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Accelerating the development of transparent graphene electrodes through basic science driven chemical functionalization

Chan, Calvin; Beechem, Thomas E.; Ohta, Taisuke; Brumbach, Michael T.; Wheeler, David R.

Chemical functionalization is required to adapt graphenes properties to many applications. However, most covalent functionalization schemes are spontaneous or defect driven and are not suitable for applications requiring directed assembly of molecules on graphene substrates. In this work, we demonstrated electrochemically driven covalent bonding of phenyl iodoniums onto epitaxial graphene. The amount of chemisorption was demonstrated by varying the duration of the electrochemical driving potential. Chemical, electronic, and defect states of phenyl-modified graphene were studied by photoemission spectroscopy, spatially resolved Raman spectroscopy, and water contact angle measurement. Covalent attachment rehybridized some of the delocalized graphene sp2 orbitals to localized sp3 states. Control over the relative spontaneity (reaction rate) of covalent graphene functionalization is an important first step to the practical realization of directed molecular assembly on graphene. More than 10 publications, conference presentations, and program highlights were produced (some invited), and follow-on funding was obtained to continue this work.

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TYPE SAND Report YEAR 2013
DOIOSTI

Band offsets of La2O3 on (0001) GaN grown by reactive molecular-beam epitaxy

Applied Physics Letters

Ihlefeld, Jon F.; Brumbach, Michael T.; Atcitty, Stanley

La2O3 films were prepared on (0001)-oriented GaN substrates via reactive molecular-beam epitaxy. Film orientation and phase were assessed using reflection high-energy electron and X-ray diffraction. Films were observed to grow as predominantly hexagonal La2O3 for thicknesses less than 10 nm while film thickness greater than 10 nm favored mixed cubic and hexagonal symmetries. Band offsets were characterized by X-ray photoelectron spectroscopy on hexagonally symmetric films and valence band offsets of 0.63 ± 0.04 eV at the La2O3/GaN interface were measured. A conduction band offset of approximately 1.5 eV could be inferred from the measured valence band offset. © 2013 AIP Publishing LLC.

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TYPE Journal Article YEAR 2013
DOIOSTIScopus

Photoelectronic Characterization of Heterointerfaces

Brumbach, Michael T.

In many devices such as solar cells, light emitting diodes, transistors, etc., the performance relies on the electronic structure at interfaces between materials within the device. The objective of this work was to perform robust characterization of hybrid (organic/inorganic) interfaces by tailoring the interfacial region for photoelectron spectroscopy. Self-assembled monolayers (SAM) were utilized to induce dipoles of various magnitudes at the interface. Additionally, SAMs of molecules with varying dipolar characteristics were mixed into spatially organized structures to systematically vary the apparent work function. Polymer thin films were characterized by depositing films of varying thicknesses on numerous substrates with and without interfacial modifications. Hard X-ray photoelectron spectroscopy (HAXPES) was performed to evaluate a buried interface between indium tin oxide (ITO), treated under various conditions, and poly(3-hexylthiophene) (P3HT). Conducting polymer films were found to be sufficiently conducting such that no significant charge redistribution in the polymer films was observed. Consequently, a further departure from uniform substrates was taken whereby electrically disconnected regions of the substrate presented ideally insulating interfacial contacts. In order to accomplish this novel strategy, interdigitated electrodes were used as the substrate. Conducting fingers of one half of the electrodes were electrically grounded while the other set of electrodes were electronically floating. This allowed for the evaluation of substrate charging on photoelectron spectra (SCOPES) in the presence of overlying semiconducting thin films. Such an experiment has never before been reported. This concept was developed out of the previous experiments on interfacial modification and thin film depositions and presents new opportunities for understanding chemical and electronic changes in a multitude of materials and interfaces.

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TYPE SAND Report YEAR 2012
DOIOSTI

Activation of erbium films for hydrogen storage

Journal of Applied Physics

Brumbach, Michael T.; Ohlhausen, J.A.; Zavadil, Kevin R.; Snow, Clark S.

Hydriding of metals can be routinely performed at high temperature in a rich hydrogen atmosphere. Prior to the hydrogen loading process, a thermal activation procedure is required to promote facile hydrogen sorption into the metal. Despite the wide spread utilization of this activation procedure, little is known about the chemical and electronic changes that occur during activation and how this thermal pretreatment leads to increased rates of hydrogen uptake. This study utilized variable kinetic energy X-ray photoelectron spectroscopy to interrogate the changes during in situ thermal annealing of erbium films, with results confirmed by time-of-flight secondary ion mass spectrometry and low energy ion scattering. Activation can be identified by a large increase in photoemission between the valence band edge and the Fermi level and appears to occur over a two stage process. The first stage involves desorption of contaminants and recrystallization of the oxide, initially impeding hydrogen loading. Further heating overcomes the first stage and leads to degradation of the passive surface oxide leading to a bulk film more accessible for hydrogen loading. © 2011 American Institute of Physics.

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TYPE Conference YEAR 2011
DOIOSTIScopus
Results 101–150 of 170
Results 101–150 of 170