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Chirag Chandrakant Palekar

Publications and source records attributed to Chirag Chandrakant Palekar.

8 recordsLinked to original sources

Resolving High-Energy States of Interlayer Excitons in MoSe$_2$/WSe$_2$ Heterostructures

High-energy states of interlayer excitons (IXs) in van der Waals heterostructures remain largely unexplored despite their importance for understanding many-body interactions and nonlinear optical phenomena. Here, we use photoluminescence excitation (PLE) spectroscopy to resolve a Rydberg-like series of excited IX states in MoSe$_2$/WSe$_2$ heterostructures. We observe multiple PLE resonances below the intralayer exciton energies, which we assign to the 2s-, 3s-, and 4s-like states of the IXs. These resonances are consistently observed across heterostructures with different twist angles, indicating that the high-energy state spectrum is only weakly affected by the twist angle. Wannier-exciton calculations incorporating screened Coulomb interactions reproduce the overall energy scale and qualitative trends of the measured Rydberg-like series, supporting the assignment of the observed resonances. Our findings demonstrate that PLE provides direct experimental access to the previously unexplored high-energy IX states in van der Waals heterostructures.

cond-mat.mes-hall↗

Anisotropic nanoscale coherent polariton transport in CrSBr

In a combined experimental and theoretical study, we demonstrate anisotropic polariton transport on the nanoscale in the van der Waals antiferromagnet CrSBr. While effective cavity-polariton formation emerges via the self-hybridization of ultra-high oscillator strength excitons with a thin slab photonic mode, the absence of external mirrors facilitates spectroscopic investigation of these polaritons via cathodoluminescence (CL) on length scales determined by the electron wavelength. This direct access allows us to perform precise charting of the polariton landscape with nanometric resolution, and to probe polariton interference phenomena. The main finding of the work highlights that the coherent polariton transport follows the $C_{2v}$ symmetry of CrSBr, allowing exclusive transport along the crystallographic a-axis, while no coherent feature is found along the b-axis direction. Our work sets the foundation to use CL spectroscopy in cavity-polaritonics in more advanced landscapes, such as photonic crystals or optical lattices, and establishes the technique as a powerful tool to probe anisotropic expansion and relaxation phenomena on the nanoscale

cond-mat.mtrl-sci↗

Localized Excitonic Emission in Wafer-Scale MOCVD-Grown GaSe 2D Nanosheets for Classical and Non-Classical Light Sources

Wafer-scale growth of two-dimensional semiconductors remains a key challenge for their integration into photonic technologies. While most studies of two-dimensional semiconductors have focused on transition metal dichalcogenides and their scalable fabrication, comparatively little attention has been given to III-VI monochalcogenides. Here, we report wafer-scale growth of gallium selenide (GaSe) by metal-organic chemical vapor deposition (MOCVD) and investigate its structural and optical properties for visible-range classical and quantum light emission. Two samples with thicknesses ranging from a few monolayers to several micrometers, controlled via the growth time, were investigated. The 30-minute grown sample yields intense, broad photoluminescence spanning 1.7--2.0$\,$eV, whereas the thinner 3-minute sample exhibits discrete narrow emission lines and single-photon emission with $(g^{(2)}(0) = 0.15 \pm 0.10)$. Remarkably, cathodoluminescence mapping reveals pronounced spatial localization of both spectrally narrow and broad emission centers. Together with temperature-dependent power-law analysis and Raman mapping, our results indicate defect-induced emission rather than intrinsic excitonic recombination. These findings establish wafer-scale MOCVD grown 2D GaSe as a platform for classical and non-classical light sources and highlight defect-engineered localization as a route toward scalable quantum photonics.

cond-mat.mes-hall↗

Robust Interlayer Exciton Interplay in Twisted van der Waals Heterotrilayer on a Broadband Bragg Reflector up to Room Temperature

We report robust room temperature interlayer excitons in transition metal dichalcogenide heterostructures engineered via precise stacking orientation and twist-angle control. We integrate 2H-stacked MoSe$_{2}$/$^{1}$WSe$_{2}$/$^{2}$WSe$_{2}$ heterotrilayer onto a chirped distributed Bragg reflector that acts as a backside mirror. This way, we fabricate a platform that hosts distinct heterotrilayer, heterobilayer, and homobilayer regions with enhanced excitonic features at elevated temperatures. Although the heterobilayer supports temperature-tunable singlet and triplet interlayer excitons, it exhibits low emission yield at 4 K. In comparison, the heterotrilayer shows remarkable excitonic properties, including pronounced band modulation, intervalley interlayer exciton transitions, and a tenfold photoluminescence enhancement along with a sevenfold increase in exciton decay time at cryogenic temperatures compared to the heterobilayer system. Temperature-dependent studies reveal intriguing interlayer exciton dynamics in the heterotrilayer, including the emergence of valley-polarized interlayer excitons, and the ability to maintain optical stability up to room temperature. Our results establish a clear strategy for engineering excitonic states across multilayer van der Waals heterostructures from 4 K to room temperature, providing a versatile platform for excitonic optoelectronics, quantum photonics, and tunable long-lived interlayer exciton states in scalable TMD heterostructures.

cond-mat.mes-hall↗

In-situ spontaneous emission control of MoSe$_2$-WSe$_2$ interlayer excitons with near-unity quantum yield

Optical resonators are a powerful platform to control the spontaneous emission dynamics of excitons in solid-state nanostructures. Here, we study a MoSe$_2$-WSe$_2$ van-der-Waals heterostructure that is integrated in a widely tunable open optical microcavity to gain insights into fundamental optical properties of the emergent interlayer charge-transfer excitons. First, we utilize an ultra-low quality factor open planar vertical cavity and investigate the modification of the excitonic lifetime as on- and off-resonant conditions are met with consecutive longitudinal modes. Time-resolved photoluminescence measurements reveal that the interlayer exciton lifetime can thus be periodically tuned with an amplitude of 110 ps. The resulting oscillations of the interlayer exciton lifetime allows us to extract a 0.5 ns free-space radiative lifetime and a quantum efficiency as high as 81 \%. We subsequently engineer the local density of optical states by introducing a spatially confined and fully spectrally tunable Tamm-plasmon resonance. The dramatic redistribution of the local optical modes in this setting allows us to encounter a profound inhibition of spontaneous emission of the interlayer excitons by a factor of 3.2. We expect that specifically engineering the inhibition of radiation from moiré excitons is a powerful tool to steer their thermalization, and eventually their condensation into coherent condensate phases.

cond-mat.mtrl-sci↗

Twist Angle Dependence of Exciton Resonances in WSe$_2$/MoSe$_2$ Moiré Heterostructures

Van der Waals heterostructures based on TMDC semiconducting materials have emerged as promising materials due to their spin-valley properties efficiently contrived by the stacking-twist angle. The twist angle drastically alters the interlayer excitonic response by determining the spatial modulation, confining moiré potential, and atomic reconstruction in those systems. Nonetheless, the impact of the interlayer twist angle on the band alignment of the monolayers composing the heterostructure has received scant attention in the current research. Here, we systematically investigate the twist-angle dependence of intra- and inter-layer excitons in twisted WSe2/MoSe2 heterobilayers. By performing photoluminescence excitation spectroscopy, we identify the twist-angle dependence of interlayer emission response, where an energy redshift of about 100 meV was observed for increasing twist angles. The applied microscopic theory predicts, on the contrary, a blueshift, which suggests that additional features, such as atomic reconstruction, may also surpass the moiré potential confinement. Those findings also prompt the effects of dielectric screening by addressing the redshift response to the stacking layer order. Furthermore, our findings support the evidence of a band offset dependence on the twist angle for the adjacent monolayers composing the heterobilayer system. Our fundamental study of exciton resonances deepens the current understanding of the physics of twisted TMDC heterostructures and paves the way for future experiments and theoretical works.

cond-mat.mes-hall↗

Development of High-Quality Polymer/Air-Bragg Micromirror Structures for Nanophotonic Applications

We report the design, nanofabrication, and characterization of high-quality polymer-based micromirror structures employing the 3D two-photon polymerization lithography technique. Compared to conventional microcavity approaches, our innovative concept provides microstructures which allow fast prototyping. Moreover, our polymer-based mirrors are cost effective, environmentally sensitive, as well as compatible with a wide range of wavelengths from NIR to the telecom C-band. We demonstrate polymer/air distributed Bragg reflectors and full microcavity structures with up to 14 mirror pairs with a target wavelength of 1550 nm and a reflectivity close to 99%. Additionally, our 3D printed micromirrors are reproducible, mechanically stable, and enable hybrid nanophotonic devices based on quantum dots, molecules or 2D quantum materials as active medium.

physics.optics↗

Tunable Polymer/Air Bragg Optical Microcavity Configurations for Controllable Light-Matter Interaction Scenarios

Complex optical systems such as high-quality microcavities enabled by advanced lithography and processing techniques paved the way to various light-matter interactions (LMI) studies. Without lattice-matching constraints in epitaxy, coating techniques or shaky open cavity constructions, sub-micrometer-precise lithographic development of a polymer photoresist paves the way to polymer microcavity structures for various spectral regions based on the material's transparency and the geometrical sizes. We introduce a new approach based on 3D nanowriting in photoresist, which can be employed to achieve microscopic photonic Fabry-Pérot cavity structures with mechanically-tunable resonator modes and polymer/air Bragg mirrors, directly on a chip or device substrate. We demonstrate by transfer-matrix calculations and computer-assisted modelling that open microcavities with up to two "air-Bragg" reflectors comprising alternating polymer/air mirror-pair layers enable compression-induced mode tuning that can benefit many LMI experiments, such as with 2D materials, nanoparticles and molecules.

physics.optics↗