Dynamics of silver nanoparticle formation and agglomeration inside the cavitation bubble after pulsed laser ablation in liquid
Open accessAbstract
The formation of nanoparticles within the laser-induced cavitation bubble is studied in situ using small angle X-ray scattering with high spatiotemporal resolution. Directly after laser ablation, two different particle fractions consisting of compact primary particles of 8-10 nm size and agglomerates of 40-60 nm size are formed. The abundance of these species is strongly influenced by the dynamics of the oscillating cavitation bubble. Primary particle mass is most abundant during maximal expansion of the first bubble and reappears a little weaker in the rebound. In contrast to this, the mass abundance of agglomerates is relatively low in the first bubble but strongly increases during first bubble collapse and following rebound. Although most of the ablated material is trapped inside the bubble and follows its oscillation, a minor fraction of both species could be detected outside the cavitation bubble even before its final collapse.
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Claims the paper makes
0 of 7 cited sources checked · 0 supported · 0 flagged
- Findingown data
The fit suggests a ratio of 20-100 between primary particle and agglomerate number.
“The fit suggests a ratio of 20-100 between primary particle and agglomerate number.”
Quote in the paperNot a substantial claim - Findingown data
The primary particles have a tendency to grow during the life time of the cavitation bubble.
“This tendency of the primary particles to grow during the life time of the cavitation bubble is also shown in Fig. 5.”
Quote in the paperSubstantial claim - Findingown data
The smaller particles in the range of 8-10 nm are best fitted with high exponents close to 4.
“These smaller particles in the range of 8-10 nm are best fitted with high exponents close to 4.”
Quote in the paperSubstantial claim - Findingown data
There is an experimental indication of small sub-nm-sized clusters or ionic species which are below the resolution of the experimental set-up.
“Furthermore, it is important to note that there is an experimental indication of small sub-nm-sized clusters or ionic species which are below the resolution of our experimental set-up.”
Quote in the paperNot a substantial claim - Findingown data
The SAXS data distinguish size fractions around 8-10 nm and a second fraction of up to 60 nm diameter.
“The data allow us to distinguish between size fractions around 8-10 nm and a second fraction of up to 60 nm diameter.”
Quote in the paperSubstantial claim
- Findingcitation
Close to the target (0.17 mm), the primary particle size shows a trend of increase during the bubble rebound.
“Close to the target (0.17 mm) there is a trend of increase in the primary particle size during the bubble rebound, probably by growth or coalescence due to high temperatures at the bubble collapse.25”
Quote in the paperSubstantial claim0 of 1 sources checked- cites [25] 25. W. Soliman, T. Nakano, N. Takada and K. Sasaki, Jpn. J. Appl. Phys., 2010, 49, 116202.
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
- Findingown data
Above the bubble (1.0 and 1.2 mm), no temporal trend of particle size change can be seen.
“Above the bubble (1.0 and 1.2 mm), no temporal trend of particle size change can be seen.”
Quote in the paperNot a substantial claim - Findingown data
The larger size fraction requires a power-law exponent at or below 2.
“The larger size fraction needs to be described by a small exponent at or below 2.”
Quote in the paperSubstantial claim - Findingown data
Two different particle fractions consisting of compact primary particles of 8-10 nm size and agglomerates of 40-60 nm size are formed directly after laser ablation.
“Directly after laser ablation, two different particle fractions consisting of compact primary particles of 8-10 nm size and agglomerates of 40-60 nm size are formed.”
- Also stated in: § 3.2 Spatiotemporal particle distribution in the cavitation bubble · plain
“The data allow us to distinguish between size fractions around 8-10 nm and a second fraction of up to 60 nm diameter.”
- Also stated in: § 4 Conclusions · plain
“Inside the cavitation bubble two individual species can be identified: compact primary particles of 8-10 nm size and bigger agglomerates of 40-60 nm size.”
Quote in the paperSubstantial claim - Also stated in: § 3.2 Spatiotemporal particle distribution in the cavitation bubble · plain
- Findingreasoning
The primary particle size is almost constant with a small trend towards smaller particles at larger height.
“The primary particle size is almost constant with a small trend towards smaller particles at larger height, which is in good agreement with recent measurements on laser ablation of gold.29”
Quote in the paperNot a substantial claim0 of 1 sources checked- cites [29] 29. S. Ibrahimkutty, P. Wagener, A. Plech, A. Menzel and S. Barcikowski, Appl. Phys. Lett., 2012, 101, 103104.
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
- Findingown data
Agglomerates are also seen to grow in the rebound at 0.17 and 0.5 mm.
“Agglomerates are also seen to grow in the rebound at 0.17 and 0.5 mm.”
Quote in the paperNot a substantial claim - Findingown data
The abundance of the two particle species is strongly influenced by the dynamics of the oscillating cavitation bubble.
“The abundance of these species is strongly influenced by the dynamics of the oscillating cavitation bubble.”
- Also stated in: § 3.2 Spatiotemporal particle distribution in the cavitation bubble · hedged
“Inside the bubble, primary particles and agglomerates in principle follow the cavitation bubble dynamics (0.17 and 0.5 mm).”
- Also stated in: § 4 Conclusions · boosted
“The particle abundance is strongly linked to cavitation bubble dynamics: during maximum elongation of the cavitation bubble, the primary particle mass goes through a maximum and reappears in the rebound, probably then contained in agglomerates.”
Quote in the paperSubstantial claim - Also stated in: § 3.2 Spatiotemporal particle distribution in the cavitation bubble · hedged
- Findingown data
The particle mass development is closely connected to the bubble dynamics.
“It can be resolved clearly that the particle mass development is closely connected to the bubble dynamics.”
Quote in the paperSubstantial claim - Findingnone given
There is a slight tendency for growth of primary particles and agglomerates during the first rebound.
“Furthermore, there is a slight tendency for growth of primary particles and agglomerates during the first rebound.”
Quote in the paperSubstantial claim - Findingown data
The increase in the agglomerate abundance during the rebound is significant.
“The increase in the agglomerate abundance during the rebound is significant.”
Quote in the paperSubstantial claim - Findingown data
A strong release of agglomerates is seen at later times beyond 400 μs where no macroscopic bubbles were detected by the X-ray beam down to 170 μm above the target.
“Additionally, a strong release of agglomerates is seen at later times beyond 400 ms where no macroscopic bubbles were detected by the X-ray beam down to 170 mm above the target.”
Quote in the paperSubstantial claim - Interpretationreasoning
Ripening processes take part after final collapse of the cavitation bubble and release of primary particles.
“Thus, ripening processes take part after final collapse of the cavitation bubble and release of primary particles.”
Quote in the paperSubstantial claim - Interpretationown data
The values of 3.6-4 for the primary particles are indicative of compact objects.
“The values of 3.6-4 for the primary particles are indicative of compact objects.”
Quote in the paperSubstantial claim - Interpretationown data
The peak shoulder is interpreted as a second rebound of the bubble after collapse due to oscillation described by the Rayleigh-Plesset equation.
“We interpret this behavior as a second rebound of the bubble after collapse due to oscillation described by the Rayleigh-Plesset equation.”
Quote in the paperNot a substantial claim - Interpretationown data
The variability of agglomerate size within the first bubble, the rebound and after bubble collapse supports the notion that these agglomerates are rather loose networks than compact objects.
“The variability of agglomerate size within the first bubble, the rebound and after bubble collapse supports the notion that these agglomerates are rather loose networks than compact objects.”
Quote in the paperSubstantial claim - Interpretationreasoning
The primary particles are emitted from the target with a distinct distribution in nascence and/or drift velocity.
“The primary particles are emitted from the target with a distinct distribution in nascence and/or drift velocity.”
Quote in the paperSubstantial claim - Premisecitation
Silver nanoparticles fabricated in pure water using similar laser parameters show an average particle diameter of about 18 nm, almost twice the diameter of primary particles identified within the cavitation bubble.
“Silver nanoparticles fabricated in pure water using similar laser parameters show an average particle diameter of about 18 nm 37 which is almost twice the diameter of primary particles identified within the cavitation bubble.”
Quote in the paperSubstantial claim0 of 1 sources checked- cites [37] 37. P. Wagener, A. Schwenke and S. Barcikowski, Langmuir, 2012, 28, 6132.
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
- Interpretationreasoning
Agglomerates can finally be released after the rebound has decayed.
“Agglomerates can finally be released after the rebound has decayed.”
Quote in the paperSubstantial claim - Interpretationcitation
The increase in primary particle size during the rebound is probably due to growth or coalescence at high temperatures during bubble collapse.
“Close to the target (0.17 mm) there is a trend of increase in the primary particle size during the bubble rebound, probably by growth or coalescence due to high temperatures at the bubble collapse.25”
Quote in the paperSubstantial claim0 of 1 sources checked- cites [25] 25. W. Soliman, T. Nakano, N. Takada and K. Sasaki, Jpn. J. Appl. Phys., 2010, 49, 116202.
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
- Premisereasoning
A partial integral over I(q)q^2 in the borders of the Guinier region of the respective hierarchy level gives a good approximation for the mass fraction at this size.
“Therefore a partial integral over I(q)q 2 in the borders of the Guinier region of the respective hierarchy level gives a good approximation for the mass fraction at this size.”
Quote in the paperSubstantial claim - Interpretationreasoning
Most of the mass release happens after recompaction onto the surface during bubble collapse.
“A picture is finally established that implies that most of the mass release happens after recompaction onto the surface during bubble collapse.”
Quote in the paperSubstantial claim - Interpretationreasoning
Primary particles may enter the liquid already during the bubble expansion phase possibly due to high ejection velocities.
“Primary particles may enter the liquid already during the bubble expansion phase possibly due to high ejection velocities.”
Quote in the paperSubstantial claim - Premisecitation
At low filling fractions F << 1, the Porod invariant is proportional to the total mass (mass contrast) in the scattering volume.
“At low filling fractions F { 1 the invariant is proportional to the total mass, strictly speaking to the mass contrast in the scattering volume.”
Quote in the paperSubstantial claim0 of 2 sources checked- cites [34] 34. G. Porod, Kolloidn. Zh., 1952, 125, 109.
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
- cites [35] 35. A. Plech, A. Siems, V. Kotaidis and M. Sztucki, Phys. Chem. Chem. Phys., 2008, 10, 3888.
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
- Interpretationown data
This points towards a slow (diffusional) release of part of the ablated material after collapse-driven redeposition onto or close to the target.
“This also points towards a slow (diffusional) release of part of the ablated material after collapse-driven redeposition onto or close to the target.”
Quote in the paperSubstantial claim - Interpretationreasoning
The bubble-liquid interface is penetrable by the ablated matter.
“This indicates that bubble-liquid interface is penetrable by the ablated matter.”
Quote in the paperSubstantial claim
- May combine two claims. 14
- The quote only partly states this claim. 4
- Classified as probably not a substantial claim. 2
May combine two claims.
Findingown dataThe mass abundance of agglomerates is relatively low in the first bubble but strongly increases during first bubble collapse and following rebound.
“In contrast to this, the mass abundance of agglomerates is relatively low in the first bubble but strongly increases during first bubble collapse and following rebound.”
- Also stated in: § 3.2 Spatiotemporal particle distribution in the cavitation bubble · plain
“The agglomerations are relatively weak in the first bubble but the mass increases strongly within the rebound.”
- Also stated in: § 4 Conclusions · plain
“the total mass of agglomerates is relatively weak in the first bubble but it increases strongly within the rebound.”
Quote in the paperSubstantial claim- Also stated in: § 3.2 Spatiotemporal particle distribution in the cavitation bubble · plain
May combine two claims.
Findingown dataAt the bubble apex (1 mm height), the particle mass at the first bubble is low, but a mass maximum is seen during the collapse phase of the first bubble.
“Here, as expected the particle mass at the first bubble is low, but a mass maximum is seen during the collapse phase of the first bubble.”
Quote in the paperSubstantial claimMay combine two claims. The quote only partly states this claim.
Findingown dataThe bubble recedes quickly after 150 μs, but then the collapse seems to stop, displaying a peak shoulder in the transmission diagram.
“A closer inspection reveals that the bubble recedes quickly after 150 ms, but then the collapse seems to stop, displaying a peak shoulder in the transmission diagram (Fig. 2).”
Quote in the paperNot a substantial claimMay combine two claims.
FindingcitationThe abundance of agglomerates in the first bubble close to the target is low and increases with height.
“As previously observed for gold, the abundance of agglomerates in the first bubble close to the target is low and increases with height.”
Quote in the paperSubstantial claimMay combine two claims.
Findingown dataPrimary particle mass is most abundant during maximal expansion of the first bubble and reappears a little weaker in the rebound.
“Primary particle mass is most abundant during maximal expansion of the first bubble and reappears a little weaker in the rebound.”
- Also stated in: § 3.2 Spatiotemporal particle distribution in the cavitation bubble · plain
“The primary particle mass is most abundant during maximal expansion of the first bubble and reappears during the rebound.”
- Also stated in: § 4 Conclusions · hedged
“during maximum elongation of the cavitation bubble, the primary particle mass goes through a maximum and reappears in the rebound, probably then contained in agglomerates.”
Quote in the paperSubstantial claim- Also stated in: § 3.2 Spatiotemporal particle distribution in the cavitation bubble · plain
May combine two claims.
Findingown dataMost of the ablated material is trapped inside the bubble and follows its oscillation, but a minor fraction of both species can be detected outside the cavitation bubble even before its final collapse.
“Although most of the ablated material is trapped inside the bubble and follows its oscillation, a minor fraction of both species could be detected outside the cavitation bubble even before its final collapse.”
- Also stated in: § 3.2 Spatiotemporal particle distribution in the cavitation bubble · plain
“Outside the bubble a very low mass of agglomerates is detected.”
- Also stated in: § 4 Conclusions · plain
“Although most of the ablated material is trapped inside the bubble and follows its oscillation, there is a certain fraction of primary particles and agglomerates which can be localized outside the bubble.”
Quote in the paperSubstantial claim- Also stated in: § 3.2 Spatiotemporal particle distribution in the cavitation bubble · plain
May combine two claims. The quote only partly states this claim.
Findingown dataThe laser-induced cavitation bubble expands to a maximum height of slightly more than 1 mm at about 80 μs, has a total duration of about 350 μs, and its rebound expands to about 0.7 mm at 220 μs.
“The rebound expands to about 0.7 mm at 220 ms.”
Quote in the paperNot a substantial claimMay combine two claims.
Findingnone givenMost of the detected particle mass is trapped inside the first bubble as primary particles with a small extent of agglomeration.
“Anyway, it is clear that most of the detected particle mass is trapped inside the first bubble as primary particles with a small extent of agglomeration.”
Quote in the paperSubstantial claimMay combine two claims.
Findingnone givenThe size of primary particles and agglomerates does not strongly depend on time and position; the average size of primary particles slightly decreases with higher distance to the target.
“The size of primary particles and agglomerates does not strongly depend on time and position, the average size of primary particles slightly decreases with higher distance to the target.”
Quote in the paperSubstantial claimMay combine two claims.
InterpretationreasoningThe collapse of the bubble retracts the ablated material towards the target, which leads to an increased rate of agglomeration.
“We conclude that the collapse of the bubble retracts the ablated material towards the target, which leads to an increased rate of agglomeration.”
Quote in the paperSubstantial claimMay combine two claims. The quote only partly states this claim.
InterpretationreasoningAn exponent of 4 is expected for compact particles, so the 8-10 nm particles are compact.
“An exponent of 4 is expected for compact particles.”
Quote in the paperSubstantial claimMay combine two claims.
InterpretationreasoningThe bubble collapse reconcentrates the particles, but also allows releasing a part through the receding bubble front.
“The bubble collapse reconcentrates the particles, but also allows releasing a part through the receding bubble front.”
Quote in the paperSubstantial claimMay combine two claims.
InterpretationreasoningIn the bubble rebound a strong agglomeration occurs, which can be released into the surrounding liquid upon complete collapse.
“In the bubble rebound a strong agglomeration occurs, which can be released into the surrounding liquid upon complete collapse.”
Quote in the paperSubstantial claimClassified as probably not a substantial claim.
InterpretationreasoningUnder the assumption that expansion of the bubble front is faster than particle drift velocity, the fastest and subsequent smallest particles accumulate in the upper part of the bubble after its formation.
“Under the assumption that expansion of the bubble front is faster than particle drift velocity, the fastest and subsequent smallest particles accumulate in the upper part of the bubble after its formation.”
Quote in the paperSubstantial claim- The authors state this as an assumption: The expansion of the bubble front is faster than the particle drift velocity.
The quote only partly states this claim.
Study design and conductreasoningThe experiment used a flow chamber to secure a stationary and reproducible process for sufficient time.
“Since pulsed laser ablation in a liquid batch chamber is not a stationary process but highly dynamic due to the changing concentration of nanoparticles, unequal flow conditions, progressing target ablation and post-irradiation of nanoparticles by subsequent pulses, 16 a stationary and reproducible process has to be secured for sufficient time.”
- Also stated in: § 2.1 Experimental set-up · plain
“A chamber, which is schematically depicted in Fig. 1 (left), has been built that allows for a continuous refreshing of the target and water column.”
Quote in the paperSubstantial claim0 of 1 sources checked- cites [16] 16. A. Schwenke, P. Wagener, S. Nolte and S. Barcikowski, Appl. Phys. A: Solid surf., 2011, 104, 77-82.
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
- Also stated in: § 2.1 Experimental set-up · plain
Probably not a substantial claim: may not pass S4 (based).
Premisenone givenFor compact particles, the scattering distribution I(q)q^2 for a hierarchy level shows a maximum at a characteristic q inversely proportional to the particle size.
“For compact particles the scattering distribution I(q)q 2 for a hierarchy level shows a maximum at a characteristic q which is inversely proportional to the particle size.”
Quote in the paperNot a substantial claimMay combine two claims.
Interpretationown dataAgglomerates stay inside the bubble with highest concentration close to the target surface and are released by the bubble only after its collapse.
“Agglomerates stay inside the bubble with highest concentration close to the target surface and are released by the bubble only after its collapse.”
Quote in the paperSubstantial claim
The authors state this as an assumption.
The expansion of the bubble front is faster than the particle drift velocity.
“Under the assumption that expansion of the bubble front is faster than particle drift velocity, the fastest and subsequent smallest particles accumulate in the upper part of the bubble after its formation.”
The authors state this as an assumption.
The scattering distribution originates from ablated nanoparticles of different size and agglomeration state.
“In our case, one can consider ablated nanoparticles of different size and agglomeration state that are the origin of the scattering distribution.”
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- Porod, 1952, Kolloidn. Zh., 125, 109
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- Authors
- Wagener, P., Ibrahimkutty, S., Menzel, A., Plech, A., & Barcikowski, S.
- Affiliations
- University of Duisburg-Essen (DE)
- Karlsruhe Institute of Technology (DE)
- Paul Scherrer Institute (CH)
- Corresponding author
- Plech, Anton
- Barcikowski, Stephan
- Venue
- Phys. Chem. Chem. Phys.
- Publisher
- Royal Society of Chemistry (RSC)
- Published
- 2013
- Volume
- 15
- Issue
- 9
- Pages
- 3068-3074
- ISSN
- 1463-9076 (ISSN-L)
- 1463-9084
- OpenAlex
- W2041579788
- Cited by
- 191
- References
- 41
- Citations by year
- 2026: 2 · 2025: 6 · 2024: 5 · 2023: 6 · 2022: 12 · 2021: 14 · 2020: 16 · 2019: 17 · 2018: 13 · 2017: 26 · 2016: 24 · 2015: 23 · 2014: 20 · 2013: 5 · 2012: 2
- FWCI
- 9.11
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Locations
- Physical Chemistry Chemical Physics (publishedVersion)
- PubMed (publishedVersion)
- DORA PSI (Paul Scherrer Institute) (submittedVersion, other-oa)
- Funders
- European Commission (226716)
- Deutsche Forschungsgemeinschaft
- Topics
- Physical Sciences › Engineering › Biomedical Engineering › Laser-Ablation Synthesis of Nanoparticles
- Physical Sciences › Materials Science › Materials Chemistry › Ultrasound and Cavitation Phenomena
- Physical Sciences › Materials Science › Electronic, Optical and Magnetic Materials › Gold and Silver Nanoparticles Synthesis and Applications
- Keywords
- silver nanoparticles, pulsed laser ablation in liquid, cavitation bubbles, nanoparticle agglomeration, bubble oscillation, bubble collapse, bubble rebound, in situ small-angle X-ray scattering
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