Switchable, Tunable, and Directable Exciton Funneling in Periodically Wrinkled WS2.

The extreme elastic strain of monolayer transition metal dichalcogenides provides an ideal platform to achieve efficient exciton funneling via local strain modulation; however, studies conducted thus far have focused on the use of substrates with fixed strain profiles. We prepared 1L-WS2 on a flexible substrate such that the formation of topographic wrinkles could be switched on or off, and the depth or the direction of the wrinkle could be modified by external strain, thereby providing full control of the periodic undulation of the band gap profile of 1L-WS2 in the range 0-57 meV. Nanoscale photoluminescence (PL) imaging unambiguously evinced that the photoexcited excitons of 1L-WS2 were accumulated at the top regions of the wrinkles with less band gap than the valley region. Our results of broad tunability of the two-dimensional (2D) exciton funneling suggest a promising route to control exciton drift for enhanced optoelectronic performances and future 2D exciton devices.

Dynamic Exciton Funneling by Local Strain Control in a Monolayer Semiconductor.

The ability to control excitons in semiconductors underlies numerous proposed applications, from excitonic circuits to energy transport. Two dimensional (2D) semiconductors are particularly promising for room-temperature applications due to their large exciton binding energy and enormous stretchability. Although the strain-induced static exciton flux has been observed in predetermined structures, dynamic control of exciton flux represents an outstanding challenge. Here, we introduce a method to tune the bandgap of suspended 2D semiconductors by applying a local strain gradient with a nanoscale tip. This strain allows us to locally and reversibly shift the exciton energy and to steer the exciton flux over micrometer-scale distances. We anticipate that our result not only marks an important experimental tool but will also open a broad range of new applications from information processing to energy conversion.

Nanocrystal skins with exciton funneling for photosensing.

Highly photosensitive nanocrystal (NC) skins based on exciton funneling are proposed and demonstrated using a graded bandgap profile across which no external bias is applied in operation for light-sensing. Four types of gradient NC skin devices (GNS) made of NC monolayers of distinct sizes with photovoltage readout are fabricated and comparatively studied. In all structures, polyelectrolyte polymers separating CdTe NC monolayers set the interparticle distances between the monolayers of ligand-free NCs to <1 nm. In this photosensitive GNS platform, excitons funnel along the gradually decreasing bandgap gradient of cascaded NC monolayers, and are finally captured by the NC monolayer with the smallest bandgap interfacing the metal electrode. Time-resolved measurements of the cascaded NC skins are conducted at the donor and acceptor wavelengths, and the exciton transfer process is confirmed in these active structures. These findings are expected to enable large-area GNS-based photosensing with highly efficient full-spectrum conversion.

Imaging Strain-Localized Single-Photon Emitters in Layered GaSe below the Diffraction Limit.

Nanoscale strain control of exciton funneling is an increasingly critical tool for the scalable production of single photon emitters (SPEs) in two-dimensional materials. However, conventional far-field optical microscopies remain constrained in spatial resolution by the diffraction limit and thus can provide only a limited description of nanoscale strain localization of SPEs. Here, we quantify the effects of nanoscale heterogeneous strain on the energy and brightness of GaSe SPEs on nanopillars with correlative cathodoluminescence, photoluminescence, and atomic force microscopy, supported by density functional theory simulations. We report the strain-localized SPEs have a broad range of emission wavelengths from 620 to 900 nm. We reveal substantial strain-controlled SPE wavelength tunability over a ∼100 nm spectral range and 2 orders of magnitude enhancement in the SPE brightness at the pillar center due to Type-I exciton funneling. In addition, we show that radiative biexciton cascade processes contribute to observed CL photon superbunching. Also, the GaSe SPEs show excellent stability, where their properties remain unchanged after electron beam exposure. We anticipate that this comprehensive study on the nanoscale strain control of two-dimensional SPEs will provide key insights to guide the development of truly deterministic quantum photonics.

Tip-Enhanced Photoluminescence of Freestanding Lateral Heterobubbles.

Two-dimensional (2D) semiconducting materials have promising applications in flexible optoelectronics, nanophotonics, and sensing based on the broad tunability of their optical and electronic properties. 2D nanobubbles form exciton funnels due to localized strain that can be used as local emitters for information processing. Their nanoscale optical characterization requires the use of near-field scanning probe microscopy (SPM). However, previous near-field studies of 2D materials were performed on SiO2/Si and metallic substrates using the plasmonic gap mode to increase the signal-to-noise ratio. Another challenge is the deterministic control of bubble size and location. We addressed these challenges by investigating the photoluminescence (PL) signals of freestanding monolayer lateral WSe2-MoSe2 heterostructures under the influence of strain exerted by a plasmonic SPM tip. For first time, we performed tip-enhanced PL imaging of freestanding 2D materials and studied the competition between the PL enhancement mechanisms by nanoindentation as a function of the tip-sample distance. We observed the tunability of PL as a function of bubble size, which opens new possibilities to design optoelectronic nanodevices.

Tip-Induced Nano-Engineering of Strain, Bandgap, and Exciton Funneling in 2D Semiconductors.

The tunability of the bandgap, absorption and emission energies, photoluminescence (PL) quantum yield, exciton transport, and energy transfer in transition metal dichalcogenide (TMD) monolayers provides a new class of functions for a wide range of ultrathin photonic devices. Recent strain-engineering approaches have enabled to tune some of these properties, yet dynamic control at the nanoscale with real-time and -space characterizations remains a challenge. Here, a dynamic nano-mechanical strain-engineering of naturally-formed wrinkles in a WSe2 monolayer, with real-time investigation of nano-spectroscopic properties is demonstrated using hyperspectral adaptive tip-enhanced PL (a-TEPL) spectroscopy. First, nanoscale wrinkles are characterized through hyperspectral a-TEPL nano-imaging with <15 nm spatial resolution, which reveals the modified nano-excitonic properties by the induced tensile strain at the wrinkle apex, for example, an increase in the quantum yield due to the exciton funneling, decrease in PL energy up to ≈10 meV, and a symmetry change in the TEPL spectra caused by the reconfigured electronic bandstructure. Then the local strain is dynamically engineered by pressing and releasing the wrinkle apex through an atomic force tip control. This nano-mechanical strain-engineering allows to tune the exciton dynamics and emission properties at the nanoscale in a reversible fashion. In addition, a systematic switching and modulation platform of the wrinkle emission is demonstrated, which provides a new strategy for robust, tunable, and ultracompact nano-optical sources in atomically thin semiconductors.