arXiv subjects

Stephan Hofmann

Publications and source records attributed to Stephan Hofmann.

At least 19 recordsLinked to original sources

arXiv2025

The role of non-equilibrium populations in dark exciton formation

In two-dimensional transition metal dichalcogenide structures, the optical excitation of a bright exciton may be followed by the formation of a plethora of lower energy dark states. In these formation and relaxation processes between different exciton species, non-equilibrium exciton and phonon populations play a dominant role, but remain so far largely unexplored as most states are inaccessible by regular spectroscopies. Here, on the example of homobilayer 2H-MoS$_2$, we realize direct access to the full exciton relaxation cascade from experiment and theory. By measuring the energy- and in-plane momentum-resolved photoemission spectral function, we reveal a distinct fingerprint for dark excitons in a non-equilibrium excitonic occupation distribution. In excellent agreement with microscopic many-particle calculations, we quantify the timescales for the formation of a non-equilibrium dark excitonic occupation and its subsequent thermalization to 85~fs and 150~fs, respectively. Our results provide a previously inaccessible view of the complete exciton relaxation cascade, which is of paramount importance for the future characterization of non-equilibrium excitonic phases and the efficient design of optoelectronic devices based on two-dimensional materials.

cond-mat.mes-hall↗

arXiv2025

The 2D Materials Roadmap

Over the past two decades, 2D materials have rapidly evolved into a diverse and expanding family of material platforms. Many members of this materials class have demonstrated their potential to deliver transformative impact on fundamental research and technological applications across different fields. In this roadmap, we provide an overview of the key aspects of 2D material research and development, spanning synthesis, properties and commercial applications. We specifically present roadmaps for high impact 2D materials, including graphene and its derivatives, transition metal dichalcogenides, MXenes as well as their heterostructures and moir\'e systems. The discussions are organized into thematic sections covering emerging research areas (e.g., twisted electronics, moir\'e nano-optoelectronics, polaritronics, quantum photonics, and neuromorphic computing), breakthrough applications in key technologies (e.g., 2D transistors, energy storage, electrocatalysis, filtration and separation, thermal management, flexible electronics, sensing, electromagnetic interference shielding, and composites) and other important topics (computational discovery of novel materials, commercialization and standardization). This roadmap focuses on the current research landscape, future challenges and scientific and technological advances required to address, with the intent to provide useful references for promoting the development of 2D materials.

cond-mat.mtrl-sci↗

arXiv2024

Selective synthesis of large-area monolayer tin sulfide from simple substances

Both tin monosulfide (SnS) and tin disulfide (SnS2) are thermodynamically stable layered materials with potential for spin-valleytronic devices and photodetectors. Notably, monolayer SnS, owing to its low symmetry, exhibits interesting properties such as ferroelectricity, shift-current, and a persistent spin helix state in the monolayer limit. However, creating atomic-thickness crystals of SnS is challenging owing to the enhanced interlayer interactions caused by lone pair electrons, unlike to SnS2. Here, we demonstrate that p-type SnS can be selectively grown by simply varying the sulfur vapor concentration relative to tin using single-element precursors. We show that monolayer SnS crystals, up to several tens of micrometers in lateral scale, can be easily and safely obtained by high-temperature etching of bulk SnS in a pure nitrogen gas atmosphere. These findings pave the way for device applications based on high-quality tin sulfide.

cond-mat.mtrl-sci↗

arXiv2024

Recommendations and tools to enable reproducibility in 2D materials research

Research on 2D materials has achieved significant milestones and fuelled a rapidly growing industrial sector. This progress, however, is accompanied by challenges in reproducibility, arising from the atomic thinness, fragility, and environmental sensitivity of these materials. Subtle variations in methods or materials can lead to drastically different outcomes, undermining reliability and slowing down both scientific and technological advances. At the same time, academic publishing and funding systems continue to place greater value on novelty than on efforts to improve reproducibility. This Expert Recommendation outlines concrete, actions researchers can take to improve reproducibility in 2D materials science. We introduce two tools - STEP (Standardised Template for Experimental Procedures) and ReChart (Reproducibility Charter) - designed to support rigorous documentation and transparent sharing of protocols, failure modes, and raw data. To illustrate the application of STEP, we provide three detailed examples covering key processes in 2D materials research: graphene growth by chemical vapour deposition (CVD) on copper foil, wet transfer of CVD graphene, and dry assembly of van der Waals heterostructures. We offer practical recommendations that spans the full research process and show how researchers can engage constructively with stakeholders across academia, funding, publishing, and industry to create a stronger basis for reproducibility, transparency and trust in the field.

physics.soc-ph↗

arXiv2024

Forming and Compliance-free Operation of Low-energy, Fast-switching HfO$_x$S$_y$/HfS$_2$ Memristors

We demonstrate low energy, forming and compliance-free operation of a resistive memory obtained by the partial oxidation of a two-dimensional layered van-der-Waals semiconductor: hafnium disulfide (HfS$_2$). Semiconductor - oxide heterostructures are achieved by low temperature ($<300^{o}$C) thermal oxidation of HfS$_2$ in dry conditions, carefully controlling process parameters. The resulting HfO$_x$S$_y$/HfS$_2$ heterostructures are integrated between metal contacts, forming vertical crossbar devices. Forming-free, compliance-free resistive switching between non-volatile states is demonstrated by applying voltage pulses and measuring the current response in time. We show non-volatile memory operation with an R$_{ON}$/ R$_{OFF}$ of 102, programmable by 80ns WRITE and ERASE operations. Multiple stable resistance states are achieved by modulating pulse width and amplitude, down to 60ns, $<$ 20pJ operation. This demonstrates the capability of these devices for low - energy, fast-switching and multi-state programming. Resistance states were retained without fail at 150$^o$C over 10$^4$s, showcasing the potential of these devices for long retention times and resilience to ageing. Low-energy resistive switching measurements were repeated in vacuum (8.6 mbar) showing unchanged characteristics and no dependence of the device on surrounding oxygen or water vapour. Using a technology computer-aided design (TCAD) tool, we explore the role of the semiconductor layer in tuning the device conductance and driving gradual resistive switching in 2D HfO$_x$ - based devices.

physics.app-ph↗

arXiv2024

Controlled Fabrication of Native Ultra-Thin Amorphous Gallium Oxide from 2D Gallium Sulfide for Emerging Electronic Applications

Oxidation of two-dimensional (2D) layered materials has proven advantageous in creating oxide/2D material heterostructures, opening the door for a new paradigm of low-power electronic devices. Gallium (II) sulfide ($\beta$-GaS), a hexagonal phase group III monochalcogenide, is a wide bandgap semiconductor with a bandgap exceeding 3 eV in single and few layer form. Its oxide, gallium oxide (Ga$_2$O$_3$), combines large bandgap (4.4-5.3 eV) with high dielectric constant (~10). Despite the technological potential of both materials, controlled oxidation of atomically-thin $\beta$-GaS remains under-explored. This study focuses into the controlled oxidation of $\beta$-GaS using oxygen plasma treatment, achieving ultrathin native oxide (GaS$_x$O$_y$, ~4 nm) and GaS$_x$O$_y$/GaS heterostructures where the GaS layer beneath remains intact. By integrating such structures between metal electrodes and applying electric stresses as voltage ramps or pulses, we investigate their use for resistive random-access memory (ReRAM). The ultrathin nature of the produced oxide enables low operation power with energy use as low as 0.22 nJ per operation while maintaining endurance and retention of 350 cycles and 10$^4$ s, respectively. These results show the significant potential of the oxidation-based GaS$_x$O$_y$/GaS heterostructure for electronic applications and, in particular, low-power memory devices.

physics.app-ph↗

arXiv2023

A foundation model for atomistic materials chemistry

Atomistic simulations of matter, especially those that leverage first-principles (ab initio) electronic structure theory, provide a microscopic view of the world, underpinning much of our understanding of chemistry and materials science. Over the last decade or so, machine-learned force fields have transformed atomistic modeling by enabling simulations of ab initio quality over unprecedented time and length scales. However, early ML force fields have largely been limited by: (i) the substantial computational and human effort of developing and validating potentials for each particular system of interest; and (ii) a general lack of transferability from one chemical system to the next. Here we show that it is possible to create a general-purpose atomistic ML model, trained on a public dataset of moderate size, that is capable of running stable molecular dynamics for a wide range of molecules and materials. We demonstrate the power of the MACE-MP-0 model - and its qualitative and at times quantitative accuracy - on a diverse set of problems in the physical sciences, including properties of solids, liquids, gases, chemical reactions, interfaces and even the dynamics of a small protein. The model can be applied out of the box as a starting or "foundation" model for any atomistic system of interest and, when desired, can be fine-tuned on just a handful of application-specific data points to reach ab initio accuracy. Establishing that a stable force-field model can cover almost all materials changes atomistic modeling in a fundamental way: experienced users get reliable results much faster, and beginners face a lower barrier to entry. Foundation models thus represent a step towards democratising the revolution in atomic-scale modeling that has been brought about by ML force fields.

physics.chem-ph↗

arXiv2023

Achieving 100% amplitude modulation depth in a graphene-based tuneable capacitance metamaterial

Effective control of terahertz radiation requires the development of efficient and fast modulators with a large modulation depth. This challenge is often tackled by using metamaterials, artificial sub-wavelength optical structures engineered to resonate at the desired terahertz frequency. Metamaterial-based devices exploiting graphene as the active tuneable element have been proven to be a highly effective solution for THz modulation. However, whilst the graphene conductivity can be tuned over a wide range, it cannot be reduced to zero due to the gapless nature of graphene, which directly limits the maximum achievable modulation depth for single-layer metamaterial modulators. Here, we demonstrate two novel solutions to circumvent this restriction: Firstly, we excite the modulator from the back of the substrate, and secondly, we incorporate air gaps into the graphene patches. This results in a ground-breaking graphene-metal metamaterial terahertz modulator, operating at 2.0-2.5 THz, which demonstrates a 99.01 % amplitude and a 99.99 % intensity modulation depth at 2.15 THz, with a reconfiguration speed in excess of 3 MHz. Our results open up new frontiers in the area of terahertz technology.

physics.optics↗

arXiv2023

Ultrafast nano-imaging of dark excitons

The role and impact of spatial heterogeneity in two-dimensional quantum materials represents one of the major research quests regarding the future application of these materials in optoelectronics and quantum information science. In the case of transition-metal dichalcogenide heterostructures, in particular, direct access to heterogeneities in the dark-exciton landscape with nanometer spatial and ultrafast time resolution is highly desired, but remains largely elusive. Here, we introduce ultrafast dark field momentum microscopy to spatio-temporally resolve dark exciton formation dynamics in a twisted WSe$_2$/MoS$_2$ heterostructure with 55 femtosecond time- and 500~nm spatial resolution. This allows us to directly map spatial heterogeneity in the electronic and excitonic structure, and to correlate these with the dark exciton formation and relaxation dynamics. The benefits of simultaneous ultrafast nanoscale dark-field momentum microscopy and spectroscopy is groundbreaking for the present study, and opens the door to new types of experiments with unprecedented spectroscopic and spatiotemporal capabilities.

cond-mat.mes-hall↗

arXiv2023

Ultrafast dynamics of bright and dark excitons in monolayer WSe$_2$ and heterobilayer WSe$_2$/MoS$_2$

The energy landscape of optical excitations in mono- and few-layer transition metal dichalcogenides (TMDs) is dominated by optically bright and dark excitons. These excitons can be fully localized within a single TMD layer, or the electron- and the hole-component of the exciton can be charge-separated over multiple TMD layers. Such intra- or interlayer excitons have been characterized in detail using all-optical spectroscopies, and, more recently, photoemission spectroscopy. In addition, there are so-called hybrid excitons whose electron- and/or hole-component are delocalized over two or more TMD layers, and therefore provide a promising pathway to mediate charge-transfer processes across the TMD interface. Hence, an in-situ characterization of their energy landscape and dynamics is of vital interest. In this work, using femtosecond momentum microscopy combined with many-particle modeling, we quantitatively compare the dynamics of momentum-indirect intralayer excitons in monolayer WSe$_2$ with the dynamics of momentum-indirect hybrid excitons in heterobilayer WSe$_2$/MoS$_2$, and draw three key conclusions: First, we find that the energy of hybrid excitons is reduced when compared to excitons with pure intralayer character. Second, we show that the momentum-indirect intralayer and hybrid excitons are formed via exciton-phonon scattering from optically excited bright excitons. And third, we demonstrate that the efficiency for phonon absorption and emission processes in the mono- and the heterobilayer is strongly dependent on the energy alignment of the intralayer and hybrid excitons with respect to the optically excited bright exciton. Overall, our work provides microscopic insights into exciton dynamics in TMD mono- and bilayers.

cond-mat.mes-hall↗

arXiv2023

Imaging Light-Induced Migration of Dislocations in Halide Perovskites with 3D Nanoscale Strain Mapping

In recent years, halide perovskite materials have been used to make high performance solar cell and light-emitting devices. However, material defects still limit device performance and stability. Here, we use synchrotron-based Bragg Coherent Diffraction Imaging to visualise nanoscale strain fields, such as those local to defects, in halide perovskite microcrystals. We find significant strain heterogeneity within MAPbBr$_{3}$ (MA = CH$_{3}$NH$_{3}^{+}$) crystals in spite of their high optoelectronic quality, and identify both $\langle$100$\rangle$ and $\langle$110$\rangle$ edge dislocations through analysis of their local strain fields. By imaging these defects and strain fields in situ under continuous illumination, we uncover dramatic light-induced dislocation migration across hundreds of nanometres. Further, by selectively studying crystals that are damaged by the X-ray beam, we correlate large dislocation densities and increased nanoscale strains with material degradation and substantially altered optoelectronic properties assessed using photoluminescence microscopy measurements. Our results demonstrate the dynamic nature of extended defects and strain in halide perovskites and their direct impact on device performance and operational stability.

cond-mat.mtrl-sci↗

arXiv2023

Probing correlations in the exciton landscape of a moir\'e heterostructure

Excitons are two-particle correlated bound states that are formed due to Coulomb interaction between single-particle holes and electrons. In the solid-state, cooperative interactions with surrounding quasiparticles can strongly tailor the exciton properties and potentially even create new correlated states of matter. It is thus highly desirable to access such cooperative and correlated exciton behavior on a fundamental level. Here, we find that the ultrafast transfer of an exciton's hole across a type-II band-aligned moir\'e heterostructure leads to a surprising sub-200-fs upshift of the single-particle energy of the electron being photoemitted from the two-particle exciton state. While energy relaxation usually leads to an energetic downshift of the spectroscopic signature, we show that this unusual upshift is a clear fingerprint of the correlated interactions of the electron and hole parts of the exciton quasiparticle. In this way, time-resolved photoelectron spectroscopy is straightforwardly established as a powerful method to access exciton correlations and cooperative behavior in two-dimensional quantum materials. Our work highlights this new capability and motivates the future study of optically inaccessible correlated excitonic and electronic states in moir\'e heterostructures.

cond-mat.mtrl-sci↗

arXiv2022

Electrochemically-gated Graphene Broadband Microwave Waveguides for Ultrasensitive Biosensing

Identification of non-amplified DNA sequences and single-base mutations is essential for molecular biology and genetic diagnostics. This paper reports a novel sensor consisting of electrochemically-gated graphene coplanar waveguides coupled with a microfluidic channel. Upon exposure to analytes, propagation of electromagnetic waves in the waveguides is modified as a result of interactions with the fringing field and modulation of graphene dynamic conductivity resulting from electrostatic gating. Probe DNA sequences are immobilised on the graphene surface, and the sensor is exposed to DNA sequences which either perfectly match the probe, contain a singlebase mismatch or are unrelated. By monitoring the scattering parameters at frequencies between 50 MHz and 50 GHz, unambiguous and reproducible discrimination of the different strands is achieved at concentrations as low as 1 attomole per litre (1 aM). By controlling and synchronising frequency sweeps, electrochemical gating, and liquid flow in the microfluidic channel, the sensor generates multidimensional datasets. Advanced data analysis techniques are utilised to take full advantage of the richness of the dataset. A classification accuracy > 97% between all three sequences is achieved using different Machine Learning models, even in the presence of simulated noise and low signal-to-noise ratios. The sensor exceeds state-of-the-art sensitivity of field-effect transistors and microwave sensors for the identification of single-base mismatches.

physics.bio-ph↗

arXiv2022

Properties of quantum emitters in different hBN sample types particularly suited for nanophotonic integration

Single photon emitters in two-dimensional (2D) hexagonal boron nitride (hBN) are promising solid-state quantum emitters for photonic applications and quantum networks. Despite their favorable properties, much is still unknown about their characteristics and their atomic origin. We focus on two different kinds of hBN samples that particularly lend themselves for integration with nanophotonic devices, multilayer nanoflakes produced by liquid phase exfoliation (LPE) and a layer-engineered sample from hBN grown by chemical vapour deposition (CVD). We investigate their inherent defects and fit their emission properties to computationally simulated optical properties of likely carbon-related defects. Thereby we compare and elucidate the properties in different sample types particularly suited for photonic quantum networks and narrow down the origin of emitters found in these samples. Our work is thus an important step towards harnessing the full potential of single photon emitters in hBN.

quant-ph↗

arXiv2022

Putting high-index Cu on the map for high-yield, dry-transferred CVD graphene

Reliable, clean transfer and interfacing of 2D material layers is technologically as important as their growth. Bringing both together remains a challenge due to the vast, interconnected parameter space. We introduce a fast-screening descriptor approach to demonstrate holistic data-driven optimization across the entirety of process steps for the graphene-Cu model system. We map the crystallographic dependencies of graphene chemical vapor deposition, interfacial Cu oxidation to decouple graphene, and its dry delamination across inverse pole figures. Their overlay enables us to identify hitherto unexplored (168) higher index Cu orientations as overall optimal. We show the effective preparation of such Cu orientations via epitaxial close-space sublimation and achieve mechanical transfer with very high yield (>95%) and quality of graphene domains, with room-temperature electron mobilities in the range of 40000 cm$^2$/(Vs). Our approach is readily adaptable to other descriptors and 2D materials systems, and we discuss the opportunities of such holistic optimization.

cond-mat.mtrl-sci↗

arXiv2022

Plasma-enhanced atomic layer deposition of Al$_2$O$_3$ on graphene using monolayer hBN as interfacial layer

The deposition of dielectric materials on graphene is one of the bottlenecks for unlocking the potential of graphene in electronic applications. In this paper we demonstrate the plasma enhanced atomic layer deposition of 10 nm thin high quality Al$_2$O$_3$ on graphene using a monolayer of hBN as protection layer. Raman spectroscopy was performed to analyze possible structural changes of the graphene lattice caused by the plasma deposition. The results show that a monolayer of hBN in combination with an optimized deposition process can effectively protect graphene from damage, while significant damage was observed without an hBN layer. Electrical characterization of double gated graphene field effect devices confirms that the graphene did not degrade during the plasma deposition of Al$_2$O$_3$. The leakage current densities were consistently below 1 nA/mm for electric fields across the insulators of up to 8 MV/cm, with irreversible breakdown happening above. Such breakdown electric fields are typical for Al$_2$O$_3$ and can be seen as an indicator for high quality dielectric films.

cond-mat.mtrl-sci↗

arXiv2022

GFET Lab: A Graphene Field-Effect Transistor TCAD Tool

Graphene field-effect transistors (GFETs) are experimental devices which are increasingly seeing commercial and research applications. Simulation and modelling forms an important stage in facilitating this transition, however the majority of GFET modelling relies on user implementation. To this end, we present GFET Lab, a user-friendly, open-source software tool for simulating GFETs. We first provide an overview of approaches to device modelling and a brief survey of GFET compact models and limitations. From this survey, we identify three key criteria for a suitable predictive model for circuit design: it must be a compact model; it must be SPICE-compatible; it must have a minimal number of fitting parameters. We selected Jimenez's drain-current model as it best matched these criteria, and we introduce some modifications to improve the predictive properties, namely accounting for saturation velocity and the asymmetry in n- and p-type carrier mobilities. We then validate the model by comparing GFETs simulated in our tool against experimentally-obtained GFET characteristics with the same materials and geometries and find good agreement between GFET Lab and experiment. We demonstrate the ability to export SPICE models for use in higher level circuit simulations and compare SPICE simulations of GFETs against GFETs simulated in GFET Lab, again showing good agreement. Lastly, we provide a brief tutorial of GFET Lab to demonstrate and encourage its use as a community-developed piece of software with both research and educational applications.

cond-mat.mes-hall↗

arXiv2022

Multi-dimensional microwave sensing using graphene waveguides

This paper presents an electrolytically gated broadband microwave sensor where atomically-thin graphene layers are integrated into coplanar waveguides and coupled with microfluidic channels. The interaction between a solution under test and the graphene surface causes material and concentration-specific modifications of graphene's DC and AC conductivity. Moreover, wave propagation in the waveguide is modified by the dielectric properties of materials in its close proximity via the fringe field, resulting in a combined sensing mechanism leading to an enhanced S-parameter response compared to metallic microwave sensors. The possibility of further controlling the graphene conductivity via an electrolytic gate enables a new, multi-dimensional approach merging chemical field-effect sensing and microwave measurement methods. By controlling and synchronizing frequency sweeps, electrochemical gating and liquid flow in the microfluidic channel, we generate multidimensional datasets that enable a thorough investigation of the solution under study. As proof of concept, we functionalize the graphene surface in order to identify specific single-stranded DNA sequences dispersed in phosphate buffered saline solution. We achieve a limit of detection of ~1 attomole per litre for a perfect match DNA strand and a sensitivity of ~3 dB/decade for sub-pM concentrations. These results show that our devices represent a new and accurate metrological tool for chemical and biological sensing.

cond-mat.mes-hall↗