Experimental and computational investigation into the hydrodynamics and chemical dynamics of laser ablation aluminum plasmas

Kwapis, Emily H.; Posey, Jacob W.; Medici, Enrique; Berg, Kira; Houim, Ryan W.; Hartig, Kyle C.

doi:10.1039/d3cp01586f

Experimental and computational investigation into the hydrodynamics and chemical dynamics of laser ablation aluminum plasmas

Journal Article · Wed May 31 00:00:00 EDT 2023 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/d3cp01586f· OSTI ID:2417916

^[1]; ^[2]; Medici, Enrique ^[2]; Berg, Kira ^[2]; Houim, Ryan W. ^[2]; Hartig, Kyle C. ^[2]

Univ. of Florida, Gainesville, FL (United States); OSTI
Univ. of Florida, Gainesville, FL (United States)

Laser ablation plasma chemistry is governed by a complex interplay between hydrodynamic plasma-gas mixing processes, thermodynamics, and rapid high-temperature chemical reactions. Here, in this work, we investigate the gas-phase oxidation chemistry of ns-laser ablation aluminum plasmas in air using optical spectroscopy combined with advanced multi-physics modeling. Experimental measurements demonstrate the formation of AlO in the plasma plume as early as 1 μs while computational results reveal that several Al_xO_y species are distributed in the periphery of the plume at even earlier times (<20 ns) in the presence of large temperature gradients and strong shockwaves. Interactions with the ablation crater during rapid plume expansion are shown to initiate vortex formation, followed by mixing dynamics that work to pull AlO into the vortices to react with gas-phase Al to form Al₂O. Oxygen and several aluminum oxides are simultaneously pulled up through the stem of the fireball, encouraging further intermixing between reacting species and enhanced molecular formation. This work concludes that chemical dynamics in laser ablation plasmas is driven by diffusion processes, concentration gradients, and plume hydrodynamics while strong shockwaves generated during laser ablation do not impede chemical reactions.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Michigan, Ann Arbor, MI (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); Defense Threat Reduction Agency (DTRA); National Science Foundation (NSF)

Grant/Contract Number:: NA0003920

OSTI ID:: 2417916

Alternate ID(s):: OSTI ID: 1975878

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 23 Vol. 25; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (71)

Effects of pulsed laser and plasma interaction on Fe, Ni, Ti, and their oxides for LIBS Raman analysis in extraterrestrial environments Schröder, Susanne; Rammelkamp, Kristin; Hanke, Franziska Journal of Raman Spectroscopy, Vol. 51, Issue 9 https://doi.org/10.1002/jrs.5650	journal	July 2019
Nonideal thermoequilibrium calculations using a large product species data base Hobbs, M. L.; Baer, M. R. Shock Waves, Vol. 2, Issue 3 https://doi.org/10.1007/BF01414640	journal	September 1992
Analysis of mixing in high-explosive fireballs using small-scale pressurised spheres Courtiaud, S.; Lecysyn, N.; Damamme, G. Shock Waves, Vol. 29, Issue 2 https://doi.org/10.1007/s00193-018-0814-4	journal	February 2018
A simplified burn model for simulating explosive effects and afterburning Houim, R. W. Shock Waves, Vol. 31, Issue 8 https://doi.org/10.1007/s00193-021-01054-2	journal	November 2021
Numerical study of the expansion of metallic vapor plasma by a nanosecond laser pulse Aggoune, S.; Vidal, F.; Amara, E. H. Applied Physics A, Vol. 101, Issue 1 https://doi.org/10.1007/s00339-010-5783-0	journal	June 2010
Modeling chemical reactions in laser-induced plasmas Shabanov, S. V.; Gornushkin, I. B. Applied Physics A, Vol. 121, Issue 3 https://doi.org/10.1007/s00339-015-9445-0	journal	September 2015
Effect of sample morphology on the spectral and spatiotemporal characteristics of laser-induced plasmas from aluminum Wainwright, Elliot R.; Dean, Steven W.; De Lucia, Frank C. Applied Physics A, Vol. 126, Issue 2 https://doi.org/10.1007/s00339-019-3201-9	journal	January 2020
Spherical expansion of the vapor plume into ambient gas: an analytical model Arnold, N.; Gruber, J.; Heitz, J. Applied Physics A: Materials Science & Processing, Vol. 69, Issue 7 https://doi.org/10.1007/s003390051360	journal	December 1999
Absolute band strengths for the AlO blue-green (B2σ−X2σ) band system Hébert, G. R.; Nicholls, R. W.; Linton, C. Journal of Quantitative Spectroscopy and Radiative Transfer, Vol. 23, Issue 2 https://doi.org/10.1016/0022-4073(80)90010-2	journal	February 1980
Quantitative laser-induced breakdown spectroscopy analysis of calcified tissue samples Samek, O.; Beddows, D. C. S.; Telle, H. H. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 56, Issue 6 https://doi.org/10.1016/S0584-8547(01)00198-7	journal	June 2001
Laser-induced breakdown spectroscopy for quantitative spectrochemical analysis of geological materials: Effects of the matrix and simultaneous determination Anzano, Jesús M.; Villoria, Mark A.; Ruíz-Medina, Antonio Analytica Chimica Acta, Vol. 575, Issue 2 https://doi.org/10.1016/j.aca.2006.05.077	journal	August 2006
Elemental imaging using laser-induced breakdown spectroscopy: A new and promising approach for biological and medical applications Busser, Benoit; Moncayo, Samuel; Coll, Jean-Luc Coordination Chemistry Reviews, Vol. 358 https://doi.org/10.1016/j.ccr.2017.12.006	journal	March 2018
Numerical analysis of nanoaluminum combustion in steam Starik, Alexander M.; Kuleshov, Pavel S.; Sharipov, Alexander S. Combustion and Flame, Vol. 161, Issue 6 https://doi.org/10.1016/j.combustflame.2013.12.007	journal	June 2014
A low-dissipation and time-accurate method for compressible multi-component flow with variable specific heat ratios Houim, Ryan W.; Kuo, Kenneth K. Journal of Computational Physics, Vol. 230, Issue 23 https://doi.org/10.1016/j.jcp.2011.07.031	journal	September 2011
Influence of thermal radiation on layered dust explosions Guhathakurta, Swagnik; Houim, Ryan W. Journal of Loss Prevention in the Process Industries, Vol. 72 https://doi.org/10.1016/j.jlp.2021.104509	journal	September 2021
Fourier transform spectral study of B2Σ+–X2Σ+ system of AlO Saksena, M. D.; Deo, M. N.; Sunanda, K. Journal of Molecular Spectroscopy, Vol. 247, Issue 1 https://doi.org/10.1016/j.jms.2007.10.002	journal	January 2008
Spectroscopy of AlO: Combined analysis of the A2Πi→X2Σ+ and B2Σ+→X2Σ+ transitions Launila, O.; Berg, L. -E. Journal of Molecular Spectroscopy, Vol. 265, Issue 1 https://doi.org/10.1016/j.jms.2010.10.005	journal	January 2011
Modeling of nonequilibrium CO Fourth-Positive and CN Violet emission in CO 2 –N 2 gases Johnston, C. O.; Brandis, A. M. Journal of Quantitative Spectroscopy and Radiative Transfer, Vol. 149 https://doi.org/10.1016/j.jqsrt.2014.08.025	journal	December 2014
PGOPHER: A program for simulating rotational, vibrational and electronic spectra Western, Colin M. Journal of Quantitative Spectroscopy and Radiative Transfer, Vol. 186 https://doi.org/10.1016/j.jqsrt.2016.04.010	journal	January 2017
Detonation initiation from shock and material interface interactions in hydrogen-air mixtures Houim, Ryan W.; Taylor, Brian D. Proceedings of the Combustion Institute, Vol. 37, Issue 3 https://doi.org/10.1016/j.proci.2018.06.037	journal	January 2019
Laser-induced plasma expansion: theoretical and experimental aspects Capitelli, M.; Casavola, A.; Colonna, G. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 59, Issue 3 https://doi.org/10.1016/j.sab.2003.12.017	journal	March 2004
Recognition of archeological materials underwater by laser induced breakdown spectroscopy Lazic, V.; Colao, F.; Fantoni, R. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 60, Issue 7-8 https://doi.org/10.1016/j.sab.2005.06.014	journal	August 2005
Evaluation of self-absorption coefficients of aluminum emission lines in laser-induced breakdown spectroscopy measurements El Sherbini, A. M.; El Sherbini, Th. M.; Hegazy, H. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 60, Issue 12 https://doi.org/10.1016/j.sab.2005.10.011	journal	December 2005
Forensic comparative glass analysis by laser-induced breakdown spectroscopy Bridge, Candice M.; Powell, Joseph; Steele, Katie L. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 62, Issue 12 https://doi.org/10.1016/j.sab.2007.10.015	journal	December 2007
High resolution applications of laser-induced breakdown spectroscopy for environmental and forensic applications Martin, Madhavi Z.; Labbé, Nicole; André, Nicolas Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 62, Issue 12 https://doi.org/10.1016/j.sab.2007.10.046	journal	December 2007
Two-dimensional axisymmetric models of laser induced plasmas relevant to laser induced breakdown spectroscopy Shabanov, S. V.; Gornushkin, I. B. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 100 https://doi.org/10.1016/j.sab.2014.08.026	journal	October 2014
Impact of oxygen chemistry on the emission and fluorescence spectroscopy of laser ablation plumes Hartig, K. C.; Brumfield, B. E.; Phillips, M. C. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 135 https://doi.org/10.1016/j.sab.2017.07.002	journal	September 2017
Advances in Laser-Induced Breakdown Spectroscopy analysis for geology: A critical review Fabre, Cécile Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 166 https://doi.org/10.1016/j.sab.2020.105799	journal	April 2020
Time-resolved formation of uranium and silicon oxides subsequent to the laser ablation of U3Si2 Weerakkody, Emily N.; Weisz, David G.; Crowhurst, Jonathan Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 170 https://doi.org/10.1016/j.sab.2020.105925	journal	August 2020
Analytical characterization of laser induced plasmas towards uranium isotopic analysis in gaseous uranium hexafluoride Chan, George C. -Y.; Martin, Leigh R.; Trowbridge, Lee D. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 176 https://doi.org/10.1016/j.sab.2020.106036	journal	February 2021
Laser ablation spectrometry for studies of uranium plasmas, reactor monitoring, and spent fuel safety Burger, M.; Finney, L. A.; Garrett, L. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 179 https://doi.org/10.1016/j.sab.2021.106095	journal	May 2021
Influence of silicon particle morphology on laser-induced plasma properties Wainwright, Elliot R.; Miller, Clayton J.; Giri, Lily Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 199 https://doi.org/10.1016/j.sab.2022.106597	journal	January 2023
Spectroscopic signatures and oxidation characteristics of nanosecond laser-induced cerium plasmas Kwapis, Emily H.; Villa-Aleman, Eliel; Hartig, Kyle C. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 200 https://doi.org/10.1016/j.sab.2022.106610	journal	February 2023
Photoemission of surface oxides and hydrides of delta plutonium Butterfield, M. T.; Durakiewicz, T.; Guziewicz, E. Surface Science, Vol. 571, Issue 1-3 https://doi.org/10.1016/j.susc.2004.07.054	journal	November 2004
A multiphase model for compressible granular–gaseous flows: formulation and initial tests Houim, Ryan W.; Oran, Elaine S. Journal of Fluid Mechanics, Vol. 789 https://doi.org/10.1017/jfm.2015.728	journal	January 2016
Shock Wave Mediated Plume Chemistry for Molecular Formation in Laser Ablation Plasmas Harilal, Sivanandan S.; Brumfield, Brian E.; Cannon, Bret D. Analytical Chemistry, Vol. 88, Issue 4 https://doi.org/10.1021/acs.analchem.5b04136	journal	January 2016
Effects of Plume Hydrodynamics and Oxidation on the Composition of a Condensing Laser-Induced Plasma Weisz, David G.; Crowhurst, Jonathan C.; Finko, Mikhail S. The Journal of Physical Chemistry A, Vol. 122, Issue 6 https://doi.org/10.1021/acs.jpca.7b11994	journal	February 2018
The effect of oxygen concentration on the speciation of laser ablated uranium Burton, Mark A.; Auner, Alex W.; Crowhurst, Jonathan C. Scientific Reports, Vol. 12, Issue 1 https://doi.org/10.1038/s41598-022-07834-9	journal	March 2022
Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry Hartig, Kyle C.; Ghebregziabher, Isaac; Jovanovic, Igor Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/srep43852	journal	March 2017
Influence of exothermic chemical reactions on laser-induced shock waves Gottfried, Jennifer L. Phys. Chem. Chem. Phys., Vol. 16, Issue 39 https://doi.org/10.1039/C4CP02903H	journal	January 2014
Applications of laser-induced breakdown spectroscopy in cultural heritage and archaeology: a critical review Botto, Asia; Campanella, Beatrice; Legnaioli, Stefano Journal of Analytical Atomic Spectrometry, Vol. 34, Issue 1 https://doi.org/10.1039/C8JA00319J	journal	January 2019
Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas Kautz, E. J.; Skrodzki, P. J.; Burger, M. Journal of Analytical Atomic Spectrometry, Vol. 34, Issue 11 https://doi.org/10.1039/C9JA00228F	journal	January 2019
Quantitative molecular analysis with molecular bands emission using laser-induced breakdown spectroscopy and chemometrics Doucet, François R.; Faustino, Patrick J.; Sabsabi, Mohamad Journal of Analytical Atomic Spectrometry, Vol. 23, Issue 5 https://doi.org/10.1039/b714219f	journal	January 2008
Semi-quantitative analysis of metal alloys, brass and soil samples by calibration-free laser-induced breakdown spectroscopy: recent results and considerations Herrera, Kathleen K.; Tognoni, Elisabetta; Omenetto, Nicoló Journal of Analytical Atomic Spectrometry, Vol. 24, Issue 4 https://doi.org/10.1039/b820493d	journal	January 2009
Laser plasma spectrochemistry Russo, Richard E.; Suen, Timothy W.; Bol'shakov, Alexander A. Journal of Analytical Atomic Spectrometry, Vol. 26, Issue 8 https://doi.org/10.1039/c1ja10107b	journal	January 2011
Expansion of the laser ablation vapor plume into a background gas. I. Analysis Wen, Sy-Bor; Mao, Xianglei; Greif, Ralph Journal of Applied Physics, Vol. 101, Issue 2 https://doi.org/10.1063/1.2431080	journal	January 2007
Laser ablation characteristics of yttria-doped zirconia in the nanosecond and femtosecond regimes Heiroth, S.; Koch, J.; Lippert, T. Journal of Applied Physics, Vol. 107, Issue 1 https://doi.org/10.1063/1.3275868	journal	January 2010
Experimental and computational study of complex shockwave dynamics in laser ablation plumes in argon atmosphere Harilal, S. S.; Miloshevsky, G. V.; Diwakar, P. K. Physics of Plasmas, Vol. 19, Issue 8 https://doi.org/10.1063/1.4745867	journal	August 2012
Characterization of laser-induced plasmas as a complement to high-explosive large-scale detonations Kimblin, Clare; Trainham, Rusty; Capelle, Gene A. AIP Advances, Vol. 7, Issue 9 https://doi.org/10.1063/1.4999793	journal	September 2017
Optical spectroscopy of laser-produced plasmas for standoff isotopic analysis Harilal, S. S.; Brumfield, B. E.; LaHaye, N. L. Applied Physics Reviews, Vol. 5, Issue 2 https://doi.org/10.1063/1.5016053	journal	June 2018
Plume dynamics and gas-phase molecular formation in transient laser-produced uranium plasmas Skrodzki, P. J.; Burger, M.; Jovanovic, I. Physics of Plasmas, Vol. 26, Issue 8 https://doi.org/10.1063/1.5087704	journal	August 2019
Thermodynamic Properties of Key Organic Oxygen Compounds in the Carbon Range C ₁ to C ₄ . Part 1. Properties of Condensed Phases Wilhoit, Randolph C.; Chao, Jing; Hall, Kenneth R. Journal of Physical and Chemical Reference Data, Vol. 14, Issue 1 https://doi.org/10.1063/1.555747	journal	January 1985
Mechanisms of prompt and delayed ignition and combustion of explosively dispersed aluminum powder Posey, Jacob W.; Roque, Brayden; Guhathakurta, Swagnik Physics of Fluids, Vol. 33, Issue 11 https://doi.org/10.1063/5.0065312	journal	November 2021
Oxidation in laser-generated metal plumes Kautz, Elizabeth J.; Phillips, Mark C.; Zelenyuk, Alla Physics of Plasmas, Vol. 29, Issue 5 https://doi.org/10.1063/5.0090155	journal	May 2022
The role of spontaneous waves in the deflagration-to-detonation transition in submillimetre channels Houim, Ryan W.; Ozgen, Alp; Oran, Elaine S. Combustion Theory and Modelling, Vol. 20, Issue 6 https://doi.org/10.1080/13647830.2016.1249523	journal	November 2016
Time-resolved observation of gas-dynamic discontinuities arising during excimer laser ablation and their interpretation Callies, G.; Berger, P.; Hugel, H. Journal of Physics D: Applied Physics, Vol. 28, Issue 4 https://doi.org/10.1088/0022-3727/28/4/026	journal	April 1995
Laser-induced plasma emission: from atomic to molecular spectra De Giacomo, Alessandro; Hermann, Jörg Journal of Physics D: Applied Physics, Vol. 50, Issue 18 https://doi.org/10.1088/1361-6463/aa6585	journal	April 2017
Laser-generated plasma plume expansion: Combined continuous-microscopic modeling Itina, Tatiana E.; Hermann, Jörg; Delaporte, Philippe Physical Review E, Vol. 66, Issue 6 https://doi.org/10.1103/PhysRevE.66.066406	journal	December 2002
Simulation of emission spectra from nonuniform reactive laser-induced plasmas Hermann, Jörg; Lorusso, Antonella; Perrone, Alessio Physical Review E, Vol. 92, Issue 5 https://doi.org/10.1103/PhysRevE.92.053103	journal	November 2015
Synthesis of Novel Thin-Film Materials by Pulsed Laser Deposition Lowndes, D. H.; Geohegan, D. B.; Puretzky, A. A. Science, Vol. 273, Issue 5277, p. 898-903 https://doi.org/10.1126/science.273.5277.898	journal	August 1996
Shock Waves and Radiation Zel'dovich, Y. B.; Raizer, Y. P. Annual Review of Fluid Mechanics, Vol. 1, Issue 1 https://doi.org/10.1146/annurev.fl.01.010169.002125	journal	January 1969
Evolution of uranium monoxide in femtosecond laser-induced uranium plasmas Hartig, Kyle C.; Harilal, Sivanandan S.; Phillips, Mark C. Optics Express, Vol. 25, Issue 10 https://doi.org/10.1364/OE.25.011477	journal	January 2017
Determination of detonation characteristics by laser-induced plasma spectra and micro-explosion dynamics Wang, Xianshuang; Liu, Ruibin; He, Yage Optics Express, Vol. 30, Issue 4 https://doi.org/10.1364/OE.449382	journal	January 2022
Investigation of multi-timescale processing phenomena in femtosecond laser drilling of zirconia ceramics Zhang, Yanming; Ito, Yusuke; Sun, Huijie Optics Express, Vol. 30, Issue 21 https://doi.org/10.1364/OE.474090	journal	September 2022
Shock physics and shadowgraphic measurements of laser-produced cerium plasmas Kwapis, Emily H.; Hewitt, Maya; Hartig, Kyle C. Optics Express, Vol. 31, Issue 6 https://doi.org/10.1364/OE.483055	journal	March 2023
Zapping Mars: Using Lasers to Determine the Chemistry of the Red Planet Melikechi, Noureddine; Wiens, Roger; Newsom, Horton Optics and Photonics News, Vol. 24, Issue 1 https://doi.org/10.1364/OPN.24.1.000026	journal	January 2013
Aluminum Monoxide Emission Measurements in a Laser-Induced Plasma Surmick, David M.; Parigger, Christian G. Applied Spectroscopy, Vol. 68, Issue 9 https://doi.org/10.1366/13-07379	journal	September 2014
Planetary Geochemical Investigations Using Raman and Laser-Induced Breakdown Spectroscopy Clegg, Samuel M.; Wiens, Roger; Misra, Anupam K. Applied Spectroscopy, Vol. 68, Issue 9 https://doi.org/10.1366/13-07386	journal	September 2014
Standoff Chemical Detection Using Laser Absorption Spectroscopy: A Review Li, Jinyi; Yu, Ziwei; Du, Zhenhui Remote Sensing, Vol. 12, Issue 17 https://doi.org/10.3390/rs12172771	journal	August 2020
The Stark Effect, Zeeman Effect, and Transition Dipole Moments for the B ²Σ⁺−X ²Σ⁺ Band of Aluminum Monoxide, AlO Bai, Xilin; Steimle, Timothy C. The Astrophysical Journal, Vol. 889, Issue 2 https://doi.org/10.3847/1538-4357/ab6327	journal	February 2020
Predicting propagation limits of laser-supported detonation by Hugoniot analysis Shimamura, Kohei; Ofosu, Joseph A.; Komurasaki, Kimiya Japanese Journal of Applied Physics, Vol. 54, Issue 1 https://doi.org/10.7567/JJAP.54.016201	journal	December 2014

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