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Daniel Erkensten

Publications and source records attributed to Daniel Erkensten.

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Coulomb-mediated interactions of charge-transfer excitons in TMD lateral heterostructures

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 study the mutual interactions between these highly dipolar CT excitons on a microscopic footing. 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.

cond-mat.mes-hall

Valley-controlled many-body exciton interactions in monolayer WSe$_2$ phototransistors

Many-body exciton interactions shape the optoelectronic response of atomically-thin transition metal dichalcogenides, yet optical control of these interactions remains largely unexplored. To date, modulation of exciton-exciton interactions has primarily relied on electrical gating or van der Waals engineering. Here, we demonstrate all-optical control of many-body exciton interactions in monolayer WSe$_2$ via valley-selective excitation using polarization-resolved pulsed-laser photocurrent spectroscopy. Circular excitation selectively populates excitons in a single valley, whereas linear excitation populates both valleys, inducing a valley-dependent nonlinear photoresponse. We observe helicity-dependent exciton renormalization, alongside a two-fold enhancement of sublinear photocurrent scaling under circular excitation, reflecting single-valley population of interacting excitons. A microscopic model incorporating intervalley-exchange and exciton-exciton annihilation mediated by dark and bright exciton populations reproduces the nonlinear valley-selective response. These results establish the valley degree of freedom as an all-optical control parameter for tuning many-body excitonic effects and, exploring correlated exciton states and valleytronic applications in two-dimensional semiconductors.

cond-mat.mes-hall

Exciton Polariton-Polariton Interactions in Transition-Metal Dichalcogenides

Microscopic insights into nonlinear interactions are essential for advancing polaritonic devices. Existing studies often rely on phenomenological models that overlook important many-body processes. Based on a material-specific and predictive approach, we investigate monolayer and homobilayer MoS$_2$ embedded in a Fabry-P\'erot cavity to characterize the exchange, saturation, and dipole-dipole contributions to polariton-polariton interactions in these technologically promising materials. A key finding is that the exchange interaction induces asymmetric energy shifts of the lower and upper polariton branches in a detuned cavity, a behavior driven by the difference in their excitonic character. Furthermore, we demonstrate that temperature and electron-photon coupling determine the energy renormalization through the equilibrium polariton distribution. In homobilayers, the dipole-dipole interaction is mediated by the interlayer character, enabling electrical control and facilitating the electric-field-induced closing of anti-crossings due to dipolar-interaction shifts. The gained insights on polariton-polariton interactions are important for the development of ultra-compact polaritonic circuitry.

cond-mat.mes-hall

Impact of an electron Wigner crystal on exciton propagation

The strong Coulomb interaction in 2D materials facilitates the formation of tightly bound excitons and charge-ordered phases of matter. A prominent example is the formation of a crystalline phase from free charges due to mutual Coulomb repulsion, known as the Wigner crystal. While exciton-electron interactions have been used as a sensor for Wigner crystallization, its impact on exciton properties has been poorly understood so far. Here, we show that the weak potential induced by periodically ordered Wigner crystal electrons has a major impact on exciton propagation, albeit having only a minor influence on exciton energy. The effect is tunable with carrier density determining the Wigner crystal confinement and temperature via thermal occupation of higher subbands. Our work provides microscopic insights into the interplay between excitons and charge-ordered states identifying key signatures in exciton transport, and establishes a theoretical framework for understanding exciton propagation in the presence of strong electronic correlations.

cond-mat.mtrl-sci

Electrically tunable ultrafast dynamics and interactions of hybrid excitons in a 2D semiconductor bilayer

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.

cond-mat.mes-hall

Stability of Wigner crystals and Mott insulators in twisted moir\'e structures

Transition metal dichalcogenides (TMDs) constitute an intriguing platform for studying charge-ordered states including conventional and generalized Wigner crystals as well as Mott insulating states. In this work, we combine a phonon mode expansion of the electronic crystal vibrations with the Lindemann criterion to investigate the quantum and thermal stability of these strongly correlated phases in the exemplary materials of MoSe$_2$ monolayers and twisted MoSe$_2$-WSe$_2$ heterostructures. We find that the moir\'e potential in heterobilayers acts as a harmonic trap, flattening the energy dispersion of phonon excitations and resulting in an order of magnitude larger melting temperatures compared to monolayer Wigner crystals. Furthermore, we explore the tunability of the correlated states with respect to dielectric environment and bilayer stacking. In particular, we show that the reduced screening in free-standing TMDs results in a tenfold increase in the melting temperature compared to hBN-encapsulated TMDs. Moreover, the deeper moir\'e potential in R-type stacked heterostructures makes generalized Wigner crystals more stable than in H-type stacking. Overall, our study provides important microscopic insights on the stability and tunability of charge-ordered states in TMD-based structures.

cond-mat.mtrl-sci

Electrically tunable dipolar interactions between layer-hybridized excitons

Transition-metal dichalcogenide bilayers exhibit a rich exciton landscape including layer-hybridized excitons, i.e. excitons which are of partly intra- and interlayer nature. In this work, we study hybrid exciton-exciton interactions in naturally stacked WSe$_2$ homobilayers. In these materials, the exciton landscape is electrically tunable such that the low-energy states can be rendered more or less interlayer-like depending on the strength of the external electric field. Based on a microscopic and material-specific many-particle theory, we reveal two intriguing interaction regimes: a low-dipole regime at small electric fields and a high-dipole regime at larger fields, involving interactions between hybrid excitons with a substantially different intra- and interlayer composition in the two regimes. While the low-dipole regime is characterized by weak inter-excitonic interactions between intralayer-like excitons, the high-dipole regime involves mostly interlayer-like excitons which display a strong dipole-dipole repulsion and give rise to large spectral blue-shifts and a highly anomalous diffusion. Overall, our microscopic study sheds light on the remarkable electrical tunability of hybrid exciton-exciton interactions in atomically thin semiconductors and can guide future experimental studies in this growing field of research.

cond-mat.mes-hall

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

Interlayer exciton polaritons in homobilayers of transition metal dichalcogenides

Transition metal dichalcogenides integrated within a high-quality microcavity support well-defined exciton polaritons. While the role of intralayer excitons in 2D polaritonics is well studied, interlayer excitons have been largely ignored due to their weak oscillator strength. Using a microscopic and material-realistic Wannier-Hopfield model, we demonstrate that MoS$_2$ homobilayers in a Fabry-Perot cavity support polaritons that exhibit a large interlayer exciton contribution, while remaining visible in linear optical spectra. Interestingly, with suitable tuning of the cavity length, the hybridization between intra- and interlayer excitons can be 'unmixed' due to the interaction with photons. We predict formation of polaritons where > 90% of the total excitonic contribution is stemming from the interlayer exciton. Furthermore, we explore the conditions on the tunneling strength and exciton energy landscape to push this to even 100%. Despite the extremely weak oscillator strength of the underlying interlayer exciton, optical energy can be effectively fed into the polaritons once the critical coupling condition of balanced radiative and scattering decay channels is met. These findings have a wide relevance for fields ranging from nonlinear optoelectronic devices to Bose-Einstein condensation.

cond-mat.mes-hall

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

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

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

Topology of critical chiral phases: multiband insulators and superconductors

Recent works have proved the existence of symmetry-protected edge states in certain one-dimensional topological band insulators and superconductors at the gap-closing points which define quantum phase transitions between two topologically nontrivial phases. We show how this picture generalizes to multiband critical models belonging to any of the chiral symmetry classes AIII, BDI, or CII of noninteracting fermions in one dimension.

cond-mat.mes-hall

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