Gerasimos Konstantatos

Ultrasensitive solution-cast quantum dot photodetectors.

Solution-processed electronic and optoelectronic devices offer low cost, large device area, physical flexibility and convenient materials integration compared to conventional epitaxially grown, lattice-matched, crystalline semiconductor devices. Although the electronic or optoelectronic performance of these solution-processed devices is typically inferior to that of those fabricated by conventional routes, this can be tolerated for some applications in view of the other benefits. Here we report the fabrication of solution-processed infrared photodetectors that are superior in their normalized detectivity (D*, the figure of merit for detector sensitivity) to the best epitaxially grown devices operating at room temperature. We produced the devices in a single solution-processing step, overcoating a prefabricated planar electrode array with an unpatterned layer of PbS colloidal quantum dot nanocrystals. The devices showed large photoconductive gains with responsivities greater than 103 A W-1. The best devices exhibited a normalized detectivity D* of 1.8 × 1013 jones (1 jones = 1 cm Hz1/2 W-1) at 1.3 µm at room temperature: todays highest performance infrared photodetectors are photovoltaic devices made from epitaxially grown InGaAs that exhibit peak D* in the 1012 jones range at room temperature, whereas the previous record for D* from a photoconductive detector lies at 1011 jones. The tailored selection of absorption onset energy through the quantum size effect, combined with deliberate engineering of the sequence of nanoparticle fusing and surface trap functionalization, underlie the superior performance achieved in this readily fabricated family of devices.

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

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.

Nanostructured materials for photon detection

The detection of photons underpins imaging, spectroscopy, fibre-optic communications and time-gated distance measurements. Nanostructured materials are attractive for detection applications because they can be integrated with conventional silicon electronics and flexible, large-area substrates, and can be processed from the solution phase using established techniques such as spin casting, spray coating and layer-by-layer deposition. In addition, their performance has improved rapidly in recent years. Here we review progress in light sensing using nanostructured materials, focusing on solution-processed materials such as colloidal quantum dots and metal nanoparticles. These devices exhibit phenomena such as absorption of ultraviolet light, plasmonic enhancement of absorption, size-based spectral tuning, multiexciton generation, and charge carrier storage in surface and interface traps.

Depleted-Heterojunction Colloidal Quantum Dot Solar Cells

Colloidal quantum dot (CQD) photovoltaics combine low-cost solution processability with quantum size-effect tunability to match absorption with the solar spectrum. Rapid recent advances in CQD photovoltaics have led to impressive 3.6% AM1.5 solar power conversion efficiencies. Two distinct device architectures and operating mechanisms have been advanced. The first-the Schottky device-was optimized and explained in terms of a depletion region driving electron-hole pair separation on the semiconductor side of a junction between an opaque low-work-function metal and a p-type CQD film. The second-the excitonic device-employed a CQD layer atop a transparent conductive oxide (TCO) and was explained in terms of diffusive exciton transport via energy transfer followed by exciton separation at the type-II heterointerface between the CQD film and the TCO. Here we fabricate CQD photovoltaic devices on TCOs and show that our devices rely on the establishment of a depletion region for field-driven charge transport and separation, and that they also exploit the large bandgap of the TCO to improve rectification and block undesired hole extraction. The resultant depleted-heterojunction solar cells provide a 5.1% AM1.5 power conversion efficiency. The devices employ infrared-bandgap size-effect-tuned PbS CQDs, enabling broadband harvesting of the solar spectrum. We report the highest open-circuit voltages observed in solid-state CQD solar cells to date, as well as fill factors approaching 60%, through the combination of efficient hole blocking (heterojunction) and very small minority carrier density (depletion) in the large-bandgap moiety.

Prospects of Nanoscience with Nanocrystals

Colloidal nanocrystals (NCs, i.e., crystalline nanoparticles) have become an important class of materials with great potential for applications ranging from medicine to electronic and optoelectronic devices. Todays strong research focus on NCs has been prompted by the tremendous progress in their synthesis. Impressively narrow size distributions of just a few percent, rational shape-engineering, compositional modulation, electronic doping, and tailored surface chemistries are now feasible for a broad range of inorganic compounds. The performance of inorganic NC-based photovoltaic and light-emitting devices has become competitive to other state-of-the-art materials. Semiconductor NCs hold unique promise for near- and mid-infrared technologies, where very few semiconductor materials are available. On a purely fundamental side, new insights into NC growth, chemical transformations, and self-organization can be gained from rapidly progressing in situ characterization and direct imaging techniques. New phenomena are constantly being discovered in the photophysics of NCs and in the electronic properties of NC solids. In this Nano Focus, we review the state of the art in research on colloidal NCs focusing on the most recent works published in the last 2 years.

Fast, sensitive and spectrally tuneable colloidal-quantum-dot photodetectors

Solution-processed semiconductors are compatible with a range of substrates, which enables their direct integration with organic circuits, microfluidics, optical circuitry and commercial microelectronics. Ultrasensitive photodetectors based on solution-process colloidal quantum dots operating in both the visible and infrared have been demonstrated, but these devices have poor response times (on the scale of seconds) to changes in illumination, and rapid-response devices based on a photodiode architecture suffer from low sensitivity. Here, we show that the temporal response of these devices is determined by two components--electron drift, which is a fast process, and electron diffusion, which is a slow process. By building devices that exclude the diffusion component, we are able to demonstrate a >1,000-fold improvement in the sensitivity-bandwidth product of tuneable colloidal-quantum-dot photodiodes operating in the visible and infrared.

Hybrid 2D–0D MoS2–PbS Quantum Dot Photodetectors

A hybrid phototransistor consisting of colloidal PbS quantum dots and few layers of MoS2 (≥2 layers) is demonstrated. The hybrid benefits from tailored light absorption in the quantum dots throughout the visible/near infrared region, efficient charge-carrier separation at the p-n interface, and fast carrier transport through the MoS2 channel. It shows responsivity of up to 10(6) A W(-1) and backgate-dependent sensitivity.

Engineering the Temporal Response of Photoconductive Photodetectors via Selective Introduction of Surface Trap States

Photoconductive photodetectors fabricated using simple solution-processing have recently been shown to exhibit high gains (>1000) and outstanding sensitivities ( D* > 10(13) Jones). One ostensible disadvantage of exploiting photoconductive gain is that the temporal response is limited by the release of carriers from trap states. Here we show that it is possible to introduce specific chemical species onto the surfaces of colloidal quantum dots to produce only a single, desired trap state having a carefully selected lifetime. In this way we demonstrate a device that exhibits an attractive photoconductive gain (>10) combined with a response time ( approximately 25 ms) useful in imaging. We achieve this by preserving a single surface species, lead sulfite, while eliminating lead sulfate and lead carboxylate. In doing so we preserve the outstanding sensitivity of these devices, achieving a specific detectivity of 10(12) Jones in the visible, while generating a temporal response suited to imaging applications.

Highly Sensitive, Encapsulated MoS2 Photodetector with Gate Controllable Gain and Speed

Semiconducting, two-dimensional molybdenum disulfide (MoS2) is considered a promising new material for highly sensitive photodetection, because of its atomically thin profile and favorable bandgap. However, reported photodetectors to date show strong variation in performance due to the detrimental and uncontrollable effects of environmental adsorbates on devices due to large surface to volume ratio. Here, we report on highly stable and high-performance monolayer and bilayer MoS2 photodetectors encapsulated with atomic layer deposited hafnium oxide. The protected devices show enhanced electronic properties by isolating them from the ambience as strong n-type doping, vanishing hysteresis, and reduced device resistance. By controlling the gate voltage the responsivity and temporal response can be tuned by several orders of magnitude with R ∼ 10-10(4) A/W and t ∼ 10 ms to 10 s. At strong negative gate voltage, the detector is operated at higher speed and simultaneously exhibits a low-bound, record sensitivity of D* ≥ 7.7 × 10(11) Jones. Our results lead the way for future application of ultrathin, flexible, and high-performance MoS2 detectors and prompt for further investigation in encapsulated transition metal dichalcogenide optoelectronics.

Solution‐Processed Heterojunction Solar Cells Based on p‐type PbS Quantum Dots and n‐type Bi2S3 Nanocrystals

Bi2S3 nanocrystals are employed as an n-type, non-toxic, inorganic, solution-processed semiconductor in thin film solar cells. The first solution processed-inorganic p-n junction based on p-type PbS QDs and n-type Bi2S3 nanocrystals with both phases contributing to photocarrier generation is demonstrated. The reported devices show a power conversion efficiency of 1.6% for 860 nm PbS QDs and over 1% for 1300 nm PbS QDs.