arXiv subjects

Matthias Wuttig

Publications and source records attributed to Matthias Wuttig.

At least 19 recordsLinked to original sources

arXiv2026

Bonding Signatures of Incipient Electron Localization in Topological Chiral Semimetals Near the Metal-Insulator Transition

How do electronic localization and delocalization compete in solids beyond the traditional limiting cases of metals and iono-covalent insulators? Topological chiral semimetals (TCSMs), characterized by their unique crystal symmetry, offer an intriguing platform to explore this question. Here, we systematically compare TCSMs with covalent compounds, ordinary metals, and metavalent solids (incipient metals), and show that TCSMs occupy a distinct region in a multidimensional property fingerprint. Atom probe tomography reveals an unusual bond-rupture signature, consistent with a bonding regime intermediate between electron localization and delocalization. This interpretation is supported by measurements of optical properties showing a transfer of spectral weight from interband to intraband transitions. For highly conductive TCSMs, this transition is accompanied by the disappearance of the Born effective charge, a measure of chemical bond polarizability, while less conductive TCSMs retain a nonzero value. Together, these results identify a property based bonding perspective on TCSMs that distinguishes them from metals, covalent solids, and metavalent compounds. Although metavalent solids and TCSMs both lie near the metal-insulator transition and exhibit distorted crystal structures, ultrafast coherent phonon spectroscopy reveals fundamentally different lattice-dynamical responses: a phonon-driven Peierls-like instability in metavalent solids versus a robust chiral B20 bonding motif in TCSMs.

cond-mat.mtrl-sci↗

arXiv2026

Classification of Metal - Insulator Transitions: Relating characteristic Properties to Quantum Chemical Bonding Descriptors

Pressure induced metal insulator transitions (MIT) are classified by the evolution of characteristic optoelectronic and vibrational properties calculated with density functional theory. Three classes emerge: ionic solids metallize continuously at band-gap closure with hardening phonons; covalent solids show discontinuous changes in atomic arrangement and optical phonon frequencies; a third class exhibits complete lattice softening and drastically enhanced electron phonon coupling. A one dimensional hydrogen chain reproduces this behavior and serves as a toy model of the underlying bonding mechanism, termed metavalent. Two quantum-chemical descriptors capture the distinct bonding changes behind the three classes. In metavalent solids, competing electron localization and delocalization yield soft optical modes and Peierls distortions on the insulating side, superconductivity on the metallic side, and low lattice thermal conductivity near the MIT.

cond-mat.mtrl-sci↗

arXiv2026

Nonresonant optomechanical control of structural phases

Optical tweezers demonstrate how light can exert forces to trap, repel, and manipulate microscopic particles without absorption. Recent theory has suggested that such forces can extend beyond particle manipulation to drive structural phase transitions in solids. Here we apply this optomechanical principle to tin selenide (SnSe), a material where proximity to several different structural phases gives rise to its high thermoelectric figure of merit and makes it a candidate for a switchable topological crystalline insulator. Whereas the force for standard optical tweezers arises from a gradient in the intensity of a light field, the optomechanical force is mediated by a gradient in the dielectric constant as a function of phonon coordinate. Unlike conventional methods that rely on resonant excitation and absorption through the imaginary part of the dielectric function, this approach operates dispersively through the real part and can be directly driven by Raman processes, enabling selective transitions with reduced energy cost and ultrafast response. Using time-domain Raman scattering, we show that above a critical mid-infrared field strength the $A_g$ Raman modes disappear abruptly without softening, signaling the formation of a new structural phase. This phase, distinct from those induced by heating or carrier excitation, exhibits large-amplitude and long-lived modulations in its optical response. Complementing this observation, we show also evidence for an equivalent DC-field-driven structural phase transformation to a higher symmetry phase, as observed by atom probe tomography. Our study demonstrates the concept of nonresonant optomechanical phase control and defines novel opportunities for synthesizing hidden structural phases with unique functional properties.

physics.optics↗

arXiv2026

Understanding and Designing Phase Change Materials: Insights from Atom Probe Tomography

Phase Change Materials (PCMs) can be rapidly and reversibly switched between their amorphous and crystalline state; a transition which is accompanied by a pronounced change of optoelectronic properties. Here progress is reviewed to explain these property changes, focusing on advances by atom probe tomography (APT). This technique classifies bonding by providing two crucial bonding descriptors. Most important is the Probability of Multiple Events (PME), which is related to the likelihood that more than one ion is dislodged per successful laser pulse in laser assisted field evaporation. Crystalline PCMs are characterized by a PME above 55%, not found for metals or iono-covalent solids. This confirms that crystalline PCMs employ a unique bonding mechanism coined metavalent bonding (MVB). While crystalline PCMs employ MVB, amorphous PCMs behave as covalent solids characterized by a much lower PME. PCMs thus change their bonding upon crystallization, consistent with quantum-chemical calculations of bonding. Crystalline solids with a high PME lie in a narrow conductivity range between metals and iono-covalent solids, indicative for a competition between electron localization and delocalization. A map quantifying chemical bonding locates metavalent solids in a region where approximately one electron is shared between adjacent atoms and bonding is not too ionic. This quantum chemical bonding map is now used to find and explain property trends relevant for PCMs in various application domains.

cond-mat.mtrl-sci↗

arXiv2026

Divergent Coherent Phonon Responses Across the Metal-Insulator Crossover

Ultrafast laser control of material properties hinges on understanding light-matter interactions. We use two experimentally accessible response functions, laser fluence induced phonon softening and the amplitude of coherent reflectance oscillations, to compare how strongly different materials respond to ultrafast photoexcitation. Comparing a diverse set of materials, we find that only a narrow class, including Sb, GeTe, and Bi2Te3, shows exceptional responses such as pronounced phonon softening and a giant increase of reflectance oscillations with increasing fluence. These response functions peak in an intermediate conductivity regime of about 102 - 104 S/cm, at the crossover between localized and delocalized electronic states. The corresponding class of solids also shows other unconventional properties including high dielectric constants, enhanced Born effective charges, coordination numbers exceeding the 8-N rule and uncommon bond rupture. This suggests that these materials employ a unique bonding mechanism, coined metavalent bonding. Frozen-phonon DFT calculations show that the strong fluence dependence arises from Peierls-like instabilities, leading to large deformation potentials and anharmonic double-well potentials. These findings identify metavalent bonding as a design principle for enhanced coherent phonon control and provide a quantitative framework for identifying materials with exceptional ultrafast responses.

cond-mat.mtrl-sci↗

arXiv2026

Understanding inhomogeneous crystallization dynamics of phase-change materials in the vicinity of metallic nanoantennas

Optical metasurfaces composed of metallic or dielectric scatterers (meta-atoms) promise a powerful way of tailoring light-matter interactions. Phase-change materials (PCMs) are prime candidates for non-volatile resonance tuning of metasurfaces based on a refractive index change. Precise resonance control can be achieved by locally applying laser pulses to crystallize a PCM, modifying the dielectric surrounding of meta-atoms. However, the complex crystallization kinetics of PCMs in the vicinity of metallic meta-atoms have not been studied yet. Here, we experimentally investigate metallic dimer antennas on top of the PCM Ge3Sb2Te6 and address these nanoantennas with laser pulses. Our study reveals inhomogeneous crystallization caused by the absorption and heat conduction of the metallic nanoantennas. A self-consistent multiphysics model, including electromagnetic, thermal, and phase-transition processes, is employed to simulate the crystallization and understand the resulting resonance shift of the antennas. This model enables the optimization of the laser parameters and the geometry of the meta-atoms to achieve an optimal crystallization pattern and resonance shift. Our work paves the way towards complex antenna geometries optimized for local addressing of PCMs to achieve sophisticated crystallization patterns, enabling on-demand programming of individual nanoantennas within metasurfaces.

physics.optics↗

arXiv2026

Fast Programming of In-Plane Hyperbolic Phonon Polariton Optics Through van der Waals Crystals using the Phase-Change Material In3SbTe2

The high directionality of hyperbolic phonon polaritons (HPhPs) has opened radically new ways to route and steer the flow of energy at the nanoscale. However, launching HPhPs requires fabricating efficient and precisely aligned polariton launching structures, which remains time-consuming and expensive with conventional nanofabrication approaches. Recently, using optical laser pulses, polariton launching structures have been programmed into the plasmonic phase-change material In3SbTe2. Here, we leverage this approach to reconfigure HPhPs by programming a variety of launching and confining nanostructures through {\alpha}-MoO3 flakes deposited onto In3SbTe2. Importantly, optical programming after flake deposition enables alignment of launching stripes to the [001]-axis of the flake, essential to control the directional polariton propagation. We showcase these capabilities in a variety of structures: i) an optically programmed disk, showing similar tuning ranges and confinement as focusing by gold disks; and ii) a cavity for in-plane HPhPs created by reconfiguring the single disk to a double disk structure, tailoring the confinement by simply reprogramming the disk distance. Our fabrication scheme offers fast turn-around times, flexible alignment and the opportunity to reconfigure the structures. Thus, it is a fast, efficient and versatile way to tailor propagation and confinement of highly directional polaritons on demand.

physics.optics↗

arXiv2025

Atomistic understanding of two-dimensional monatomic phase-change material for non-volatile optical applications

Elemental antimony (Sb) is a promising material for phase-change memory, neuromorphic computing and nanophotonic applications, because its compositional simplicity can prevent phase segregation upon extensive programming. Scaling down the film thickness is a necessary step to prolong the lifetime of amorphous Sb, but the optical properties of Sb are also significantly altered as the thickness is reduced to a few nanometers, adding complexity to device optimization. In this work, we aim to provide atomistic understanding of the thickness-dependent optical responses in Sb thin films. As thickness decreases, both the extinction coefficient and optical contrast reduce in the near-infrared spectrum, consistent with previous optical measurements. Such thickness dependence gives rise to a bottom thickness limit of 2 nm in photonic applications, as predicted by coarse-grained device simulations. Further bonding analysis reveals a fundamentally different behavior for amorphous and crystalline Sb upon downscaling, resulting in the reduction of optical contrast. Thin film experiments are also carried out to validate our predictions. The thickness-dependent optical trend is fully demonstrated by our ellipsometric spectroscopy experiments, and the bottom thickness limit of 2 nm is confirmed by structural characterization experiments. Finally, we show that the greatly improved amorphous-phase stability of the 2 nm Sb thin film enables robust and reversible optical switching in a silicon-based waveguide device.

cond-mat.mtrl-sci↗

arXiv2025

Robust Material Properties in Epitaxial In$_2$Te$_3$ Thin Films Across Varying Thicknesses

Sesqui-chalcogenides serve as a critical bridge between traditional semiconductors and quantum materials, offering significant potential in applications such as thermoelectrics, phase change memory, and topological insulators. While considerable attention has been focused on antimony- and bismuth-based compounds, characterized by substantial property changes upon reduction in film thickness, indium containing sesqui-chalcogenides like In$_2$Te$_3$ are emerging as promising candidates for photovoltaics and electronic devices. However, the effects of film thickness on the properties of In$_2$Te$_3$ remain largely unexplored. In this study, we investigate high-quality In$_2$Te$_3$ thin films grown by molecular beam epitaxy on Si(111) substrates across a thickness range from 2.7 nm to 24 nm. We employ X-ray diffraction, reflective high-energy electron diffraction and atomic force microscopy to analyze both the crystal structure and film morphology. Additionally, we utilize broadband optical spectroscopy alongside femtosecond pump-probe measurements and Raman spectroscopy to assess optical and vibrational properties, respectively. Our analysis reveals that material properties exhibit minimal dependence on film thickness, contrasting sharply with behavior observed in other chalcogenides such as Sb$_2$Te$_3$, Bi$_2$Se$_3$, or GeTe. This phenomenon can be attributed to covalent bonding present in In$_2$Te$_3$, which differs from those in its antimony- and bismuth-containing counterparts.

cond-mat.mtrl-sci↗

arXiv2025

Isothermal Annealing Effects on $\beta$-Relaxations and Crystallization Behaviors in Amorphous GeTe

A secondary $\beta$-relaxation process is often the dominant source of atomic dynamics below $T_\mathrm{g}$ in many glass forming systems. Recent studies reported the presence of $\beta$-relaxations in amorphous phase-change materials (PCMs) and showed that suppressing the $\beta$-relaxation via annealing in Ge$_{15}$Sb$_{85}$ can effectively slow down its crystallization kinetics. Yet, when Sb is replaced by Te, similar annealing protocol has little effect on the Te-rich alloy Ge$_{15}$Te$_{85}$. Here, we investigate amorphous GeTe that is a Sb-free PCM, but with faster crystallization kinetics than Ge$_{15}$Te$_{85}$. Using powder mechanical dynamic spectroscopy, we observe a clear reduction of the excess-wing in the loss modulus upon isothermal annealing, indicating a suppression of its $\beta$-relaxation. Ultrafast calorimetric analysis and time-resolved optical reflectivity measurements show that, whereas as-deposited GeTe exhibit stochastic crystallization behaviors, annealed samples crystallize more slowly with reduced stochasticity. Synchrotron X-ray scattering experiments reveal reinforced Peierls-like distortions in the amorphous structure after annealing, and demonstrate that, even if annealing introduces nucleation sites, it nonetheless slows down crystallization kinetics. These finding suggests that, in annealed GeTe, crystallization is limited by crystal growth rate, which is retarded through the suppression of $\beta$-relaxation.

cond-mat.mtrl-sci↗

arXiv2025

Tailoring hBN's Phonon Polaritons with the Plasmonic Phase-Change Material In3SbTe2

Polaritons in van-der-Waals materials (vdWM) promise high confinement and multiple tailoring options by optical structures, e.g., resonators, launching structures and lenses. These optical structures are conventionally fabricated using cumbersome multi-process lithography techniques. In contrast, phase-change materials (PCMs) offer fast and reconfigurable programming of optical structures. PCMs can reversibly be switched between two stable phases with distinct permittivities by local heating, e.g., by optical laser pulses. While the well-known dielectric PCM GeSbTe-alloys feature only a permittivity change, the PCM In3SbTe2 can be switched between a dielectric and metallic phase. This makes In3SbTe2 promising for programming metallic launching structures. Here, we demonstrate direct optical programming and thereby rapid prototyping of optical launching structures in In3SbTe2 to tailor and confine polaritons in vdWM. We combine the vdWM hexagonal boron nitride (hBN) with In3SbTe2 and optically program circular resonators for hBN's phonon polaritons through hBN into In3SbTe2. We investigate the polariton resonators with near-field optical microscopy. Demonstrating the reconfigurability, we decrease the resonator diameter to increase the polariton confinement. Finally, we fabricate focusing structures for hBN's phonon polaritons whose focal point is changed in a second post-processing step. We promote In3SbTe2 as a versatile platform for rapid prototyping of polariton optics in vdWM.

physics.optics↗

arXiv2024

Infrared Beam-shaping on Demand via Tailored Geometric Phase Metasurfaces employing the Plasmonic Phase-Change Material In3SbTe2

Conventional optical elements are bulky and limited to specific functionalities, contradicting the increasing demand of miniaturization and multi-functionalities. Optical metasurfaces enable tailoring light-matter interaction at will, especially important for the infrared spectral range which lacks commercially available beam-shaping elements. While the fabrication of those metasurfaces usually requires cumbersome techniques, direct laser writing promises a simple and convenient alternative. Here, we exploit the non-volatile laser-induced insulator-to-metal transition of the plasmonic phase-change material In3SbTe2 (IST) for optical programming of large-area metasurfaces for infrared beam-shaping. We tailor the geometric phase of metasurfaces with rotated crystalline IST rod antennas to achieve beam steering, lensing, and beams carrying orbital angular momenta. Finally, we investigate multi-functional and cascaded metasurfaces exploiting enlarged holography, and design a single metasurface creating two different holograms along the optical axis. Our approach facilitates fabrication of large-area metasurfaces within hours, enabling rapid-prototyping of customized infrared meta-optics for sensing, imaging and quantum information.

physics.optics↗

arXiv2024

Atom probe tomography: a local probe for chemical bonds in solids

Atom probe tomography is frequently employed to characterize the elemental distribution in solids with atomic resolution. Here we review and discuss the potential of this technique to locally probe chemical bonds. Two processes characterize the bond rupture in laser-assisted field emission, the probability of molecular ions, i.e. the probability that molecular ions (PMI) are evaporated instead of single (atomic) ions, and the probability of multiple events, i.e. the correlated field-evaporation of more than a single fragment (PME) upon laser- or voltage pulse excitation. Here we demonstrate that one can clearly distinguish solids with metallic, covalent, and metavalent bonds based on their bond rupture, i.e. their PME and PMI values. Differences in the field penetration depth can largely explain these differences in bond breaking. These findings open new avenues in understanding and designing advanced materials, since they allow a quantification of bonds in solids on a nanometer scale, as will be shown for several examples. These possibilities would even justify calling the present approach bonding probe tomography (BPT).

cond-mat.mtrl-sci↗

arXiv2023

Direct programming of confined Surface Phonon Polariton Resonators using the plasmonic Phase-Change Material In$_3$SbTe$_2$

Tailoring light-matter interaction is essential to realize nanophotonic components. It can be achieved with surface phonon polaritons (SPhPs), an excitation of photons coupled with phonons of polar crystals, which also occur in 2d materials such as hexagonal boron nitride or anisotropic crystals. Ultra-confined resonances are observed by restricting the SPhPs to cavities. Phase-change materials (PCMs) enable non-volatile programming of these cavities based on a change in the refractive index. Recently, the new plasmonic PCM In$_3$SbTe$_2$ (IST) was introduced which can be reversibly switched from an amorphous dielectric state to a crystalline metallic one in the entire infrared to realize numerous nanoantenna geometries. However, reconfiguring SPhP resonators to modify the confined polaritons modes remains elusive. Here, we demonstrate direct programming of confined SPhP resonators by phase-switching IST on top of a polar silicon carbide crystal and investigate the strongly confined resonance modes with scanning near-field optical microscopy. Reconfiguring the size of the resonators themselves result in enhanced mode confinements up to a value of $\lambda/35$. Finally, unconventional cavity shapes with complex field patterns are explored as well. This study is a first step towards rapid prototyping of reconfigurable SPhP resonators that can be easily transferred to hyperbolic and anisotropic 2d materials.

physics.optics↗

arXiv2023

Machine learning-enabled tomographic imaging of chemical short-range atomic ordering

In solids, chemical short-range order (CSRO) refers to the self-organisation of atoms of certain species occupying specific crystal sites. CSRO is increasingly being envisaged as a lever to tailor the mechanical and functional properties of materials. Yet quantitative relationships between properties and the morphology, number density, and atomic configurations of CSRO domains remain elusive. Herein, we showcase how machine learning-enhanced atom probe tomography (APT) can mine the near-atomically resolved APT data and jointly exploit the technique's high elemental sensitivity to provide a 3D quantitative analysis of CSRO in a CoCrNi medium-entropy alloy. We reveal multiple CSRO configurations, with their formation supported by state-of-the-art Monte-Carlo simulations. Quantitative analysis of these CSROs allows us to establish relationships between processing parameters and physical properties. The unambiguous characterization of CSRO will help refine strategies for designing advanced materials by manipulating atomic-scale architectures.

cond-mat.mtrl-sci↗

arXiv2023

A Universal Strategy of Perovskite Ink-Substrate Interaction to Overcome the Poor Wettability of a Self-Assembled Monolayer for Reproducible Perovskite Solar Cells

Perovskite solar cells employing self assembled monolayers such as Me-4PACz as hole transport layer has been reported to demonstrate high device efficiency. However, the poor perovskite wetting on the Me-4PACz caused by poor perovskite ink interaction with the underlying Me-4PACz presents significant challenges for fabricating efficient perovskite devices. A triple co-solvent system comprising of dimethylformamide (DMF), dimethyl sulfoxide (DMSO) and N-methyl-2-pyrrolidone (NMP) is employed to improve the perovskite ink-substrate interaction and obtain a uniform perovskite layer. In comparison to DMF, DMSO-based inks, the inclusion of NMP shows considerably higher binding energies of the perovskite ink with Me-4PACz as revealed by density-functional theory calculations. With the optimized triple co-solvent ratio, the perovskite devices deliver high power conversion efficiencies of >20%, 19.5% and ~18.5% for active areas of 0.16 cm2, 0.72 cm2 and 1.08 cm2 respectively. Importantly, this perovskite ink-substrate interaction approach is universal and helps in obtaining a uniform layer and high photovoltaic device performance for other perovskite compositions such as MAPbI3, FAMAPbI3-xBrx, and MA-free FACsPbI3-xBrx.

physics.app-ph↗

arXiv2022

In situ characterization of vacancy ordering in Ge-Sb-Te phase-change memory alloys

Tailoring the degree of structural disorder in Ge-Sb-Te alloys is important for the development of non-volatile phase-change memory and neuro-inspired computing. Upon crystallization from the amorphous phase, these alloys form a cubic rocksalt-like structure with a high content of intrinsic vacancies. Further thermal annealing results in a gradual structural transition towards a layered structure and an insulator-to-metal transition. In this work, we elucidate the atomic-level details of the structural transition in crystalline GeSb2Te4 by in situ high-resolution transmission electron microscopy (HRTEM) experiments and ab initio density functional theory (DFT) calculations, providing a comprehensive real-time and real-space view of the vacancy ordering process. We also discuss the impact of vacancy ordering on altering the electronic and optical properties of GeSb2Te4, which is relevant to multilevel storage applications. The phase evolution paths in Ge-Sb-Te alloys are illustrated using a summary diagram, which serves as a guide for designing phase-change memory devices.

cond-mat.mtrl-sci↗

arXiv2022

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↗