The isolation of various two-dimensional (2D) materials, and the possibility to combine them in vertical stacks, has created a new paradigm in materials science: heterostructures based on 2D crystals. Such a concept has already proven fruitful for a number of electronic applications in the area of ultrathin and flexible devices. Here, we expand the range of such structures to photoactive ones by using semiconducting transition metal dichalcogenides (TMDCs)/graphene stacks. Van Hove singularities in the electronic density of states of TMDC guarantees enhanced light-matter interactions, leading to enhanced photon absorption and electron-hole creation (which are collected in transparent graphene electrodes). This allows development of extremely efficient flexible photovoltaic devices with photoresponsivity above 0.1 ampere per watt (corresponding to an external quantum efficiency of above 30%).
Raman Spectroscopy is able to probe disorder in graphene through defect-activated peaks. It is of great interest to link these features to the nature of disorder. Here we present a detailed analysis of the Raman spectra of graphene containing different type of defects. We found that the intensity ratio of the D and D' peak is maximum (~ 13) for sp 3 -defects, it decreases for vacancy-like defects (~ 7) and reaches a minimum for boundaries in graphite (~3.5).
When a crystal is subjected to a periodic potential, under certain circumstances (such as when the period of the potential is close to the crystal periodicity; the potential is strong enough, etc.) it might adjust itself to follow the periodicity of the potential, resulting in a, so called, commensurate state 1-3 .Such commensurate-incommensurate transitions are ubiquitous phenomena in many areas of condensed matter physics: from magnetism and dislocations in crystals, to vortices in superconductors, and atomic layers adsorbed on a crystalline surface 1 . Of particular interest might be the properties of topological defects between the two commensurate phases: solitons 2,4 , domain walls 1 , and dislocation walls 5-7 . Here we report a commensurate-incommensurate transition for graphene on top of hexagonal boron nitride (hBN) 8,9 . Depending on the rotational angle between the two hexagonal lattices, graphene can either stretch to adjust to a slightly different hBN periodicity (the commensurate state found for small rotational angles) or exhibit little adjustment (the incommensurate state). In the commensurate state, areas with matching lattice constants are separated by domain walls that accumulate the resulting strain. Such soliton-like objects present significant fundamental interest 1 , and their presence might explain recent observations when the electronic, optical, Raman and other properties of graphene-hBN heterostructures have been notably altered 10 .
We present a detailed Raman study of defective graphene samples containing specific types of defects. In particular, we compared sp 3 sites, vacancies, and substitutional Boron atoms. We find that the ratio between the D and G peak intensities, I(D)/I(G), does not depend on the geometry of the defect (within the Raman spectrometer resolution). In contrast, in the limit of low defect concentration, the ratio between the D and G peak intensities is higher for vacancies than sp 3 sites. By using the local activation model, we attribute this difference to the term C S,x , representing the Raman cross section of I(x)/I(G) associated with the distortion of the crystal lattice after defect introduction per unit of damaged area, where x = D or D. We observed that C S,D = 0 for all the defects analyzed, while C S,D of vacancies is 2.5 times larger than C S,D of sp 3 sites. This makes I(D)/I(D) strongly sensitive to the nature of the defect. We also show that the exact dependence of I(D)/I(D) on the excitation energy may be affected by the nature of the defect. These results can be used to obtain further insights into the Raman scattering process (in particular for the D peak) in order to improve our understanding and modeling of defects in graphene.
The new paradigm of heterostructures based on two-dimensional (2D) atomic crystals has already led to the observation of exciting physical phenomena and creation of novel devices. The possibility of combining layers of different 2D materials in one stack allows unprecedented control over the electronic and optical properties of the resulting material. Still, the current method of mechanical transfer of individual 2D crystals, though allowing exceptional control over the quality of such structures and interfaces, is not scalable. Here we show that such heterostructures can be assembled from chemically exfoliated 2D crystals, allowing for low-cost and scalable methods to be used in device fabrication.
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