arXiv subjects

Samuel Brem

Publications and source records attributed to Samuel Brem.

At least 37 records · Page 2Linked to original sources

arXiv2023

Link between interlayer hybridization and ultrafast charge transfer in WS$_2$-graphene heterostructures

Ultrafast charge separation after photoexcitation is a common phenomenon in various van-der-Waals (vdW) heterostructures with great relevance for future applications in light harvesting and detection. Theoretical understanding of this phenomenon converges towards a coherent mechanism through charge transfer states accompanied by energy dissipation into strongly coupled phonons. The detailed microscopic pathways are material specific as they sensitively depend on the band structures of the individual layers, the relative band alignment in the heterostructure, the twist angle between the layers, and interlayer interactions resulting in hybridization. We used time- and angle-resolved photoemission spectroscopy combined with tight binding and density functional theory electronic structure calculations to investigate ultrafast charge separation and recombination in WS$_2$-graphene vdW heterostructures. We identify several avoided crossings in the band structure and discuss their relevance for ultrafast charge transfer. We relate our own observations to existing theoretical models and propose a unified picture for ultrafast charge transfer in vdW heterostructures where band alignment and twist angle emerge as the most important control parameters.

cond-mat.mtrl-sci↗

arXiv2023

Electrical control of hybrid exciton transport in a van der Waals heterostructure

Interactions between out-of-plane dipoles in bosonic gases enable the long-range propagation of excitons. The lack of direct control over collective dipolar properties has hitherto limited the degrees of tunability and the microscopic understanding of exciton transport. In this work, we modulate the layer hybridization and interplay between many-body interactions of excitons in a van der Waals heterostructure with an applied vertical electric field. By performing spatiotemporally resolved measurements supported by microscopic theory, we uncover the dipole-dependent properties and transport of excitons with different degrees of hybridization. Moreover, we find constant emission quantum yields of the transporting species as a function of excitation power with dominating radiative decay mechanisms over nonradiative ones, a fundamental requirement for efficient excitonic devices. Our findings provide a complete picture of the many-body effects in the transport of dilute exciton gases and have crucial implications for the study of emerging states of matter, such as Bose-Einstein condensation, as well as for optoelectronic applications based on exciton propagation.

cond-mat.mes-hall↗

arXiv2023

A room-temperature moiré interlayer exciton laser

Moiré superlattices in van der Waals heterostructures offer highly tunable quantum systems with emergent electronic and excitonic properties such as superconductivity, topological edge states, and moiré-trapped excitons. Theoretical calculations predicted the existence of the moiré potential at elevated temperatures; however, its impact on the optical properties of interlayer excitons (IXs) at room temperature is lacking, and the benefits of the moiré effects for lasing applications remain unexplored. We report that the moiré potential in a molybdenum disulfide/tungsten diselenide (MoS2/WSe2) heterobilayer system can significantly enhance light emission, elongate the IX lifetime, and modulate the IX emission energy at room temperature. By integrating a moiré superlattice with a silicon topological nanocavity, we achieve ultra-low-threshold lasing at the technologically important telecommunication O-band thanks to the significant moiré modulation. Moreover, the high-quality topological nanocavities facilitate the highest spectral coherence of < 0.1 nm linewidth among all reported two-dimensional material-based laser systems. Our findings not only open a new avenue for studying correlated states at elevated temperatures, but also enable novel architectures for integrated on-chip photonics and optoelectronics.

physics.optics↗

arXiv2022

Exciton optics, dynamics and transport in atomically thin semiconductors

Atomically thin semiconductors such as transition metal dichalcogenide (TMD) monolayers exhibit a very strong Coulomb interaction, giving rise to a rich exciton landscape. This makes these materials highly attractive for efficient and tunable optoelectronic devices. In this article, we review the recent progress in the understanding of exciton optics, dynamics and transport, which crucially govern the operation of TMD-based devices. We highlight the impact of hBN-encapsulation, which reveals a plethora of many-particle states in optical spectra, and we outline the most novel breakthroughs in the field of exciton-polaritonics. Moreover, we underline the direct observation of exciton formation and thermalization in TMD monolayers and heterostructures in recent time-resolved ARPES studies. We also show the impact of exciton density, strain and dielectric environment on exciton diffusion and funneling. Finally, we put forward relevant research directions in the field of atomically thin semiconductors for the near future.

cond-mat.mes-hall↗

arXiv2022

Exciton transport in a moiré potential: from hopping to dispersive regime

The propagation of excitons in TMD monolayers has been intensively studied revealing interesting many-particle effects, such as halo formation and non-classical diffusion. Initial studies have investigated how exciton transport changes in twisted TMD bilayers, including Coulomb repulsion and Hubbard-like exciton hopping. In this work, we investigate the twist-angle-dependent transition of the hopping regime to the dispersive regime of effectively free excitons. Based on a microscopic approach for excitons in the presence of a moiré potential, we show that the hopping regime occurs up to an angle of approximately 2° and is well described by the Hubbard model. At large angles, however, the Hubbard model fails due to increasingly delocalized exciton states. Here, the quantum mechanical dispersion of free particles with an effective mass determines the propagation of excitons. Overall, our work provides microscopic insights into the character of exciton propagation in twisted van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2022

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.

cond-mat.mes-hall↗

arXiv2022

Trion-phonon interaction in atomically thin semiconductors

Optical and transport properties of doped monolayer semiconductors are dominated by trions, which are three-particle compounds formed by two electrons and one hole or vice versa. In this work, we investigate the trion-phonon interaction on a microscopic footing and apply our model to the exemplary case of a molybdenum diselenide (MoSe2) monolayer. We determine the trion series of states and their internal quantum structure by solving the trion Schrödinger equation. Transforming the system into a trion basis and solving equations of motion, including the trion-phonon interaction within the second-order Born-Markov approximation, provides a microscopic access to the trion dynamics. In particular, we investigate trion propagation and compute the diffusion coefficient and mobility. In the low density limit, we find that trions propagate less efficiently than excitons and electrons due to their stronger coupling with phonons and their larger mass. For increasing densities, we predict a drastic enhancement of diffusion caused by the build-up of a large pressure by the degenerate trion gas, which is a direct consequence of the fermionic character of trions. Our work provides microscopic insights into the trion-phonon interaction and its impact on the diffusion behaviour in atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2022

Microscopic origin of anomalous interlayer exciton transport in van der Waals heterostructures

Van der Waals heterostructures constitute a platform for investigating intriguing many-body quantum phenomena. In particular, transition-metal dichalcogenide (TMD) hetero-bilayers host long-lived interlayer excitons which exhibit permanent out-of-plane dipole moments. Here, we develop a microscopic theory for interlayer exciton-exciton interactions including both the dipolar nature of interlayer excitons as well as their fermionic substructure, which gives rise to an attractive fermionic exchange. We find that these interactions contribute to a drift force resulting in highly non-linear exciton propagation at elevated densities in the MoSe$_2$-WSe$_2$ heterostructure. We show that the propagation can be tuned by changing the number of hBN spacers between the TMD layers or by adjusting the dielectric environment. In particular, although counter-intuitive, we reveal that interlayer excitons in free-standing samples propagate slower than excitons in hBN-encapsulated TMDs - due to an enhancement of the net Coulomb-drift with stronger environmental screening. Overall, our work contributes to a better microscopic understanding of the interlayer exciton transport in technologically promising atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2022

Electrical tuning of moiré excitons in MoSe$_2$ bilayers

Recent advances in the field of vertically stacked 2D materials have revealed a rich exciton landscape. In particular, it has been demonstrated that out-of-plane electrical fields can be used to tune the spectral position of spatially separated interlayer excitons. Other studies have shown that there is a strong hybridization of exciton states, resulting from the mixing of electronic states in both layers. However, the connection between the twist-angle dependent hybridization and field-induced energy shifts has remained in the dark. Here, we investigate on a microscopic footing the interplay of electrical and twist-angle tuning of moiré excitons in MoSe$_2$ homobilayers. We reveal distinct energy regions in PL spectra that are clearly dominated by either intralayer or interlayer excitons, or even dark excitons. Consequently, we predict twist-angle-dependent critical electrical fields at which the material is being transformed from a direct into an indirect semiconductor. Our work provides new microscopic insights into experimentally accessible knobs to significantly tune the moiré exciton physics in atomically thin nanomaterials.

cond-mat.mes-hall↗

arXiv2022

The moiré potential in twisted transition metal dichalcogenide bilayers

Moiré superlattices serve as a playground for emerging phenomena, such as localization of band states, superconductivity, and localization of excitons. These superlattices are large and are often modeled in the zero angle limit, which obscures the effect of finite twist angles. Here, by means of first-principles calculations we quantify the twist-angle dependence of the moiré potential in the MoS$_2$ homobilayer and identify the contributions from the constituent elements of the moiré potential. Furthermore, by considering the zero-angle limit configurations, we show that the moiré potential is rather homogeneous across the transition metal dichalcogenides (TMDs) and briefly discuss the separate effects of potential shifts and hybridization on the bilayer hybrid excitons. We find that the moiré potential in TMDs exhibits both an electrostatic component and a hybridization component, which are intertwined and have different relative strengths in different parts of the Brillouin zone. The electrostatic component of the moiré potential is a varying dipole field, which has a strong twist angle dependence. In some cases, the hybridization component can be interpreted as a tunneling rate but the interpretation is not generally applicable over the full Brillouin zone.

cond-mat.mtrl-sci↗

arXiv2022

Exciton landscape in van der Waals heterostructures

van der Waals heterostructures consisting of vertically stacked transition-metal dichalcogenides (TMDs) exhibit a rich landscape of bright and dark intra- and interlayer excitons. In spite of a growing literature in this field of research, the type of excitons dominating optical spectra in different van der Waals heterostructures has not yet been well established. The spectral position of exciton states depends strongly on the strength of hybridization and energy renormalization due to the periodic moiré potential. Combining exciton density-matrix formalism and density-functional theory, we shed light on the exciton landscape in TMD homo- and heterobilayers at different stackings. This allows us to identify on a microscopic footing the energetically lowest-lying exciton state for each material and stacking. Furthermore, we disentangle the contribution of hybridization and layer polarization-induced alignment shifts of dark and bright excitons in photoluminescence spectra. By revealing the exciton landscape in van der Waals heterostructures, our work provides the basis for further studies of the optical, dynamical, and transport properties of this technologically promising class of nanomaterials.

cond-mat.mes-hall↗

arXiv2021

Dark exciton-exciton annihilation in monolayer WSe$_2$

The exceptionally strong Coulomb interaction in semiconducting transition-metal dichalcogenides (TMDs) gives rise to a rich exciton landscape consisting of bright and dark exciton states. At elevated densities, excitons can interact through exciton-exciton annihilation (EEA), an Auger-like recombination process limiting the efficiency of optoelectronic applications. Although EEA is a well-known and particularly important process in atomically thin semiconductors determining exciton lifetimes and affecting transport at elevated densities, its microscopic origin has remained elusive. In this joint theory-experiment study combining microscopic and material-specific theory with time- and temperature-resolved photoluminescence measurements, we demonstrate the key role of dark intervalley states that are found to dominate the EEA rate in monolayer WSe$_2$. We reveal an intriguing, characteristic temperature dependence of Auger scattering in this class of materials with an excellent agreement between theory and experiment. Our study provides microscopic insights into the efficiency of technologically relevant Auger scattering channels within the remarkable exciton landscape of atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2021

Terahertz fingerprint of monolayer Wigner crystals

The strong Coulomb interaction in monolayer semiconductors represents a unique opportunity for the realization of Wigner crystals without external magnetic fields. In this work, we predict that the formation of monolayer Wigner crystals can be detected by their terahertz response spectrum, which exhibits a characteristic sequence of internal optical transitions. We apply the density matrix formalism to derive the internal quantum structure and the optical conductivity of the Wigner crystal and to microscopically analyze the multi-peak shape of the obtained terahertz spectrum. Moreover, we predict a characteristic shift of the peak position as function of charge density for different atomically thin materials and show how our results can be generalized to an arbitrary two-dimensional system.

cond-mat.str-el↗

arXiv2021

Valley-exchange coupling probed by angle-resolved photoluminescence

The optical properties of monolayer transition metal dichalcogenides are dominated by tightly-bound excitons. They form at distinct valleys in reciprocal space, and can interact via the valley-exchange coupling, modifying their dispersion considerably. Here, we predict that angle-resolved photoluminescence can be used to probe the changes of the excitonic dispersion. The exchange-coupling leads to a unique angle dependence of the emission intensity for both circularly and linearly-polarised light. We show that these emission characteristics can be strongly tuned by an external magnetic field due to the valley-specific Zeeman-shift. We propose that angle-dependent photoluminescence measurements involving both circular and linear optical polarisation as well as magnetic fields should act as strong verification of the role of valley-exchange coupling on excitonic dispersionand its signatures in optical spectra

cond-mat.mes-hall↗

arXiv2021

Nonclassical Exciton Diffusion in Monolayer WSe2

We experimentally demonstrate time-resolved exciton propagation in a monolayer semiconductor at cryogenic temperatures. Monitoring phonon-assisted recombination of dark states, we find a highly unusual case of exciton diffusion. While at 5 K the diffusivity is intrinsically limited by acoustic phonon scattering, we observe a pronounced decrease of the diffusion coefficient with increasing temperature, far below the activation threshold of higher-energy phonon modes. This behavior corresponds neither to well-known regimes of semiclassical free-particle transport nor to the thermally activated hopping in systems with strong localization. Its origin is discussed in the framework of both microscopic numerical and semi-phenomenological analytical models illustrating the observed characteristics of nonclassical propagation. Challenging the established description of mobile excitons in monolayer semiconductors, these results open up avenues to study quantum transport phenomena for excitonic quasiparticles in atomically-thin van der Waals materials and their heterostructures.

cond-mat.mes-hall↗

arXiv2021

Momentum-resolved observation of exciton formation dynamics in monolayer WS$_2$

The dynamics of exciton formation in transition metal dichalcogenides is difficult to measure experimentally, since many momentum-indirect exciton states are not accessible to optical interband spectroscopy. Here, we combine a tuneable pump, high-harmonic probe laser source with a 3D momentum imaging technique to map photoemitted electrons from monolayer WS$_2$. This provides momentum-, energy- and time-resolved access to excited states on an ultrafast timescale. The high temporal resolution of the setup allows us to trace the early-stage exciton dynamics on its intrinsic timescale and observe the formation of a momentum-forbidden dark K$Σ$ exciton a few tens of femtoseconds after optical excitation. By tuning the excitation energy we manipulate the temporal evolution of the coherent excitonic polarization and observe its influence on the dark exciton formation. The experimental results are in excellent agreement with a fully microscopic theory, resolving the temporal and spectral dynamics of bright and dark excitons in WS$_2$.

cond-mat.mtrl-sci↗

arXiv2021

Non-equilibrium diffusion of dark excitons in atomically thin semiconductors

Atomically thin semiconductors provide an excellent platform to study intriguing many-particle physics of tightly-bound excitons. In particular, the properties of tungsten-based transition metal dichalcogenides are determined by a complex manifold of bright and dark exciton states. While dark excitons are known to dominate the relaxation dynamics and low-temperature photoluminescence, their impact on the spatial propagation of excitons has remained elusive. In our joint theory-experiment study, we address this intriguing regime of dark state transport by resolving the spatio-temporal exciton dynamics in hBN-encapsulated WSe$_2$ monolayers after resonant excitation. We find clear evidence of an unconventional, time-dependent diffusion during the first tens of picoseconds, exhibiting strong deviation from the steady-state propagation. Dark exciton states are initially populated by phonon emission from the bright states, resulting in creation of hot excitons whose rapid expansion leads to a transient increase of the diffusion coefficient by more than one order of magnitude. These findings are relevant for both fundamental understanding of the spatio-temporal exciton dynamics in atomically thin materials as well as their technological application by enabling rapid diffusion.

cond-mat.mes-hall↗

arXiv2021

Exciton-exciton interaction in transition metal dichalcogenide monolayers and van der Waals heterostructures

Due to a strong Coulomb interaction, excitons dominate the excitation kinetics in 2D materials. While Coulomb-scattering between electrons has been well studied, the interaction of excitons is more challenging and remains to be explored. As neutral composite bosons consisting of electrons and holes, excitons show a non-trivial scattering dynamics. Here, we study on microscopic footing exciton-exciton interaction in transition-metal dichalcogenides and related van der Waals heterostructures. We demonstrate that the crucial criterion for efficient scattering is a large electron/hole mass asymmetry giving rise to internal charge inhomogeneities of excitons and emphasizing their cobosonic substructure. Furthermore, both exchange and direct exciton-exciton interactions are boosted by enhanced exciton Bohr radii. We also predict an unexpected temperature dependence that is usually associated to phonon-driven scattering and we reveal an orders of magnitude stronger interaction of interlayer excitons due to their permanent dipole moment. The developed approach can be generalized to arbitrary material systems and will help to study strongly correlated exciton systems, such as moire super lattices.

cond-mat.mtrl-sci↗