SearcharxivSearch

arXiv subjects

Georg S. Duesberg

Publications and source records attributed to Georg S. Duesberg.

At least 19 recordsLinked to original sources

Visible and Terahertz Nonlinear Responses in the Topological Noble Metal Dichalcogenide PdTe2

Nonlinear processes can offer pathways to next-generation sensors and frequency mixing devices to overcome modern imaging, detection, and communication challenges. In this article, we report on strong second and third-order nonlinear optical responses in visible and terahertz (THz) light in single crystals of the noble metal dichalcogenide PdTe$_2$. We find that buried conduction and valence topological surface states of PdTe$_2$ lead to resonant optical second-harmonic generation. On the other hand, although the nonlinear responses obtained with THz excitation are not close to this resonance, they can be clearly observed in reflection geometry, even in the presence of broadband excitation, where optical filters are not necessary to observe the enhanced odd-order higher harmonic output. By carefully considering the radiative photocurrent framework of stimulated THz emission, we are able to extract fingerprints of both second- and third-order processes in the THz regime, and show that PdTe$_2$ is a promising material candidate for radio frequency rectification, frequency mixing, and beam focusing.

cond-mat.mtrl-sci

How to Identify Suitable Gate Dielectrics for Transistors based on Two-Dimensional Semiconductors

The recent progress in nanosheet transistors has established two-dimensional (2D) semiconductors as viable candidates for future ultra-scaled electronic devices. Next to reducing contact resistance, identifying good gate dielectrics is a fundamental challenge, as the dielectric/channel interface dramatically impacts virtually all performance parameters. While several promising gate dielectrics have recently been reported, the evaluation of their quality and suitability is often fragmentary and focused on selected important performance metrics of the gate stack, such as the capacitive gate control, leakage currents, reliability, and ease of fabrication and integration. However, identifying a suitable gate stack is a complex problem that has not yet been approached systematically. In this perspective, we aim to formulate general criteria for good gate dielectrics.

physics.app-ph

Toward All 2D-based Printed Raindrop Triboelectric Nanogenerators

The raindrop triboelectric nanogenerator (RD-TENG) is an emerging technology that is designed to harvest energy from raindrops. This application requires materials with negative triboelectric effect, high surface charge density, mechanical flexibility, and a large surface area, which are key characteristics of 2D materials. However, fundamental research is necessary to understand the potential of 2D materials in this context. This study introduces all-2D-based RD-TENG devices using graphene and transition metal dichalcogenide (TMD) nanosheets. Liquid phase exfoliation (LPE) and liquid cascade centrifugation are used for nanosheet preparation and size selection. The TENGs are fabricated through a rapid, low-cost solution deposition technique based on liquid-liquid interface deposition, which allows screening of different active films and device geometries. Among the tested layered materials, medium-sized molybdenum disulfide (MoS2) nanosheets (average lateral size~160 nm, volume-fraction weighted average layer number ~9) exhibit the highest short-circuit current (microampere per drop) and voltage (mV per drop) output due to their most suited electron affinity, capacitance, and surface charge exchange properties. The variations in the performance of the TMD films were further evaluated with X-ray photoelectron spectroscopy (XPS), showing the influence of oxidation differences on charge transfer and charge decay time.

physics.app-ph

Piezoresistive PtSe$_2$ pressure sensors with reliable high sensitivity and their integration into CMOS ASIC substrates

Membrane-based sensors are an important market for microelectromechanical systems (MEMS). Two-dimensional (2D) materials, with their low mass, are excellent candidates for suspended membranes to provide high sensitivity, small footprint sensors. The present work demonstrates pressure sensors employing large-scale-synthesized 2D platinum diselenide (PtSe${_2}$) films as piezoresistive membranes supported only by a thin polymer layer. We investigate three different synthesis methods with contrasting growth parameters and establish a reliable high yield fabrication process for suspended PtSe${_2}$/PMMA membranes across sealed cavities. The pressure sensors reproducibly display sensitivities above 6 x 10${^4}$ kPa${^{-1}}$. We show that the sensitivity clearly depends on the membrane diameter and the piezoresistive gauge factor of the PtSe${_2}$ film. Reducing the total device size by decreasing the number of membranes within a device leads to a significant increase in the area-normalized sensitivity. This allows the manufacturing of pressure sensors with high sensitivity but a much smaller device footprint than the current state-of-the-art MEMS technology. We further integrate PtSe${_2}$ pressure sensors with CMOS technology, improving the technological readiness of PtSe${_2}$-based MEMS and NEMS devices.

physics.app-ph

3D printing of hierarchical structures made of inorganic silicon-rich glass featuring self-forming nanogratings

Hierarchical structures are abundant in nature, such as in the superhydrophobic surfaces of lotus leaves and the structural coloration of butterfly wings. They consist of ordered features across multiple size scales, and their unique properties have attracted enormous interest in wide-ranging fields, including energy storage, nanofluidics, and nanophotonics. Femtosecond lasers, capable of inducing various material modifications, have shown promise for manufacturing tailored hierarchical structures. However, existing methods such as multiphoton lithography and 3D printing using nanoparticle-filled inks typically involve polymers and suffer from high process complexity. Here, we demonstrate 3D printing of hierarchical structures in inorganic silicon-rich glass featuring self-forming nanogratings. This approach takes advantage of our finding that femtosecond laser pulses can induce simultaneous multiphoton crosslinking and self-formation of nanogratings in hydrogen silsesquioxane (HSQ). The 3D printing process combines the 3D patterning capability of multiphoton lithography and the efficient generation of periodic structures by the self-formation of nanogratings. We 3D-printed micro-supercapacitors with large surface areas and a remarkable areal capacitance of 1 mF/cm^2 at an ultrahigh scan rate of 50 V/s, thereby demonstrating the utility of our 3D printing approach for device applications in emerging fields such as energy storage.

physics.app-ph

Non-Volatile Resistive Switching of Polymer Residues in 2D Material Memristors

Two-dimensional (2D) materials are popular candidates for emerging nanoscale devices, including memristors. Resistive switching (RS) in such 2D material memristors has been attributed to the formation and dissolution of conductive filaments created by the diffusion of metal ions between the electrodes. However, the area-scalable fabrication of patterned devices involves polymers that are difficult to remove from the 2D material interfaces without damage. Remaining polymer residues are often overlooked when interpreting the RS characteristics of 2D material memristors. Here, we demonstrate that the parasitic residues themselves can be the origin of RS. We emphasize the necessity to fabricate appropriate reference structures and employ atomic-scale material characterization techniques to properly evaluate the potential of 2D materials as the switching layer in vertical memristors. Our polymer-residue-based memristors exhibit RS typical for a filamentary mechanism with metal ion migration, and their performance parameters are strikingly similar to commonly reported 2D material memristors. This reveals that the exclusive consideration of electrical data without a thorough verification of material interfaces can easily lead to misinterpretations about the potential of 2D materials for memristor applications.

cond-mat.mes-hall

Graphene thermal infrared emitters integrated into silicon photonic waveguides

Cost-efficient and easily integrable broadband mid-infrared (mid-IR) sources would significantly enhance the application space of photonic integrated circuits (PICs). Thermal incandescent sources are superior to other common mid-IR emitters based on semiconductor materials in terms of PIC compatibility, manufacturing costs, and bandwidth. Ideal thermal emitters would radiate directly into the desired modes of the PIC waveguides via near-field coupling and would be stable at very high temperatures. Graphene is a semi-metallic two-dimensional material with comparable emissivity to thin metallic thermal emitters. It allows maximum coupling into waveguides by placing it directly into their evanescent fields. Here, we demonstrate graphene mid-IR emitters integrated with photonic waveguides that couple directly into the fundamental mode of silicon waveguides designed for a wavelength of 4,2 μm relevant for CO${_2}$ sensing. High broadband emission intensity is observed at the waveguide-integrated graphene emitter. The emission at the output grating couplers confirms successful coupling into the waveguide mode. Thermal simulations predict emitter temperatures up to 1000°C, where the blackbody radiation covers the mid-IR region. A coupling efficiency η, defined as the light emitted into the waveguide divided by the total emission, of up to 68% is estimated, superior to data published for other waveguide-integrated emitters.

physics.optics

Metal-Organic Chemical Vapor Deposition of PtSe2

Platinum diselenide (PtSe2), a novel two-dimensional material from the class of noble-metal dichalcogenide (NMD), has recently received significant attention due to its outstanding properties. PtSe2, which undergoes a semi metallic to semiconductor transition when thinned, offers a band-gap in the infrared range and good air stability. These properties make it a prime active material in optoelectronic and chemical sensing devices. However, a synthesis method that can produce large-scale and reliable high quality PtSe2 is highly sought after. Here, we present PtSe2 growth by metal organic chemical vapor deposition. Films were grown on a variety of centimeter scale substrates and were characterized by Raman, X-ray photoelectron and X-ray diffraction spectroscopy, as well as scanning tunneling microscopy and spectroscopy. Domains within the films are found to be up to several hundred nanometers in size, and atomic scale measurements show their highly ordered crystalline structure. The thickness of homogenous films can be controlled via the growth time. This work provides fundamental guidance for the synthesis and implementation of high quality, large-scale PtSe2 layers, hence offering the key requirement for the implementation of PtSe2 in future electronic devices.

cond-mat.mtrl-sci

Post-Synthetic Treatment of Nickel-Iron Layered Double Hydroxides for the Optimum Catalysis of the Oxygen Evolution Reaction

Nickel-iron layered double hydroxide (NiFe LDH) platelets with high morphological regularity and sub-micrometre lateral dimensions were synthesized using a homogeneous precipitation technique for highly efficient catalysis of the oxygen evolution reaction (OER). Considering edge sites are the point of activity, efforts were made to control platelet size within the synthesized dispersions. The goal is to controllably isolate and characterize size-reduced NiFe LDH particles. Synthetic approaches for size control of NiFe LDH platelets have not been transferable based on published work with other LDH materials and for that reason, we instead use post-synthetic treatment techniques to improve edge-site density. In the end, size reduced NiFe LDH/single-wall carbon nanotube (SWCNT) composites allowed to further reduce the OER overpotential to 237 plus/minus 7 mV ( L = 0.16 plus/minus 0.01 micrometres, 20 wt% SWCNT), which is one of the best values reported to date. This approach as well improved the long term activity of the catalyst in operating conditions.

cond-mat.mtrl-sci

Two-dimensional Platinum Diselenide Waveguide-Integrated Infrared Photodetectors

Low cost, easily integrable photodetectors (PDs) for silicon (Si) photonics are still a bottleneck for photonic integrated circuits (PICs), especially for wavelengths above 1.8 $μ$m. Multilayered platinum diselenide (PtSe$_2$) is a semi-metallic two-dimensional (2D) material that can be synthesized below 450$°$C. We integrate PtSe$_2$ based PDs directly by conformal growth on Si waveguides. The PDs operate at 1550 nm wavelength with a maximum responsivity of 11 mA/W and response times below 8.4 $μ$s. Fourier transform infrared spectroscopy (FTIR) in the wavelength range from 1.25 $μ$m to 28 $μ$m indicates the suitability of PtSe$_2$ for PDs far into the infrared wavelength range. Our PtSe$_2$ PDs integrated by direct growth outperform PtSe$_2$ PDs manufactured by standard 2D layer transfer. The combination of IR responsivity, chemical stability, selective and conformal growth at low temperatures, and the potential for high carrier mobility, make PtSe$_2$ an attractive 2D material for optoelectronics and PICs.

physics.app-ph

Synthesis and thermal stability of TMD thin films: A comprehensive XPS and Raman study

Transition metal dichalcogenides (TMDs) have been a core constituent of 2D material research throughout the last decade. Over this time, research focus has progressively shifted from synthesis and fundamental investigations, to exploring their properties for applied research such as electrochemical applications and integration in electrical devices. Due to the rapid pace of development, priority is often given to application-oriented aspects while careful characterisation and analysis of the TMD materials themselves is occasionally neglected. This can be particularly evident for characterisations involving X-ray photoelectron spectroscopy (XPS), where measurement, peak-fitting, and analysis can be complex and nuanced endeavours requiring specific expertise. To improve the availability and accessibility of reference information, here we present a detailed peak-fitted XPS analysis of ten transition metal chalcogenides. The materials were synthesised as large-area thin-films on SiO2 using direct chalcogenisation of pre-deposited metal films. Alongside XPS, the Raman spectra with several excitation wavelengths for each material are also provided. These complementary characterisation methods can provide a more complete understanding of the composition and quality of the material. As material stability is a crucial factor when considering applications, the in-air thermal stability of the TMDs was investigated after several annealing points up to 400 °C. This delivers a trend of evolving XPS and Raman spectra for each material which improves interpretation of their spectra while also indicating their ambient thermal limits. This provides an accessible library and set of guidelines to characterise, compare, and discuss TMD XPS and Raman spectra.

cond-mat.mtrl-sci

Correlating Nanocrystalline Structure with Electronic Properties in 2D Platinum Diselenide

Platinum diselenide (PtSe${_2}$) is a two-dimensional (2D) material with outstanding electronic and piezoresistive properties. The material can be grown at low temperatures in a scalable manner which makes it extremely appealing for many potential electronics, photonics, and sensing applications. Here, we investigate the nanocrystalline structure of different PtSe${_2}$ thin films grown by thermally assisted conversion (TAC) and correlate them with their electronic and piezoresistive properties. We use scanning transmission electron microscopy for structural analysis, X-ray photoelectron spectroscopy (XPS) for chemical analysis, and Raman spectroscopy for phase identification. Electronic devices are fabricated using transferred PtSe${_2}$ films for electrical characterization and piezoresistive gauge factor measurements. The variations of crystallite size and their orientations are found to have a strong correlation with the electronic and piezoresistive properties of the films, especially the sheet resistivity and the effective charge carrier mobility. Our findings may pave the way for tuning and optimizing the properties of TAC-grown PtSe${_2}$ towards numerous applications.

cond-mat.mtrl-sci

Synthesis and characterisation of thin-film platinum disulfide and platinum sulfide

Group-10 transition metal dichalcogenides (TMDs) are rising in prominence within the highly innovative field of 2D materials. While PtS2 has been investigated for potential electronic applications, due to its high charge-carrier mobility and strong layer-dependent bandgap, it has proven to be one of the more difficult TMDs to synthesise. In contrast to most TMDs, Pt has a significantly more stable monosulfide, the non-layered PtS. The existence of two stable platinum sulfides, sometimes within the same sample, has resulted in much confusion between the materials in the literature. Neither of these Pt sulfides have been thoroughly characterised as-of-yet. Here we utilise time-efficient, scalable methods to synthesise high-quality thin films of both Pt sulfides on a variety of substrates. The competing nature of the sulfides and limited thermal stability of these materials is demonstrated. We report peak-fitted X-ray photoelectron spectra, and Raman spectra using a variety of laser wavelengths, for both materials. This systematic characterisation provides a guide to differentiate between the sulfides using relatively simple methods which is essential to enable future work on these interesting materials.

cond-mat.mtrl-sci

Slippery Polymer Monoliths: Surface Functionalization with Ordered MoS2 Microparticle Arrays

Components of technical systems and devices often require self-lubricating properties, which are implemented by means of dry lubricants. However, continuous lubricant coatings on the components' surfaces often suffer from poor adhesion, delamination and crack propagation. The replacement of continuous coatings with dense ordered arrays of microparticles consisting of dry lubricants may overcome these drawbacks. Using the well-established solid lubricant MoS2 as model system, we demonstrate that the sliding capability of polymeric monoliths can be significantly enhanced by integration of arrays of micron-sized dry lubricant microparticles into their contact surfaces. To synthesize the MoS2 microparticle arrays, we first prepared ordered hexagonal arrays of ammonium tetrathiomolybdate (ATM) microparticles on Si wafers by molding against poly(dimethylsiloxane) templates followed by high-temperature conversion of the ATM microparticles into MoS2 microparticles under Ar/H2 atmosphere in the presence of elemental sulfur. Finally, the obtained large-scale hexagonal MoS2 microparticle arrays were transferred to the surfaces of polymer monoliths under conservation of the array ordering. Self-lubrication of components of technical systems by incorporation of dry lubricant microparticle arrays into their contact surfaces is an example for overcoming the drawbacks of continuous functional coatings by replacing them with microparticle arrays.

physics.app-ph

Nanoelectromechanical Sensors based on Suspended 2D Materials

The unique properties and atomic thickness of two-dimensional (2D) materials enable smaller and better nanoelectromechanical sensors with novel functionalities. During the last decade, many studies have successfully shown the feasibility of using suspended membranes of 2D materials in pressure sensors, microphones, accelerometers, and mass and gas sensors. In this review, we explain the different sensing concepts and give an overview of the relevant material properties, fabrication routes, and device operation principles. Finally, we discuss sensor readout and integration methods and provide comparisons against the state of the art to show both the challenges and promises of 2D material-based nanoelectromechanical sensing.

physics.app-ph

Spectroscopic thickness and quality metrics for PtSe$_2$ layers produced by top-down and bottom-up techniques

Thin films of noble-metal-based transition metal dichalcogenides, such as PtSe$_2$, have attracted increasing attention due to their interesting layer-number dependent properties and application potential. While it is difficult to cleave bulk crystals down to mono- and few-layers, a range of growth techniques have been established producing material of varying quality and layer number. However, to date, no reliable high-throughput characterization to assess layer number exists. Here, we use top-down liquid phase exfoliation (LPE) coupled with centrifugation to produce widely basal plane defect-free PtSe$_2$ nanosheets of varying sizes and thicknesses. Quantification of the lateral dimensions by statistical atomic force microscopy allows us to quantitatively link information contained in optical spectra to the dimensions. For LPE nanosheets we establish metrics for lateral size and layer number based on extinction spectroscopy. Further, we compare the Raman spectroscopic response of LPE nanosheets with micromechanically exfoliated PtSe$_2$, as well as thin films produced by a range of bottom up techniques. We demonstrate that the Eg1 peak position and the intensity ratio of the Eg1/ A1g1 peaks can serve as robust metric for layer number across all sample types and will be of importance in future benchmarking of PtSe$_2$ films.

physics.app-ph

Three-dimensional printing of silica-glass structures with submicrometric features

Humanity's interest in manufacturing silica-glass objects extends back over three thousand years. Silica glass is resistant to heating and exposure to many chemicals, and it is transparent in a wide wavelength range. Due to these qualities, silica glass is used for a variety of applications that shape our modern life, such as optical fibers in medicine and telecommunications. However, its chemical stability and brittleness impede the structuring of silica glass, especially on the small scale. Techniques for three-dimensional (3D) printing of silica glass, such as stereolithography and direct ink writing, have recently been demonstrated, but the achievable minimum feature size is several tens of micrometers. While submicrometric silica-glass structures have many interesting applications, for example in micro-optics, they are currently manufactured using lithography techniques, which severely limits the 3D shapes that can be realized. Here, we show 3D printing of optically transparent silica-glass structures with submicrometric features. We achieve this by cross-linking hydrogen silsesquioxane to silica glass using nonlinear absorption of laser light followed by the dissolution of the unexposed material. We print a functional microtoroid resonator with out-of-plane fiber couplers to demonstrate the new possibilities for designing and building silica-glass microdevices in 3D.

physics.app-ph

Synthesis of WTe2 thin films and highly-crystalline nanobelts from pre-deposited reactants

Tungsten ditelluride is a layered transition metal dichalcogenide (TMD) that has attracted increasing research interest in recent years. WTe2 has demonstrated large non-saturating magnetoresistance, potential for spintronic applications and promise as a type-II Weyl semimetal. The majority of works on WTe2 have relied on mechanically-exfoliated flakes from chemical vapour transport (CVT) grown crystals for their investigations. While producing high-quality samples, this method is hindered by several disadvantages including long synthesis times, high-temperature anneals and an inherent lack of scalability. In this work, a synthesis method is demonstrated that allows the production of large-area polycrystalline films of WTe2. This is achieved by the reaction of pre-deposited films of W and Te at a relatively low temperature of 550 degC. Sputter X-ray photoelectron spectroscopy reveals the rapid but self-limiting nature of the oxidation of these WTe2 films in ambient conditions. The WTe2 films are composed of areas of micrometre sized nanobelts that can be isolated and offer potential as an alternative to CVT-grown samples. These nanobelts are highly crystalline with low defect densities indicated by TEM and show promising initial electrical results.

cond-mat.mtrl-sci