Realizing nonlinear optical response in the low photon density limit in solid-state systems has been a long-standing challenge. Semiconductor microcavities in the strong coupling regime hosting exciton-polaritons have emerged as attractive candidates in this context. However, the weak interaction between these quasiparticles has been a hurdle in this quest. Dipolar excitons provide an attractive strategy to overcome this limitation but are often hindered by their weak oscillator strength. The interlayer dipolar excitons in naturally occurring homobilayer MoS alleviates this issue owing to their formation via hybridization of interlayer charge transfer exciton with intralayer B exciton. Here we demonstrate the formation of dipolar exciton polaritons in bilayer MoS resulting in unprecedented nonlinear interaction strengths. A ten-fold increase in nonlinearity is observed for the interlayer dipolar excitons compared to the conventional A excitons. These highly nonlinear dipolar polaritons will likely be a frontrunner in the quest for solid-state quantum nonlinear devices.
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http://dx.doi.org/10.1038/s41467-022-33940-3 | DOI Listing |
J Phys Condens Matter
December 2024
School of Physical Science and Technology, Inner Mongolia University, Hohhot 010021, People's Republic of China.
The introduction of intermediate hexagonal boron nitride (hBN) between the bilayer transition metal dichalcogenide (TMD) heterostructures has been considered an efficient approach to manipulate the interlayer excitations. However, the hBN intercalation primarily serves as a spacer to increase the interlayer distance and alter the screening, without producing a significant band offset shift. Here, we use Janus monolayer CSiH, possessing a prominent out-of-plane intrinsic dipole moment and large enough band gap, as an intercalation to build trilayer MoS/CSiH/WSheterostructures.
View Article and Find Full Text PDFScience
November 2024
State Key Laboratory of Surface Physics, Key Laboratory of Micro- and Nano-Photonic Structures (Ministry of Education), Shanghai Key Laboratory of Metasurfaces for Light Manipulation, and Department of Physics, Fudan University, Shanghai 200433, China.
Bright dipolar excitons, which contain electrical dipoles and have high oscillator strength, are an ideal platform for studying correlated quantum phenomena. They usually rely on carrier tunneling between two quantum wells or two layers to hybridize with nondipolar excitons to gain oscillator strength. In this work, we uncovered a new type of bright infrared dipolar exciton by stacking 90°-twisted black phosphorus (BP) structures.
View Article and Find Full Text PDFJ Phys Chem Lett
October 2024
Department of Chemical Sciences, Indian Institute of Science Education and Research Kolkata, Mohanpur, Nadia, West Bengal 741246, India.
Instances of magic angle excitonic coupling and its optical consequences are infrequently documented in the literature, yet they hold fundamental significance in understanding excited state electronic processes within molecular aggregates. Weak/null long-range dipolar Coulombic coupling is the characteristic of chromophore arrays positioned in a magic angle configuration. This study presents a rare example of such phenomena in CFDPT solids, resulting in a high fluorescence quantum efficiency of 62 ± 3% in the aggregated solid state.
View Article and Find Full Text PDFMRS Bull
September 2024
Institute of Physics, University of Münster, Münster, Germany.
Abstract: Interlayer excitons (IXs), composed of electron and hole states localized in different layers, excel in bilayers composed of atomically thin van der Waals materials such as semiconducting transition-metal dichalcogenides (TMDs) due to drastically enlarged exciton binding energies, exciting spin-valley properties, elongated lifetimes, and large permanent dipoles. The latter allows modification by electric fields and the study of thermalized bosonic quasiparticles, from the single particle level to interacting degenerate dense ensembles. Additionally, the freedom to combine bilayers of different van der Waals materials without lattice or relative twist-angle constraints leads to layer-hybridized and Moiré excitons, which can be widely engineered.
View Article and Find Full Text PDFNano Lett
September 2024
Cambridge Graphene Centre, University of Cambridge, 9 JJ Thomson Avenue, CB3 0FA Cambridge, U.K.
Interlayer excitons in transition-metal dichalcogenide heterobilayers combine high binding energy and valley-contrasting physics with a long optical lifetime and strong dipolar character. Their permanent electric dipole enables electric-field control of the emission energy, lifetime, and location. Device material and geometry impact the nature of the interlayer excitons via their real- and momentum-space configurations.
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