Iris Niehues

Nanoscale Positioning of Single-Photon Emitters in Atomically Thin WSe2

Single-photon emitters in monolayer WSe2 are created at the nanoscale gap between two single-crystalline gold nanorods. The atomically thin semiconductor conforms to the metal nanostructure and is bent at the position of the gap. The induced strain leads to the formation of a localized potential well inside the gap. Single-photon emitters are localized there with a precision better than 140 nm.

Reversible uniaxial strain tuning in atomically thin WSe2

Due to their unique band structure, single layers of transition metal dichalcogenides are promising for new atomic-scale physics and devices. It has been shown that the band structure and the excitonic transitions can be tuned by straining the material. Recently, the discovery of single-photon emission from localized excitons has put monolayer WSe2 in the spotlight. The localized light emitters might be related to local strain potentials in the monolayer. Here, we measure strain-dependent energy shifts for the A, B, C, and D excitons for uniaxial tensile strain up to 1.4% in monolayer WSe2 by performing absorption measurements. A gauge factor of and is derived for the A, B, C, and D exciton, respectively. These values are in good agreement with ab initio GW-BSE calculations. Furthermore, we examine the spatial strain distribution in the WSe2 monolayer at different applied strain levels. We find that the size of the monolayer is crucial for an efficient transfer of strain from the substrate to the monolayer.

Strain Control of Exciton–Phonon Coupling in Atomically Thin Semiconductors

Semiconducting transition metal dichalcogenide (TMDC) monolayers have exceptional physical properties. They show bright photoluminescence due to their unique band structure and absorb more than 10% of the light at their excitonic resonances despite their atomic thickness. At room temperature, the width of the exciton transitions is governed by the exciton-phonon interaction leading to strongly asymmetric line shapes. TMDC monolayers are also extremely flexible, sustaining mechanical strain of about 10% without breaking. The excitonic properties strongly depend on strain. For example, exciton energies of TMDC monolayers significantly redshift under uniaxial tensile strain. Here, we demonstrate that the width and the asymmetric line shape of excitonic resonances in TMDC monolayers can be controlled with applied strain. We measure photoluminescence and absorption spectra of the A exciton in monolayer MoSe2, WSe2, WS2, and MoS2 under uniaxial tensile strain. We find that the A exciton substantially narrows and becomes more symmetric for the selenium-based monolayer materials, while no change is observed for atomically thin WS2. For MoS2 monolayers, the line width increases. These effects are due to a modified exciton-phonon coupling at increasing strain levels because of changes in the electronic band structure of the respective monolayer materials. This interpretation based on steady-state experiments is corroborated by time-resolved photoluminescence measurements. Our results demonstrate that moderate strain values on the order of only 1% are already sufficient to globally tune the exciton-phonon interaction in TMDC monolayers and hold the promise for controlling the coupling on the nanoscale.

Phonon Sidebands in Monolayer Transition Metal Dichalcogenides

Excitons dominate the optical properties of monolayer transition metal dichalcogenides (TMDs). Besides optically accessible bright exciton states, TMDs exhibit also a multitude of optically forbidden dark excitons. Here, we show that efficient exciton-phonon scattering couples bright and dark states and gives rise to an asymmetric excitonic line shape. The observed asymmetry can be traced back to phonon-induced sidebands that are accompanied by a polaron redshift. We present a joint theory-experiment study investigating the microscopic origin of these sidebands in different TMD materials taking into account intra- and intervalley scattering channels opened by optical and acoustic phonons. The gained insights contribute to a better understanding of the optical fingerprint of these technologically promising nanomaterials.

Inverted valley polarization in optically excited transition metal dichalcogenides

Large spin–orbit coupling in combination with circular dichroism allows access to spin-polarized and valley-polarized states in a controlled way in transition metal dichalcogenides. The promising application in spin-valleytronics devices requires a thorough understanding of intervalley coupling mechanisms, which determine the lifetime of spin and valley polarizations. Here we present a joint theory–experiment study shedding light on the Dexter-like intervalley coupling. We reveal that this mechanism couples A and B excitonic states in different valleys, giving rise to an efficient intervalley transfer of coherent exciton populations. We demonstrate that the valley polarization vanishes and is even inverted for A excitons, when the B exciton is resonantly excited and vice versa. Our theoretical findings are supported by energy-resolved and valley-resolved pump-probe experiments and also provide an explanation for the recently measured up-conversion in photoluminescence. The gained insights might help to develop strategies to overcome the intrinsic limit for spin and valley polarizations.In atomically thin transition metal dichalcogenides, spin- and valley-polarised states can be addressed thanks to large spin–orbit coupling and circular dichroism. Here, the authors investigate theoretically and experimentally the decay dynamics of spin and valley polarisation in transition metal dichalcogenide monolayers.

Single-photon emitters in GaSe

Single-photon sources are important building blocks for quantum technology. Recently, non-classical light emitters have been found in the transition metal dichalcogenide WSe2 [1].

Deterministic positioning of single-photon emitters in monolayer WSe 2 on the nanoscale

Single-photon sources are important building blocks for quantum technology. Recently, bright and stable single-photon emitters have been reported in the atomically thin semiconductor WSe2. However, the localized light sources appear at random positions at the edges of the material [1]. Here, we demonstrate the deterministic positioning of single-photon emitters in monolayer WSe2 on the nanoscale [2]. The monolayer is placed on top of a gapped single-crystalline gold rod. The atomically thin semiconductor folds around the metal nanostructure and is bent at the position of the gap (Fig. 1a).