17O
Formation of 18O:
14N(α, γ)18F(β+)18O
Data is taken from Washington University Presolar Grain Database
Presolar Grains: Classification
18. Presolar Grains: Classification
Data is taken from Washington University Presolar Grain Database
Formation of 28Si:
16O+16O →28Si+ α
24Mg(α, γ) 28Si
Formation of 29Si:
28Si(n,γ)29Si
25Mg(α, γ)29Si
Formation of 30Si:
28Si(n,γ)29Si(n, γ)30Si
26Mg(α, γ)30Si
20. Neutron Capture Nucleosynthesis
• Creation of elements heavier than Fe through fusion is an endothermic
process.
• Coulomb repulsion is high for high Z.
• Thus, heavy element creation is not favoured by primary fusion or
charge particle reaction.
• Neutron capture is not hindered by Coulomb repulsion.
• Seed nuclei encounters an external neutron flux.
• Based on neutron density, slow (s-process) and rapid (r-process)
processes have been identified.
s- process (slow) r-process (rapid)
τ (n capture) >> τ (β- decay) τ (n capture) << τ (β- decay)
N Density ~ 108 n/cm3 N Density ~ 1021 n/cm3
Major Sites: AGB stars Major Sites: Core collapse Supernovae
21. Major neutron sources for sustaining s-
process in AGB stars:
13C(α, n)16O 22Ne(α, n)25Mg
T ~ 1×108 K T ~ 2-3×108 K
n ~ 107 n/cm3 n ~ 108-11 n/cm3
τ ~ 1000 years τ ~ few years
Characterized by an inert carbon-
oxygen core, surrounded by two
separate nuclear burning layers - an
inner layer of Helium and an outer
layer of Hydrogen. These layers are in
turn surrounded by a strongly
convective outer envelope.
Asymptotic Giant Branch (AGB) stars
22. Presolar Grains: A probe to AGB stars
❖ About 90% Silicon Carbide grains
(mainstream) and large fraction of
Oxide and Silicate grains show the
signature of AGB star origin.
❖ Characterized by lower 12C/13C and
higher 14N/15N than solar, enriched
in 17O.
Hoppe et al, 1994
Lambert et al, 1986
Mass Number
142 144 146 148 150
0
100
200
300
400
Mass Number
130 132 134 136 138
0
100
200
300
400
Neodymium Barium
Overabundance(%)
Prombo et al. (1993)Richter et al. (1995)
From Thermal Ionization Mass Spectrometer (TIMS) measurements on bulk
presolar SiC
Problems with data from bulk measurements
23. Marhas et al. (2007)
Before this work: 13C pocket size was almost a free parameter (ST/12 to STx2)
After this work: Needed 13C spread reduced from factors ~20 down to 2.
Constraining on 13C can help in understanding complex physical process.
ST: M(13C) = 3X10−6 Mʘ burnt per pulse
Signatures of s-process: Single grain analysis for Barium
24. Signatures of s-process: Single grain analysis for Neodymium
Branching at 141Ce.
Isobaric, Hydride, molecular interference
Branching at 147Nd
25. Required instrumental condition for measurement
Marhas et al. (2007)
First of all, we need standards of similar matrix for measurements i.e. synthetic
grains rich in trace elements.
Detectors arrangements according to our need i.e. resolve interferences with least
analysis time.
For C, N, and Si isotopic data: Cs+ primary ion beam, ~100 nm , ~1pA
For Nd isotopic data: O- primary ion beam, ~300 nm, ~10pA
Need to be vary careful about contaminations.