arXiv subjects

Ioannis Paradisanos

Publications and source records attributed to Ioannis Paradisanos.

At least 19 recordsLinked to original sources

arXiv2026

Alloy engineering of excitonic properties in TMD monolayers

We investigate monolayer MoS$_{2x}$Se$_{2(1-x)}$ alloys across the full composition range using optical spectroscopy. We demonstrate continuous tuning of the optical gap over $\sim$0.35 eV, accompanied by a systematic reduction of the B--A exciton splitting, in agreement with density functional theory calculations. Temperature-dependent measurements reveal a progressive increase of the average phonon energy from Se-rich to S-rich alloys that follows a simple reduced-mass scaling model. Polarization-resolved spectroscopy further shows a monotonic increase of the circular polarization from nearly zero in MoSe$_2$ to $\sim$15\% in MoS$_2$ at 78 K. The observed evolution of the polarization is attributed to alloy-induced modifications of the electronic structure that modify bright--dark exciton mixing and the associated valley depolarization. These findings establish alloy engineering as an effective strategy for controlling excitonic properties in TMD monolayers.

cond-mat.mtrl-sci↗

arXiv2026

Highly Efficient Exciton Modulation in MoSe$_2$/PdSe$_2$ Heterostructures

Controlling exciton recombination in atomically thin semiconductors is central to their optoelectronic functionality, as the competition between radiative and non-radiative decay channels governs emission efficiency. Existing approaches, such as defect passivation, chemical doping, dielectric engineering, and strain tuning, primarily aim to suppress non-radiative losses. Here, we report a pronounced $\sim$6-fold enhancement of room-temperature A-exciton emission in a type-I MoSe$_2$/PdSe$_2$ van der Waals heterostructure, yielding a photoluminescence quantum yield of 6 %, compared to $\sim$1 % for as-exfoliated monolayer MoSe$_2$. This enhancement is accompanied by strong quenching of the B-exciton, consistent with interlayer electronic coupling that redistributes exciton populations toward the radiative A-exciton channel. Power- and temperature-dependent measurements reveal a suppression of exciton-exciton annihilation and a crossover to quenched emission at low temperature, indicating a redistribution of exciton relaxation pathways. Photoluminescence excitation spectroscopy further reveals a broadband enhancement spanning 450-725 nm, ruling out a resonance-specific mechanism. These results demonstrate that interlayer electronic coupling can be used as an efficient means to redirect exciton populations toward radiative channels, enhancing emission efficiency in two-dimensional semiconductors without chemical modification or strain.

cond-mat.mes-hall↗

arXiv2026

Valleytronics in 2D Materials Roadmap

Valleytronics exploits non-equivalent energy extrema in the electronic band structure of crystalline solids -- the valley degree of freedom -- to encode, manipulate, and read out information. The advent of 2D materials, first graphene and then transition-metal dichalcogenides, made valley control practical through optical, electrical, and magnetic routes. This foundation has enabled remarkable progress in recent years spanning established frontiers, such as valley exciton physics and valley Hall effects, as well as emerging directions including lightwave valleytronics, nanophotonic integration, flat-band valleytronics, and spin-valley qubits. In parallel, there are sustained efforts to scale up valleytronic materials and to predict new valleytronic platforms. This Roadmap brings together perspectives from leading experts to chart the key opportunities and challenges at the forefront of 2D material valleytronics. Each section captures a snapshot of progress in a key research area, identifies critical open challenges, and outlines pathways toward future valleytronics breakthroughs.

cond-mat.mes-hall↗

arXiv2025

Silicon nanoantennas for tailoring the optical properties of MoS2 monolayers

Silicon-based dielectric nanoantennas provide an effective platform for engineering light-matter interactions in van der Waals semiconductors. Here, we demonstrate near-field coupling between monolayer MoS2 and silicon nanoantennas arranged in hexagonal lattices with tunable geometric parameters, leading to a three-fold enhancement in photoluminescence and an excitation-wavelength-dependent emission that aligns with Mie-resonant modes. Raman spectroscopy reveals an up to 8-fold enhancement in the vibrational modes of MoS2, while second-harmonic generation exhibits a 20 to 30-fold increase in efficiency, closely correlating with the presence of the underlying nanoantennas. Our experiments and simulations quantify the tunable benefits of the near-field interactions, taking into account thin-film interference and strain-induced effects. Our findings present dielectric nanoantennas as a promising platform for tailoring linear and nonlinear optical properties in 2D materials, with potential applications in nanophotonic devices and integrated photonics.

physics.optics↗

arXiv2024

Two dimensional semiconductors: optical and electronic properties

In the last decade atomically thin 2D materials have emerged as a perfect platform for studying and tuning light-matter interaction and electronic properties in nanostructures. The optoelectronic properties in layered materials such as transition-metal-dichalcogenides (TMDs) are governed by excitons, Coulomb bound electron-hole pairs, even at room temperature. The energy, wave function extension, spin and valley properties of optically excited conduction electrons and valence holes are controllable via multiple experimentally accessible knobs, such as lattice strain, varying atomic registries, dielectric engineering as well as electric and magnetic fields. This results in a multitude of fascinating physical phenomena in optics and transport linked to excitons with very specific properties, such as bright and dark excitons, interlayer and charge transfer excitons as well as hybrid and moiré excitons. In this book chapter we introduce general optoelectronic properties of 2D materials and energy landscapes in TMD monolayers as well as their vertical and lateral heterostructures, including twisted TMD hetero- and homobilayer bilayers with moiré excitons and lattice recombination effects. We review the recently gained insights and open questions on exciton diffusion, strain- and field-induced exciton drift. We discuss intriguing non-linear many-particle effects, such as exciton halo formation, negative and anomalous diffusion, the surprising anti-funneling of dark excitons.

cond-mat.mes-hall↗

arXiv2023

Valley Polarization-Electric Dipole Interference and Nonlinear Chiral Selection Rules in Monolayer WSe$_2$

In monolayer transition metal dichalcogenides time-reversal symmetry, combined with space-inversion symmetry, defines the spin-valley degree of freedom. As such, engineering and control of time-reversal symmetry by optical or magnetic fields constitutes the foundation of valleytronics. Here, we propose a new approach for the detection of broken time-reversal symmetry and valley polarization in monolayer WSe$_2$ based on second harmonic generation. Our method can selectively and simultaneously generate and detect a valley polarization at the $\pm K$ valleys of transition metal dichalcogenides at room temperature. Furthermore, it allows to measure the interference between the real and imaginary parts of the intrinsic (electric dipole) and valley terms of the second order nonlinear susceptibility. This work demonstrates the potential and unique capabilities of nonlinear optics as a probe of broken time-reversal symmetry and as a tool for ultrafast and non-destructive valleytronic operations.

physics.optics↗

arXiv2023

Kapitza-resistance-like exciton dynamics in atomically flat MoSe$_{2}$-WSe$_{2}$ lateral heterojunction

Being able to control the neutral excitonic flux is a mandatory step for the development of future room-temperature two-dimensional excitonic devices. Semiconducting Monolayer Transition Metal Dichalcogenides (TMD-ML) with extremely robust and mobile excitons are highly attractive in this regard. However, generating an efficient and controlled exciton transport over long distances is a very challenging task. Here we demonstrate that an atomically sharp TMD-ML lateral heterostructure (MoSe$_{2}$-WSe$_{2}$) transforms the isotropic exciton diffusion into a unidirectional excitonic flow through the junction. Using tip-enhanced photoluminescence spectroscopy (TEPL) and a modified exciton transfer model, we show a discontinuity of the exciton density distribution on each side of the interface. We introduce the concept of exciton Kapitza resistance, by analogy with the interfacial thermal resistance referred to as Kapitza resistance. By comparing different heterostructures with or without top hexagonal boron nitride (hBN) layer, we deduce that the transport properties can be controlled, over distances far greater than the junction width, by the exciton density through near-field engineering and/or laser power density. This work provides a new approach for controlling the neutral exciton flow, which is key toward the conception of excitonic devices.

cond-mat.mes-hall↗

arXiv2023

Interface engineering of charge-transfer excitons in 2D lateral heterostructures

The existence of bound charge transfer (CT) excitons at the interface of monolayer lateral heterojunctions has been debated in literature, but contrary to the case of interlayer excitons in vertical heterostructure their observation still has to be confirmed. Here, we present a microscopic study investigating signatures of bound CT excitons in photoluminescence spectra at the interface of hBN-encapsulated lateral MoSe$_2$-WSe$_2$ heterostructures. Based on a fully microscopic and material-specific theory, we reveal the many-particle processes behind the formation of CT excitons and how they can be tuned via interface- and dielectric engineering. For junction widths smaller than the Coulomb-induced Bohr radius we predict the appearance of a low-energy CT exciton. The theoretical prediction is compared with experimental low-temperature photoluminescence measurements showing emission in the bound CT excitons energy range. Our joint theory-experiment study presents a significant step towards a microscopic understanding of optical properties of technologically promising 2D lateral heterostructures.

cond-mat.mes-hall↗

arXiv2022

Probing the optical near-field interaction of Mie nanoresonators with atomically thin semiconductors

Optical Mie resonators based on silicon nanostructures allow tuning of light-matter-interaction with advanced design concepts based on CMOS compatible nanofabrication. Optically active materials such as transition-metal dichalcogenide (TMD) monolayers can be placed in the near-field region of such Mie resonators. Here, we experimentally demonstrate and verify by numerical simulations coupling between a MoSe2 monolayer and the near-field of dielectric nanoresonators. Through a comparison of dark-field (DF) scattering spectroscopy and photoluminescence excitation experiments (PLE), we show that the MoSe2 absorption can be enhanced via the near-field of a nanoresonator. We demonstrate spectral tuning of the absorption via the geometry of individual Mie resonators. We show that we indeed access the optical near-field of the nanoresonators, by measuring a spectral shift between the typical near-field resonances in PLE compared to the far-field resonances in DF scattering. Our results prove that using MoSe2 as an active probe allows accessing the optical near-field above photonic nanostructures, without the requirement of highly complex near-field microscopy equipment.

physics.optics↗

arXiv2022

One pot chemical vapor deposition of high optical quality large area monolayer Janus transition metal dichalcogenides

We report one-pot chemical vapor deposition (CVD) growth of large-area Janus SeMoS monolayers, with the asymmetric top (Se) and bottom (S) chalcogen atomic planes with respect to the central transition metal (Mo) atoms. The formation of these two-dimensional semiconductor monolayers takes place upon the thermodynamic equilibrium-driven exchange of the bottom Se atoms of the initially grown MoSe2 single crystals on gold foils with S atoms. The growth process is characterized by complementary experimental techniques including Raman and X-ray photoelectron spectroscopy and the growth mechanisms are rationalized by first principle calculations. The remarkably high optical quality of the synthesized Janus monolayers is demonstrated by optical and magneto-optical measurements which reveal the strong exciton-phonon coupling and enable to obtain the exciton g-factor of -3.3.

cond-mat.mtrl-sci↗

arXiv2022

Exciton spectroscopy and diffusion in MoSe2-WSe2 lateral heterostructures encapsulated in hexagonal boron nitride

Chemical vapor deposition (CVD) allows lateral edge epitaxy of transition metal dichalcogenide heterostructures with potential applications in optoelectronics. Critical for carrier and exciton transport is the quality of the two materials that constitute the monolayer and the nature of the lateral heterojunction. Important details of the optical properties were inaccessible in as-grown heterostructure samples due to large inhomogeneous broadening of the optical transitions. Here we perform optical spectroscopy at T = 4 K and also at 300 K to access the optical transitions in CVD grown MoSe2-WSe2 lateral heterostructures that are transferred from the growth-substrate and are encapsulated in hBN. Photoluminescence (PL), reflectance contrast and Raman spectroscopy reveal considerably narrowed optical transition linewidth similar to high quality exfoliated monolayers. In high-resolution transmission electron microscopy (HRTEM) we find near-atomically sharp junctions with a typical extent of 3nm for the covalently bonded MoSe2-WSe2. In PL imaging experiments we find effective excitonic diffusion length that are longer for WSe2 than for MoSe2 at low T=4 K, whereas at 300 K this trend is reversed.

cond-mat.mtrl-sci↗

arXiv2022

Electrically tuneable nonequilibrium optical response of graphene

The ability to tune the optical response of a material via electrostatic gating is crucial for optoelectronic applications, such as electro-optic modulators, saturable absorbers, optical limiters, photodetectors and transparent electrodes. The band structure of single layer graphene (SLG), with zero-gap, linearly dispersive conduction and valence bands, enables an easy control of the Fermi energy E$_F$ and of the threshold for interband optical absorption. Here, we report the tunability of the SLG non-equilibrium optical response in the near-infrared (1000-1700nm/0.729-1.240eV), exploring a range of E$_F$ from -650 to 250 meV by ionic liquid gating. As E$_F$ increases from the Dirac point to the threshold for Pauli blocking of interband absorption, we observe a slow-down of the photobleaching relaxation dynamics, which we attribute to the quenching of optical phonon emission from photoexcited charge carriers. For E$_F$ exceeding the Pauli blocking threshold, photobleaching eventually turns into photoinduced absorption, due to hot electrons' excitation increasing SLG absorption. The ability to control both recovery time and sign of nonequilibrium optical response by electrostatic gating makes SLG ideal for tunable saturable absorbers with controlled dynamics.

cond-mat.mtrl-sci↗

arXiv2021

Second harmonic generation control in twisted bilayers of transition metal dichalcogenides

The twist angle in transition metal dichalcogenide (TMD) heterobilayers is a compelling degree of freedom that determines electron correlations and the period of lateral confinement of moiré excitons. Here we perform polarization-resolved second harmonic generation (SHG) spectroscopy of MoS2/WSe2 heterostructures. We demonstrate that by choosing suitable laser energies the twist angle between two monolayers can be measured directly on the assembled heterostructure. We show that the amplitude and polarization of the SHG signal from the heterostructure are determined by the twist angle between the layers and exciton resonances at the SH energy. For heterostructures with close to zero twist angle, we observe changes of exciton resonance energies and the appearance of new resonances in the linear and non-linear susceptibilities.

cond-mat.mes-hall↗

arXiv2021

Capacitively-coupled and inductively-coupled excitons in bilayer MoS$_2$

The interaction of intralayer and interlayer excitons is studied in a two-dimensional semiconductor, homobilayer MoS$_2$. It is shown that the measured optical susceptibility reveals both the magnitude and the sign of the coupling constants. The interlayer exciton interacts capacitively with the intralayer B-exciton (positive coupling constant) consistent with hole tunnelling from one monolayer to the other. Conversely, the interlayer exciton interacts inductively with the intralayer A-exciton (negative coupling constant). First-principles many-body calculations show that this coupling arises via an intravalley exchange-interaction of A- and B-excitons.

cond-mat.mes-hall↗

arXiv2021

Giant Stark splitting of an exciton in bilayer MoS$_2$

Transition metal dichalcogenides (TMDs) constitute a versatile platform for atomically thin optoelectronics devices and spin-valley memory applications. In monolayers optical absorption is strong, but the transition energy is not tunable as the neutral exciton has essentially no out-of-plane electric dipole. In contrast, interlayer exciton transitions in heterobilayers are widely tunable in applied electric fields, but their coupling to light is considerably reduced. Here, we show tuning over 120 meV of interlayer excitons with high oscillator strength in bilayer MoS2. These shifts are due to the quantum confined Stark effect, here the electron is localised to one of the layers yet the hole is delocalised across the bilayer. We optically probe the interaction between intra- and interlayer excitons as they are energetically tuned into resonance. This allows studying their mixing supported by beyond standard density functional theory calculations including excitonic effects. In MoS2 trilayers our experiments uncover two types of interlayer excitons with and without in-built electric dipoles, respectively. Highly tunable excitonic transitions with large oscillator strength and in-built dipoles, that lead to considerable exciton-exciton interactions, hold great promise for non-linear optics with polaritons.

cond-mat.mes-hall↗

arXiv2021

Interlayer exciton mediated second harmonic generation in bilayer MoS2

Second harmonic generation (SHG) is a non-linear optical process, where two photons coherently combine into one photon of twice their energy. Efficient SHG occurs for crystals with broken inversion symmetry, such as transition metal dichalcogenide monolayers. Here we show tuning of non-linear optical processes in an inversion symmetric crystal. This tunability is based on the unique properties of bilayer MoS2, that shows strong optical oscillator strength for the intra- but also inter-layer exciton resonances. As we tune the SHG signal onto these resonances by varying the laser energy, the SHG amplitude is enhanced by several orders of magnitude. In the resonant case the bilayer SHG signal reaches amplitudes comparable to the off-resonant signal from a monolayer. In applied electric fields the interlayer exciton energies can be tuned due to their in-built electric dipole via the Stark effect. As a result the interlayer exciton degeneracy is lifted and the bilayer SHG response is further enhanced by an additional two orders of magnitude, well reproduced by our model calculations.

cond-mat.mtrl-sci↗

arXiv2020

Prominent room temperature valley polarization in WS2/graphene heterostructures grown by chemical vapor deposition

We examine different cases of heterostructures consisting of WS2 monolayers grown by chemical vapor deposition (CVD) as the optically active material. We show that the degree of valley polarization of WS2 is considerably influenced by the material type used to form the heterostructure. Our results suggest the interaction between WS2 and graphene (WS2/Gr) has a strong effect on the temperature dependent depolarization (i.e. decrease of polarization with increasing temperature), with polarization degrees reaching 24% at room temperature under near-resonant excitation. This contrasts to hBN- encapsulated WS2, which exhibits a room temperature polarization degree of only 11%. The observed low depolarization rate in WS2/Gr heterostructure is attributed to the nearly temperature independent scattering rate due to phonons and fast charge and energy transfer processes from WS2 to graphene. Significant variations in the degree of polarization are also observed at 4K between the different heterostructure configurations. Intervalley hole scattering in the valence band proximity between the K and Γ points of WS2 is sensitive to the immediate environment, leading to the observed variations.

cond-mat.mtrl-sci↗

arXiv2020

Low-loss integrated nanophotonic circuits with layered semiconductor materials

Monolayer transition metal dichalcogenides with direct bandgaps are emerging candidates for microelectronics, nano-photonics, and optoelectronics. Transferred onto photonic integrated circuits (PICs), these semiconductor materials have enabled new classes of light-emitting diodes, modulators and photodetectors, that could be amenable to wafer-scale manufacturing. For integrated photonic devices, the optical losses of the PICs are critical. In contrast to silicon, silicon nitride (Si3N4) has emerged as a low-loss integrated platform with a wide transparency window from ultraviolet to mid-infrared and absence of two-photon absorption at telecommunication bands. Moreover, it is suitable for nonlinear integrated photonics due to its high Kerr nonlinearity and high-power handing capability. These features of Si3N4 are intrinsically beneficial for nanophotonics and optoelectronics applications. Here we report a low-loss integrated platform incorporating monolayer molybdenum ditelluride (1L-MoTe2) with Si3N4 photonic microresonators. We show that, with the 1L-MoTe2, microresonator quality factors exceeding 3 million in the telecommunication O-band to E-band are maintained. We further investigate the change of microresonator dispersion and resonance shift due to the presence of 1L-MoTe2, and extrapolate the optical loss introduced by 1L-MoTe2 in the telecommunication bands, out of the excitonic transition region. Our work presents a key step for low-loss, hybrid PICs with layered semiconductors without using heterogeneous wafer bonding.

physics.optics↗