A graphene-based broadband optical modulator.

Integrated optical modulators with high modulation speed, small footprint and large optical bandwidth are poised to be the enabling devices for on-chip optical interconnects. Semiconductor modulators have therefore been heavily researched over the past few years. However, the device footprint of silicon-based modulators is of the order of millimetres, owing to its weak electro-optical properties. Germanium and compound semiconductors, on the other hand, face the major challenge of integration with existing silicon electronics and photonics platforms. Integrating silicon modulators with high-quality-factor optical resonators increases the modulation strength, but these devices suffer from intrinsic narrow bandwidth and require sophisticated optical design; they also have stringent fabrication requirements and limited temperature tolerances. Finding a complementary metal-oxide-semiconductor (CMOS)-compatible material with adequate modulation speed and strength has therefore become a task of not only scientific interest, but also industrial importance. Here we experimentally demonstrate a broadband, high-speed, waveguide-integrated electroabsorption modulator based on monolayer graphene. By electrically tuning the Fermi level of the graphene sheet, we demonstrate modulation of the guided light at frequencies over 1 GHz, together with a broad operation spectrum that ranges from 1.35 to 1.6 µm under ambient conditions. The high modulation efficiency of graphene results in an active device area of merely 25 µm(2), which is among the smallest to date. This graphene-based optical modulation mechanism, with combined advantages of compact footprint, low operation voltage and ultrafast modulation speed across a broad range of wavelengths, can enable novel architectures for on-chip optical communications.

Controlling inelastic light scattering quantum pathways in graphene.

Inelastic light scattering spectroscopy has, since its first discovery, been an indispensable tool in physical science for probing elementary excitations, such as phonons, magnons and plasmons in both bulk and nanoscale materials. In the quantum mechanical picture of inelastic light scattering, incident photons first excite a set of intermediate electronic states, which then generate crystal elementary excitations and radiate energy-shifted photons. The intermediate electronic excitations therefore have a crucial role as quantum pathways in inelastic light scattering, and this is exemplified by resonant Raman scattering and Raman interference. The ability to control these excitation pathways can open up new opportunities to probe, manipulate and utilize inelastic light scattering. Here we achieve excitation pathway control in graphene with electrostatic doping. Our study reveals quantum interference between different Raman pathways in graphene: when some of the pathways are blocked, the one-phonon Raman intensity does not diminish, as commonly expected, but increases dramatically. This discovery sheds new light on the understanding of resonance Raman scattering in graphene. In addition, we demonstrate hot-electron luminescence in graphene as the Fermi energy approaches half the laser excitation energy. This hot luminescence, which is another form of inelastic light scattering, results from excited-state relaxation channels that become available only in heavily doped graphene.

Polymer Adsorption on Graphite and CVD Graphene Surfaces Studied by Surface-Specific Vibrational Spectroscopy.

Sum-frequency vibrational spectroscopy was employed to probe polymer contaminants on chemical vapor deposition (CVD) graphene and to study alkane and polyethylene (PE) adsorption on graphite. In comparing the spectra from the two surfaces, it was found that the contaminants on CVD graphene must be long-chain alkane or PE-like molecules. PE adsorption from solution on the honeycomb surface results in a self-assembled ordered monolayer with the C-C skeleton plane perpendicular to the surface and an adsorption free energy of ∼42 kJ/mol for PE(H(CH2CH2)nH) with n ≈ 60. Such large adsorption energy is responsible for the easy contamination of CVD graphene by impurity in the polymer during standard transfer processes. Contamination can be minimized with the use of purified polymers free of PE-like impurities.

Electrical control of optical plasmon resonance with graphene.

Surface plasmon has the unique capability to concentrate light into subwavelength volume. Active plasmon devices using electrostatic gating can enable flexible control of the plasmon excitations, which has been demonstrated recently in terahertz plasmonic structures. Controlling plasmon resonance at optical frequencies, however, remains a significant challenge because gate-induced free electrons have very weak responses at optical frequencies. Here we achieve efficient control of near-infrared plasmon resonance in a hybrid graphene-gold nanorod system. Exploiting the uniquely strong and gate-tunable optical transitions of graphene, we are able to significantly modulate both the resonance frequency and quality factor of gold nanorod plasmon. Our analysis shows that the plasmon-graphene coupling is remarkably strong: even a single electron in graphene at the plasmonic hotspot could have an observable effect on plasmon scattering intensity. Such hybrid graphene-nanometallic structure provides a powerful way for electrical control of plasmon resonances at optical frequencies and could enable novel plasmonic sensing down to single charge transfer events.

The interaction of Li+ with single-layer and few-layer graphene.

The interaction of Li(+) with single and few layer graphene is reported. In situ Raman spectra were collected during the electrochemical lithiation of the single- and few-layer graphene. While the interaction of lithium with few layer graphene seems to resemble that of graphite, single layer graphene behaves very differently. The amount of lithium absorbed on single layer graphene seems to be greatly reduced due to repulsion forces between Li(+) at both sides of the graphene layer.

Large-size and high performance visible-light photodetectors based on two-dimensional hybrid materials SnS/RGO.

We report a facile solvothermal method to synthesize two-dimensional hybrid materials consisting of layered SnS nanosheets and reduced graphene oxide (SnS/RGO). Large-size photodetectors with a channel length/width = 2 mm/7 mm are fabricated on Si/SiO2 substrates, showing an excellent photoresponsivity of 0.18 A W-1 under visible-light illumination with a detectivity of 4.18 × 1010 Jones, as well as fast rise and decay times (τ rise = τ decay = 0.4 s). SnS/RGO hybrids are therefore promising candidates for potential applications in optoelectronics and low cost, high performance, and reliable photodetectors.

Graphene plasmonics for tunable terahertz metamaterials.

Plasmons describe collective oscillations of electrons. They have a fundamental role in the dynamic responses of electron systems and form the basis of research into optical metamaterials. Plasmons of two-dimensional massless electrons, as present in graphene, show unusual behaviour that enables new tunable plasmonic metamaterials and, potentially, optoelectronic applications in the terahertz frequency range. Here we explore plasmon excitations in engineered graphene micro-ribbon arrays. We demonstrate that graphene plasmon resonances can be tuned over a broad terahertz frequency range by changing micro-ribbon width and in situ electrostatic doping. The ribbon width and carrier doping dependences of graphene plasmon frequency demonstrate power-law behaviour characteristic of two-dimensional massless Dirac electrons. The plasmon resonances have remarkably large oscillator strengths, resulting in prominent room-temperature optical absorption peaks. In comparison, plasmon absorption in a conventional two-dimensional electron gas was observed only at 4.2 K (refs 13, 14). The results represent a first look at light-plasmon coupling in graphene and point to potential graphene-based terahertz metamaterials.

Transfer-free batch fabrication of large-area suspended graphene membranes.

We demonstrate a process for batch production of large-area (100-3000 microm(2)) patterned free-standing graphene membranes on Cu scaffolds using chemical vapor deposition (CVD)-grown graphene. This technique avoids the use of silicon and transfers of graphene. As one application of this technique, we fabricate transmission electron microscopy (TEM) sample supports. TEM characterization of the graphene membranes reveals relatively clean, highly TEM-transparent, single-layer graphene regions ( approximately 50% by area) and, despite the polycrystalline nature of CVD graphene, membrane yields as high as 75-100%. This high yield verifies that the intrinsic strength and integrity of CVD-grown graphene films is sufficient for sub-100 microm width membrane applications. Elemental analysis (electron energy loss spectroscopy (EELS) and X-ray energy-dispersive spectroscopy (EDS)) of the graphene membranes reveals some nanoscaled contamination left over from the etching process, and we suggest several ways to reduce this contamination and improve the quality of the graphene for electronic device applications. This large-scale production of suspended graphene membranes facilitates access to the two-dimensional physics of graphene that are suppressed by substrate interactions and enables the widespread use of graphene-based sample supports for electron and optical microscopy.

A tunable phonon-exciton Fano system in bilayer graphene.

Fano resonances are features in absorption, scattering or transport spectra resulting from the interaction of discrete and continuum states. They have been observed in a variety of systems. Here, we report a many-body Fano resonance in bilayer graphene that is continuously tunable by means of electrical gating. Discrete phonons and continuous exciton (electron-hole pair) transitions are coupled by electron-phonon interactions, yielding a new hybrid phonon-exciton excited state. It may also be possible to control the phonon-exciton coupling with an optical field. This tunable phonon-exciton system could allow novel applications such as phonon lasers.