Ermin Malic

Lateral heterostructures of transition-metal dichalcogenides (TMDs) host spatially separated charge-transfer (CT) excitons. While analogous to interlayer excitons in vertical TMD heterostructures, these interfacial excitons possess much larger in-plane dipoles of several nanometers and an additional center-of-mass quantization. Here, we investigate mutual interactions between these highly dipolar CT excitons using a quantum mechanical approach. Accounting for the dipolar and quantum exchange interactions, we evaluate the experimentally accessible density-dependent energy renormalization and predict a net energy blueshift of a few meV for bound CT excitons. Interestingly, for small dipole moments, the energy renormalization displays a quadratic dependence with respect to the dipole moment, in contrast to the linear dependence found in vertical TMD heterostructures. We show that spatial energy offset and temperature are the key tuning knobs for controlling the density-dependent excitonic response. Overall, our results contribute to a better microscopic understanding of CT excitons and their interactions in lateral TMD heterostructures.

Modern short-scale information transmission mainly relies on dissipative charge transport, with electrons scattered by defects and phonons, leading to significant power losses. By contrast, excitons—charge-neutral quasiparticles—offer a playground for electro-optical energy-efficient information transduction and processing owing to their extended lifetimes, charge neutrality and efficient electrostatic control. In this work, we report the observation of fast exciton transport in a van der Waals heterostructure over distances exceeding 10 µm, constrained only by the heterostructure finite size. We observe the presence of excitonic potential ramps that leads to long-range rapid exciton drift and enables rapid dilution of the initial exciton population. Our measurements reveal fast exciton propagation, with interlayer exciton drift velocities of approximately 2.66 × 10 ⁴ m s ⁻¹ , within a transport regime that remains robust across a wide range of exciton densities and temperatures up to 150 K. Our work opens avenues for the development of high-speed, energy-efficient excitonic devices, such as field-effect switches and modulators.

Extended efforts have been devoted to the study of strongly-interacting excitons and their dynamics, towards macroscopic quantum states of matter such as Bose-Einstein condensates of excitons and polaritons. Momentum-direct layer-hybridized excitons in transition metal dichalcogenides have attracted considerable attention due to their high oscillator strength and dipolar nature. However, the tunability of their interactions and dynamics remains unexplored. Here, we achieve an unprecedented control over the nonlinear properties of dipolar layer-hybridized excitons in an electrically gated van der Waals homobilayer monitored by transient optical spectroscopy. By applying a vertical electric field, we reveal strong Coulomb interactions of dipolar hybrid excitons, leading to opposite density-dependent energy shifts of the two main hybrid species based on their dipolar orientation, together with a strongly enhanced optical saturation of their absorption. Furthermore, by electrically tuning the interlayer tunneling between the hybridized carriers, we significantly extend the formation time of hybrid excitons, while simultaneously increasing their decay times. Our findings have implications for the search on quantum blockade and condensation of excitons and dipolaritons in two-dimensional materials.

Controlling exciton relaxation and energy conversion pathways via their coupling to photonic modes is a central task in cavity-mediated quantum materials research. In this context, the light-matter hybridization in optical cavities can lead to intriguing effects, such as modified carrier transport, enhancement of optical quantum yield, and control of chemical reaction pathways. Here, we investigate the impact of the strong light-matter coupling regime on energy conversion, both in relaxation and upconversion schemes, by utilizing a strongly charged MoSe ₂ monolayer embedded in a spectrally tunable open-access cavity. We find that the charge carrier gas yields a significantly modified photoluminescence response of cavity exciton-polaritons, dominated by an intra-cavity like pump scheme. In addition, upconversion luminescence emerges from a population transfer from fermionic trions to bosonic exciton-polaritons. Due to the availability of multiple optical modes in the tunable open cavity, it seamlessly meets the cavity-enhanced double resonance condition required for an efficient upconversion. The latter can be actively tuned via the cavity length in-situ, displaying nonlinear scaling in intensity and fingerprints of the valley polarization. This suggests mechanisms that include both trion-trion Auger scattering and phonon absorption as its underlying microscopic origin.

Extended efforts have been devoted to the study of strongly-interacting excitons and their dynamics, towards macroscopic quantum states of matter such as Bose-Einstein condensates of excitons and polaritons. Momentum-direct layer-hybridized excitons in transition metal dichalcogenides have attracted considerable attention due to their high oscillator strength and dipolar nature. However, the tunability of their interactions and dynamics remains unexplored. Here, we achieve an unprecedented control over the nonlinear properties of dipolar layer-hybridized excitons in an electrically gated van der Waals homobilayer monitored by transient optical spectroscopy. By applying a vertical electric field, we reveal strong Coulomb interactions of dipolar hybrid excitons, leading to opposite density-dependent energy shifts of the two main hybrid species based on their dipolar orientation, together with a strongly enhanced optical saturation of their absorption. Furthermore, by electrically tuning the interlayer tunneling between the hybridized carriers, we significantly extend the formation time of hybrid excitons, while simultaneously increasing their decay times. Our findings have implications for the search on quantum blockade and condensation of excitons and dipolaritons in two-dimensional materials.

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.

Controlling exciton relaxation and energy conversion pathways via their coupling to photonic modes is a central task in cavity-mediated quantum materials research. In this context, the light-matter hybridization in optical cavities can lead to intriguing effects, such as modified carrier transport, enhancement of optical quantum yield, and control of chemical reaction pathways. Here, we investigate the impact of the strong light-matter coupling regime on energy conversion, both in relaxation and upconversion schemes, by utilizing a strongly charged MoSe ₂ monolayer embedded in a spectrally tunable open-access cavity. We find that the charge carrier gas yields a significantly modified photoluminescence response of cavity exciton-polaritons, dominated by an intra-cavity like pump scheme. In addition, upconversion luminescence emerges from a population transfer from fermionic trions to bosonic exciton-polaritons. Due to the availability of multiple optical modes in the tunable open cavity, it seamlessly meets the cavity-enhanced double resonance condition required for an efficient upconversion. The latter can be actively tuned via the cavity length in-situ, displaying nonlinear scaling in intensity and fingerprints of the valley polarization. This suggests mechanisms that include both trion-trion Auger scattering and phonon absorption as its underlying microscopic origin.

Optical microcavities provide a powerful and versatile framework for manipulating the dynamics of photonic emission from optically active materials through light recirculation. Spatially indirect interlayer excitons (IXs) exhibit broad tunability of their emission energy via the quantum-confined Stark effect. However, the electrical tunability of IXs has not been exploited in cavity-coupled systems until now. Here we modulate the detuning between the cavity resonance and the IX emission in a monolithic Fabry–Perot cavity using an applied vertical electric field. We reveal a simultaneous enhancement of both the emission intensity and lifetime of weakly coupled IXs when in resonance with the optical cavity owing to strong Purcell inhibition and cavity transparency effects. We further investigate the tunable momentum dispersion of coupled IXs through back-focal-plane imaging and explain our results by the cavity coupling of IX transition dipoles as supported by theoretical modelling. Our work demonstrates an integration effort enabling the versatile tuning of highly interacting IXs within monolithic cavities, revealing the attractiveness of electrically tunable IX cavity coupling for both fundamental studies towards exciton condensate manipulation and future integration of excitonic devices.

MoTe 2 monolayers and bilayers are unique within the family of van der Waals materials since they pave the way toward atomically thin infrared light-matter quantum interfaces, potentially reaching the important telecommunication windows. Here, we report emergent exciton polaritons based on MoTe 2 monolayers and bilayers in a low-temperature open microcavity in a joint experiment-theory study. Our experiments clearly evidence both the enhanced oscillator strength and enhanced luminescence of MoTe 2 bilayers, signified by a 38% increase of the Rabi splitting and a strongly enhanced relaxation of polaritons to low-energy states. The latter is distinct from polaritons in MoTe 2 monolayers, which feature a bottlenecklike relaxation inhibition. Both the polaritonic spin valley locking in monolayers and the spin-layer locking in bilayers are revealed via the Zeeman effect, which we map and control via the light-matter composition of our polaritonic resonances.