The interplay of optics, dynamics and transport is crucial for the design of novel optoelectronic devices, such as photodetectors and solar cells. In this context, transition metal dichalcogenides (TMDs) have received much attention. Here, strongly bound excitons dominate optical excitation, carrier dynamics and diffusion processes. While the first two have been intensively studied, there is a lack of fundamental understanding of non-equilibrium phenomena associated with exciton transport that is of central importance e.g. for high efficiency light harvesting. In this work, we provide microscopic insights into the interplay of exciton propagation and many-particle interactions in TMDs. Based on a fully quantum mechanical approach and in excellent agreement with photoluminescence measurements, we show that Auger recombination and emission of hot phonons act as a heating mechanism giving rise to strong spatial gradients in excitonic temperature. The resulting thermal drift leads to an unconventional exciton diffusion characterized by spatial exciton halos.
Indirect excitons (IXs), also known as interlayer excitons, can form the medium for excitonic devices whose operation is based on controlled propagation of excitons. A proof of principle for excitonic devices was demonstrated in GaAs heterostructures where the operation of excitonic devices is limited to low temperatures. IXs in van der Waals transition-metal dichalcogenide (TMD) heterostructures are characterized by high binding energies making IXs robust at room temperature and offering an opportunity to create excitonic devices operating at high temperatures suitable for applications. Howev…
Long lifetimes of spatially indirect excitons (IXs), also known as interlayer excitons, make possible long-range IX propagation. Van der Waals heterostructures composed of atomically thin layers of transition-metal dichalcogenides (TMDs) give an opportunity to realize excitons with high binding energies and provide a materials platform for the realization of both excitonic quantum phenomena and excitonic devices. Propagation of IXs in TMD heterostructures is intensively studied. However, in spite of long IX lifetimes, orders of magnitude longer than lifetimes of spatially direct excitons (DXs)…
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 ang…
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 excito…
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 h…
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 d…
We perform explicit time-dependent classical and quantum propagation of a spatially indirect exciton (SIX) driven by surface acoustic waves (SAWs) in a semiconductor heterostructure device. We model the SIX dynamics at different levels of description, from the Euler-Lagrange propagation of structureless classical particles to unitary Schrödinger propagation of an electron-hole wave packet in a mean field and to the full quantum propagation of the two-particle complex. A recently proposed beyond mean-field self-energy approach, adding internal virtual transitions to the c.m. dynamics, has been …
Excitonic insulators host a condensate of electron-hole pairs at equilibrium, giving rise to collective many-body effects. Although several materials have emerged as excitonic insulator candidates, evidence of long-range coherence is lacking and the origin of the ordered phase in these systems remains controversial. Here, using ultrafast pump-probe microscopy, we investigate the possible excitonic insulator Ta$_2$NiSe$_5$. Below 328 K, we observe the anomalous micrometer-scale propagation of coherent modes at velocities of the order of $\sim10^5$ m/s, which we attribute to the hybridization be…
We investigate the propagation of surface plasmons (SPPs) in a thin layer of copper surrounded by copper oxide Cu$_2$O. It is shown that particularly strong excitons in Cu$_2$O can have considerable impact on plasmon propagation, providing many opportunities for plasmon-exciton and plasmon-plasmon interactions. It is demonstrated that by the use of sufficiently thin metal layer, one can excite the so-called long range plasmons (LRSPPs) which can overcome the inherently high ohmic losses of Cu as compared to usual plasmonic metals such as silver. Analytical results are confirmed by numerical ca…
Phonon wind and drag of excitons in monolayer semiconductors
从理论上研究了过渡金属双硫族化合物单层膜中激子的非平衡输运。我们考虑激子与非平衡声子相互作用的情况，例如，在局部激发的条件下形成“热点”。我们发展了声子对激子拖曳的理论，并详细分析了声子的扩散传播和声子的弹道传播的声子风形成的制度。我们证明了类似于在[Phys. Rev. Lett. 120，207401（2018）]可以由于非平衡声子或塞贝克效应的激子拖曳而形成。
The exciton polariton (EP), a half-light and half-matter quasiparticle, is potentially an important element for future photonic and quantum technologies. It provides both strong light-matter interactions and long-distance propagation that is necessary for applications associated with energy or information transfer. Recently, strongly-coupled cavity EPs at room temperature have been demonstrated in van der Waals (vdW) materials due to their strongly-bound excitons. Here we report a nano-optical imaging study of waveguide EPs in MoSe2, a prototypical vdW semiconductor. The measured propagation l…
Exciton transport driven by spin excitations in an antiferromagnet
TUD Dresden University of Technology（德累斯顿工业大学）；Technical University of Munich（慕尼黑工业大学）；Ioffe Institute（约费研究所）；University of Chemistry and Technology Prague（布拉格化工大学）；Rheinland-Pfälzische Technische Universität Kaiserslautern-Landau（莱茵兰-普法尔茨技术大学凯泽斯劳滕-兰道分校）；Universidad Autónoma de Madrid（马德里自治大学）
In recent years, novel materials supporting in-plane anisotropic polaritons have attracted a lot of research interest due to their capability of shaping nanoscale field distributions and controlling nanophotonic energy flows. Here we report a nano-optical imaging study of waveguide exciton polaritons (EPs) in tin sulfide (SnS) in the near-infrared (IR) region using the scattering-type scanning near-field optical microscopy (s-SNOM). With s-SNOM, we mapped in real space the propagative EPs in SnS, which show sensitive dependence on the excitation energy and sample thickness. Moreover, we found …
Hyperbolic materials exhibit unique properties that enable a variety of intriguing applications in nanophotonics. The topological insulator Bi2Se3 represents a natural hyperbolic optical medium, both in the THz and visible range. Here, using cathodoluminescence spectroscopy and electron energy-loss spectroscopy, we demonstrate that Bi2Se3, in addition to being a hyperbolic material, supports room-temperature exciton polaritons. Moreover, we explore the behavior of hyperbolic edge exciton polaritons in Bi2Se3. Edge polaritons are hybrid modes that result from the coupling of the polaritons boun…
Hyperbolic polaritons exhibit large photonic density of states and can be collimated in certain propagation directions. The majority of hyperbolic polaritons are sustained in man-made metamaterials. However, natural-occurring hyperbolic materials also exist. Particularly, natural in-plane hyperbolic polaritons in layered materials have been demonstrated in MoO3 and WTe2, which are based on phonon and plasmon resonances respectively. Here, by determining the anisotropic optical conductivity (dielectric function) through optical spectroscopy, we predict that monolayer black phosphorus naturally …
Atomically-thin transition metal dichalcogenide crystals (TMDCs) hold great promise for future semiconductor optoelectronics due to their unique electronic and optical properties. In particular, electron-hole pairs (excitons) in TMDCs are stable at room temperature and interact strongly with light. When TMDCs are embedded in an optical microcavity, the excitons can hybridise with cavity photons to form exciton polaritons (polaritons herein), which display both ultrafast velocities and strong interactions. The ability to manipulate and trap polaritons on a microchip is critical for future appli…
We consider theoretically the dynamics of exciton-polaritons in a zigzag chain of coupled elliptical micropillars subjected to incoherent excitation. The driven-dissipative nature of the system along with the naturally present polarization splitting inside the pillars gives rise to the non-reciprocal dynamics, which eventually leads to the non-Hermitian skin effect, where all the modes of the system collapse to one edge. As a result, the polaritons propagate only in one direction along the chain, independent of the excitation position, and the propagation in the opposite direction is suppresse…
