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Micro-Raman spectroscopy has become an important tool in probing thermophysical properties in functional materials. Localized heating by the focused Raman excitation laser beam can produce both stress and local nonequilibrium phonons in the material. Here, we investigate the effects of hot optical phonons in the Raman spectra of molybdenum disulfide and distinguish them from those caused by thermally induced compressive stress, which causes a Raman frequency blue shift. We use a thermomechanical analysis to correct for this stress effect in the equivalent lattice temperature extracted from the measured Raman peak shift. When the heating Gaussian laser beam is reduced to 0.71 μm, the corrected peak shift temperature rise is 17% and 8%, respectively, higher than those determined from the measured peak shift and linewidth without the stress correction, and 32% smaller than the optical phonon temperature rise obtained from the anti-Stokes to Stokes intensity ratio. This nonequilibrium between the hot optical phonons and the lattice vanishes as the beam width increases to 1.53 μm. Much less pronounced than those reported in prior micro-Raman measurements of suspended graphene, this observed hot phonon behavior agrees with a first-principles based multitemperature model of overpopulated zone-center optical phonons compared to other optical phonons in the Brillouin zone and acoustic phonons of this prototypical transition metal dichalcogenide. The findings provide detailed insight into the energy relaxation processes in this emerging electronic and optoelectronic material and clarify an important question in micro-Raman measurements of thermal transport in this and other two-dimensional materials.
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In situ monitoring of electrical and optoelectronic properties of suspended graphene ribbons during laser-induced morphological changes
Exploring ways to tune and improve the performance of graphene is of paramount importance in creating functional graphene-based electronic and optoelectronic devices. Recent advancements have shown that altering the morphology of graphene can have a pronounced effect on its properties. Here, we present a practical and facile method to manipulate the morphology of a suspended graphene ribbon using a laser to locally induce heating while monitoring its electrical and optoelectronic properties in situ . Electrical measurements reveal that the conductance of suspended graphene transistors can be tuned by modifying its morphology. Additionally, scanning photocurrent measurements show that laser-induced folded graphene ribbons display significantly enhanced localized photocurrent responses in comparison with their flat counterparts. Moreover, the localization of the laser-induced heating allows for a series of folds to be induced along the entire graphene ribbon, creating targeted photocurrent enhancement. Through further investigations, it is revealed that the photo-thermoelectric effect is the primary mechanism for the increased photocurrent response of the device. Our experimental results explore the mechanisms and consequences of the folding process as well as provide a strategy to manipulate morphology and physical properties of graphene for future engineering of electronics and optoelectronics.
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- Award ID(s):
- 1810088
- PAR ID:
- 10258179
- Date Published:
- Journal Name:
- Nanoscale Advances
- Volume:
- 2
- Issue:
- 9
- ISSN:
- 2516-0230
- Page Range / eLocation ID:
- 4034 to 4040
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/D0NA00413H
