We present the science and technology roadmap for graphene, related two-dimensional crystals, and hybrid systems, targeting an evolution in technology, that might lead to impacts and benefits reaching into most areas of society. This roadmap was developed within the framework of the European Graphene Flagship and outlines the main targets and research areas as best understood at the start of this ambitious project. We provide an overview of the key aspects of graphene and related materials (GRMs), ranging from fundamental research challenges to a variety of applications in a large number of sectors, highlighting the steps necessary to take GRMs from a state of raw potential to a point where they might revolutionize multiple industries. We also define an extensive list of acronyms in an effort to standardize the nomenclature in this emerging field.

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Science and technology roadmap for graphene, related two-dimensional crystals, and hybrid systems

Light modulation is an essential operation in photonics and optoelectronics. With existing and emerging technologies increasingly demanding compact, efficient, fast and broadband optical modulators, high-performance light modulation solutions are becoming indispensable. The recent realization that 2D layered materials could modulate light with superior performance has prompted intense research and significant advances, paving the way for realistic applications. In this Review, we cover the state of the art of optical modulators based on 2D materials, including graphene, transition metal dichalcogenides and black phosphorus. We discuss recent advances employing hybrid structures, such as 2D heterostructures, plasmonic structures, and silicon and fibre integrated structures. We also take a look at the future perspectives and discuss the potential of yet relatively unexplored mechanisms, such as magneto-optic and acousto-optic modulation.

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Optical modulators with 2D layered materials

In recent years, nanocrystals of metal sulfide materials have attracted scientific research interest for renewable energy applications due to the abundant choice of materials with easily tunable electronic, optical, physical and chemical properties. Metal sulfides are semiconducting compounds where sulfur is an anion associated with a metal cation; and the metal ions may be in mono-, bi- or multi-form. The diverse range of available metal sulfide materials offers a unique platform to construct a large number of potential materials that demonstrate exotic chemical, physical and electronic phenomena and novel functional properties and applications. To fully exploit the potential of these fascinating materials, scalable methods for the preparation of low-cost metal sulfides, heterostructures, and hybrids of high quality must be developed. This comprehensive review indicates approaches for the controlled fabrication of metal sulfides and subsequently delivers an overview of recent progress in tuning the chemical, physical, optical and nano- and micro-structural properties of metal sulfide nanocrystals using a range of material fabrication methods. For hydrogen energy production, three major approaches are discussed in detail: electrocatalytic hydrogen generation, powder photocatalytic hydrogen generation and photoelectrochemical water splitting. A variety of strategies such as structural tuning, composition control, doping, hybrid structures, heterostructures, defect control, temperature effects and porosity effects on metal sulfide nanocrystals are discussed and how they are exploited to enhance performance and develop future energy materials. From this literature survey, energy conversion currently relies on a limited range of metal sulfides and their composites, and several metal sulfides are immature in terms of their dissolution, photocorrosion and long-term durability in electrolytes during water splitting. Future research directions for innovative metal sulfides should be closely allied to energy and environmental issues, along with their advanced characterization, and developing new classes of metal sulfide materials with well-defined fabrication methods.

Recent advances in metal sulfides: from controlled fabrication to electrocatalytic, photocatalytic and photoelectrochemical water splitting and beyond

Nanotubes and graphene have emerged as promising materials for use in ultrafast fibre lasers. Their unique electrical and optical properties enable them to be used as saturable absorbers that have fast responses and broadband operation and that can be easily integrated in fibre lasers.

Nanotube and graphene saturable absorbers for fibre lasers

Direct printing of functional inks is critical for applications in diverse areas including electrochemical energy storage, smart electronics and healthcare. However, the available printable ink formulations are far from ideal. Either surfactants/additives are typically involved or the ink concentration is low, which add complexity to the manufacturing and compromises the printing resolution. Here, we demonstrate two types of two-dimensional titanium carbide (Ti3C2Tx) MXene inks, aqueous and organic in the absence of any additive or binary-solvent systems, for extrusion printing and inkjet printing, respectively. We show examples of all-MXene-printed structures, such as micro-supercapacitors, conductive tracks and ohmic resistors on untreated plastic and paper substrates, with high printing resolution and spatial uniformity. The volumetric capacitance and energy density of the all-MXene-printed micro-supercapacitors are orders of magnitude greater than existing inkjet/extrusion-printed active materials. The versatile direct-ink-printing technique highlights the promise of additive-free MXene inks for scalable fabrication of easy-to-integrate components of printable electronics.

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Additive-free MXene inks and direct printing of micro-supercapacitors

Black phosphorus is a two-dimensional material of great interest, in part because of its high carrier mobility and thickness dependent direct bandgap. However, its instability under ambient conditions limits material deposition options for device fabrication. Here we show a black phosphorus ink that can be reliably inkjet printed, enabling scalable development of optoelectronic and photonic devices. Our binder-free ink suppresses coffee ring formation through induced recirculating Marangoni flow, and supports excellent consistency (  30 days) oxidation. We demonstrate printed black phosphorus as a passive switch for ultrafast lasers, stable against intense irradiation, and as a visible to near-infrared photodetector with high responsivities. Our work highlights the promise of this material as a functional ink platform for printed devices. Atomically thin black phosphorus shows promise for optoelectronics and photonics, yet its instability under environmental conditions and the lack of well-established large-area synthesis protocols hinder its applications. Here, the authors demonstrate a stable black phosphorus ink suitable for printed ultrafast lasers and photodetectors.

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Black phosphorus ink formulation for inkjet printing of optoelectronics and photonics

We demonstrate mode-locking of a thulium-doped fiber laser operating at 1.94 μm, using a graphene-polymer based saturable absorber. The laser outputs 3.6 ps pulses, with ~0.4 nJ energy and an amplitude fluctuation ~0.5%, at 6.46 MHz. This is a simple, low-cost, stable and convenient laser oscillator for applications where eye-safe and low-photon-energy light sources are required, such as sensing and biomedical diagnostics.

Tm-doped fiber laser mode-locked by graphene-polymer composite

We fabricate a free-standing few-layer molybdenum disulfide (MoS2)-polymer composite by liquid phase exfoliation of chemically pristine MoS2 crystals and use this to demonstrate a wideband tunable, ultrafast mode-locked fiber laser. Stable, picosecond pulses, tunable from 1,535 nm to 1,565 nm, are generated, corresponding to photon energies below the MoS2 material bandgap. These results contribute to the growing body of work studying the nonlinear optical properties of transition metal dichalcogenides that present new opportunities for ultrafast photonic applications.

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Solution processed MoS2-PVA composite for sub-bandgap mode-locking of a wideband tunable ultrafast er:fiber laser

We demonstrate mode-locking of a thulium-doped fiber laser operating at 1.94\mu m, using a graphene-based saturable absorber. The laser outputs 3.6ps pulses, with~0.4nJ energy and an amplitude fluctuation~0.5%, at 6.46MHz. This is a simple, low-cost, stable and convenient laser oscillator for applications where eye-safe and low-photon-energy light sources are required, such as sensing and biomedical diagnostics

Meng Zhang

Papers

Black phosphorus ink formulation for inkjet printing of optoelectronics and photonics

Tm-doped fiber laser mode-locked by graphene-polymer composite

Solution processed MoS2-PVA composite for sub-bandgap mode-locking of a wideband tunable ultrafast er:fiber laser

Tm-doped fiber laser mode-locked by graphene-polymer composite

2D Black Phosphorus Saturable Absorbers for Ultrafast Photonics