Publications by authors named "Herman Duim"

Article Synopsis
  • The optical response of 2D layered perovskites features closely spaced spectral signatures, interpreted as phonon replicas, with an energy separation ranging from 12 to 40 meV, depending on the material.
  • These materials also show a strong scattering response in resonant Raman spectroscopy above roughly 200 cm (or 25 meV), which is linked to the presence of polarons, exhibiting a distinctive spectral pattern deviating from the Rayleigh line.
  • A significant Huang-Rhys factor (S > 6) suggests strong coupling between charge carriers and the lattice, with polaron binding energies between 20-35 meV, influencing the optical properties critical for future opto-electronic applications.
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Metal halide perovskites show the capability of performing structural transformation, allowing the formation of functional heterostructures. Unfortunately, the elusive mechanism governing these transformations limits their technological application. Herein, the mechanism of 2D-3D structural transformation is unraveled as catalyzed by solvents.

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Scarce information is available on the thin film morphology of Dion-Jacobson halide perovskites. However, the microstructure can have a profound impact on a material's photophysics and its potential for optoelectronic applications. The microscopic mechanisms at play in the prototypical 1,4-phenylenedimethanammonium lead iodide (PDMAPbI) Dion-Jacobson compound are here elucidated through a combination of hyperspectral photoluminescence and Raman spectro-microscopy supported by x-ray diffraction.

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Conjugated polymers with narrow band gaps are particularly useful for sorting and discriminating semiconducting single-walled carbon nanotubes (s-SWCNT) due to the low charge carrier injection barrier for transport. In this paper, we report two newly synthesized narrow-band-gap conjugated polymers ( and ) based on naphthalene diimide (NDI) and thienylennevinylene (TVT) building blocks, decorated with different polar side chains that can be used for dispersing and discriminating s-SWCNT. Compared with the mid-band-gap conjugated polymer , which is composed of naphthalene diimide (NDI) and head-to-head bithiophene building blocks, the addition of a vinylene linker eliminates the steric congestion present in head-to-head bithiophene, which promotes backbone planarity, extending the π-conjugation length and narrowing the band gap.

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Lead halide perovskite nanocrystals are highly attractive for next-generation optoelectronics because they are easy to synthesize and offer great compositional and morphological tunability. However, the replacement of lead by tin for sustainability reasons is hampered by the unstable nature of Sn oxidation state and by an insufficient understanding of the chemical processes involved in the synthesis. Here, an optimized synthetic route is demonstrated to obtain stable, tunable, and monodisperse CsSnI nanocrystals, exhibiting well-defined excitonic peaks.

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Optically inactive dark exciton states play an important role in light emission processes in semiconductors because they provide an efficient nonradiative recombination channel. Understanding the exciton fine structure in materials with potential applications in light-emitting devices is therefore critical. Here, we investigate the exciton fine structure in the family of two-dimensional (2D) perovskites (PEA)SnI, (PEA)PbI, and (PEA)PbBr.

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The recent development of phase transfer ligand exchange methods for PbS quantum dots (QD) has enhanced the performance of quantum dots solar cells and greatly simplified the complexity of film deposition. However, the dispersions of PbS QDs (inks) used for film fabrication often suffer from colloidal instability, which hinders large-scale solar cell production. In addition, the wasteful spin-coating method is still the main technique for the deposition of QD layer in solar cells.

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Phase-transfer exchange of pristine organic ligands for inorganic ones is essential for the integration of colloidal quantum dots (CQDs) in optoelectronic devices. This method results in a colloidal dispersion (ink) which can be directly deposited by various solution-processable techniques to fabricate conductive films. For PbS CQDs capped with methylammonium lead iodide ligands (MAPbI), the most commonly employed solvent is butylamine, which enables only a short-term (hours) colloidal stability and thus brings concerns on the possibility of manufacturing CQD devices on a large scale in a reproducible manner.

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Recent works demonstrate that polyelectrolytes as a hole transport layer (HTL) offers superior performance in Ruddlesden-Popper perovskite solar cells (RPPSCs) compared to poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS). The factors contributing to such improvement need to be systematically investigated. To achieve this, we have systematically investigated how the two HTLs affect the morphology, crystallinity, and orientation of the Ruddlesden-Popper perovskite (RPP) films as well as the charge extraction of the RPPSCs.

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Article Synopsis
  • Recent research highlights the importance of two-dimensional metal halide perovskites, particularly Ruddlesden-Popper types, for their potential in light generation and stabilizing their 3D versions.
  • The common belief that broad luminescence in these materials is due to self-trapped excitons from strong carrier-phonon interactions is challenged by new findings.
  • Investigating lead-iodide single crystals reveals that the broad emission originates from in-gap states in the crystal, prompting a reevaluation of the assumptions surrounding luminescence in metal halide perovskites.
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Formamidinium lead iodide (FAPbI3) is one of the most extensively studied perovskite materials due to its narrow band gap and high absorption coefficient, which makes it highly suitable for optoelectronic applications. Deposition of a solution containing lead iodide (PbI2) and formamidinium iodide (FAI) or sequential deposition of PbI2 and FAI usually leads to the formation of films with a poor morphology and an unstable crystal structure that readily crystallize into two different polymorphs: the photoinactive yellow phase and the photoactive black phase. In this work, 2D 2-phenylethylammonium lead iodide (PEA2PbI4) thin films are deposited by a scalable doctor-blade coating technique and used as a growth template for the high-quality 3D FAPbI3 perovskite thin films which are obtained by organic cation exchange.

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In this article it is investigated how the hole extraction layer (HEL) influence the charge recombination and performance in half tin and half lead (FASn Pb I ) based solar cells (HPSCs). FASn Pb I film grown on PEDOT:PSS displays a large number of pin-holes and open grain boundaries, resulting in a high defect density and shunts in the perovskite film causing significant bulk and interfacial charge recombination in the HPSCs. By contrast, FASn Pb I films grown on PCP-Na, an anionic conjugated polymer, show compact and pin-hole free morphology over a large area, which effectively eliminates the shunts and trap states.

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In this review we discuss systems of self-replicating molecules in the context of the origin of life and the synthesis of de novo life. One of the important aspects of life is the ability to reproduce and evolve continuously. In this review we consider some of the prerequisites for obtaining unbounded evolution of self-replicating molecules and describe some recent advances in this field.

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