Synthesis and properties of free-standing monolayer amorphous carbon.

Bulk amorphous materials have been studied extensively and are widely used, yet their atomic arrangement remains an open issue. Although they are generally believed to be Zachariasen continuous random networks1, recent experimental evidence favours the competing crystallite model in the case of amorphous silicon2-4. In two-dimensional materials, however,  the corresponding questions remain unanswered. Here we report the synthesis, by laser-assisted chemical vapour deposition5, of centimetre-scale, free-standing, continuous and stable monolayer amorphous carbon, topologically distinct from disordered graphene. Unlike in bulk materials, the structure of monolayer amorphous carbon can be determined by atomic-resolution imaging. Extensive characterization by Raman and X-ray spectroscopy and transmission electron microscopy reveals the complete absence of long-range periodicity and a threefold-coordinated structure with a wide distribution of bond lengths, bond angles, and five-, six-, seven- and eight-member rings. The ring distribution is not a Zachariasen continuous random network, but resembles the competing (nano)crystallite model6. We construct a corresponding model that enables density-functional-theory calculations of the properties of monolayer amorphous carbon, in accordance with observations. Direct measurements confirm that it is insulating, with resistivity values similar to those of boron nitride grown by chemical vapour deposition. Free-standing monolayer amorphous carbon is surprisingly stable and deforms to a high breaking strength, without crack propagation from the point of fracture. The excellent physical properties of this stable, free-standing monolayer amorphous carbon could prove useful for permeation and diffusion barriers in applications such as magnetic recording devices and flexible electronics.

Graphene-Based Adaptive Thermal Camouflage.

In nature, adaptive coloration has been effectively utilized for concealment and signaling. Various biological mechanisms have evolved to tune the reflectivity for visible and ultraviolet light. These examples inspire many artificial systems for mimicking adaptive coloration to match the visual appearance to their surroundings. Thermal camouflage, however, has been an outstanding challenge which requires an ability to control the emitted thermal radiation from the surface. Here we report a new class of active thermal surfaces capable of efficient real-time electrical-control of thermal emission over the full infrared (IR) spectrum without changing the temperature of the surface. Our approach relies on electro-modulation of IR absorptivity and emissivity of multilayer graphene via reversible intercalation of nonvolatile ionic liquids. The demonstrated devices are light (30 g/m2), thin (<50 µm), and ultraflexible, which can conformably coat their environment. In addition, by combining active thermal surfaces with a feedback mechanism, we demonstrate realization of an adaptive thermal camouflage system which can reconfigure its thermal appearance and blend itself with the varying thermal background in a few seconds. Furthermore, we show that these devices can disguise hot objects as cold and cold ones as hot in a thermal imaging system. We anticipate that, the electrical control of thermal radiation would impact on a variety of new technologies ranging from adaptive IR optics to heat management for outer space applications.

Generation of sub-20-fs pulses from a graphene mode-locked laser.

We demonstrate, what is to our knowledge, the shortest pulses directly generated to date from a solid-state laser, mode locked with a graphene saturable absorber (GSA). In the experiments, a low-threshold diode-pumped Cr3+:LiSAF laser was used near 850 nm. At a pump power of 275 mW provided by two pump diodes, the Cr3+:LiSAF laser produced nearly transform-limited, 19-fs pulses with an average output power of 8.5 mW. The repetition rate was around 107 MHz, corresponding to a pulse energy and peak power of 79 pJ and 4.2 kW, respectively. Once mode locking was initiated with the GSA, stable, uninterrupted femtosecond pulse generation could be obtained. In addition, the femtosecond output of the laser could be tuned from 836 nm to 897 nm with pulse durations in the range of 80-190 fs. We further performed detailed mode locking initiation tests across the full cavity stability range of the laser to verify that pulse generation was indeed started by the GSA and not by Kerr lens mode locking.

Femtosecond pulse generation from a Ti3+:sapphire laser near 800 nm with voltage reconfigurable graphene saturable absorbers.

We experimentally show that a voltage-controlled graphene-gold supercapacitor saturable absorber (VCG-gold-SA) can be operated as a fast saturable absorber with adjustable linear absorption at wavelengths as low as 795 nm. This was made possible by the use of a novel supercapacitor architecture, consisting of a high-dielectric electrolyte sandwiched between a graphene and a gold electrode. The high-dielectric electrolyte allowed continuous, reversible adjustment of the Fermi level and, hence, the optical loss of the VCG-gold-SA up to the visible wavelengths at low bias voltages of the order of a few volts (0-2 V). The fast saturable absorber action of the VCG-gold-SA and the bias-dependent reduction of its loss were successfully demonstrated inside a femtosecond Ti3+:sapphire laser operating near 800 nm. Dispersion compensation was employed by using dispersion control mirrors and a prism pair. At a bias voltage of 1.2 V, the laser operated with improved power performance in comparison with that at zero bias, and the VCG-gold-SA initiated the generation of nearly transform-limited pulses as short as 48 fs at a pulse repetition rate of 131.7 MHz near 830 nm. To the best of our knowledge, this represents the shortest wavelength where a VCG-gold-SA has been employed as a mode locker with adjustable loss.

Graphene-gold supercapacitor as a voltage controlled saturable absorber for femtosecond pulse generation.

We report, for the first time to the best of our knowledge, use of a graphene-gold supercapacitor as a voltage controlled fast saturable absorber for femtosecond pulse generation. The unique design involving only one graphene electrode lowers the insertion loss of the device, in comparison with capacitor designs with two graphene electrodes. Furthermore, use of the high-dielectric electrolyte allows reversible, adjustable control of the absorption level up to the visible region with low bias voltages of only a few volts (0-2 V). The fast saturable absorber action of the graphene-gold supercapacitor was demonstrated inside a multipass-cavity Cr:forsterite laser to generate nearly transform-limited, sub-100 fs pulses at a pulse repetition rate of 4.51 MHz at 1.24 µm.

Dynamic tuning of plasmon resonance in the visible using graphene.

We report active electrical tuning of plasmon resonance of silver nanoprisms (Ag NPs) in the visible spectrum. Ag NPs are placed in close proximity to graphene which leads to additional tunable loss for the plasmon resonance. The ionic gating of graphene modifies its Fermi level from 0.2 to 1 eV, which then affects the absorption of graphene due to Pauli blocking. Plasmon resonance frequency and linewidth of Ag NPs can be reversibly shifted by 20 and 35 meV, respectively. The coupled graphene-Ag NPs system can be classically described by a damped harmonic oscillator model. Atomic layer deposition allows for controlling the graphene-Ag NP separation with atomic-level precision to optimize coupling between them.

Graphene mode-locked Cr:LiSAF laser at 850 nm.

We report, for the first time to our knowledge, a mode-locked femtosecond Cr:LiSAF laser initiated with a high-quality monolayer graphene saturable absorber (GSA), synthesized by chemical-vapor deposition. The tight-focusing resonator architecture made it possible to operate the Cr:LiSAF laser with only two 135 mW, 660 nm low-cost single-mode diode lasers. At a pump power of 270 mW, the laser produced nearly transform-limited 68 fs pulses with an average power of 11.5 mW at 850 nm. The repetition rate was around 132 MHz, corresponding to a pulse energy and peak power of 86 pJ and 1.26 kW, respectively. Once mode locking was initiated with the GSA, stable, uninterrupted femtosecond pulse generation could be sustained for hours. The saturation fluence and the modulation depth of the GSA were further determined to be 28 µJ/cm2 and 0.62%, respectively.

Graphene-enabled electrically controlled terahertz spatial light modulators.

In this Letter, we demonstrate a broadband terahertz (THz) spatial light modulator using 5×5 arrays of large area graphene supercapacitors. Our approach relies on controlling spatial charge distribution on a passive matrix array of patterned graphene electrodes. By changing the voltage bias applied to the rows and columns, we were able to pattern the THz transmittance through the device with high modulation depth and low operation voltage. We anticipate that the simplicity of the device architecture with high contrast THz modulation over a broad spectral range could provide new tools for THz imaging and communication systems.

Topological engineering of terahertz light using electrically tunable exceptional point singularities.

The topological structure associated with the branch point singularity around an exceptional point (EP) can provide tools for controlling the propagation of light. Through use of graphene-based devices, we demonstrate the emergence of EPs in an electrically controlled interaction between light and a collection of organic molecules in the terahertz regime at room temperature. We show that the intensity and phase of terahertz pulses can be controlled by a gate voltage, which drives the device across the EP. Our electrically tunable system allows reconstruction of the Riemann surface associated with the complex energy landscape and provides topological control of light by tuning the loss imbalance and frequency detuning of interacting modes. Our approach provides a platform for developing topological optoelectronics and studying the manifestations of EP physics in light-matter interactions.

Electrically switchable metadevices via graphene.

Metamaterials bring subwavelength resonating structures together to overcome the limitations of conventional materials. The realization of active metadevices has been an outstanding challenge that requires electrically reconfigurable components operating over a broad spectrum with a wide dynamic range. However, the existing capability of metamaterials is not sufficient to realize this goal. By integrating passive metamaterials with active graphene devices, we demonstrate a new class of electrically controlled active metadevices working in microwave frequencies. The fabricated active metadevices enable efficient control of both amplitude (>50 dB) and phase (>90°) of electromagnetic waves. In this hybrid system, graphene operates as a tunable Drude metal that controls the radiation of the passive metamaterials. Furthermore, by integrating individually addressable arrays of metadevices, we demonstrate a new class of spatially varying digital metasurfaces where the local dielectric constant can be reconfigured with applied bias voltages. In addition, we reconfigure resonance frequency of split-ring resonators without changing its amplitude by damping one of the two coupled metasurfaces via graphene. Our approach is general enough to implement various metamaterial systems that could yield new applications ranging from electrically switchable cloaking devices to adaptive camouflage systems.

Graphene as a Reversible and Spectrally Selective Fluorescence Quencher.

We report reversible and spectrally selective fluorescence quenching of quantum dots (QDs) placed in close proximity to graphene. Controlling interband electronic transitions of graphene via electrostatic gating greatly modifies the fluorescence lifetime and intensity of nearby QDs via blocking of the nonradiative energy transfer between QDs and graphene. Using ionic liquid (IL) based electrolyte gating, we are able to control Fermi energy of graphene in the order of 1 eV, which yields electrically controllable fluorescence quenching of QDs in the visible spectrum. Indeed, our technique enables us to perform voltage controllable spectral selectivity among quantum dots at different emission wavelengths. We anticipate that our technique will provide tunable light-matter interaction and energy transfer that could yield hybrid QDs-graphene based optoelectronic devices with novel functionalities, and additionally, may be useful as a spectroscopic ruler, for example, in bioimaging and biomolecular sensing. We propose that graphene can be used as an electrically tunable and wavelength selective fluorescence quencher.

Graphene-enabled electrically switchable radar-absorbing surfaces.

Radar-absorbing materials are used in stealth technologies for concealment of an object from radar detection. Resistive and/or magnetic composite materials are used to reduce the backscattered microwave signals. Inability to control electrical properties of these materials, however, hinders the realization of active camouflage systems. Here, using large-area graphene electrodes, we demonstrate active surfaces that enable electrical control of reflection, transmission and absorption of microwaves. Instead of tuning bulk material property, our strategy relies on electrostatic tuning of the charge density on an atomically thin electrode, which operates as a tunable metal in microwave frequencies. Notably, we report large-area adaptive radar-absorbing surfaces with tunable reflection suppression ratio up to 50 dB with operation voltages <5 V. Using the developed surfaces, we demonstrate various device architectures including pixelated and curved surfaces. Our results provide a significant step in realization of active camouflage systems in microwave frequencies.

Synthesis of Large Area Graphene for High Performance in Flexible Optoelectronic Devices.

This work demonstrates an attractive low-cost route to obtain large area and high-quality graphene films by using the ultra-smooth copper foils which are typically used as the negative electrodes in lithium-ion batteries. We first compared the electronic transport properties of our new graphene film with the one synthesized by using commonly used standard copper foils in chemical vapor deposition (CVD). We observed a stark improvement in the electrical performance of the transistors realized on our graphene films. To study the optical properties on large area, we transferred CVD based graphene to transparent flexible substrates using hot lamination method and performed large area optical scanning. We demonstrate the promise of our high quality graphene films for large areas with ~400 cm(2) flexible optical modulators. We obtained a profound light modulation over a broad spectrum by using the fabricated large area transparent graphene supercapacitors and we compared the performance of our devices with the one based on graphene from standard copper. We propose that the copper foils used in the lithium-ion batteries could be used to obtain high-quality graphene at much lower-cost, with the improved performance of electrical transport and optical properties in the devices made from them.