Micro-pillars compression of different

silicate glasses compositions

M. Bourguignon1, E. Barthel1
S. Sao-Jao2, S. Girard2, G. Kermouche2

1
Laboratory of Soft Matter Sciences and Engineering, EPSCI-PSL, Paris
2
Laboratory of Physics and Mechanics for Metallurgy, Mines Saint-Etienne

Matthieu BOURGUIGNON SPN Group Meeting

Supervisors : Etienne BARTHEL and Matteo CICCOTTI 2022-10-18

1
Before SIMM
Paris

2
 My PhD - Context
Multiscale experimental approach of the rupture of glasses

 Why a such difference in crack resistance among

Surface defects decrease the mechanical resistance of silicate glasses these silicate glasses ?
Y. Kato, H. Yamazaki, S. Yoshida, and J. Matsuoka, “Effect of densification on crack initiation under Vickers indentation test”, J. Non-Cryst. Solids, 2010
A. A. Griffith, ”The Phenomena of rupture and flow in solids”, 1920

3
 My PhD - Context
 Assumption : Material damage resulting from plastic shear flow initiates
fracture

 Shear bands formation during loading phase

 Tensile vertical stresses arise below the plastically deformed region right
at the end of the unloading phase

Silicate glass composition  Shear localizations  Crack initiation

T. M. Gross, J. Wu, D. E. Baker, J. J. Price, and R. Yongsunthon, "Crack-resistant glass with high shear band density", J. Non-Cryst. Solids, 2018
E. Barthel, V. Keryvin, G. Rosales-Sosa, and G. Kermouche, ”Indentation cracking in silicate glasses is directed by shear flow, not by densification”, Acta Mater. 2020

4
 In the SIMM Lab
 So why organic glasses?

J. B. C. Wu and J. C. M. Li, J. Materials Science, 1976

J.L. Halary , “Polymer materials”,2011
E. Van der Giessen. “Localized Plastic Deformations in Glassy Polymers”, European Journal of Mechanics, 1997

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Micro-pillars compression

6
Materials
 Manufacturing by Reactive Ion Etching (RIE)

On 3 compositions of silicate glasses:

• Alumino borosilicate (SiO2 - Al2O3 - B2O3)

• Soda Lime Silicate (SiO2 - NaO2 - CaO)
• Lead Silicate (SiO2 - PbO)

Efficient method on fused silica but not so simple with ionics inclusions in glasses

7
Methodology
 SEM in situ micro-compression set-up (ALEMNIS)

SEM

Punch
Pillars

8
Methodology
 Questions we want to investigate
 Ductility of silicate glasses other than silica glass
 Strain rate sensitivity
 Effect of Beam
 Effect of the environment
• Vacuum
• Various Pressure = 20 Pa of N2

 Tested conditions
• Glass type = [ABS, LS, SLS]
• Depth = [500, 1000,…, 3500] nm
• Tip speed = [100, 1000, 10000] nm/s
• Beam = [On, Off]
• VP mode = [On, Off]
• Tension = [5, 20] kV
• Current = [30, 120] nA

9
Methodology
 Perform micro-compression up to several prescribed depth

0.30 Effect of penetra

Loading
0.25 h=500nm
h=1000nm
Unloading
h=1500nm
h=2000nm
0.20

Force [N]
h=2500nm
h=3000nm
h=3500nm
0.15

0.10 10
 Constitutive relation
 Pure amorphous silica Fused silica pillars
ρ 𝑠𝑎𝑡
Δρ 𝑠𝑎𝑡 = − 1= 0.20
ρ
Plastic flow

Radial cracking
G. Molnar, G. Kermouche, E. Barthel, “Plastic response of amorphous silicates, from atomistic simulations to experiments – A general constitutive relation”, Mechanics of Materials, 2017, Volume 114, pp 1-8
R. Lacroix, G. Kermouche, J. Teisseire, et al. ‘’Plastic deformation and residual stresses in amorphous silica pillars under uniaxial loading’’, Acta Materialia, 2012, Volume 60, p. 5555-5566

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Alumino BoroSilicate (ABS)

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Results on ABS glass
 Ductile or Brittle?  Ductile at small scale!

0.30 Effect of penetra

0.25 h=500nm
h=1000nm
h=1500nm
h=2000nm
0.20

Force [N]
h=2500nm
h=3000nm
h=3500nm
 Microscale to decrease size effects
 Prevent fractures from intern defects 0.15
 Get closer to process area size (~10nm)

0.10 13
Results on ABS glass
 Effect of Beam and Vacuum

0.30 Effect of Beam and Vaccuum on ABS

0.25 Beam on 100 nm/s Radial cracking

Beam off 100 nm/s
VP Beam on 100 nm/s
0.20 VP Beam off 100 nm/s
Force [N]

0.15 4 µm
2 µm depth
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Results on ABS glass
 Effect of strain rate

0.30 Effect of tip speed on ABS

100 nm/s
1000 nm/s
0.25 1000 nm/s
Radial cracking

VP 100 nm/s
0.20
Force [N]

VP 1000 nm/s
VP 10000 nm/s
3.0
0.15 3 µm depth
4 µm

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Results on ABS glass
 Conclusions on ABS glass

 About plastic flow

• ABS glass is ductile at small scale
• Radial cracking is observed on the pillars
• Behaviour similar to silica?

 About tested conditions !

• No effects of Beam reported
• Effects of vacuum: under VP mode, hardening at large
strain is higher -> radial plastic flow is modified (or radial
cracking)
• Strain rate plays very slightly under Vacuum conditions
Finite Element Analysis could help

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Soda Lime Silicate (SLS)

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Results on SLS glass
 Is it ductile too? Yes!

0.4 Effect of penetra

h=500nm
h=1000nm
0.3 h=1500nm
h=2000nm

Force [N]
h=2500nm
h=3000nm 3.5
0.2 h=3500nm
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 Results on SLS glass
 Effect of strain rate

0.4
Effect of tip speed on SLS

100 nm/s Shear localizations and

VP 100 nm/s fracture afterwards
0.3 1000 nm/s
VP 1000 nm/s
1000 nm/s
VP 10000 nm/s
Force [N]

Shear bands Cracks from shear bands

0.2 3.0

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Results on SLS glass
 Conclusions on SLS glass

 About plastic flow

• SLS glass is ductile at small scale as well
• No radial cracking is observed
• Large radial expansion
• Shear localizations

 About tested conditions !

• No effects of Beam reported
• No effects of VP mode at 1000 nm/s
• Strain rate plays slightly under VP conditions (SLS is softer under VP
condition at 100 nm/s)

Finite Element Analysis could help again

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Lead Silicate (LS)

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Results on LS glass
 Effect of penetration depth
• Still ductile

Shear localizations

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Results on LS glass
 Effect of strain rate

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Results on LS glass
 Conclusions on LS glass

 About plastic flow

• LS glass is ductile at small scale
• No radial cracking observed
• Shear localizations then cracks !

 About tested conditions !

• No effects of Beam/VP reported
• Strain rate plays very slightly

Finite Element Analysis could help again

24
 Resume and perspectives
 Resume  Outlooks
ABS SLS LS
Ductility at  Compression of FIBed ABS/SLS/LS cylindrical
Yes Yes Yes
small scale µpillars
Radial Cracking Yes No No
 Investigate on new composition of glasses
Effect of Beam No No No
Load increases /
Effect of VP No (at 1000
Radial plastic No
mode flow is modified nm/s)

Plays slightly Plays slightly Finite Element Simulation

Effect of Strain under VP under VP Plays very
rate slightly
conditions conditions
Shear
No Seems to be Yes
localization

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Thanks for your attention!

26
 All the glass compositions

0.35
Comparison of all glass
0.30 Makes no sense
to plot because
0.25 ABS
not the same
pillar geometry !
orce [N]

SLS
0.20 LS 3.0
0.15 27
 Strain softening in epoxy resins
Objectives :
• Compression of micropillars
• Change the formulation/preparation of epoxy and observe the consequence on the strain softening

σ𝑦
Z1 Z2

Zpiezo

Z3
X
 Presence of water or plasticizers:
o Reduced the Y amount of strain softening and lowered
 The growth of sheared regions is inhibited in the post
yield stress
cured material, possibly due to a higher density of
o Effect of stress required for nucleation of sheared
cross-links Setup for micropillars compression
K. W. Thomson , L. J. Broutman, Journal of Materials Sciences, 1982
regions and little effect of their growth
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Birefringence
Diametral compression Sphere indentation in elastic regime 2D-Indentation
0

-2
10 Experiment
Experiment Calculated
Calculated
500 -4

8 Retardation
400 -6
Δ
300 -8
0
6
200 -10
-2
Retardation Δ -10 -5 0
4
Rotation 100 -4
ߜ
Retardance
-6
2
-8

Silica SiO2  Simple geometry first (diametral compression or sphere

-10 indentation)
0
-10 -5 0
Diameter 𝜙 (mm) 0 2 19.94 6 8 10
Determine stress field (analytically and numerically)
Thickness t (mm) 15.0
C (TPa-1) 3.5  Computionnaly deduce photoelastic patterns (Retardance & Rotation)
29