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1.
Nano Lett ; 24(17): 5174-5181, 2024 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-38587459

RESUMEN

Characteristic properties of secondary electrons emitted from irradiated two-dimensional materials arise from multi-length and multi-time-scale relaxation processes that connect the initial nonequilibrium excited electron distribution with their eventual emission. To understand these processes, which are critical for using secondary electrons as high-resolution thermalization probes, we combine first-principles real-time electron dynamics with irradiation experiments. Our data for cold and hot proton-irradiated graphene show signatures of kinetic and potential emission and generally good agreement for electron yields between experiment and theory. The duration of the emission pulse is about 1.5 fs, which indicates high time resolution when used as a probe. Our newly developed method to predict kinetic energy spectra shows good agreement with electron and ion irradiation experiments and prior models. We find that the lattice temperature significantly increases secondary electron emission, whereas electron temperature has a negligible effect.

2.
ACS Omega ; 6(24): 15929-15939, 2021 Jun 22.
Artículo en Inglés | MEDLINE | ID: mdl-34179637

RESUMEN

Two-dimensional semiconductors such as MoS2 are promising for future electrical devices. The interface to metals is a crucial and critical aspect for these devices because undesirably high resistances due to Fermi level pinning are present, resulting in unwanted energy losses. To date, experimental information on such junctions has been obtained mainly indirectly by evaluating transistor characteristics. The fact that the metal-semiconductor interface is typically embedded, further complicates the investigation of the underlying physical mechanisms at the interface. Here, we present a method to provide access to a realistic metal-semiconductor interface by large-area exfoliation of single-layer MoS2 on clean polycrystalline gold surfaces. This approach allows us to measure the relative charge neutrality level at the MoS2-gold interface and its spatial variation almost directly using Kelvin probe force microscopy even under ambient conditions. By bringing together hitherto unconnected findings about the MoS2-gold interface, we can explain the anomalous Raman signature of MoS2 in contact to metals [ACS Nano. 7, 2013, 11350] which has been the subject of intense recent discussions. In detail, we identify the unusual Raman mode as the A1g mode with a reduced Raman shift (397 cm-1) due to the weakening of the Mo-S bond. Combined with our X-ray photoelectron spectroscopy data and the measured charge neutrality level, this is in good agreement with a previously predicted mechanism for Fermi level pinning at the MoS2-gold interface [Nano Lett. 14, 2014, 1714]. As a consequence, the strength of the MoS2-gold contact can be determined from the intensity ratio between the reduced A1greduced mode and the unperturbed A1g mode.

3.
J Am Soc Mass Spectrom ; 28(6): 1182-1191, 2017 06.
Artículo en Inglés | MEDLINE | ID: mdl-28265969

RESUMEN

The prospect of improved secondary ion yields for secondary ion mass spectrometry (SIMS) experiments drives innovation of new primary ion sources, instrumentation, and post-ionization techniques. The largest factor affecting secondary ion efficiency is believed to be the poor ionization probability (α+) of sputtered material, a value rarely measured directly, but estimated to be in some cases as low as 10-5. Our lab has developed a method for the direct determination of α+ in a SIMS experiment using laser post-ionization (LPI) to detect neutral molecular species in the sputtered plume for an organic compound. Here, we apply this method to coronene (C24H12), a polyaromatic hydrocarbon that exhibits strong molecular signal during gas-phase photoionization. A two-dimensional spatial distribution of sputtered neutral molecules is measured and presented. It is shown that the ionization probability of molecular coronene desorbed from a clean film under bombardment with 40 keV C60 cluster projectiles is of the order of 10-3, with some remaining uncertainty arising from laser-induced fragmentation and possible differences in the emission velocity distributions of neutral and ionized molecules. In general, this work establishes a method to estimate the ionization efficiency of molecular species sputtered during a single bombardment event. Graphical Abstract .

4.
J Phys Chem A ; 118(37): 8542-52, 2014 Sep 18.
Artículo en Inglés | MEDLINE | ID: mdl-24779393

RESUMEN

The formation of neutral gas phase indium carbide clusters under C60(+) ion bombardment of solid indium was investigated using laser based postionization prior to mass spectrometric detection. Two different postionization methods were used and shown to provide saturated photoionization efficiency, thereby delivering nearly the same information about the composition of the sputtered material. The resulting size distributions of neutral In(m)C(n) clusters are compared with those of the corresponding cationic secondary cluster ions and discussed in terms of calculated cluster properties. Investigating the dependence on C60(+) ion fluence, we demonstrate that clusters containing only one carbon atom are formed in single impact events, whereas the formation of more carbon-rich clusters results from carbon accumulation at the bombarded surface.

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