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 Title: Probing Thin Films And Monolayers On Gold With Large Amplitude Temperature Jumps Author(s): Sun, Yuxiao Contributor(s): Dlott, Dana; Berg, Christopher M. Subject(s): Analytical, Combustion, Plasma Abstract: A methodology to probe localized vibrational transitions of self-assembled monolayers (SAMs) adsorbed on gold films using vibrational sum-frequency generation (SFG) is described. The gold film is subjected to heating from a 400nm pump laser, exposing the adsorbed molecules to a temperature jump in the 30-175 $^\circ$ K range, calibrated using ultrafast reflectance measurements of the gold compared to steady state oven heating . SAMs of alkyl thiols as well as nitro functionalized aryl thiols were deposited and temperature jumped while be observed with SFG, monitoring the symmetric and asymmetric methyl vibrations as well as nitro vibrations. The amplitude, center, and width of the transitions were measured and provide information about delay and orientation of the molecules, as well as providing an indicator of the overall monolayer state. All transitions probed exhibited overshoot decay plateau patterns, attributed to a fast hot electron process directly exciting the probed transitions, followed by a slower bulk heating process causing monolayer disordering. This leads to a shift in the average angle of the terminal methyl, manifesting itself as a change in the amplitude of the vibration. These techniques will be applied to thin films of energetic materials to study reactions to temperature jumps. HMX is known to have a peak in sensitivity as $\delta$-HMX transitions to $\beta$-HMX at high temperatures, but fairly little information about the reason for this is known. This technique should be able to probe that process and provide data that can be used with computational models to gain some understanding of the process. Issue Date: 2014-06-16 Publisher: International Symposium on Molecular Spectroscopy Citation Info: Sun, Y.; Dlott, D.; Berg, C.M. PROBING THIN FILMS AND MONOLAYERS ON GOLD WITH LARGE AMPLITUDE TEMPERATURE JUMPS. Proceedings of the International Symposium on Molecular Spectroscopy, Urbana, IL, June 16-21, 2014. DOI: 10.15278/isms.2014.MJ08 Genre: CONFERENCE PAPER/PRESENTATION Type: Text Language: English URI: http://hdl.handle.net/2142/50938 DOI: https://doi.org/10.15278/isms.2014.MJ08 Rights Information: Copyright 2014 by the authors. Licensed under a Creative Commons Attribution 4.0 International License. http://creativecommons.org/licenses/by/4.0/ Date Available in IDEALS: 2014-09-172015-04-14
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