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Ilka Kriegel

Publications and source records attributed to Ilka Kriegel.

At least 19 recordsLinked to original sources

Metal Halide Perovskite/Chalcohalide Heterojunctions for the Photoinduced Oxidative Coupling of p-substituted Thiophenols

The introduction of a semiconductor-semiconductor junction is an effective strategy to enhance the photocatalytic performance of perovskite nanocrystal-based systems. Herein, we optimized the synthesis of CsPbX3/Pb4S3X2 (X= Cl, Br, I) perovskites-chalcohalides heterostructures, whose band alignment can be tuned by halide composition. As a proof-of-concept, we evaluated the photooxidative coupling of p-substituted thiophenols at room temperature, under visible-light, air, and without sacrificial electron donor. Notably, CsPbBr3/Pb4S3Br2 achieved up to 94 % selectivity toward disulfide (p-OCH3 thiophenol with a turnover number of 14300) highlighting the crucial role of the type-II heterojunction to promote charge separation and efficient electron delocalization across the junction.

cond-mat.mtrl-sci

Synthesis, Growth Mechanism, and Photocatalytic Properties of Metallic-Bi/Bi13S18Br2 Nano-Bell Heterostructures

We report the synthesis of bell-shaped Bi/Bi13S18Br2 metal/semiconductor heterostructures as a photocatalyst based on non-toxic and Earth-abundant elements. Their unique morphology arises from a multi-step growth process, involving 1) the nucleation of Bi13S18Br2 nanorods, 2) the reduction of a metallic-Bi domain on their surface induced by N,N-didodecylmethylamine, and 3) the heterostructure accretion by a localized reaction at the Bi/Bi13S18Br2 interface promoted by Ostwald ripening. These heterostructures display remarkable stability in polar solvents, remaining almost unaffected by prolonged exposure to isopropanol and water, and exhibit high photocatalytic efficiency for the degradation of organic dyes (i.e., Rhodamine-B and Methylene Blue) under visible-light irradiation, with good recyclability. Additionally, preliminary tests demonstrate CO2 reduction capabilities, which make them promising for both the photocatalytic degradation of pollutants and photo-electro CO2 conversion. The straightforward synthesis process and the use of non-toxic and earth-abundant elements offers significant potential for sustainable energy conversion technologies.

cond-mat.mtrl-sci

Core@Shell AgBr@CsPbBr3 Nanocrystals as Precursors to Hollow Lead Halide Perovskite Nanocubes

We report the synthesis of colloidal core@shell AgBr@CsPbBr3 nanocubes by a one-pot approach, where the nucleation and growth of AgBr nanocrystals occurs rapidly after the injection of chemical precursors. This is immediately followed by the overgrowth of CsPbBr3, delivering AgBr@CsPbBr3 nanocubes of several tens of nanometers in size, with the volume of the AgBr core being only a small fraction of the overall nanocrystal volume. The formation of a core@shell geometry is facilitated by the epitaxial compatibility between AgBr and CsPbBr3 along multiple crystallographic directions. Exchange with Cl-ions leads to Ag@CsPbCl3 nanocubes, whereas exchange with I-ions leads to hollow CsPbI3 nanocubes, due to selective etching of the AgBr (or Ag) core region by the I-ions diffusing in the nanocubes. These hollow CsPbI3 nanocubes can then be converted into hollow CsPbBr3 and CsPbCl3 nanocubes by halide exchange. The optical emission properties of the hollow CsPbX3 (X=Cl, Br, I) nanocubes are in line with those expected from large, non-hollow halide perovskite nanocrystals, indicating that the small hollow region in the cubes has no major influence on their optical properties.

cond-mat.mtrl-sci

Electron-beam-induced Contactless Manipulation of Interlayer Twist in van der Waals Heterostructures

The ability to dynamically control the relative orientation of layers in two dimensional (2D) van der Waals (vdW) heterostructures represents a critical step toward the realization of reconfigurable nanoscale devices. Existing actuation methods often rely on mechanical contact, complex architectures, or extreme operating conditions, which limit their applicability and scalability. In this work, we present a proof-of-concept demonstration of contactless electrostatic actuation based on electron-beam-induced charge injection. By locally charging an insulating hexagonal boron nitride (hBN) flake on an electrically grounded graphene layer, we create an interfacial electric field that generates in-plane electrostatic torque and induces angular displacement. We validate the induced rotation through in-situ scanning electron microscopy (SEM) and twist-dependent Raman spectroscopy.

cond-mat.mes-hall

Ultrafast nonlinear dynamics of indium tin oxide nanocrystals probed via fieldoscopy

Scalable, high-speed, small-footprint photonic switching platforms are essential for advancing optical communication. An effective optical switch must operate at high duty cycles with fast recovery times, while maintaining substantial modulation depth and full reversibility. Colloidal nanocrystals, such as indium tin oxide (ITO), offer a scalable platform to meet these requirements. In this work, the transmission of ITO nanocrystals near their epsilon-near-zero wavelength is modulated by two-cycle optical pulses at a repetition rate of one megahertz. The modulator exhibits a broad bandwidth spanning from 2 um to 2.5 um. Sensitive fieldoscopy measurements resolve the transient electric-field response of the ITO for the first time, showing that the modulation remains reversible for excitation fluences up to 1.2 mJ/cm2 with a modulation depth of 10%, and becomes fully irreversible beyond 3.3 mJ/cm2, while reaching modulation depth of up to 20%. Field sampling further indicates that at higher excitation fluences, the relative contribution from the first cycle of the optical pulses is reduced. These findings are crucial for the development of all-optical switching, telecommunications, and sensing technologies capable of operating at terahertz switching frequencies.

physics.optics

Near-Infrared plasmon induced hot electron extraction evidence in an indium tin oxide nanoparticle / monolayer molybdenum disulphide heterostructure

In this work, we observe plasmon induced hot electron extraction in a heterojunction between indium tin oxide nanocrystals and monolayer molybdenum disulphide. We study the sample with ultrafast differential transmission exciting the sample at 1750 nm where the intense localized plasmon surface resonance of the indium tin oxide nanocrystals is and where the monolayer molybdenum disulphide does not absorb light. With the excitation at 1750 nm we observe the excitonic features of molybdenum disulphide in the visible range, close to the exciton of molybdenum disulphide. Such phenomenon can be ascribed to a charge transfer between indium tin oxide nanocrystals and monolayer molybdenum disulphide upon plasmon excitation. These results are a first step towards the implementation of near infrared plasmonic materials for photoconversion.

physics.optics

Two-Dimensional Gallium Sulfide Nanoflakes for UV-Selective Photoelectrochemical-type Photodetectors

Two-dimensional (2D) transition-metal monochalcogenides have been recently predicted to be potential photo(electro)catalysts for water splitting and photoelectrochemical (PEC) reactions. Differently from the most established InSe, GaSe, GeSe, and many other monochalcogenides, bulk GaS has a large band gap of ca. 2.5 eV, which increases up to more than 3.0 eV with decreasing its thickness due to quantum confinement effects. Therefore, 2D GaS fills the void between 2D small-band-gap semiconductors and insulators, resulting of interest for the realization of van der Waals type-I heterojunctions in photocatalysis, as well as the development of UV light-emitting diodes, quantum wells, and other optoelectronic devices. Based on theoretical calculations of the electronic structure of GaS as a function of layer number reported in the literature, we experimentally demonstrate, for the first time, the PEC properties of liquid-phase exfoliated GaS nanoflakes. Our results indicate that solution-processed 2D GaS-based PEC-type photodetectors outperform the corresponding solid-state photodetectors. In fact, the 2D morphology of the GaS flakes intrinsically minimizes the distance between the photogenerated charges and the surface area at which the redox reactions occur, limiting electron-hole recombination losses. The latter are instead deleterious for standard solid-state configurations. Consequently, PEC-type 2D GaS photodetectors display a relevant UV-selective photoresponse. In particular, they attain responsivities of 1.8 mA W-1 in 1 M H2SO4 (at 0.8 V vs reversible hydrogen electrode -RHE-), 4.6 mA W-1 in 1 M Na2SO4 (at 0.9 V vs RHE), and 6.8 mA W-1 in 1 M KOH (at 1.1 V vs RHE) under 275 nm illumination wavelength with an intensity of 1.3 mW cm-2.

physics.app-ph

Multi-charge Transfer from Photodoped ITO Nanocrystals

Metal oxide nanocrystals are emerging as extremely versatile material for addressing many of the current challenging demands of energy-conversion technology. Being able to exploit their full potential is not only an advantage but also a scientific and economic ambition for a more sustainable energy technology. In this direction, photodoping of metal oxide nanocrystals is a very notable process that allows accumulating multiple charge carriers per nanocrystals after light absorption. The reactivity of the photodoped electrons is currently the subject of an intense study. In this context, the possibility to efficiently extract the stored electrons could be beneficial for numerous processes, from photoconversion and sunlight energy storage, to photocatalysis and photoelectrochemistry. In this work we provide, via oxidative titration and optical spectroscopy, evidence for multi-electron transfer processes from photodoped Sn:In2O3 nanocrystals to a widely employed organic electron acceptor (F4TCNQ). The results of this study disclose the potential of photodoped electrons to drive chemical reactions involving more than one electron at a time.

physics.chem-ph

Control of electronic band profiles through depletion layer engineering in core-shell nanocrystals

The understanding of depletion layers is of major importance to control the optical and electronic properties of metal oxide (MO) nanocrystals (NCs). Here, we show that depletion layer engineering is the main mechanism of photodoping of MO NCs. We show that the introduction of different electronic interfaces induces a double-bending of the electronic bands and a distinct carrier density profile. We found that the light-induced depletion layer modulation and bending of the bands close to the surface of the nanocrystal is the main mechanism responsible for the storage of extra electrons after photodoping in MO NCs. We support our results by a combined experimental and theoretical approach in the case of Sn:In2O3/In2O3 core-shell NCs, in which we compare numerical simulations with empirical modeling and experiments. This allows not only to extract the main mechanism of photodoping in MO NCs but also to engineer the charge storage capability of MO NCs after photodoping. Our results are transferable to other core-multishell systems, opening up a novel direction to control the optoelectronic properties of nanoscale MOs by designing their energetic band profiles through depletion layer engineering.

physics.app-ph

Linear and Nonlinear Optical Propagation in 2D Materials

Recently, a lot of effort has been dedicated to developing next-generation optoelectronic devices based on two-dimensional materials, thanks to their unique optical properties that are significantly different from those of their bulk counterparts. In order to implement high-performance nanoscale optical devices, an in-depth study of how linear and non-linear propagation occurs in two-dimensional materials is required. Here, we focus on the theory behind the propagation of electromagnetic waves in two-dimensional materials as well as emerging applications in the fields of electronics, optics, sensors, which are summarized and discussed in the paper.

physics.optics

Electrochromism in Electrolyte-Free and Solution Processed Bragg Stacks

Achieving an active manipulation of colours has huge implications in optoelectronics, as colours engineering can be exploited in a number of applications, ranging from display to lightning. In the last decade, the synergy of the highly pure colours of 1D photonic crystals, also known as Bragg stacks, with electro-tunable materials have been proposed as an interesting route to attain such a technologically relevant effect. However, recent works rely on the use of liquid electrolytes, which can pose issues in terms of chemical and environmental stability. Here, we report on the proof-of-concept of an electrolyte free and solution-processed electrochromic Bragg stack. We integrate an electro-responsive plasmonic metal oxide, namely indium tin oxide, in a 1D photonic crystal structure made of alternating layers of ITO and TiO2 nanoparticles. In such a device we observed 15 nm blue-shift upon application of an external bias (5 V), an effect that we attribute to the increase of ITO charge density arising from the capacitive charging at the metal oxide/dielectric interface and from the current flowing throughout the porous structure. Our data suggest that electrochromism can be attained in all-solid state systems by combining a judicious selection of the constituent materials with device architecture optimisation.

physics.app-ph

Ultrafast photochromism and bacteriochromism in one dimensional hybrid plasmonic photonic structures

Hybrid plasmonic photonic structures combine the plasmonic response with the photonic band gap, holding promise for utilization as optical switches and sensors. Here, we demonstrate the active modulation of the optical response in such structures with two different external stimuli, e.g. laser pulses and bacteria. First, we report the fabrication of a miniaturized (5 x 5 mm) indium tin oxide (ITO) grating employing femtosecond laser micromachining, and we show the possibility to modulate the photonic band gap in the visible via ultrafast photoexcitation in the infrared part of the spectrum. Note that the demonstrated time response in the picosecond range of the spectral modulation have an industrial relevance. Moreover, we manufacture one-dimensional photonic crystals consisting of a solution-processed dielectric Bragg stack exposing a top-layer of bio-active silver. We assign the bacterial responsivity of the system to polarization charges at the Ag/bacterium interface, giving rise to an overall blue shift of the photonic band gap.

physics.optics

The ultrafast onset of exciton formation in 2D semiconductors

The equilibrium and non-equilibrium optical properties of single-layer transition metal dichalcogenides (TMDs) are determined by strongly bound excitons. Exciton relaxation dynamics in TMDs have been extensively studied by time-domain optical spectroscopies. However, the formation dynamics of excitons following non-resonant photoexcitation of free electron-hole pairs have been challenging to directly probe because of their inherently fast timescales. Here we use extremely short optical pulses to non-resonantly excite an electron-hole plasma and show the formation of two-dimensional excitons in single-layer MoS2 on the timescale of 30 fs via the induced changes to photo-absorption. These formation dynamics are significantly faster than in conventional 2D quantum wells and are attributed to the intense Coulombic interactions present in 2D TMDs. A theoretical model of a coherent polarization that dephases and relaxes to an incoherent exciton population reproduces the experimental dynamics on the sub-100-fs timescale and sheds light into the underlying mechanism of how the lowest-energy excitons, which are the most important for optoelectronic applications, form from higher-energy excitations. Importantly, a phonon-mediated exciton cascade from higher energy states to the ground excitonic state is found to be the rate-limiting process. These results set an ultimate timescale of the exciton formation in TMDs and elucidate the exceptionally fast physical mechanism behind this process.

cond-mat.mtrl-sci

Hybrid 1D Plasmonic/Photonic Crystals are Responsive to Escherichia Coli

Photonic crystal-based biosensors hold great promise as valid and low-cost devices for real-time monitoring of a variety of biotargets. Given the high processability and easiness of read-out even for unskilled operators, these systems can be highly appealing for the detection of bacterial contaminants in food and water. Here, we propose a novel hybrid plasmonic/photonic device that is responsive to Escherichia coli, which is one of the most hazardous pathogenic bacterium. Our system consists of a thin layer of silver, a metal that exhibits both a plasmonic behavior and a well-known biocidal activity, on top of a solution processed 1D photonic crystal. We attribute the bio-responsivity to the modification of the dielectric properties of the silver film upon bacterial contamination, an effect that likely stems from the formation of polarization charges at the Ag/bacterium interface within a sort of bio-doping mechanism. Interestingly, this triggers a blue-shift in the photonic response. This work demonstrates that our hybrid plasmonic/photonic device can be a low-cost and portable platform for the detection of common contaminants in food and water.

physics.app-ph

Indium tin oxide nanoparticle:TiO$_{2}$:air layers for one-dimensional multilayer photonic structures

In this work we study the optical properties, by means of the transfer matrix method, of one-dimensional photonic crystals in which layers of silica nanoparticles are alternated with layers of indium tin oxide nanoparticle (ITO) / titania nanoparticle mixture. The dielectric function of the mixed ITO/TiO$_{2}$ nanoparticle layer is carefully accounted for with a generalized Rayleigh equation for the ternary mixture ITO:TiO$_{2}$:air. We have studied the light transmission of the multilayer photonic crystal as a function of the ITO/TiO$_{2}$ ratio. We observe that, by increasing the ITO content in the three-phase mixture, the intensity of the plasmon resonance in the near infrared (NIR) increases and the intensity of the photonic band gap (visible) decreases. Thus, our study is of major importance for the realization of electrochromic smart windows, in which separate and independent NIR and visible light control is required.

physics.optics

Contactless photo-induced carrier density control in nanocrystal MoS2 hybrids

The ultrathin nature of two-dimensional monolayer semiconductors yields optoelectronic properties which are highly responsive to changes in free-carrier density, making it imperative to masterfully control their doping levels. We report a new photo-doping scheme that quasi-permanently dopes the monolayer MoS2 to extents competing with electrostatic gating. The photo-doping is achieved by coupling monolayer MoS2 with indium tin oxide nanocrystals that can store multiple electrons per nanocrystal after UV illumination. In the hybrid structure, the photo-generated valence band holes in the nanocrystals are filled by MoS2 electrons, photo-doping the MoS2 with holes. Reductions in carrier density by ~6x10^12 cm^-2 are observed, equivalent to the storage of ~40 electrons per nanocrystal. Long-range changes proliferating up to 40 micrometers away from the localized photodoping result from local bandstructure variations in MoS2. These studies reveal novel all-optical carrier density control in monolayer semiconductors, enabling remote-control of local charge density and innovative energy storage technologies.

cond-mat.mes-hall

TaAs Weyl semimetal based one-dimensional photonic structures

Weyl semimetals can be described as the three-dimensional analogue of graphene, showing linear dispersion around nodes (Weyl points) [1]. Tantalum arsenide (TaAs) is among the most studied Weyl semimetals. It has been demonstrated that TaAs has a very high value of the real part of the complex refractive index in the infrared region [2]. In this work we show one-dimensional photonic crystals alternating TaAs with SiO2 or TiO2 and a microcavity where a layer of TaAs is embedded between two SiO2-TiO2 multilayer.

physics.optics

Structural color tuning in 1D photonic crystals with electric field and magnetic field

A tuning of the light transmission properties of 1D photonic structures employing an external stimulus is very attracting and opens the way to the fabrication of optical switches for colour manipulation in sensing, lighting, and display technology. We present the electric field-induced tuning of the light transmission in a photonic crystal device, made by alternating layers of silver nanoparticles and titanium dioxide nanoparticles. We show a shift of around 10 nm for an applied voltage of 10 V. We ascribe the shift to an accumulation of charges at the silver/TiO2 interface due to electric field, resulting in an increase of the number of charges contributing to the plasma frequency in silver, giving rise to a blue shift of the silver plasmon band, with concomitant blue shift of the photonic band gap. The employment of a relatively low applied voltage gives the possibility to build a compact and low-cost device. We also propose the fabrication of 1D photonic crystal and microcavities employing a magneto-optical material as TGG (Tb3Ga5O12). With these structures we can observe a shift of 22 nm with a magnetic field of 5 T, at low temperature (8 K). The option to tune the colour of a photonic crystal with magnetic field is interesting because of the possibility to realize contactless optical switches. We also discuss the possibility to achieve the tuning of the photonic band gap with UV light in photonic crystals made with indium tin oxide (ITO).

physics.gen-ph