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93 result(s) for "Brem, Samuel"
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Exciton transport in atomically thin semiconductors
Atomically thin semiconductors have been in the center of one of the most active research fields. Here, we discuss the main challenges in exciton transport that is crucial for nanoelectronics. We focus on transport phenomena in monolayers, lateral heterostructures, and twisted heterostacks of transition metal dichalcogenides. In this Comment, the authors discuss the current status, the challenges, and potential technological impact of exciton transport in transition metal dichalcogenide (TMD) monolayers, lateral and vertical heterostructures as well as moiré excitons in twisted TMD heterostacks.
Spatiotemporal dynamics of moiré excitons in van der Waals heterostructures
Heterostructures of transition metal dichalcogenides (TMDs) offer unique opportunities in optoelectronics due to their strong light-matter interaction and the formation of dipolar interlayer excitons. Introducing a twist angle or lattice mismatch between layers creates a periodic moiré potential that significantly reshapes the energy landscape and introduces a high-dimensional complexity absent in aligned bilayers. Recent experimental advances have enabled direct observation and control of interlayer excitons in such moiré-patterned systems, yet a microscopic theoretical framework capturing both their thermalization and spatiotemporal dynamics remains lacking. Here, we address this challenge by developing a predictive, material-specific many-body model that tracks exciton dynamics across time, space, and momentum, fully accounting for the moiré potential and the complex non-parabolic exciton band structure. Surprisingly, we reveal that flat bands, which typically trap excitons, can significantly enhance exciton propagation. This counterintuitive behavior emerges from the interplay between the flat-band structure giving rise to a bottleneck effect for exciton relaxation and thermal occupation dynamics creating hot excitons. Our work not only reveals the microscopic mechanisms behind the enhanced propagation but also enables the control of exciton transport via twist-angle engineering. These insights lay the foundation for next-generation moiré-based optoelectronic and quantum technologies. Here, the authors develop a predictive, material-specific many-body model for moiré heterostructures of transition metal dichalcogenides that tracks exciton dynamics across time, space, and momentum, fully accounting for the moiré potential and the complex non-parabolic exciton band structure.
Dielectric disorder in two-dimensional materials
Understanding and controlling disorder is key to nanotechnology and materials science. Traditionally, disorder is attributed to local fluctuations of inherent material properties such as chemical and structural composition, doping or strain. Here, we present a fundamentally new source of disorder in nanoscale systems that is based entirely on the local changes of the Coulomb interaction due to fluctuations of the external dielectric environment. Using two-dimensional semiconductors as prototypes, we experimentally monitor dielectric disorder by probing the statistics and correlations of the exciton resonances, and theoretically analyse the influence of external screening and phonon scattering. Even moderate fluctuations of the dielectric environment are shown to induce large variations of the bandgap and exciton binding energies up to the 100 meV range, often making it a dominant source of inhomogeneities. As a consequence, dielectric disorder has strong implications for both the optical and transport properties of nanoscale materials and their heterostructures.
Dark exciton anti-funneling in atomically thin semiconductors
Transport of charge carriers is at the heart of current nanoelectronics. In conventional materials, electronic transport can be controlled by applying electric fields. Atomically thin semiconductors, however, are governed by excitons, which are neutral electron-hole pairs and as such cannot be controlled by electrical fields. Recently, strain engineering has been introduced to manipulate exciton propagation. Strain-induced energy gradients give rise to exciton funneling up to a micrometer range. Here, we combine spatiotemporal photoluminescence measurements with microscopic theory to track the way of excitons in time, space and energy. We find that excitons surprisingly move away from high-strain regions. This anti-funneling behavior can be ascribed to dark excitons which possess an opposite strain-induced energy variation compared to bright excitons. Our findings open new possibilities to control transport in exciton-dominated materials. Overall, our work represents a major advance in understanding exciton transport that is crucial for technological applications of atomically thin materials. Strain engineering can manipulate the propagation of excitons in atomically thin transition metal dichalcogenides. Here, the authors observe an anti-funnelling behavior, i.e., the exciton photoluminescence moves away from high-strain regions, and attribute it to the dominating role of propagating dark excitons.
Ultrafast phonon‐driven charge transfer in van der Waals heterostructures
Van der Waals heterostructures built by vertically stacked transition metal dichalcogenides (TMDs) exhibit a rich energy landscape, including interlayer and intervalley excitons. Recent experiments demonstrated an ultrafast charge transfer in TMD heterostructures. However, the nature of the charge transfer process has remained elusive. Based on a microscopic and material‐realistic exciton theory, we reveal that phonon‐mediated scattering via strongly hybridized intervalley excitons governs the charge transfer process that occurs on a sub‐100fs timescale. We track the time‐, momentum‐, and energy‐resolved relaxation dynamics of optically excited excitons and determine the temperature‐ and stacking‐dependent charge transfer time for different TMD bilayers. The provided insights present a major step in microscopic understanding of the technologically important charge transfer process in van der Waals heterostructures. Key Points Microscopic and fully quantum‐mechanic model is developed to calculate exciton dynamics in van der Waals heterostructures Charge transfer occurs on a femtosecond timescale and is a phonon‐mediated two‐step process Strongly hybridized dark exciton states play a crucial role for the charge transfer
Twist-tailoring Coulomb correlations in van der Waals homobilayers
The recent discovery of artificial phase transitions induced by stacking monolayer materials at magic twist angles represents a paradigm shift for solid state physics. Twist-induced changes of the single-particle band structure have been studied extensively, yet a precise understanding of the underlying Coulomb correlations has remained challenging. Here we reveal in experiment and theory, how the twist angle alone affects the Coulomb-induced internal structure and mutual interactions of excitons. In homobilayers of WSe 2 , we trace the internal 1 s –2 p resonance of excitons with phase-locked mid-infrared pulses as a function of the twist angle. Remarkably, the exciton binding energy is renormalized by up to a factor of two, their lifetime exhibits an enhancement by more than an order of magnitude, and the exciton-exciton interaction is widely tunable. Our work opens the possibility of tailoring quasiparticles in search of unexplored phases of matter in a broad range of van der Waals heterostructures. The crystallographic orientation of monolayers in van der Waals multi-layers controls their electronic and optical properties. Here the authors show how the twist angle affects Coulomb correlations governing the internal structure and the mutual interaction of excitons in homobilayers of WSe 2 .
Interlayer exciton dynamics in van der Waals heterostructures
Atomically thin transition metal dichalcogenides can be stacked to van der Waals heterostructures enabling the design of new materials with tailored properties. The strong Coulomb interaction gives rise to interlayer excitons, where electrons and holes are spatially separated in different layers. In this work, we reveal the time- and momentum-dependent elementary processes behind the formation, thermalization and photoemission of interlayer excitons for the exemplary MoSe 2 –WSe 2 heterostructure. We identify tunneling of holes from MoSe 2 to WSe 2 on a ps timescale as the crucial process for interlayer exciton formation. We also predict a drastic reduction of the formation time as a function of the interlayer energy offset suggesting that interlayer excitons can be externally tuned. Finally, we explain the experimental observation of a dominant photoluminescence from interlayer excitons despite the vanishingly small oscillator strength as a consequence of huge interlayer exciton occupations at low temperatures. Single layers of transition metal dichalcogenides are expected to be suitable for a number of applications and by stacking layers of different materials on top of each other (heterostructures) an even richer variety of properties can be explored. To this end the authors theoretically investigate cross material exciton states in a heterostructures of MoSe 2 and WSe 2 layers.
Quadrupolar excitons in MoSe2 bilayers
The quest for platforms to generate and control exotic excitonic states has greatly benefited from the advent of transition metal dichalcogenide (TMD) monolayers and their heterostructures. Among the unconventional excitonic states, quadrupolar excitons—a superposition of two dipolar excitons with anti-aligned dipole moments—are of great interest for applications in quantum simulations and for the investigation of many-body physics. Here, we unambiguously demonstrate the emergence of quadrupolar excitons in natural MoSe 2 homobilayers, whose energy shifts quadratically in electric field. In contrast to trilayer systems, MoSe 2 homobilayers have many advantages, which include a larger coupling between dipolar excitons. Our experimental observations are complemented by many-particle theory calculations offering microscopic insights in the formation of quadrupolar excitons. Our results suggest TMD homobilayers as ideal platform for the engineering of excitonic states and their interaction with light and thus candidate for carrying out on-chip quantum simulations. Quadrupolar excitons — a superposition of two dipolar excitons with anti-aligned dipole moments — are of great interest for applications in quantum simulations and for the investigation of many-body physics. Here, the authors demonstrate the emergence of quadrupolar excitons in natural MoSe2 homobilayers, whose energy shifts quadratically in electric field.
Sequential order dependent dark-exciton modulation in bi-layered TMD heterostructure
We report the emergence of dark-excitons in transition-metal-dichalcogenide (TMD) heterostructures that strongly rely on the stacking sequence, i.e., momentum-dark K-Q exciton located exclusively at the top layer of the heterostructure. The feature stems from band renormalization and is distinct from those of typical neutral excitons or trions, regardless of materials, substrates, and even homogeneous bilayers, which is further confirmed by scanning tunneling spectroscopy. To understand the unusual stacking sequence, we introduce the excitonic Elliot formula by imposing strain exclusively on the top layer that could be a consequence of the stacking process. We further find that the intensity ratio of Q- to K-excitons in the same layer is inversely proportional to laser power, unlike for conventional K-K excitons. This can be a metric for engineering the intensity of dark K-Q excitons in TMD heterostructures, which could be useful for optical power switches in solar panels. Here, the authors report the emergence of dark-excitons in transition-metal-dichalcogenide heterostructures that strongly rely on the stacking sequence, i.e., momentum-dark K-Q excitons located exclusively at the top layer of the heterostructure.
Electrically tunable layer-hybridized trions in doped WSe2 bilayers
Doped van der Waals heterostructures host layer-hybridized trions, i.e. charged excitons with layer-delocalized constituents holding promise for highly controllable optoelectronics. Combining a microscopic theory with photoluminescence (PL) experiments, we demonstrate the electrical tunability of the trion energy landscape in naturally stacked WSe 2 bilayers. We show that an out-of-plane electric field modifies the energetic ordering of the lowest lying trion states, which consist of layer-hybridized Λ -point electrons and layer-localized K-point holes. At small fields, intralayer-like trions yield distinct PL signatures in opposite doping regimes characterized by weak Stark shifts in both cases. Above a doping-asymmetric critical field, interlayer-like species are energetically favored and produce PL peaks with a pronounced Stark red-shift and a counter-intuitively large intensity arising from efficient phonon-assisted recombination. Our work presents an important step forward in the microscopic understanding of layer-hybridized trions in van der Waals heterostructures and paves the way towards optoelectronic applications based on electrically controllable atomically-thin semiconductors. Here, the authors combine theory and photoluminescence measurements on WSe 2 bilayers and demonstrate the electrical tunability of the trion energy landscape, by showing that an out-of-plane electric field modifies the energetic ordering of the lowest lying trion states.