Publications by authors named "Simon C Boehme"

Colloidal quantum dots (QDs) are promising regenerable photoredox catalysts offering broadly tunable redox potentials along with high absorption coefficients. QDs have thus far been examined for various organic transformations, water splitting, and CO reduction. Vast opportunities emerge from coupling QDs with other homogeneous catalysts, such as transition metal complexes or organic dyes, into hybrid nanoassemblies exploiting energy transfer (ET), leveraging a large absorption cross-section of QDs and long-lived triplet states of cocatalysts.

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The compositional engineering of lead-halide perovskite nanocrystals (NCs) via the A-site cation represents a lever to fine-tune their structural and electronic properties. However, the presently available chemical space remains minimal since, thus far, only three A-site cations have been reported to favor the formation of stable lead-halide perovskite NCs, i.e.

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The brightness of an emitter is ultimately described by Fermi's golden rule, with a radiative rate proportional to its oscillator strength times the local density of photonic states. As the oscillator strength is an intrinsic material property, the quest for ever brighter emission has relied on the local density of photonic states engineering, using dielectric or plasmonic resonators. By contrast, a much less explored avenue is to boost the oscillator strength, and hence the emission rate, using a collective behaviour termed superradiance.

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Understanding the origin of electron-phonon coupling in lead halide perovskites is key to interpreting and leveraging their optical and electronic properties. Here we show that photoexcitation drives a reduction of the lead-halide-lead bond angles, a result of deformation potential coupling to low-energy optical phonons. We accomplish this by performing femtosecond-resolved, optical-pump-electron-diffraction-probe measurements to quantify the lattice reorganization occurring as a result of photoexcitation in nanocrystals of FAPbBr.

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The success of colloidal semiconductor nanocrystals (NCs) in science and optoelectronics is inextricable from their surfaces. The functionalization of lead halide perovskite NCs poses a formidable challenge because of their structural lability, unlike the well-established covalent ligand capping of conventional semiconductor NCs. We posited that the vast and facile molecular engineering of phospholipids as zwitterionic surfactants can deliver highly customized surface chemistries for metal halide NCs.

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The highly controlled, microfluidic template-assisted self-assembly of CsPbBr nanocrystals into spherical supraparticles is presented, achieving precise control over average supraparticle size through the variation of nanocrystal concentration and droplet size; thus facilitating the synthesis of highly monodisperse, sub-micron supraparticles (with diameters between 280 and 700 nm).

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The success of the colloidal semiconductor quantum dots (QDs) field is rooted in the precise synthetic control of QD size, shape, and composition, enabling electronically well-defined functional nanomaterials that foster fundamental science and motivate diverse fields of applications. While the exploitation of the strong confinement regime has been driving commercial and scientific interest in InP or CdSe QDs, such a regime has still not been thoroughly explored and exploited for lead-halide perovskite QDs, mainly due to a so far insufficient chemical stability and size monodispersity of perovskite QDs smaller than about 7 nm. Here, we demonstrate chemically stable strongly confined 5 nm CsPbBr colloidal QDs via a postsynthetic treatment employing didodecyldimethylammonium bromide ligands.

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With increasing computing demands, serial processing in von Neumann architectures built with zeroth-order complexity digital circuits is saturating in computational capacity and power, entailing research into alternative paradigms. Brain-inspired systems built with memristors are attractive owing to their large parallelism, low energy consumption, and high error tolerance. However, most demonstrations have thus far only mimicked primitive lower-order biological complexities using devices with first-order dynamics.

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All-inorganic lead-halide perovskite (LHP) (CsPbX , X = Cl, Br, I) quantum dots (QDs) have emerged as a competitive platform for classical light-emitting devices (in the weak light-matter interaction regime, e.g., LEDs and laser), as well as for devices exploiting strong light-matter interaction at room temperature.

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Colloidal lead halide perovskite nanocrystals are of interest as photoluminescent quantum dots (QDs) whose properties depend on the size and shape. They are normally synthesized on subsecond time scales through hard-to-control ionic metathesis reactions. We report a room-temperature synthesis of monodisperse, isolable, spheroidal APbBr QDs ("A" indicates cesium, formamidinium, and methylammonium) that are size tunable from 3 to >13 nanometers.

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Semiconductor quantum dots have long been considered artificial atoms, but despite the overarching analogies in the strong energy-level quantization and the single-photon emission capability, their emission spectrum is far broader than typical atomic emission lines. Here, by using ab-initio molecular dynamics for simulating exciton-surface-phonon interactions in structurally dynamic CsPbBr quantum dots, followed by single quantum dot optical spectroscopy, we demonstrate that emission line-broadening in these quantum dots is primarily governed by the coupling of excitons to low-energy surface phonons. Mild adjustments of the surface chemical composition allow for attaining much smaller emission linewidths of 35-65 meV (vs.

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Attaining pure single-photon emission is key for many quantum technologies, from optical quantum computing to quantum key distribution and quantum imaging. The past 20 years have seen the development of several solid-state quantum emitters, but most of them require highly sophisticated techniques (e.g.

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CsPbBr (0D) nanocrystals at room temperature have both been reported as nonemissive and green-emissive systems in conflicting reports, with no consensus regarding both the origin of the green emission and the emission quenching mechanism. Here, via ab initio molecular dynamics (AIMD) simulations and temperature-dependent photoluminescence (PL) spectroscopy, we show that the PL in these 0D metal halides is thermally quenched well below 300 K via strong electron-phonon coupling. To unravel the source of green emission reported for bulk 0D systems, we further study two previously suggested candidate green emitters: (i) a Br vacancy, which we demonstrate to present a strong thermal emission quenching at room temperature; (ii) an impurity, based on octahedral connectivity, that succeeds in suppressing nonradiative quenching via a reduced electron-phonon coupling in the corner-shared lead bromide octahedral network.

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Article Synopsis
  • The study focuses on understanding how charge carriers interact with the polar lattice in CsPbBr perovskites under nonequilibrium conditions, essential for developing advanced optoelectronic devices.
  • Researchers identify a specific polaronic distortion caused by electron-phonon coupling, leading to significant lattice changes when exposed to light, which they quantify with high precision.
  • By combining time-resolved and temperature-dependent X-ray studies, the researchers demonstrate that structural deformations at Br and Pb sites are linked to carrier recombination, rather than just thermal effects.
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Trap states play a crucial role in the design of colloidal quantum dot (QD)-based technologies. The presence of these in-gap states can either significantly limit the efficiency of devices (e.g.

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Luminescent organic-inorganic low-dimensional ns metal halides are of rising interest as thermographic phosphors. The intrinsic nature of the excitonic self-trapping provides for reliable temperature sensing due to the existence of a temperature range, typically 50-100 K wide, in which the luminescence lifetimes (and quantum yields) are steeply temperature-dependent. This sensitivity range can be adjusted from cryogenic temperatures to above room temperature by structural engineering, thus enabling diverse thermometric and thermographic applications ranging from protein crystallography to diagnostics in microelectronics.

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We combine state-of-the-art ultrafast photoluminescence and absorption spectroscopy and nonadiabatic molecular dynamics simulations to investigate charge-carrier cooling in CsPbBr nanocrystals over a very broad size regime, from 0.8 to 12 nm. Contrary to the prevailing notion that polaron formation slows down charge-carrier cooling in lead-halide perovskites, no suppression of carrier cooling is observed in CsPbBr nanocrystals except for a slow cooling (over ∼10 ps) of "warm" electrons in the vicinity (within ∼0.

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Colloidal lead halide perovskite nanocrystals (NCs) have recently emerged as versatile photonic sources. Their processing and luminescent properties are challenged by the lability of their surfaces, i.e.

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All-inorganic cesium lead halide perovskite nanocrystals are extensively studied because of their outstanding optoelectronic properties. Being of a cubic shape and typically featuring a narrow size distribution, CsPbX (X = Cl, Br, and I) nanocrystals are the ideal starting material for the development of homogeneous thin films as required for photovoltaic and optoelectronic applications. Recent experiments reveal spontaneous merging of drop-casted CsPbBr nanocrystals, which is promoted by humidity and mild-temperature treatments and arrested by electron beam irradiation.

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Charge trapping is an ubiquitous process in colloidal quantum-dot solids and a major limitation to the efficiency of quantum dot based devices such as solar cells, LEDs, and thermoelectrics. Although empirical approaches led to a reduction of trapping and thereby efficiency enhancements, the exact chemical nature of the trapping mechanism remains largely unidentified. In this study, we determine the density of trap states in CdTe quantum-dot solids both experimentally, using a combination of electrochemical control of the Fermi level with ultrafast transient absorption and time-resolved photoluminescence spectroscopy, and theoretically, via density functional theory calculations.

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Ligand exchange is a much-used method to increase the conductivity of colloidal quantum-dot films by replacing long insulating ligands on quantum-dot surfaces with shorter ones. Here we show that while some ligands indeed replace the original ones as expected, others may be used to controllably remove the native ligands and induce epitaxial necking of specific crystal facets. In particular, we demonstrate that amines strip lead oleate from the (100) surfaces of PbSe quantum dots.

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Understanding and controlling charge transfer between different kinds of colloidal quantum dots (QDs) is important for devices such as light-emitting diodes and solar cells and for thermoelectric applications. Here we study photoinduced electron transfer between CdTe and CdSe QDs in a QD film. We find that very efficient electron trapping in CdTe QDs obstructs electron transfer to CdSe QDs under most conditions.

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Films of colloidal quantum dots (QDs) show great promise for application in optoelectronic devices. Great advances have been made in recent years in designing efficient QD solar cells and LEDs. A very important aspect in the design of devices based on QD films is the knowledge of their absolute energy levels.

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