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1 Ultrafast Dynamics of NEEMs Focus on accomplishments and problems Ultrafast t flash-heating h experiments Ultrafast heating of self-assembled monolayers Emission from flash-heated Al/Teflon Infrared probing of flash-heated Al/Teflon Summary and future work Collaborators Dr. Mikhail Zamkov (Center for Photochemical sciences, Bowling Green State University) Rusty Conner (UIUC)
2 Dynamics of a NEEM fuel passivation 100 nm oxidizer 3 (or more) part structure activation initiation ignition nascent propagation steady propagation
3 fuel passivation oxidizer 100 nm flash- time- time heating resolved -resolved SFG IR emission structure initiation ignition activation time -resolved emission transient propagation steady propagation
4 Pulsed thermal desorption of SAM passivation layers Al, Au Activation SFG is the only technique that can probe monolayers with picosecond time resolution glass 100 fs laser heating pulse SFG IR vis SFG probe (1 ps) nonlinear coherent heat to melting point in <5 picoseconds
5 SFG spectra of SAM on Al CH 3 -(CH 2 ) 17 -SH on gold CH 3 -(CH 2 ) 16 -CO 2 H on Al with oxide arb) SFG Signal ( ν s CH 2 ν s CH 3 ν FR ν as CH 3 nonresonant nonresonant background from metal SFG wavenumber (cm -1 )
6 Nonresonant suppression with time-asymmetric pulses ambient flash-heated h 20 ps ambient flash-heated 20 ps wavenumber (cm -1 ) wavenumber (cm -1 )
7 Summary of flash-heating heating of SAMs Ordinarily SAMs desorb at C Flash-heating heating to melting point C for 10 nanoseconds produced no SAM desorption Extraordinary stability of SAMs to pulsed heating Opens up a new field of research in molecular dynamics Z W J A C t A L t h Y K K h N H S Z. Wang, J. A. Carter, A. Lagutchev, Y. K. Koh, N.-H. Seong, D. G. Cahill, and D. D. Dlott, Ultrafast flash thermal conductance of molecular chains, Science 317, (2007).
8 Time-resolved emission (kinetics of energy release) attenuator near-ir flash-heating translator XY streak camera spectrograph delay sample array SPS optically thin CD YLF QS ML Nd:YLF 100 ps laser to vacuum
9 Time resolved images of Al + Teflon AF flash heated by 100 ns pulses 0 ns 50 ns 100 ns 150 ns 200 ns 300 ns 670 μm 400 ns 500 ns
10 Ultrafast emission apparatus
11 Energy release via time-resolved emission (arb) in ntensity Al atoms AlO 1% in NC 5.6 J/cm J/cm 2 18J/cm J/cm 2 2ns 1% in NC 5.6 J/cm J/cm 2 18J/cm J/cm 2 several ns wavelength (nm) time (ns) Alex in nitrocellulose flash-heated with 100 ps pulses 2003 data
12 Al (30 nm) in Teflon AF 15% laser b) inte ensity (ar Al 2 J/cm 2 2 J/cm 2 time (ns) wavelength (nm) rb) int tensity (a tensity (a arb) in time (ns) 4 J/cm 2 2 J/cm J/cm J/cm time (ns)
13 Commercial vs. engineered Al nanoparticles Novacentrix 50 nm diameter with 2 nm diameter oxide Jason Jouet NSWC Al with perfluoro SAM CF 3 -(CF 2 2) 13 -COOH passivation
14 Laser ablation data from NSWC R. J. Jouet, J. R. Carney, R. H. Granholm, H. W. Sandusky, and A. D. WArren, Preparation and reactivity analysis of novel perfluoroalkyl coated aluminium nanocomposites Mat. Sci. Tech. 22, (2006). 4 μs 6 μs Al + Al 8 μs Time (microseconds)
15 Commercial vs. engineered Al nanoparticles ntensity (arb) Novacentrix Jason Jouet NSWC 50 nm diameter with Al with CF 3 -(CF 2 ) 13 -COOH 2nmdiameteroxide passivation 15% in Teflon AF ignition laser laser fluence 2 J/cm 2 2 J/cm 2 (arb) i intensity time (ns) time (ns) 2.0
16 Femtosecond two-beam IR spectrometer
17 Flash-heating heating of NEEMs reacted material CaF 2 CaF 2 100μm 100 fs IR probe pulse spectrograph MCT IR array Al nanoparticles + Teflon AF Teflon AF + 18 wgt % Al (30 nm) 50% of the needed Al Mot torized tran nslation Al 30 nm Al 2 O 3 (2 nm)
18 IR spectra of Teflon and Teflon AF abso orbance 3 Teflon AF 2 Teflon AF + 18%Al CF PTFE no flash heating post flash heating CF 2 (s) CF 2 + CFO CF 2 (a) (a) (b) (c) F F F F F O F F O F dioxole F F F F TFE wavenumber (cm -1 )
19 Transient IR spectra after flash-heatingheating (a) absorb bance (b) -0.1 ns 02ns ns wavenumber (cm -1 )
20 Time-dependence fractio on Teflo n AF su urvival cm CF 3 only 1147 cm cm CFO 0.7 ns ps delay (ns) 16 20
21 Summary and future work Accomplishments First direct probe of passivation layer dynamics: surprising stability to transient high temperatures First direct probe of chemical reaction initiation inside a reacting energetic material Meaningful measurements of energy release of NEEMs Future work It has been difficult to see systematic effects of NEEM structures on dynamical behavior Rusty has emission apparatus functioning beautifully Detailed investigations of energy release of different NEEMs Improve IR absorption techniques Simultaneous IR absorption and emission measurements
22 Dlott NEEM Quad Chart Objective: To understand the fundamental mechanisms of energetic materials containing nanoparticles, and the relationships between nanostructure and performance, using experimental measurements with high time and space resolution. (left) block diagram of flash-heating heating laser with two- channel IR detection. (right) IR spectra of a nanoenergetic material 16% Al (30 nm) with Teflon AF after flash-heating with a 0.1 ns pulse. Chemical reaction dynamics of nanoenergetics via ultrafast IR and emission spectroscopies Dynamics of monolayer coatings on metal nanoparticles via ultrafast vibrational spectroscopy Major Accomplishments: Real-time vibrational spectroscopy of flash-heated nanoenergetic material Real-time measurement of emission of flashheated nanoenergetic material Ultrafast dynamics of self-assembled monolayers on metal surfaces with flash-heating, studied by nonlinear coherent vibrational spectroscopy Personnel: Dana Dlott PI, Mikhail Zamkov, Postdoc, Rusty Conner Graduate student Army Relevance: This work seeks to understand the fundamental mechanisms of the new generation of nanoenergetic materials and to learn how to design and control the nanostructure to optimize advanced munitions for chosen applications. Funding profile: FY06 $125K, FY07 $125K, FY08 $125K Grant # subcontract of W911NF PI Dana D. Dlott, School of Chemical Sciences and Fredrick Seitz Materials Research Laboratory, University of Illinois at Urbana Champaign. ph: , dlott@scs.uiuc.edu
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