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Alexey Chernikov

Publications and source records attributed to Alexey Chernikov.

47 records · Page 3Linked to original sources

Zeeman Splitting and Inverted Polarization of Biexciton Emission in Monolayer WS2

We investigate the magnetic-field-induced splitting of biexcitons in monolayer WS$_2$ using polarization-resolved photoluminescence spectroscopy in out-of-plane magnetic fields up to 30 T. The observed $g$ factor of the biexciton amounts to $-3.89$, closely matching the $g$ factor of the neutral exciton. The biexciton emission shows an inverted circular field-induced polarization upon linearly polarized excitation, i.e. it exhibits preferential emission from the high-energy peak in a magnetic field. This phenomenon is explained by taking into account the configuration of the biexciton constituents in momentum space and their respective energetic behavior in magnetic fields. Our findings reveal the critical role of dark excitons in the composition of this many-body state.

cond-mat.mes-hall↗

Excitons in atomically thin transition metal dichalcogenides

Atomically thin materials such as graphene and monolayer transition metal dichalcogenides (TMDs) exhibit remarkable physical properties resulting from their reduced dimensionality and crystal symmetry. The family of semiconducting transition metal dichalcogenides is an especially promising platform for fundamental studies of two-dimensional (2D) systems, with potential applications in optoelectronics and valleytronics due to their direct band gap in the monolayer limit and highly efficient light-matter coupling. A crystal lattice with broken inversion symmetry combined with strong spin-orbit interactions leads to a unique combination of the spin and valley degrees of freedom. In addition, the 2D character of the monolayers and weak dielectric screening from the environment yield a significant enhancement of the Coulomb interaction. The resulting formation of bound electron-hole pairs, or excitons, dominates the optical and spin properties of the material. Here we review recent progress in our understanding of the excitonic properties in monolayer TMDs and lay out future challenges. We focus on the consequences of the strong direct and exchange Coulomb interaction, discuss exciton-light interaction and effects of other carriers and excitons on electron-hole pairs in TMDs. Finally, the impact on valley polarization is described and the tuning of the energies and polarization observed in applied electric and magnetic fields is summarized.

cond-mat.mtrl-sci↗

Valley Dynamics of Excitons in Monolayer Dichalcogenides

Monolayer transition-metal dichalcogenides (TMDCs) have recently emerged as possible candidates for valleytronic applications, as the spin and valley pseudospin are directly coupled and stabilized by a large spin splitting. In these semiconducting materials, optically excited electron-hole pairs form tightly Coulomb-bound excitons with large binding energies. The selection rules for excitonic transitions allow for direct optical generation of a valley-polarized exciton population using resonant excitation. Here, we investigate the exciton valley dynamics in monolayers of three different TMDCs by means of time-resolved Kerr rotation at low temperatures. We observe pronounced differences in the valley dynamics of tungsten- and molybdenum-based TMDCs, which are directly related to the opposite order of the conduction-band spin splitting in these materials.

cond-mat.mes-hall↗

Giant Zeeman splitting inducing near-unity valley polarization in van der Waals heterostructures

Monolayers of semiconducting transition metal dichalcogenides exhibit intriguing fundamental physics of strongly coupled spin and valley degrees of freedom for charge carriers. While the possibility of exploiting these properties for information processing stimulated concerted research activities towards the concept of valleytronics , maintaining control over spin-valley polarization proved challenging in individual monolayers. A promising alternative route explores type II band alignment in artificial van der Waals heterostructures. The resulting formation of interlayer excitons combines the advantages of long carrier lifetimes and spin-valley locking . Here, we demonstrate direct magnetic manipulation of valley polarization in a WSe2/MoSe2 heterostructure through giant valley Zeeman splitting of interlayer transitions. Remarkably, even after non-selective injection, the observed $g$ factor as large as $-15$ induces near-unity polarization of long-lived excitons with 100 ns lifetimes under magnetic fields. The demonstrated control of the spin-valley physics highlights the exceptional aspects of novel, artificially designed material systems and their promise for atomically-thin valleytronic devices.

cond-mat.mes-hall↗

Interlayer exciton dynamics in a dichalcogenide monolayer heterostructure

In heterostructures consisting of different transition-metal dichalcogenide monolayers, a staggered band alignment can occur, leading to rapid charge separation of optically generated electron-hole pairs into opposite monolayers. These spatially separated electron-hole pairs are Coulomb-coupled and form interlayer excitons. Here, we study these interlayer excitons in a heterostructure consisting of MoSe$_2$ and WSe$_2$ monolayers using photoluminescence spectroscopy. We observe a non-trivial temperature dependence of the linewidth and the peak energy of the interlayer exciton, including an unusually strong initial redshift of the transition with temperature, as well as a pronounced blueshift of the emission energy with increasing excitation power. By combining these observations with time-resolved photoluminescence measurements, we are able to explain the observed behavior as a combination of interlayer exciton diffusion and dipolar, repulsive exciton-exciton interaction.

cond-mat.mes-hall↗

Spectral focusing of broadband silver electroluminescence in nanoscopic FRET-LEDs

Few inventions have shaped the world like the incandescent bulb. While Edison used thermal radiation from ohmically heated conductors, some noble metals exhibit "cold" electroluminescence (EL) in percolation films, tunnel diodes, electromigrated nanoparticle aggregates, optical antennae, or scanning-tunnelling microscopy (STM). The origin of this radiation, which is spectrally broad and depends on applied bias, is controversial given the low radiative yields of electronic transitions. Nanoparticle EL is particularly intriguing since it involves localized surface-plasmon resonances with large dipole moments. Such plasmons enable very efficient non-radiative fluorescence resonance energy transfer (FRET) coupling to proximal resonant dipole transitions. We demonstrate nanoscopic FRET-LEDs which exploit the opposite process, energy transfer from silver nanoparticles to exfoliated monolayers of transition-metal dichalcogenides (TMDCs). In diffraction-limited hotspots showing pronounced photon bunching, broadband silver EL is focused into the narrow excitonic resonance of the atomically thin overlayer. Such devices may offer alternatives to conventional nano-LEDs in on-chip optical interconnects.

physics.optics↗

Coulomb engineering of the bandgap in 2D semiconductors

The ability to control the size of the electronic bandgap is an integral part of solid-state technology. Atomically-thin two-dimensional crystals offer a new approach for tuning the energies of the electronic states based on the interplay between the environmental sensitivity and unusual strength of the Coulomb interaction in these materials. By engineering the surrounding dielectric environment, we are able to tune the electronic bandgap in monolayers of WS2 and WSe2 by hundreds of meV. We exploit this behavior to present an in-plane dielectric heterostructure with a spatially dependent bandgap, illustrating the feasibility of our approach for the creation of lateral junctions with nanoscale resolution. This successful demonstration of bandgap engineering based on the non-invasive modification of the Coulomb interaction should enable the design of a new class of atomically thin devices to advance the limits of size and functionality for solid-state technologies.

cond-mat.mes-hall↗

Measurement of the optical dielectric function of transition metal dichalcogenide monolayers: MoS2, MoSe2, WS2 and WSe2

We report a determination of the complex in-plane dielectric function of monolayers of four transition metal dichalcogenides: MoS2, MoSe2, WS2 and WSe2, for photon energies from 1.5 - 3 eV. The results were obtained from reflection spectra using a Kramers-Kronig constrained variational analysis. From the dielectric functions, we obtain the absolute absorbance of the monolayers. We also provide a comparison of the dielectric function for the monolayers with the corresponding bulk materials.

cond-mat.mtrl-sci↗

Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

Atomically thin transition metal dichalcogenides (TMDs) are direct-gap semiconductors with strong light-matter and Coulomb interaction. The latter accounts for tightly bound excitons, which dominate the optical properties of these technologically promising materials. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. In a recent study, an experimental evidence for the existence of such dark states has been demonstrated, as well as their strong impact on the quantum efficiency of light emission in TMDs. Here, we reveal the microscopic origin of the excitonic coherence lifetime in two representative TMD materials (WS$_2$ and MoSe$_2$) within a joint study combining microscopic theory with optical experiments. We show that the excitonic coherence lifetime is determined by phonon-induced intra- and intervalley scattering into dark excitonic states. Remarkably, and in accordance with the theoretical prediction, we find an efficient exciton relaxation in WS$_2$ through phonon emission at all temperatures.

cond-mat.mtrl-sci↗

Valley Splitting and Polarization by the Zeeman Effect in Monolayer MoSe2

We have measured circularly polarized photoluminescence in monolayer MoSe2 under perpendicular magnetic fields up to 10 T. At low doping densities, the neutral and charged excitons shift linearly with field strength at a rate of $\mp$ 0.12 meV/T for emission arising, respectively, from the K and K' valleys. The opposite sign for emission from different valleys demonstrates lifting of the valley degeneracy. The magnitude of the Zeeman shift agrees with predicted magnetic moments for carriers in the conduction and valence bands. The relative intensity of neutral and charged exciton emission is modified by the magnetic field, reflecting the creation of field-induced valley polarization. At high doping levels, the Zeeman shift of the charged exciton increases to $\mp$ 0.18 meV/T. This enhancement is attributed to many-body effects on the binding energy of the charged excitons.

cond-mat.mes-hall↗

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2

We have experimentally determined the energies of the ground and first four excited excitonic states of the fundamental optical transition in monolayer WS2, a model system for the growing class of atomically thin two-dimensional semiconductor crystals. From the spectra, we establish a large exciton binding energy of 0.32 eV and a pronounced deviation from the usual hydrogenic Rydberg series of energy levels of the excitonic states. We explain both of these results using a microscopic theory in which the non-local nature of the effective dielectric screening modifies the functional form of the Coulomb interaction. These strong but unconventional electron-hole interactions are expected to be ubiquitous in atomically thin materials.

cond-mat.mtrl-sci↗