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Nicola Gasparini

Publications and source records attributed to Nicola Gasparini.

6 recordsLinked to original sources

Matching Terahertz and Hall Mobilities as a Hallmark of Intrinsic Charge Transport in Metal-Halide Perovskites

Charge-carrier transport in soft-lattice materials, including metal-halide perovskites, is often perceived to be highly heterogeneous across different length scales, and influenced by both the intrinsic (dynamic) thermal electronic disorder and extrinsic (static) disorder due to crystal defects, impurities, grain boundaries, and surface states. As a consequence, the reported carrier mobilities obtained by different electrical and optical measurement techniques frequently disagree, raising a critical question: can a truly intrinsic charge transport regime (that is, a regime not dominated by static disorder) extend across macroscopic single crystals of these materials? Here, we demonstrate such a regime in an exemplary metal-halide perovskite system, epitaxial CsPbBr$_{3}$ single crystals, where the local mobility obtained via optical pump-terahertz probe (OPTP) spectroscopy quantitatively agrees with the macroscopic transport mobility across a broad range of experimental conditions. Using a dedicated device platform that enables concurrent Hall-effect and OPTP measurements on the same single-crystalline sample, we obtain consistent room-temperature mobilities of ~ 30 cm$^{2}$V$^{-1}$s$^{-1}$, among the highest reliably reported for CsPbBr$_{3}$. Both techniques reveal band-like temperature dependence of the hole mobility with similar power exponents, confirming that the same intrinsic transport mechanism governs the ultrafast/local and steady-state/macroscopic responses. These results show that defect-free charge transport is achievable in soft-lattice perovskites on millimetre length scales and establish a robust methodology for benchmarking intrinsic mobility in emerging semiconductors.

cond-mat.mtrl-sci

Aqueous Preparation of CsPbBr3 Perovskite Nanocrystals Under Ambient Conditio

Metal halide perovskites (MHPs) have had a profound impact on numerous emerging optoelectronic technologies, achieving performance metrics that rival or exceed incumbent materials. This impact is underpinned by the exceptional properties of MHPs, including tuneable band gaps, high absorption coefficients, long carrier diffusion lengths and combined with uncomplicated synthesis methods. However, current MHP production relies on the toxic solvents, which pose significant environmental and health risks. Moreover, these methods often require complex multi component solvent systems and thermal processing to achieve the desired material phases, further hindering scalability and sustainability. Overcoming these challenges is critical to the future development of MHP-based technologies. Overcoming these challenges is critical to the future development of MHP-based technologies. Here, we present a novel water-based solvent system and synthetic approach for the preparation of size-controlled CsPbBr3 perovskite nanocrystals in ambient air and at room temperature. The photoluminescence quantum yield (PLQY) of CsPbBr3 erovskite nanocrystals (PNCs) exceeds 60 precent. To demonstrate the light to current conversion ability of our PNCs a series of photoconductors were prepared, with the best performing devices achieving a specific detectivity (D*) of 1.2 x 10^11 Jones. Thus, this green, scalable, and low-cost approach offers a sustainable pathway for precise size and compositional control of MHP nanocrystals, opening new possibilities for environmentally friendly optoelectronic applications.

cond-mat.mtrl-sci

Polaritons in non-fullerene acceptors for high responsivity angle-independent organic narrowband infrared photodiodes

Narrowband infrared organic photodetectors are in great demand for sensing, imaging, and spectroscopy applications. However, most existing strategies for narrowband detection depend on spectral filtering either through saturable absorption, which requires active layers exceeding 500 nm, restricting the choice of materials for producing high-quality films, or cavity effects, which inherently introduce strong angular dispersion. Microcavity exciton-polariton (polariton) modes, which emerge from strong exciton-photon coupling, have recently been explored as an angular dispersion suppression strategy for organic optoelectronics. In this work, we present the first narrowband infrared polariton organic photodiode that combines angle-independent response with a record-high responsivity of 0.24 A/W at 965 nm and -2 V. This device, featuring a 100-nm-thin active layer comprising a non-fullerene acceptor, exhibits a detection mode with a full-width at half maximum of less than 30 nm and a marginal angular dispersion of under 15 nm across $\pm$$45^\circ$. This study highlights the potential of polaritons as an innovative platform for developing next-generation optoelectronic devices that achieve simultaneous enhancements in optical and electronic performance.

physics.optics

Roadmap on Photovoltaic Absorber Materials for Sustainable Energy Conversion

Photovoltaics (PVs) are a critical technology for curbing growing levels of anthropogenic greenhouse gas emissions, and meeting increases in future demand for low-carbon electricity. In order to fulfil ambitions for net-zero carbon dioxide equivalent (CO 2 eq) emissions worldwide, the global cumulative capacity of solar PVs must increase by an order of magnitude from 0.9 TWp in 2021 to 8.5 TWp by 2050 according to the International Renewable Energy Agency, which is considered to be a highly conservative estimate. In 2020, the Henry Royce Institute brought together the UK PV community to discuss the critical technological and infrastructure challenges that need to be overcome to address the vast challenges in accelerating PV deployment. Herein, we examine the key developments in the global community, especially the progress made in the field since this earlier roadmap, bringing together experts primarily from the UK across the breadth of the photovoltaics community. The focus is both on the challenges in improving the efficiency, stability and levelized cost of electricity of current technologies for utility-scale PVs, as well as the fundamental questions in novel technologies that can have a significant impact on emerging markets, such as indoor PVs, space PVs, and agrivoltaics. We discuss challenges in advanced metrology and computational tools, as well as the growing synergies between PVs and solar fuels, and offer a perspective on the environmental sustainability of the PV industry. Through this roadmap, we emphasize promising pathways forward in both the short- and long-term, and for communities working on technologies across a range of maturity levels to learn from each other.

physics.app-ph

Fast near-infrared photodetectors based on nontoxic and solution-processable AgBiS2

Solution-processable near-infrared (NIR) photodetectors are urgently needed for a wide range of next-generation electronics, including sensors, optical communications and bioimaging. However, there is currently a compromise between low toxicity and slow (<300 kHz cut-off frequency) organic materials versus faster detectors (>300 kHz cut-off frequency) based on compounds containing toxic lead or cadmium. Herein, we circumvent this trade-off by developing solution-processed AgBiS2 photodetectors with high cut-off frequencies under both white light (>1 MHz) and NIR (approaching 500 kHz) illumination. These high cut-off frequencies are due to the short transit distances of charge-carriers in the AgBiS2 photodetectors, which arise from the strong light absorption of these materials, such that film thicknesses well below 120 nm are adequate to absorb >65% of near-infrared to visible light. By finely controlling the thickness of the photoactive layer, we can modulate the charge-collection efficiency, achieve low dark current densities, and minimize the effects of ion migration to realize fast photodetectors that are stable in air. These outstanding characteristics enable real-time heartbeat sensors based on NIR AgBiS2 photodetectors. # equal contribution, * corresponding authors

cond-mat.mtrl-sci

Inkjet printed circuits with two-dimensional semiconductor inks for high-performance electronics

Air-stable semiconducting inks suitable for complementary logic are key to create low-power printed integrated circuits (ICs). High-performance printable electronic inks with two-dimensional materials have the potential to enable the next generation of high performance, low-cost printed digital electronics. Here we demonstrate air-stable, low voltage (< 5 V) operation of inkjet-printed n-type molybdenum disulfide (MoS2) and p-type indacenodithiophene-co-benzothiadiazole (IDT-BT) field-effect transistors (FETs), estimating a switching time of τ ~ 3.3 μs for the MoS2 FETs. We achieve this by engineering high-quality MoS2 and air-stable IDT-BT inks suitable for inkjet-printing complementary pairs of n-type MoS2 and p-type IDT-BT FETs. We then integrate MoS2 and IDT-BT FETs to realise inkjet-printed complementary logic inverters with a voltage gain |Av| ~ 4 when in resistive load configuration and |Av| ~ 1.36 in complementary configuration. These results represent a key enabling step towards ubiquitous long-term stable, low-cost printed digital ICs.

cond-mat.mes-hall