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Sreyan Raha

Publications and source records attributed to Sreyan Raha.

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Thermal assisted transport of biexcitons in monolayer WSe2

Studies of excitonic transport in transition metal dichalcogenide monolayers have attracted increasing interest in recent years in order to develop nano-optoelectronic devices made with 2D materials. These studies began with low to moderate optical excitation regimes, and more recently have focused on high injection regimes where nonlinear effects appear. This article is focused on the transport of biexcitons by spatially and temporally resolved photoluminescence spectroscopy at high excitation flux. The study is carried out on a high-quality WSe$_2$ monolayer encapsulated in hexagonal boron nitride. The results show that a Seebeck current affects transport in connection with the presence of hot biexcitons. In particular, we observe the formation of spatial rings, also called halos, which have been observed in other excitonic gases. These results tend to generalize the importance of high-energy populations in excitonic transport in TMD, even for complex and heavy excitonic particles.

cond-mat.mtrl-sci

Coherent multi-dimensional widefield microscopy

Understanding how electronic excitations evolve across space and time is essential for revealing the microscopic processes underlying quantum and optoelectronic materials. However, existing approaches cannot simultaneously resolve ultrafast coherent dynamics with microscopic spatial information: pump-probe microscopy lacks access to quantum coherence, while two-dimensional electronic spectroscopy (2DES) requires slow point-by-point scanning for spatial resolution. Here we introduce a widefield two-dimensional electronic spectroscopy microscope (2DESM) combining multidimensional coherent spectroscopy with widefield imaging, enabling simultaneous femtosecond temporal and micrometer spatial resolution across a broadband spectral range. Applying 2DESM to hBN-encapsulated WSe2, we directly visualize spatial variations in exciton coherence and relaxation associated with the local environment, establishing 2DESM as a powerful platform for probing many-body interactions, energy transport, and structure-function relationships in low-dimensional materials and devices.

physics.optics

Brightening of dark trions in monolayer WS$_2$ via localization of surface plasmons

Among all excitonic complexes in transition-metal dichalcogenides (TMDs), dark and semi-dark trions are poised to play a stellar role in future quantum technologies due to their long lifetimes, about two orders of magnitude greater than those of their bright counterparts. In monolayer (ML) tungsten disulphide (WS$_2$), accessing these states via a suitable brightening mechanism remains challenging, specially, at elevated temperatures. Here, we demonstrate the brightening of dark trions from ML WS$_2$ over the temperature range, 83 K-115 K, enabled by localized surface plasmon modes in a disordered gold substrate. The resulting photoluminescence (PL) spectrum reveals a distinct spectral doublet with the twin peaks of semi-dark and bright trion states, separated by $\sim$ 45 meV. The origin of the semi-dark trion state lies in intervalley electron-electron scatterings, while its visibility in the PL spectrum is made possible by the enhanced out-of-plane electromagnetic field associated with plasmon localization. We also report on the negative degree of circular polarization in ML WS$_2$ at the energy of the semi-dark trion state. Our results establish a scalable plasmonic route to access valley-polarized semi-dark trions, opening new opportunities for quantum and valleytronic applications.

cond-mat.mes-hall

Raman spectroscopy of group-IV Ge$_{1-x}$Sn$_{x}$ alloys: theory and experiment

Ge$_{1-x}$Sn$_{x}$ alloys are a promising candidate material to realise direct-gap group-IV semiconductors for applications in Si-compatible electronic and photonic devices. Here, we present a combined theoretical and experimental analysis of Raman spectroscopy in Ge$_{1-x}$Sn$_{x}$ alloys. We describe liquid-vapour-solid growth and structural characterisation of Ge$_{1-x}$Sn$_{x}$ ($x \leq 8$%) nanowires displaying high crystalline quality, and investigate the structural and vibrational properties of the nanowires using Raman spectroscopy. Our theoretical analysis is based on a fully analytic anharmonic valence force field (VFF) potential, which describes exactly - i.e. without recourse to numerical fitting - the second-order elastic constants, third-order bulk modulus, selected second- and third-order inner elastic constants and, as a consequence, the zone-centre transverse optical phonon mode frequency and its hydrostatic and axial strain dependence. We compute bulk elastic properties via density functional theory to parametrise the VFF potential for Ge$_{1-x}$Sn$_{x}$ alloys, and apply the VFF potential to explicitly compute the Raman spectra of realistic, disordered Ge$_{1-x}$Sn$_{x}$ alloy supercells. Our atomistic theoretical calculations quantitatively capture: (i) the evolution of the measured Raman spectra with Sn composition $x$, (ii) demonstrate explicitly that the presence of short-range alloy disorder can significantly impact the shift coefficients $a$ and $b$ that respectively describe the dependence of the Raman shift on Sn composition and pseudomorphic strain, (iii) elucidate the origin of the so-called "disorder activated" mode identified in previous experimental investigations, and (iv) allow for detailed atomic-scale interpretation of measured Raman spectra. Overall, our analysis provides insight relevant to the characterisation of this emerging material system.

cond-mat.mtrl-sci