?url_ver=Z39.88-2004&rft_val_fmt=info%3Aofi%2Ffmt%3Akev%3Amtx%3Adc&rft.relation=http%3A%2F%2Fd-scholarship-dev.library.pitt.edu%2F7210%2F&rft.title=Electron+and+Molecular+Dynamics%3A+Penning+Ionization+and+Molecular+Charge+Transfer&rft.creator=Madison%2C+Tamika+Arlene&rft.description=An+understanding+of+fundamental+reaction+dynamics+is+an+important+problem+in+chemistry.+In+this+work%2C+experimental+and+theoretical+methods+are+combined+to+study+the+dynamics+of+fundamental+chemical+reactions.+Molecular+collision+and+dissociation+dynamics+are+explored+with+the+Penning+ionization+of+amides%2C+while+charge+transfer+reactions+are+examined+with+charge+transport+in+organic+thin+film+devices.Mass+spectra+from+the+Penning+ionization+of+formamide+by+He*%2C+Ne*%2C+and+Ar*+were+measured+using+molecular+beam+experiments.+When+compared+to+70eV+electron+ionization+spectra%2C+the+He*+and+Ne*+spectra+show+higher+yields+of+fragments+resulting+from+C!N+and+C!H+bond+cleavage%2C+while+the+Ar*+spectrum+only+shows+the+molecular+ion%2C+H-atom+elimination%2C+and+decarbonylation.+The+differences+in+yields+and+observed+fragments+are+attributed+to+the+differences+in+the+dynamics+of+the+two+ionization+methods.+Fragmentation+in+the+Ar*+spectrum+was+analyzed+using+quantum+chemistry+and+RRKM+calculations.+Calculated+yields+for+the+Ar*+spectrum+are+in+excellent+agreement+with+experiment+and+show+that+15%25+and+50%25+of+the+yields+for+decarbonylation+and+H-atom+elimination+respectively+are+attributed+to+tunnelingThe+effects+of+defects%2C+traps%2C+and+electrostatic+interactions+on+charge+transport+in+imperfect+organic+field+effect+transistors+were+studied+using+course-grained+Monte+Carlo+simulations+with+explicit+introduction+of+defect+and+traps.+The+simulations+show+that+electrostatic+interactions+dramatically+affect+the+field+and+carrier+concentration+dependence+of+charge+transport+in+the+presence+of+a+significant+number+of+defects.+The+simulations+also+show+that+while+charge+transport+decreases+linearly+as+a+function+of+neutral+defect+concentration%2C+it+is+roughly+unaffected+by+charged+defect+concentration.+In+addition%2C+the+trap+concentration+dependence+on+charge+transport+is+shown+to+be+sensitive+to+the+distribution+of+trap+sites.Finally%2C+density+functional+theory+calculations+were+used+to+study+how+charge+localization+affects+the+orbital+energies+of+positively+charged+bithiophene+clusters.+These+calculations+show+that+the+charge+delocalizes+over+at+least+seven+molecules%2C+is+more+likely+to+localize+on+%22tilted%22+molecules+due+to+polarization+effects%2C+and+affects+molecules+anisotropically.+These+results+suggest+that+models+for+charge+transport+in+organic+semiconductors+should+be+modified+to+account+for+charge+delocalization+and+intermolecular+interactions.&rft.date=2011-06-30&rft.type=University+of+Pittsburgh+ETD&rft.type=PeerReviewed&rft.format=application%2Fpdf&rft.language=en&rft.identifier=http%3A%2F%2Fd-scholarship-dev.library.pitt.edu%2F7210%2F1%2Fdissertation_tamadison_04252011.pdf&rft.identifier=++Madison%2C+Tamika+Arlene++(2011)+Electron+and+Molecular+Dynamics%3A+Penning+Ionization+and+Molecular+Charge+Transfer.++Doctoral+Dissertation%2C+University+of+Pittsburgh.++++(Unpublished)++