Graphene's success has shown that it is possible to create stable, single and few-atom-thick layers of van der Waals materials, and also that these materials can exhibit fascinating and technologically useful properties. Here we review the state-of-the-art of 2D materials beyond graphene. Initially, we will outline the different chemical classes of 2D materials and discuss the various strategies to prepare single-layer, few-layer, and multilayer assembly materials in solution, on substrates, and on the wafer scale. Additionally, we present an experimental guide for identifying and characterizing single-layer-thick materials, as well as outlining emerging techniques that yield both local and global information. We describe the differences that occur in the electronic structure between the bulk and the single layer and discuss various methods of tuning their electronic properties by manipulating the surface. Finally, we highlight the properties and advantages of single-, few-, and many-layer 2D materials in field-effect transistors, spin- and valley-tronics, thermoelectrics, and topological insulators, among many other applications.
Covalent organic frameworks (COFs), in which molecular building blocks form robust microporous networks, are usually synthesized as insoluble and unprocessable powders. We have grown two-dimensional (2D) COF films on single-layer graphene (SLG) under operationally simple solvothermal conditions. The layered films stack normal to the SLG surface and show improved crystallinity compared with COF powders. We used SLG surfaces supported on copper, silicon carbide, and transparent fused silica (SiO(2)) substrates, enabling optical spectroscopy of COFs in transmission mode. Three chemically distinct COF films grown on SLG exhibit similar vertical alignment and long-range order, and two of these are of interest for organic electronic devices for which thin-film formation is a prerequisite for characterizing their optoelectronic properties.
Using ultrafast optical pump-probe spectroscopy, we have measured carrier relaxation times in epitaxial graphene layers grown on SiC wafers. We find two distinct time scales associated with the relaxation of nonequilibrium photogenerated carriers. An initial fast relaxation transient in the 70-120 fs range is followed by a slower relaxation process in the 0.4-1.7 ps range. The slower relaxation time is found to be inversely proportional to the degree of crystalline disorder in the graphene layers as measured by Raman spectroscopy. We relate the measured fast and slow time constants to carrier-carrier and carrier-phonon intraband and interband scattering processes in graphene.
The ultrafast relaxation and recombination dynamics of photogenerated electrons and holes in epitaxial graphene are studied using optical-pump Terahertz-probe spectroscopy. The conductivity in graphene at Terahertz frequencies depends on the carrier concentration as well as the carrier distribution in energy. Time-resolved studies of the conductivity can therefore be used to probe the dynamics associated with carrier intraband relaxation and interband recombination. We report the electron-hole recombination times in epitaxial graphene for the first time. Our results show that carrier cooling occurs on sub-picosecond time scales and that interband recombination times are carrier density dependent.Graphene is a 2D lattice of carbon atoms arranged in a honeycomb crystal structure with a zero (or nearzero) bandgap and a linear energy-momentum dispersion relation for both electrons and holes [1,2]. The unique electronic and optical properties of graphene make it a promising material for the development of high-speed electron devices, including field-effect transistors, pn-diodes, Terahertz oscillators, and electronic and optical sensors [2,3,4,5,6,7]. The realization of graphene-based devices requires understanding the nonequilibrium carrier dynamics as well as the rate at which electron-hole recombination occurs.Measurements of the ultrafast intraband relaxation dynamics of photogenerated electrons and holes in epitaxial graphene using both degenerate [8] and non-degenerate [9] optical-pump optical-probe spectroscopy have been previously reported. Similar measurements for exfoliated graphene mono-and multi-layers have also been carried out [10]. These measurements were sensitive to the interband conductivity of graphene and probed the time evolution of the carrier occupation at specific energies in the bands. Consequently, they were not able to directly measure the time scales associated with carrier recombination. At room temperature, the optical response of graphene in the THz frequency range is described by the intraband conductivity -the free carrier responsewhich depends not only on the total carrier concentration but also on the carrier distribution in energy [11]. Therefore, THz radiation can be used to study the carrier relaxation and recombination dynamics in graphene. In this paper, we present results obtained from opticalpump THz-probe spectroscopy of epitaxial graphene in which the time-dependent conductivity of graphene that has been excited with an optical pump pulse is probed with a few-cycle THz pulse. We observe cooling of the photogenerated carrier distribution as well as electronhole recombination in graphene in real time. Our results indicate that the recombination times in graphene depend on the carrier density and material disorder.The epitaxial graphene samples used in this work were grown on the carbon face of semi-insulating 6H-SiC wafers using techniques that have been reported previously [12]. As discussed in [8,11], X-ray photoemission, Raman, and optical/IR/THz transmission spectroscopy ...
We investigate the distribution and temperature-dependent optical properties of sharp, zero-phonon emission from defect-based single photon sources in multilayer hexagonal boron nitride (h-BN) flakes. We observe sharp emission lines from optically active defects distributed across an energy range that exceeds 500 meV. Spectrally resolved photon-correlation measurements verify single photon emission, even when multiple emission lines are simultaneously excited within the same h-BN flake. We also present a detailed study of the temperature-dependent line width, spectral energy shift, and intensity for two different zero-phonon lines centered at 575 and 682 nm, which reveals a nearly identical temperature dependence despite a large difference in transition energy. Our temperature-dependent results are well described by a lattice vibration model that considers piezoelectric coupling to in-plane phonons. Finally, polarization spectroscopy measurements suggest that whereas the 575 nm emission line is directly excited by 532 nm excitation, the 682 nm line is excited indirectly.
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