Manipulating light in two-dimensional layered materials

Graphene and layered two-dimensional (2D) materials have set a new paradigm in modern solid-state physics and technology. In particular their exceptional optical and electronic properties have shown great promise for novel applications in light detection. However, several challenges remain to fully exploit such properties in commercial devices. Such challenges include the limited linear dynamic range (LDR) of graphene-based photodetectors (PDs), the efficient extraction of photoexcited charges and ultimately the environmental stability of such atomically-thin materials. In order to overcome the aforementioned limits, novel approaches to tune the properties of graphene and semiconducting \ce{HfS2} are explored in this work, using chemical functionalisation and laser-irradiation. Intercalation of graphene with \ce{FeCl3} is shown to lead to a highly tunable material, with unprecedented stability in ambient conditions. This material is used to define photo-active junctions with an unprecedented LDR via laser-irradiation. Intercalation with \ce{FeCl3} is also used to demonstrate the first all-graphene position-sensitive photodetector (PSD) promising for novel sensing applications. Finally, laser-irradiation is employed, to perform controlled oxidation of ultra-thin \ce{HfS2}, which leads to induced strain in the material and a consequent spatially-varying bandgap. Such structure is used to demonstrate, for the first time, efficient extraction of photogenerated carriers trough the so-called ``charge-funnel'' effect, paving the way to the development of ultra-thin straintronic devices.European Commissio

Extraordinary linear dynamic range in laser-defined functionalized graphene photodetectors

Graphene-based photodetectors have demonstrated mechanical flexibility, large operating bandwidth, and broadband spectral response. However, their linear dynamic range (LDR) is limited by graphene's intrinsichot-carrier dynamics, which causes deviation from a linear photoresponse at low incident powers. At the same time, multiplication of hot carriers causes the photoactive region to be smeared over distances of a few micro-meters, limiting the use of graphene in high-resolution applications. We present a novel method for engineer-ing photoactive junctions in FeCl3-intercalated graphene using laser irradiation. Photocurrent measured at these planar junctions shows an extraordinary linear response with an LDR value at least 4500 times larger than that of other graphene devices (44 dB) while maintaining high stability against environmental contamination without the need for encapsulation. The observed photoresponse is purely photovoltaic, demonstrating complete quenching of hot-carrier effects. These results pave the way toward the design of ultrathin photode-tectors with unprecedented LDR for high-definition imaging and sensing.Comment: 44 pages, includes supplementar

Functionalised hexagonal-domain graphene for position-sensitive photodetectors

Graphene's unique photoresponse has been largely used in a multitude of optoelectronics applications ranging from broadband photodetectors to wave-guide modulators. In this work we extend the range of applications to position-sensitive photodetectors (PSDs) using FeCl3-intercalated hexagonal domains of graphene grown by atmospheric pressure chemical vapour deposition (APCVD). The FeCl3-based chemical functionalisation of APCVD graphene crystals is affected by the presence of wrinkles and results in a non-uniform doping of the graphene layers. This doping profile creates multiple p–p+ photoactive junctions which show a linear and bipolar photoresponse with respect to the position of a focused light spot, which is ideal for the realization of a PSD. Our study paves the way towards the fabrication of flexible and transparent PSDs that could be embedded in smart textile and wearable electronics

Strain-engineered inverse charge-funnelling in layered semiconductors

The control of charges in a circuit due to an external electric field is ubiquitous to the exchange, storage and manipulation of information in a wide range of applications. Conversely, the ability to grow clean interfaces between materials has been a stepping stone for engineering built-in electric fields largely exploited in modern photovoltaics and opto-electronics. The emergence of atomically thin semiconductors is now enabling new ways to attain electric fields and unveil novel charge transport mechanisms. Here, we report the first direct electrical observation of the inverse charge-funnel effect enabled by deterministic and spatially resolved strain-induced electric fields in a thin sheet of HfS2. We demonstrate that charges driven by these spatially varying electric fields in the channel of a phototransistor lead to a 350% enhancement in the responsivity. These findings could enable the informed design of highly efficient photovoltaic cells

Extraordinary linear dynamic range in laser-defined functionalized graphene photodetectors

Graphene-based photodetectors have demonstrated mechanical flexibility, large operating bandwidth, and broadband spectral response. However, their linear dynamic range (LDR) is limited by graphene’s intrinsic hot-carrier dynamics, which causes deviation from a linear photoresponse at low incident powers. At the same time, multiplication of hot carriers causes the photoactive region to be smeared over distances of a few micrometers, limiting the use of graphene in high-resolution applications. We present a novel method for engineering photoactive junctions in FeCl3-intercalated graphene using laser irradiation. Photocurrent measured at these planar junctions shows an extraordinary linear response with an LDR value at least 4500 times larger than that of other graphene devices (44 dB) while maintaining high stability against environmental contamination without the need for encapsulation. The observed photoresponse is purely photovoltaic, demonstrating complete quenching of hot-carrier effects. These results pave the way toward the design of ultrathin photodetectors with unprecedented LDR for high-definition imaging and sensing.Peer Reviewe