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Preprints
213. P. Werner, W. Bennecke, J. P. Bange, G. Meneghini, D. Schmitt, M. Merboldt, A. M. Seiler, A. AlMutairi, K. Watanabe, T. Taniguchi, G. S. Matthijs Jansen, J. Liu, D. Steil, S. Hofmann, R. Thomas Weitz, E. Malic, S. Mathias, M. Reutzel "The role of non-equilibrium populations in dark exciton formation", arXiv: 2505.06074
In two-dimensional transition metal dichalcogenide structures, the optical excitation of a bright exciton may be followed by the formation of a plethora of lower energy dark states. In these formation and relaxation processes between different exciton species, non-equilibrium exciton and phonon populations play a dominant role, but remain so far largely unexplored as most states are inaccessible by regular spectroscopies. Here, on the example of homobilayer 2H-MoS, we realize direct access to the full exciton relaxation cascade from experiment and theory. By measuring the energy- and in-plane momentum-resolved photoemission spectral function, we reveal a distinct fingerprint for dark excitons in a non-equilibrium excitonic occupation distribution. In excellent agreement with microscopic many-particle calculations, we quantify the timescales for the formation of a non-equilibrium dark excitonic occupation and its subsequent thermalization to 85~fs and 150~fs, respectively. Our results provide a previously inaccessible view of the complete exciton relaxation cascade, which is of paramount importance for the future characterization of non-equilibrium excitonic phases and the efficient design of optoelectronic devices based on two-dimensional materials.
arXiv: 2505.06074212. H. Shan, J. M. Fitzgerald, R. Rosati, G. Leibeling, K. Watanabe, T. Taniguchi, S. Ariel Tongay, F. Eilenberger, M. Esmann, S. Höfling, E. Malic and C. Schneider "Tuning relaxation and nonlinear upconversion of valley-exciton-polaritons in a monolayer semiconductor", arXiv: 2505.00385
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 MoSe2 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.
arXiv: 2505.00385211. R. Rosati, S. Shradha, J. Picker, A. Turchanin, B. Urbaszek, E. Malic "Impact of charge transfer excitons on unidirectional exciton transport in lateral TMD heterostructures", arXiv: 2503.01833
Lateral heterostructures built of monolayers of transition metal dichalcogenides (TMDs) are characterized by a thin 1D interface exhibiting a large energy offset. Recently, the formation of spatially separated charge-transfer (CT) excitons at the interface has been demonstrated. The technologically important exciton propagation across the interface and the impact of CT excitons has remained in the dark so far. In this work, we microscopically investigate the spatiotemporal exciton dynamics in the exemplary hBN-encapsulated WSe2-MoSe2 lateral heterostructure and reveal a highly interesting interplay of energy offset-driven unidirectional exciton drift across the interface and efficient capture into energetically lower CT excitons at the interface. This interplay triggers a counterintuitive thermal control of exciton transport with a less efficient propagation at lower temperatures - opposite to the behavior in conventional semiconductors. We predict clear signatures of this intriguing exciton propagation both in far- and near-field photoluminescence experiments. Our results present an important step toward a microscopic understanding of the technologically relevant unidirectional exciton transport in lateral heterostructures.
arXiv: 2503.01833210. A. M. Kumar, D. J. Bock, D. Yagodkin, E. Wietek, B. Höfer, M. Sinner, P. Hernández López, S. Heeg, C. Gahl, F. Libisch, A. Chernikov, E. Malic, R. Rosati, K. I. Bolotin "Strain engineering of valley-polarized hybrid excitons in a 2D semiconductor", arXiv: 2502.11232
Encoding and manipulating digital information in quantum degrees of freedom is one of the major challenges of today's science and technology. The valley indices of excitons in transition metal dichalcogenides (TMDs) are well-suited to address this challenge. Here, we demonstrate a new class of strain-tunable, valley-polarized hybrid excitons in monolayer TMDs, comprising a pair of energy-resonant intra- and intervalley excitons. These states combine the advantages of bright intravalley excitons, where the valley index directly couples to light polarization, and dark intervalley excitons, characterized by low depolarization rates. We demonstrate that the hybridized state of dark KK' intervalley and defect-localized excitons exhibits a degree of circular polarization of emitted photons that is three times higher than that of the constituent species. Moreover, a bright KK intravalley and a dark KQ exciton form a coherently coupled hybrid state under energetic resonance, with their valley depolarization dynamics slowed down a hundredfold. Overall, these valley-polarized hybrid excitons with strain-tunable valley character emerge as prime candidates for valleytronic applications in future quantum and information technology.
arXiv: 2502.11232209. B. Kundu, P. Chakrabarty, A. Dhara, R. Rosati, C. Samanta, S. K. Chakraborty, S. Sahoo, S. Dhara, Saroj P. Dash, E. Malic, S. Lodha, P. K. Sahoo "Trion-Engineered Multimodal Transistors in Two-dimensional Bilayer Semiconductor Lateral Heterostructures", arXiv: 2411.01257
Multimodal device operations are essential to advancing the integration of 2D semiconductors in electronics, photonics, information and quantum technology. Precise control over carrier dynamics, particularly exciton generation and transport, is crucial for finetuning the functionality of optoelectronic devices based on 2D semiconductor heterostructure. However, the traditional exciton engineering methods in 2D semiconductors are mainly restricted to the artificially assembled vertical pn heterostructures with electrical or strain induced confinements. In this study, we utilized bilayer 2D lateral npn multijunction heterostructures with intrinsically spatially separated energy landscapes to achieve preferential exciton generation and manipulation without external confinement. In lateral npn FET geometry, we uncover unique and nontrivial properties, including dynamic tuning of channel photoresponsivity from positive to negative. The multimodal operation of these 2D FETs is achieved by carefully adjusting electrical bias and the impinging photon energy, enabling precise control over the trions generation and transport. Cryogenic photoluminescence measurement revealed the presence of trions in bilayer MoSe2 and intrinsic trap states in WSe2. Measurements in different FET device geometries show the multifunctionality of 2D lateral heterostructure phototransistors for efficient tuning and electrical manipulation of excitonic characteristics. Our findings pave the way for developing practical exciton-based transistors, sensors, multimodal optoelectronic and quantum technologies.
arXiv: 2411.01257