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.
more »
« less
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.
more »
« less
- 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
More Like this
-
-
This research introduces a readily available and non-chemical combinatorial production approach, known as the laser-induced writing process, to achieve laser-processed conductive graphene traces. The laser-induced graphene (LIG) structure and properties can be improved by adjusting the laser conditions and printing parameters. This method demonstrates the ability of laser-induced graphene (LIG) to overcome the electrothermal issues encountered in electronic devices. To additively process the PEI structures and the laser-induced surface, a high-precision laser nScrypt printer with different power, speed, and printing parameters was used. Raman spectroscopy and scanning electron microscopy analysis revealed similar results for laser-induced graphene morphology and structural chemistry. Significantly, the 3.2 W laser-induced graphene crystalline size (La; 159 nm) is higher than the higher power (4 W; 29 nm) formation due to the surface temperature and oxidation. Under four-point probe electrical property measurements, at a laser power of 3.8 W, the resistivity of the co-processed structure was three orders of magnitude larger. The LIG structure and property improvement are possible by varying the laser conditions and the printing parameters. The lowest gauge factor (GF) found was 17 at 0.5% strain, and the highest GF found was 141.36 at 5%.more » « less
-
Wetting experiments show pure graphene to be weakly hydrophilic, but its contact angle (CA) also reflects the character of the supporting material. Measurements and Molecular Dynamics simulations on suspended and supported graphene often reveal a CA reduction due to the presence of the supporting substrate. A similar reduction is consistently observed when graphene is wetted from both sides. The effect has been attributed to transparency to molecular interactions across the graphene sheet, however, the possibility of substrate-induced graphene polarization has also been considered. Computer simulations of CA on graphene have so far been determined by ignoring the material’s conducting properties. We improve the graphene model by incorporating its conductivity according to the Constant Applied Potential Molecular Dynamics. Using this method, we compare the wettabilities of suspended graphene and graphene supported by water by measuring the CA of cylindrical water drops on the sheets. The inclusion of graphene conductivity and concomitant polarization effects lead to a lower CA on suspended graphene but the CA reduction is significantly bigger when the sheets are also wetted from the opposite side. The stronger adhesion is accompanied by a profound change in the correlations among water molecules across the sheet. While partial charges on water molecules interacting across an insulator sheet attract charges of the opposite sign, apparent attraction among like charges is manifested across the conducting graphene. The change is associated with graphene polarization, as the image charges inside the conductor attract equally signed partial charges of water molecules on both sides of the sheet. Additionally, by using a non-polar liquid (diiodomethane), we affirm a detectable wetting translucency when liquid-liquid forces are dominated by dispersive interactions. Our findings are important for predictive modeling toward a variety of applications including sensors, fuel cell membranes, water filtration, and graphene-based electrode materials in high-performance supercapacitors.more » « less
-
null (Ed.)Group IVB transition metal dichalcogenides (TMDCs) have attracted significant attention due to their predicted high charge carrier mobility, large sheet current density, and enhanced thermoelectric power. Here, we investigate the electrical and optoelectronic properties of few-layer titanium diselenide (TiSe 2 )-metal junctions through spatial-, wavelength-, temperature-, power- and temporal-dependent scanning photocurrent measurements. Strong photocurrent responses have been detected at TiSe 2 -metal junctions, which is likely attributed to both photovoltaic and photothermoelectric effects. A fast response time of 31 μs has been achieved, which is two orders of magnitude better than HfSe 2 based devices. More importantly, our experimental results reveal a significant enhancement in the response speed upon cooling to the charge-density-wave (CDW) phase transition temperature ( T CDW = 206 K), which may result from dramatic reduction in carrier scattering that occurs as a result of the switching between the normal and CDW phases of TiSe 2 . Additionally, the photoresponsivity at 145 K is up to an order of magnitude higher than that obtained at room temperature. These fundamental studies not only offer insight for the photocurrent generation mechanisms of group IVB TMDC materials, but also provide a route to engineering future temperature-dependent, two-dimensional, fast electronic and optoelectronic devices.more » « less
-
Abstract Nanomechanical resonators are built into phones, as filters or accelerometers, but they lack a knob to effectively tune the frequency at the nanoscale when it’s easy to tune on an octave the tone of a classical musical instrument like a guitar string. Moreover, the control of deformation in nanomaterials, as two-dimensional (2D) materials, to tailor their electronic properties, i.e., straintronic, opens up avenues for applications in force detection, bolometry or quantum emitters. An accurate control of the deformation within these materials is thus necessary to fully exploit their potential. The precise study of deformations in 2D materials involves measurements of vibration modes and nanomechanics. By using a suspended MoS 2 membrane heated by the Joule effect, we induce a strong softening of the mechanical resonance frequency as a function of the electrothermal heating, over one octave. A simple electrical tension is used to modulate the thermal mechanical tuning. Its amplitude is very large, greater than 100% modulation for one volt, compared to other approaches on 2D or 1D materials and, moreover, a very wide frequency range is accessible. Finally, we have related a photo-induced softening of the membrane over very long times with the current measurements and a photothermal effect.more » « less
An official website of the United States government

