Explore the vast range of titles available.

Quantum information processing—which relies on spin defects or single-photon emission—has shown quantum advantage in proof-of-principle experiments including microscopic imaging of electromagnetic fields, strain and temperature in applications ranging from battery research to neuroscience. However, critical gaps remain on the path to wider applications, including a need for improved functionalization, deterministic placement, size homogeneity and greater programmability of multifunctional properties. Colloidal semiconductor nanocrystals can close these gaps in numerous application areas, following years of rapid advances in synthesis and functionalization. In this Review, we specifically focus on three key topics: optical interfaces to long-lived spin states, deterministic placement and delivery for sensing beyond the standard quantum limit, and extensions to multifunctional colloidal quantum circuits. This Review highlights the current potential for colloidal quantum dots for applications in quantum sensing and quantum circuits.

Low-dimensional perovskites have—in view of their high radiative recombination rates—shown great promise in achieving high luminescence brightness and colour saturation. Here we investigate the effect of electron–phonon interactions on the luminescence of single crystals of two-dimensional perovskites, showing that reducing these interactions can lead to bright blue emission in two-dimensional perovskites. Resonance Raman spectra and deformation potential analysis show that strong electron–phonon interactions result in fast non-radiative decay, and that this lowers the photoluminescence quantum yield (PLQY). Neutron scattering, solid-state NMR measurements of spin–lattice relaxation, density functional theory simulations and experimental atomic displacement measurements reveal that molecular motion is slowest, and rigidity greatest, in the brightest emitter. By varying the molecular configuration of the ligands, we show that a PLQY up to 79% and linewidth of 20 nm can be reached by controlling crystal rigidity and electron–phonon interactions. Designing crystal structures with electron–phonon interactions in mind offers a previously underexplored avenue to improve optoelectronic materials' performance.

A special perovskite material design is demonstrated to operate as a wideband, achromatic quarter-wave plate.

By switching shell growth on and off on the (0001) facet of wurtzite CdSe cores to produce a built-in biaxial strain that lowers the optical gain threshold, we achieve continuous-wave lasing in colloidal quantum dot films. SQUEEZED LIGHT The electronic structure of colloidal quantum dots lends them a host of desirable optical properties, but they typically perform poorly as laser materials. Fengjia Fan et al. have developed a scheme for tuning this electronic structure in such a way that the barriers to laser action might be overcome. Specifically, they developed a synthesis strategy in which the shell of material encompassing the core of the quantum dot is asymmetric and compressive. This effectively squeezes the particle, thereby modifying the electronic structure to favour laser-like emissions. Colloidal quantum dots (CQDs) feature a low degeneracy of electronic states at the band edges compared with the corresponding bulk material 1 , as well as a narrow emission linewidth 2 , 3 . Unfortunately for potential laser applications, this degeneracy is incompletely lifted in the valence band, spreading the hole population among several states at room temperature 4 , 5 , 6 . This leads to increased optical gain thresholds, demanding high photoexcitation levels to achieve population inversion (more electrons in excited states than in ground states—the condition for optical gain). This, in turn, increases Auger recombination losses 7 , limiting the gain lifetime to sub-nanoseconds and preventing steady laser action 8 , 9 . State degeneracy also broadens the photoluminescence linewidth at the single-particle level 10 . Here we demonstrate a way to decrease the band-edge degeneracy and single-dot photoluminescence linewidth in CQDs by means of uniform biaxial strain. We have developed a synthetic strategy that we term facet-selective epitaxy: we first switch off, and then switch on, shell growth on the (0001) facet of wurtzite CdSe cores, producing asymmetric compressive shells that create built-in biaxial strain, while still maintaining excellent surface passivation (preventing defect formation, which otherwise would cause non-radiative recombination losses). Our synthesis spreads the excitonic fine structure uniformly and sufficiently broadly that it prevents valence-band-edge states from being thermally depopulated. We thereby reduce the optical gain threshold and demonstrate continuous-wave lasing from CQD solids, expanding the library of solution-processed materials 11 , 12 that may be capable of continuous-wave lasing. The individual CQDs exhibit an ultra-narrow single-dot linewidth, and we successfully propagate this into the ensemble of CQDs.

Quantum dot and well architectures are attractive for infrared optoelectronics, and have led to the realization of compelling light sensors. However, they require well-defined passivated interfaces and rapid charge transport, and this has restricted their efficient implementation to costly vacuum-epitaxially grown semiconductors. Here we report solution-processed, sensitive infrared field-emission photodetectors. Using quantum-dots-in-perovskite, we demonstrate the extraction of photocarriers via field emission, followed by the recirculation of photogenerated carriers. We use in operando ultrafast transient spectroscopy to sense bias-dependent photoemission and recapture in field-emission devices. The resultant photodiodes exploit the superior electronic transport properties of organometal halide perovskites, the quantum-size-tuned absorption of the colloidal quantum dots and their matched interface. These field-emission quantum-dot-in-perovskite photodiodes extend the perovskite response into the short-wavelength infrared and achieve measured specific detectivities that exceed 10 12 Jones. The results pave the way towards novel functional photonic devices with applications in photovoltaics and light emission. Efficient implementation of quantum dot and well architectures are restricted to costly vacuum-epitaxially-grown semiconductors. The authors use quantum dots in perovskite to build field-emission photodiodes that are sensitive across the visible and into the short-wavelength infrared.

Bandtail states in disordered semiconductor materials result in losses in open-circuit voltage ( V oc ) and inhibit carrier transport in photovoltaics. For colloidal quantum dot (CQD) films that promise low-cost, large-area, air-stable photovoltaics, bandtails are determined by CQD synthetic polydispersity and inhomogeneous aggregation during the ligand-exchange process. Here we introduce a new method for the synthesis of solution-phase ligand-exchanged CQD inks that enable a flat energy landscape and an advantageously high packing density. In the solid state, these materials exhibit a sharper bandtail and reduced energy funnelling compared with the previous best CQD thin films for photovoltaics. Consequently, we demonstrate solar cells with higher V oc and more efficient charge injection into the electron acceptor, allowing the use of a closer-to-optimum bandgap to absorb more light. These enable the fabrication of CQD solar cells made via a solution-phase ligand exchange, with a certified power conversion efficiency of 11.28%. The devices are stable when stored in air, unencapsulated, for over 1,000 h. An improved ligand-exchange process allows the realization of solution-deposited films of quantum dots with reduced energetic disorder and, as a result, solar cells with improved open-circuit voltage, charge-carrier transport and stability.

Reduced-dimensional perovskites are attractive light-emitting materials due to their efficient luminescence, color purity, tunable bandgap, and structural diversity. A major limitation in perovskite light-emitting diodes is their limited operational stability. Here we demonstrate that rapid photodegradation arises from edge-initiated photooxidation, wherein oxidative attack is powered by photogenerated and electrically-injected carriers that diffuse to the nanoplatelet edges and produce superoxide. We report an edge-stabilization strategy wherein phosphine oxides passivate unsaturated lead sites during perovskite crystallization. With this approach, we synthesize reduced-dimensional perovskites that exhibit 97 ± 3% photoluminescence quantum yields and stabilities that exceed 300 h upon continuous illumination in an air ambient. We achieve green-emitting devices with a peak external quantum efficiency (EQE) of 14% at 1000 cd m −2 ; their maximum luminance is 4.5 × 10 4  cd m −2 (corresponding to an EQE of 5%); and, at 4000 cd m −2 , they achieve an operational half-lifetime of 3.5 h. Reduced-dimensional halide perovskites are promising for light-emitting diodes but suffer from photo-degradation. Here Quan et al. identify the edge of the perovskite nanoplatelets as the degradation channels and use phosphine oxides to passivate the edges and boost device performance and lifetime.

The light-driven generation of H ₂, the reductive side of water splitting, requires a light absorber or photosensitizer (PS) for electron-hole creation and photoinduced electron transfer. To increase the effectiveness of charge transfer chromophores as PSs, this report describes the attachment of a strongly absorbing organic dye (dipyrromethene-BF ₂, commonly known as Bodipy) to Pt diimine dithiolate charge transfer chromophores and examination of systems containing these dyads for the light-driven generation of H ₂. The use of these dyads increases system activity under green light irradiation (530 nm) relative to systems with either chromophore alone, validating such an approach in designing artificial photosynthetic systems. One dyad system exhibits both high activity and substantial durability (40,000 turnovers relative to PSs over 12 d). New dyads consisting of a strongly absorbing Bodipy (dipyrromethene-BF ₂) dye and a platinum diimine dithiolate (PtN ₂S ₂) charge transfer (CT) chromophore have been synthesized and studied in the context of the light-driven generation of H ₂ from aqueous protons. In these dyads, the Bodipy dye is bonded directly to the benzenedithiolate ligand of the PtN ₂S ₂ CT chromophore. Each of the new dyads contains either a bipyridine (bpy) or phenanthroline (phen) diimine with an attached functional group that is used for binding directly to TiO ₂ nanoparticles, allowing rapid electron photoinjection into the semiconductor. The absorption spectra and cyclic voltammograms of the dyads show that the spectroscopic and electrochemical properties of the dyads are the sum of the individual chromophores (Bodipy and the PtN ₂S ₂ moieties), indicating little electronic coupling between them. Connection to TiO ₂ nanoparticles is carried out by sonication leading to in situ attachment to TiO ₂ without prior hydrolysis of the ester linking groups to acids. For H ₂ generation studies, the TiO ₂ particles are platinized (Pt-TiO ₂) so that the light absorber (the dyad), the electron conduit (TiO ₂), and the catalyst (attached colloidal Pt) are fully integrated. It is found that upon 530 nm irradiation in a H ₂O solution (pH 4) with ascorbic acid as an electron donor, the dyad linked to Pt-TiO ₂ via a phosphonate or carboxylate attachment shows excellent light-driven H ₂ production with substantial longevity, in which one particular dyad [4(bpyP)] exhibits the highest activity, generating ∼40,000 turnover numbers of H ₂ over 12 d (with respect to dye).

The remarkable properties of metal halide perovskites arising from their impressive charge carrier diffusion lengths have led to rapid advances in solution-processed optoelectronics. Unfortunately, diffusion lengths reported in perovskite single crystals have ranged widely – from 3 μm to 3 mm – for ostensibly similar materials. Here we report a contactless method to measure the carrier mobility and further extract the diffusion length: our approach avoids both the effects of contact resistance and those of high electric field. We vary the density of quenchers – epitaxially included within perovskite single crystals – and report the dependence of excited state lifetime in the perovskite on inter-quencher spacing. Our results are repeatable and self-consistent (i.e. they agree on diffusion length for many different quencher concentrations) to within ± 6%. Using this method, we obtain a diffusion length in metal-halide perovskites of 2.6 μm ± 0.1 μm. Reliable and consistent measurement of the carrier diffusion length in metal halide perovskite single crystals has proven difficult. Here Gong, Huang et al. systematically included very dilute quantum dot quenchers into perovskite crystals and develop a contactless and self-consistent method for the task.

In luminescent solar concentrator (LSC) systems, broadband solar energy is absorbed, down-converted and waveguided to the panel edges where peripheral photovoltaic cells convert the concentrated light to electricity. Achieving a low-loss LSC requires reducing the reabsorption of emitted light within the absorbing medium while maintaining high photoluminescence quantum yield (PLQY). Here we employ layered hybrid metal halide perovskites—ensembles of two-dimensional perovskite domains—to fabricate low-loss large-area LSCs that fulfil this requirement. We devised a facile synthetic route to obtain layered perovskite nanoplatelets (PNPLs) that possess a tunable number of layers within each platelet. Efficient ultrafast non-radiative exciton routing within each PNPL (0.1 ps −1 ) produces a large Stokes shift and a high PLQY simultaneously. Using this approach, we achieve an optical quantum efficiency of 26% and an internal concentration factor of 3.3 for LSCs with an area of 10 × 10 cm 2 , which represents a fourfold enhancement over the best previously reported perovskite LSCs. Luminescent solar concentrators are promising for semi-transparent, building-integrated photovoltaic systems. Here the authors minimize the absorption losses by relying on fast energy transfer in multiphase perovskite nanoplatelets to achieve optical quantum efficiency of 26% on 100 cm 2 devices.