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Pranjal Kumar Gogoi

Publications and source records attributed to Pranjal Kumar Gogoi.

8 recordsLinked to original sources

Point Defects and Localized Excitons in 2D WSe2

Identifying the point defects in 2D materials is important for many applications. Recent studies have proposed that W vacancies are the predominant point defect in 2D WSe2, in contrast to theoretical studies, which predict that chalcogen vacancies are the most likely intrinsic point defects in transition metal dichalcogenide semiconductors. We show using first principles calculations, scanning tunneling microscopy (STM) and scanning transmission electron microscopy experiments, that W vacancies are not present in our CVD-grown 2D WSe2. We predict that O-passivated Se vacancies (O_Se) and O interstitials (Oins) are present in 2D WSe2, because of facile O2 dissociation at Se vacancies, or due to the presence of WO3 precursors in CVD growth. These defects give STM images in good agreement with experiment. The optical properties of point defects in 2D WSe2 are important because single photon emission (SPE) from 2D WSe2 has been observed experimentally. While strain gradients funnel the exciton in real space, point defects are necessary for the localization of the exciton at length scales that enable photons to be emitted one at a time. Using state-of-the-art GW-Bethe-Salpeter-equation calculations, we predict that only Oins defects give localized excitons within the energy range of SPE in previous experiments, making them a likely source of previously observed SPE. No other point defects (O_Se, Se vacancies, W vacancies and Se_W antisites) give localized excitons in the same energy range. Our predictions suggest ways to realize SPE in related 2D materials and point experimentalists toward other energy ranges for SPE in 2D WSe2.

cond-mat.mtrl-sci

Momentum Conserved Ultrafast Charge Transfer Dynamics of Interlayer Excitons in vdW Heterostructures

Heterostructures comprising van der Waals (vdW) stacked transition metal dichalcogenide (TMDC) monolayers are a fascinating class of two-dimensional (2D) materials with unique properties. The presence of interlayer excitons, where the electron and the hole remain spatially separated in the two layers due to ultrafast charge transfer, is an intriguing feature of these heterostructures. Inevitably, the efficiency of 2D heterostructure devices is critically dependent on the charge transfer dynamics. However, the role of the relative rotation angle of the constituent layers on this charge transfer dynamics is hitherto unknown. Here, we investigate MoS$_2$/WSe$_2$ vdW heterostructures (hMWs) using monochromated low-loss electron energy loss (EEL) spectroscopy combined with aberration-corrected scanning transmission electron microscopy (STEM), and report that momentum conservation is a critical factor in the charge transfer dynamics of TMDC vdW heterostructures. The low-loss EEL spectra of the heterostructures with various rotation angles reveal that the charge transfer rate can be about one order-of-magnitude faster in the aligned (or anti-aligned) case than the misaligned cases. These results provide a deeper insight into the role of the fundamental principle of momentum conservation in 2D vdW heterostructure charge transfer dynamics.

cond-mat.mes-hall

Oxygen passivation mediated tunability of trion and excitons in MoS$_2$

Using wide spectral range in situ spectroscopic ellipsometry with systematic ultra high vacuum annealing and in situ exposure to oxygen, we report the complex dielectric function of MoS$_2$ isolating the environmental effects and revealing the crucial role of unpassivated and passivated sulphur vacancies. The spectral weights of the A ($1.92$ eV) and B ($2.02$ eV) exciton peaks in the dielectric function reduce significantly upon annealing, accompanied by spectral weight transfer in a broad energy range. Interestingly, the original spectral weights are recovered upon controlled oxygen exposure. This tunability of the excitonic effects is likely due to passivation and reemergence of the gap states in the bandstructure during oxygen adsorption and desorption, respectively, as indicated by ab initio density functional theory calculation results. This work unravels and emphasizes the important role of adsorbed oxygen in the optical spectra and many-body interactions of MoS$_2$.

cond-mat.mes-hall

Temperature-dependent dielectric function of bulk SrTiO$_3$: Urbach tail, band edges, and excitonic effects

We report the temperature-dependent complex dielectric function of pristine bulk SrTiO$_3$ between 4.2 and 300 K within the energy range of 0.6-6.5 eV determined by spectroscopic ellipsometry. Fundamental indirect and direct band-gap energies have been extracted and are discussed with regard to existing state-of-the-art theoretical calculations. Furthermore, the dielectric function around the fundamental direct gap is analyzed by considering excitonic states. The excitonic effects, including the Coulomb enhancement of the continuum, are characterized using an extension of the Elliott's formula considering both the real and imaginary parts of the dielectric function. The Urbach tail below the indirect edge shows an unconventional temperature-dependent behavior correlated to the microstructural changes near the structural phase transition around 105 K from the low-temperature tetragonal phase to the cubic phase. The temperature-dependent characterization reveals that the fundamental indirect edge as well as the Urbach tail are affected conspicuously by the structural phase transition while the fundamental direct edge is not. Moreover, the indirect edge follows Varshni's rule only in the cubic phase and the direct edge exhibits an anomalous linear increase with increasing temperature.

cond-mat.mtrl-sci

Anomalous excitons and screenings unveiling strong electronic correlations in SrTi$_{1-x}$Nb$_x$O$_3$, 0$\leq$x$\leq$0.005

Electron-electron (e-e) and electron-hole (e-h) interactions are often associated with many exotic phenomena in correlated electron systems. Here, we report an observation of anomalous excitons at 3.75 , 4.67 and 6.11 eV at 4.2 K in bulk-SrTiO$_3$. Fully supported by ab initio GW Bethe-Salpeter equation calculations, these excitons are due to surprisingly strong e-h and e-e interactions with different characters: 4.67 and 6.11 eV are resonant excitons and 3.75 eV is a bound Wannier-like exciton with an unexpectedly higher level of delocalization. Measurements and calculations on SrTi$_{1-x}$Nb$_x$O$_3$ for 0.0001$\leq$x$\leq$0.005 further show that energy and spectral-weight of the excitonic peaks vary as a function of electron doping (x) and temperature, which are attributed to screening effects. Our results show the importance of e-h and e-e interactions yielding to anomalous excitons and thus bring out a new fundamental perspective in SrTiO$_3$.

cond-mat.str-el

Optical conductivity renormalization of graphene on SrTiO$_{3}$ due to resonant excitonic effects mediated by Ti 3\textit{d} orbitals

We present evidence of a drastic renormalization of the optical conductivity of graphene on SrTiO$_3$ resulting in almost full transparency in the ultraviolet region. These findings are attributed to resonant excitonic effects further supported by \emph{ab initio} Bethe-Salpeter equation and density functional theory calculations. The ($π$,$π$*)-orbitals of graphene and Ti-3\textit{d} $t_{2g}$ orbitals of SrTiO$_3$ are strongly hybridized and the interactions of electron-hole states residing in those orbitals play dominant role in the graphene optical conductivity. These interactions are present much below the optical band gap of bulk SrTiO$_3$. These results open a possibility of manipulating interaction strengths in graphene via \textit {d}-orbitals which could be crucial for optical applications.

cond-mat.str-el

Tunable optical absorption and interactions in graphene via oxygen plasma

We report significant changes of optical conductivity in single layer graphene induced by mild oxygen plasma exposure, and explore the interplay between carrier doping, disorder, and many-body interactions from their signatures in the absorption spectrum. The first distinctive effect is the reduction of the excitonic binding energy that can be extracted from the renormalized saddle point resonance at 4.64 eV. Secondly, the real part of the frequency-dependent conductivity is nearly completely suppressed below an exposure-dependent threshold in the near infrared range. The clear step-like suppression follows the Pauli blocking behaviour expected for doped monolayer graphene. The nearly zero residual conductivity at frequencies below 2Ef can be interpreted as arising from the weakening of the electronic self-energy. Our data shows that mild oxygen exposure can be used to controlably dope graphene without introducing the strong physical and chemical changes that are common in other approaches to oxidized graphene, allowing a controllable manipulation of the optical properties of graphene.

cond-mat.mes-hall

Optical conductivity study of screening of many-body effects in graphene interfaces

Theoretical studies have shown that electron-electron (e-e) and electron-hole (e-h) interactions play important roles in many observed quantum properties of graphene making this an ideal system to study many body effects. In this report we show that spectroscopic ellipsometry can enable us to measure this interactions quantitatively. We present spectroscopic data in two extreme systems of graphene on quartz (GOQ), an insulator, and graphene on copper (GOC), a metal which show that for GOQ, both e-e and e-h interactions dominate while for GOC e-h interactions are screened. The data further enables the estimation of the strength of the many body interaction through the effective fine structure constant, $α_{g}^{*}$. The $α_{g}^{*}$ for GOQ indicates a strong correlation with an almost energy independent value of about 1.37. In contrast, $α_{g}^{*}$ value of GOC is photon energy dependent, is almost two orders of magnitude lower at low energies indicating very weak correlation.

cond-mat.mes-hall