Room Temperature, Twist Angle Independent, Momentum Direct Interlayer Excitons in van der Waals Heterostructures with Wide Spectral Tunability.

Interlayer excitons (IXs) in van der Waals heterostructures with static out of plane dipole moment and long lifetime show promise in the development of exciton based optoelectronic devices and the exploration of many body physics. However, these IXs are not always observed, as the emission is very sensitive to lattice mismatch and twist angle between the constituent materials. Moreover, their emission intensity is very weak compared to that of corresponding intralayer excitons at room temperature. Here we report the room-temperature realization of twist angle independent momentum direct IX in the heterostructures of bulk PbI2 and bilayer WS2. Momentum conserving transitions combined with the large band offsets between the constituent materials enable intense IX emission at room temperature. A long lifetime (∼100 ns), noticeable Stark shift, and tunability of IX emission from 1.70 to 1.45 eV by varying the number of WS2 layers make these heterostructures promising to develop room temperature exciton based optoelectronic devices.

Layer-Number Engineered Momentum-Indirect Interlayer Excitons with Large Spectral Tunability.

Interlayer excitons (IXs) in type II van der Waals (vdW) heterostructures are equipped with an oriented permanent dipole moment and long lifetime and thus would allow promising applications in excitonic and optoelectronic devices. However, based on the widely studied heterostructures of transition-metal dichalcogenides (TMDs), IX emission is greatly influenced by the lattice mismatch and geometric misalignment between the constituent layers, increasing the complexity of the device fabrication. Here, we report on the robust momentum-indirect IX emission in TMD/two-dimensional (2D) perovskite vdW heterostructures, which were fabricated without considering the orientation arrangement or momentum mismatch. The IXs show a large diffusion coefficient of ∼10 cm2 s-1, and importantly the IX emission energy can be widely tuned from 1.3 to 1.6 eV via changing the layer number of the 2D perovskite or the thickness of TMD flakes, shedding light on the applications of vdW interface engineering to broad-spectrum optoelectronics.

Enhancing Plasmonic Spectral Tunability with Anomalous Material Dispersion.

The field confinement of plasmonic systems enables spectral tunability under structural variations or environmental perturbations, which is the principle for various applications including nanorulers, sensors, and color displays. Here, we propose and demonstrate that materials with anomalous dispersion, such as Ge in the visible, improve spectral tunability. We introduce our proposal with a semianalytical guided mode picture. Using Ge-based film (Ag/Au)-coupled gap plasmon resonators, we implement two architectures and demonstrate the improved tunability with single-particle dark-field scattering, ensemble reflection, and color generation. We observe three-fold enhancement of tunability with Ge nanodisks compared with that of Si, a normal-dispersion material in the visible. The structural color generation of large array systems, made of inversely fabricated Ge-Ag resonators, exhibits a wide gamut. Our results introduce anomalous material dispersion as an extra degree of freedom to engineer the spectral tunability of plasmonic systems, especially relevant for actively tunable plasmonics and metasurfaces.

On-demand engineerable visible spectrum by fine control of electrochemical reactions.

Tunability of optical performance is one of the key technologies for adaptive optoelectronic applications, such as camouflage clothing, displays, and infrared shielding. High-precision spectral tunability is of great importance for some special applications with on-demand adaptability but remains challenging. Here we demonstrate a galvanostatic control strategy to achieve this goal, relying on the finding of the quantitative correlation between optical properties and electrochemical reactions within materials. An electrochromic electro-optical efficiency index is established to optically fingerprint and precisely identify electrochemical redox reactions in the electrochromic device. Consequently, the charge-transfer process during galvanostatic electrochemical reaction can be quantitatively regulated, permitting precise control over the final optical performance and on-demand adaptability of electrochromic devices as evidenced by an ultralow deviation of <3.0%. These findings not only provide opportunities for future adaptive optoelectronic applications with strict demand on precise spectral tunability but also will promote in situ quantitative research in a wide range of spectroelectrochemistry, electrochemical energy storage, electrocatalysis, and material chemistry.