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Chakradhar Sahoo

Publications and source records attributed to Chakradhar Sahoo.

11 recordsLinked to original sources

Observation of dodecagonal replica bands in 30$^{\circ}$-twisted bilayer WSe$_2$

Twisted bilayers of two-dimensional (2D) transition metal dichalcogenides are promising systems for achieving tunable quasicrystalline orders with emergent properties. The underpinning electronic structure and scattering processes in 2D quasicrystals with multiorbital dodecagonal replica bands have so far not been determined. Here, we utilize angle-resolved photoemission spectroscopy (ARPES) with micrometer spatial resolution to directly observe replica bands in 30$^{\circ}$-twisted bilayer WSe$_2$. The symmetry and intensity distribution of the observed replicas are explained by interlayer Umklapp scattering from bottom to top WSe$_2$ layers. Our spectral function measurements are consistent with the presence of a van Hove singularity adjacent to the $\mathrm{K}$-valleys, which underlines the possibility of inducing electronic reconstructions in bilayers with a large interlayer twist angle.

cond-mat.mes-hall

Band offsets and stability of WSe$_2$/RuCl$_3$ van der Waals charge-transfer contacts

The layered Mott insulator $\alpha$-RuCl$_3$ induces degenerate hole-doping in two-dimensional semiconductors due to its large electron affinity, making it a promising charge-transfer material for establishing ohmic contacts in electronic devices. In order to assess the applicability and guide the design of devices incorporating RuCl$_3$ it is critical to determine the electronic structure and robustness of the band offsets that underpin the transport properties of semiconductors in contact with RuCl$_3$. Here, we apply micro-focused angle-resolved photoemission spectroscopy to determine the electronic structure of single-layer WSe$_2$ contacted to RuCl$_3$ on hexagonal boron nitride substrates. We find that formation of a functioning WSe$_2$/RuCl$_3$ contact leads to a valence band shift of $(0.68 \pm 0.05)$ eV towards the Fermi energy in WSe$_2$. The charge transfer effect is challenging to observe as it depends sensitively on fabrication conditions such as solvent exposure, quality of interface encapsulation and heating of RuCl$_3$, imposing strict requirements on device design to attain high-quality contacts.

cond-mat.mes-hall

Direct nanoscale mapping of band alignment in single-layer semiconducting lateral heterojunctions

Atomic-scale control over band alignment in single-layer lateral heterostructures (LHSs) of dissimilar transition metal dichalcogenides (TMDCs) is critical for nextgeneration electronic, optoelectronic, and quantum technologies. However, direct experimental access to interfacial electronic states with nanometer precision remains a significant challenge. Here, we employ angle-resolved photoemission spectroscopy with nanoscale spatial resolution (nanoARPES) to directly map the epitaxial alignment and valence band evolution across MoSe2-WSe2 LHSs. By combining nanoARPES with spatially resolved photoluminescence, we correlate the evolution of the valence band maximum and exciton features across both atomically sharp and compositionally graded diffusive interfaces. We identified type-II band alignments governed by both material composition and interstitial-induced modifications of band offsets, in close agreement with density functional theory calculations. These results reveal fundamental mechanisms of electronic structure modulation at 1D TMDC heterointerfaces and provide a robust platform for tailored band engineering in van der Waals materials.

cond-mat.mes-hall

Quasiparticle gap renormalization driven by internal and external screening in a WS$_2$ device

The electronic band gap of a two-dimensional semiconductor within a device architecture is sensitive to variations in screening properties of adjacent materials in the device and to gate-controlled doping. Here, we employ micro-focused angle resolved photoemission spectroscopy to separate band gap renormalization effects stemming from environmental screening and electron-doping during \textit{in situ} gating of a single-layer WS$_{2}$ device. The WS$_{2}$ is supported on hBN and contains a section that is exposed to vacuum and another section that is encapsulated by a graphene contact. We directly observe the doping-induced semiconductor-metal transition and band gap renormalization in the two sections of WS$_2$. Surprisingly, a larger band gap renormalization is observed in the vacuum-exposed section than in the graphene-encapsulated - and thus ostensibly better screened - section of the WS$_2$. Using $GW$ calculations, we determine that intrinsic screening due to stronger doping in vacuum exposed WS$_2$ exceeds the external environmental screening in graphene-encapsulated WS$_2$.

cond-mat.mes-hall

Multi Moire Networks in Engineered Lateral Hetero-Bilayers: Programmable Phononic Reconfiguration and Second Harmonic Generation

Moire engineering in two-dimensional transition metal dichalcogenides enables access to correlated quantum phenomena. Realizing such effects demands simultaneous control over twist angle and material composition to modulate phonons, excitons, and their interactions. However, most studies rely on exfoliated flakes, limiting scalability and systematic exploration. Here, we demonstrate a scalable multi-moire network by vertically stacking CVD-grown monolayer lateral heterostructures. Signatures of moire non-rigidity, including phonon frequency softening, linewidth broadening, and strain localization, are attributed to two lattice relaxation modes; rotational reconstruction and volumetric dilation. Micro-angle-resolved photoemission spectroscopy reveals that interfacial orbital interactions modulate interlayer coupling. At aligned angles, molybdenum diselenides exhibit reduced valley polarization and Davydov splitting, indicating strain-induced symmetry breaking and chiral phonon effects. Notably, SHG modulation was obderved with variation in twist angle due to lower coherence and band-offset-driven phase delay. First-principles calculations support these findings. This work provides a route to programmable, scalable multi-moire platforms for opto-straintronics, quantum sensing, and on-chip photonics.

cond-mat.mes-hall

Van der Waals engineering of ultrafast carrier dynamics in magnetic heterostructures

Heterostructures composed of the intrinsic magnetic topological insulator MnBi$_2$Te$_4$ and its non-magnetic counterpart Bi$_2$Te$_3$ host distinct surface electronic band structures depending on the stacking order and exposed termination. Here, we probe the ultrafast dynamical response of MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$ following near-infrared optical excitation using time- and angle-resolved photoemission spectroscopy, and disentangle surface from bulk dynamics based on density functional theory slab calculations of the surface-projected electronic structure. We gain access to the out-of-equilibrium charge carrier populations of both MnBi$_2$Te$_4$ and Bi$_2$Te$_3$ surface terminations of MnBi$_4$Te$_7$, revealing an instantaneous occupation of states associated with the Bi$_2$Te$_3$ surface layer followed by carrier extraction into the adjacent MnBi$_2$Te$_4$ layers with a laser fluence-tunable delay of up to 350 fs. The ensuing thermal relaxation processes are driven by phonon scattering with significantly slower relaxation times in the magnetic MnBi$_2$Te$_4$ septuple layers. The observed competition between interlayer charge transfer and intralayer phonon scattering demonstrates a method to control ultrafast charge transfer processes in MnBi$_2$Te$_4$-based van der Waals compounds.

cond-mat.mtrl-sci

Direct view of gate-tunable miniband dispersion in graphene superlattices near the magic twist angle

Superlattices from twisted graphene mono- and bi-layer systems give rise to on-demand many-body states such as Mott insulators and unconventional superconductors. These phenomena are ascribed to a combination of flat bands and strong Coulomb interactions. However, a comprehensive understanding is lacking because the low-energy band structure strongly changes when the electron filling is varied. Here, we gain direct access to the filling-dependent low energy bands of twisted bilayer graphene (TBG) and twisted double bilayer graphene (TDBG) by applying micro-focused angle-resolved photoemission spectroscopy to in situ gated devices. Our findings for the two systems are in stark contrast: The doping dependent dispersion for TBG can be described in a simple model, combining a filling-dependent rigid band shift with a many-body related bandwidth change. In TDBG, on the other hand, we find a complex behaviour of the low-energy bands, combining non-monotonous bandwidth changes and tuneable gap openings. Our work establishes the extent of electric field tunability of the low energy electronic states in twisted graphene superlattices and can serve to underpin the theoretical understanding of the resulting phenomena.

cond-mat.mes-hall

Revealing flat bands and hybridization gaps in a twisted bilayer graphene device with microARPES

Controlling the electronic structure of two-dimensional materials using the combination of twist angle and electrostatic doping is an effective means to induce emergent phenomena. In bilayer graphene with an interlayer twist angle near the magic angle, the electronic dispersion is strongly modified by a manifold of hybridizing moiré Dirac cones leading to flat band segments with strong electronic correlations. Numerous technical challenges arising from spatial inhomogeneity of interlayer interactions, twist angle and device functionality have so far limited momentum-resolved electronic structure measurements of these systems to static conditions. Here, we present a detailed characterization of the electronic structure exhibiting miniband dispersions for twisted bilayer graphene, near the magic angle, integrated in a functional device architecture using micro-focused angle-resolved photoemission spectroscopy. The optimum conditions for visualizing the miniband dispersion are determined by exploiting the spatial resolution and photon energy tunability of the light source and applied to extract a hybridization gap size of $(0.14 \pm 0.03)$~eV and flat band segments extending across a moiré mini Brillouin zone. \textit{In situ} electrostatic gating of the sample enables significant electron-doping, causing the conduction band states to shift below the Fermi energy. Our work emphasizes key challenges in probing the electronic structure of magic angle bilayer graphene devices and outlines conditions for exploring the doping-dependent evolution of the dispersion that underpins the ability to control many-body interactions in the material.

cond-mat.mes-hall

Moiré-localized interlayer exciton wavefunctions captured by imaging its electron and hole constituents

Interlayer excitons (ILXs) - electron-hole pairs bound across two atomically thin layered semiconductors - have emerged as attractive platforms to study exciton condensation, single-photon emission and other quantum-information applications. Yet, despite extensive optical spectroscopic investigations, critical information about their size, valley configuration and the influence of the moiré potential remains unknown. Here, we captured images of the time- and momentum-resolved distribution of both the electron and the hole that bind to form the ILX in a WSe2/MoS2 heterostructure. We thereby obtain a direct measurement of the interlayer exciton diameter of ~5.4 nm, comparable to the moiré unit-cell length of 6.1 nm. Surprisingly, this large ILX is well localized within the moiré cell to a region of only 1.8 nm - smaller than the size of the exciton itself. This high degree of localization of the interlayer exciton is backed by Bethe-Salpeter equation calculations and demonstrates that the ILX can be localized within small moiré unit cells. Unlike large moiré cells, these are uniform over large regions, thus allowing the formation of extended arrays of localized excitations for quantum technology.

physics.optics

Experimental measurement of the intrinsic excitonic wavefunction

An exciton, a two-body composite quasiparticle formed of an electron and hole, is a fundamental optical excitation in condensed-matter systems. Since its discovery nearly a century ago, a measurement of the excitonic wavefunction has remained beyond experimental reach. Here, we directly image the excitonic wavefunction in reciprocal space by measuring the momentum distribution of electrons photoemitted from excitons in monolayer WSe2. By transforming to real space, we obtain a visual of the distribution of the electron around the hole in an exciton. Further, by also resolving the energy coordinate, we confirm the elusive theoretical prediction that the photoemitted electron exhibits an inverted energy-momentum dispersion relationship reflecting the valence band where the partner hole remains, rather than that of conduction-band states of the electron.

cond-mat.mes-hall

Directly visualizing the momentum forbidden dark excitons and their dynamics in atomically thin semiconductors

Resolving the momentum degree of freedom of excitons - electron-hole pairs bound by the Coulomb attraction in a photoexcited semiconductor, has remained a largely elusive goal for decades. In atomically thin semiconductors, such a capability could probe the momentum forbidden dark excitons, which critically impact proposed opto-electronic technologies, but are not directly accessible via optical techniques. Here, we probe the momentum-state of excitons in a WSe2 monolayer by photoemitting their constituent electrons, and resolving them in time, momentum and energy. We obtain a direct visual of the momentum forbidden dark excitons, and study their properties, including their near-degeneracy with bright excitons and their formation pathways in the energy-momentum landscape. These dark excitons dominate the excited state distribution - a surprising finding that highlights their importance in atomically thin semiconductors.

cond-mat.mtrl-sci