Reproducible dry and wet transfer techniques were developed to improve the transfer of large-area monolayer graphene grown on copper foils by chemical vapor deposition (CVD). The techniques reported here allow transfer onto three different classes of substrates: substrates covered with shallow depressions, perforated substrates, and flat substrates. A novel dry transfer technique was used to make graphene-sealed microchambers without trapping liquid inside. The dry transfer technique utilizes a polydimethylsiloxane frame that attaches to the poly(methyl methacrylate) spun over the graphene film, and the monolayer graphene was transferred onto shallow depressions with 300 nm depth. The improved wet transfer onto perforated substrates with 2.7 μm diameter holes yields 98% coverage of holes covered with continuous films, allowing the ready use of Raman spectroscopy and transmission electron microscopy to study the intrinsic properties of CVD-grown monolayer graphene. Additionally, monolayer graphene transferred onto flat substrates has fewer cracks and tears, as well as lower sheet resistance than previous transfer techniques. Monolayer graphene films transferred onto glass had a sheet resistance of ∼980 Ω/sq and a transmittance of 97.6%. These transfer techniques open up possibilities for the fabrication of various graphene devices with unique configurations and enhanced performance.
We demonstrate the continuous and reversible tuning of the optical band gap of suspended monolayer MoS 2 membranes by as much as 500 meV by applying very large biaxial strains. By using chemical vapor deposition (CVD) to grow crystals that are highly impermeable to gas, we are able to apply a pressure difference across suspended membranes to induce biaxial strains. We observe the effect of strain on the energy and intensity of the peaks in the photoluminescence (PL) spectrum, and find a linear tuning rate of the optical band gap of 99 meV/%. This method is then used to study the PL spectra of bilayer and trilayer devices under strain, and to find the shift rates and Grüneisen parameters of two Raman modes in monolayer MoS 2 . Finally, we use this result to show that we can apply biaxial strains as large as 5.6% across micron sized areas, and report evidence for the strain tuning of higher level optical transitions.KEYWORDS: Strain engineering, MoS 2 , photoluminescence, bandgap, Raman spectroscopy, biaxial strain 3 The ability to produce materials of truly nanoscale dimensions has revolutionized the potential for modulating or enhancing the physical properties of semiconductors by mechanical strain 1 . Strain engineering is routinely used in semiconductor manufacturing, with essential electrical components such as the silicon transistor or quantum well laser using strain to improve efficiency and performance 2,3 . Nano-structured materials are particularly suited to this technique, as they are often able to remain elastic when subject to strains many times larger than their bulk counterparts can withstand 4 . For instance, bulk silicon fractures when strained to just 1.2%, whereas silicon nanowires can reach strains of as much as 3.5% 5 . Parameters such as the band gap energy or carrier mobility of a semiconductor, which are often crucial to the electronic or photonic device performance, can be highly sensitive to the application of only small strains. The combination of this sensitivity with the ultra-high strains possible at the nanoscale could lead to an unprecedented ability to modify the electrical or photonic properties of materials in a continuous and reversible manner.Monolayer MoS 2, a 2D atomic crystal, has been shown in both theory 6,7 and experiment [8][9][10][11][12] to be an ideal candidate for strain engineering. It belongs to the class of 2D transition metal dichalcogonides (TMD's), and as a direct-gap semiconductor 13 has received significant interest as a channel material in transistors 14 , photovoltaics 15 and photodetection 16 devices. It has a breaking strain of 6-11% as measured by nanoindentation, which approaches its maximum theoretical strain limit 17 and classifies it as an ultra-strength material. Its electronic structure has also proven to be highly sensitive to strain, with experiments showing that the optical band gap reduces by ~50 meV/% for 4 uniaxial strain 8,11 , and is predicted to reduce by ~100 meV/% for biaxial strain 18,19 . This reversible modulation of the band...
We report G-band resonance Raman spectra of single-wall carbon nanotubes ͑SWNTs͒ at the singlenanotube level. By measuring 62 different isolated SWNTs resonant with the incident laser, and having diameters d t ranging between 0.95 nm and 2.62 nm, we have conclusively determined the dependence of the two most intense G-band features on the nanotube structure. The higher-frequency peak is not diameter dependent (G ϩ ϭ1591 cm Ϫ1), while the lower-frequency peak is given by G Ϫ ϭ G ϩ ϪC/d t 2 , with C being different for metallic and semiconducting SWNTs (C M ϾC S). The peak frequencies do not depend on nanotube chiral angle. The intensity ratio between the two most intense features is in the range 0.1ϽI G Ϫ /I G ϩϽ 0.3 for most of the isolated SWNTs (ϳ90%). Unusually high or low I G Ϫ /I G ϩ ratios are observed for a few spectra coming from SWNTs under special resonance conditions, i.e., SWNTs for which the incident photons are in resonance with the E 44 S interband transition and scattered photons are in resonance with E 33 S. Since the E ii values depend sensitively on both nanotube diameter and chirality, the (n,m) SWNTs that should exhibit such a special G-band spectra can be predicted by resonance Raman theory. The agreement between theoretical predictions and experimental observations about these special G-band phenomena gives additional support for the (n,m) assignment from resonance Raman spectroscopy.
Uniaxial strain is induced by pushing single-wall carbon nanotubes ͑SWNTs͒ with an atomic force microscope tip. The vibrational and electronic energies of nanotubes are found to be very sensitive to strain. For both metallic and semiconducting SWNTs under strain, the D, G, and GЈ band Raman modes are downshifted by up to 27, 15, and 40 cm −1 , respectively. The relative strain-induced shifts of the D, G, and GЈ bands vary significantly from nanotube to nanotube, implying that there is a strong chirality dependence of the relative shifts. Semiconducting SWNTs remain strongly resonant under these large deformations, while metallic SWNTs appear to move in and out of resonance with strain, indicating a strain-induced shifting of the electronic subbands. Tight-binding calculations of the electronic band structure of semiconducting and metallic nanotubes under uniaxial strain predict significant shifting of the subband energies, leading to strain-induced changes in the Raman intensity. These theoretical predictions are consistent with what we observe experimentally for metallic nanotubes, but not for semiconducting nanotubes.
Measurements on graphene exfoliated over a substrate prepatterned with shallow depressions demonstrate that graphene does not remain free-standing but instead adheres to the substrate despite the induced biaxial strain. The strain is homogeneous over the depression bottom as determined by Raman measurements. We find higher Raman shifts and Gruneisen parameters of the phonons underlying the G and 2D bands under biaxial strain than previously reported. Interference modeling is used to determine the vertical position of the graphene and to calculate the optimum dielectric substrate stack for maximum Raman signal.
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