Self-Adaptive Synthesis of Non-Covalent Crosslinkers while Folding Single-Chain Polymers.

Peptide folding is a dynamic process driven by non-covalent cross-linking leading to functional nanostructures for essential biochemical activities. However, replicating this process in synthetic systems is challenging due to the difficulty in mimicking nature's real-time regulation of non-covalent crosslinking for single-chain polymer folding. Here, we address this by employing anionic dithiol building blocks to create macrocyclic disulfides as non-covalent crosslinkers that adapted to the folding process. Initially, small macrocycles facilitated a low degree folding of a polycation. Then, this preorganized structure catalysed the production of larger macrocycles that enhanced the folding conversely. The self-adaptive synthesis was verified through the encapsulation of an anticancer drug, showing an updated production distribution of non-covalent crosslinkers and maximizing drug-loading efficiency against drug-resistant cancer in vitro. Our research advances the understanding of molecular systems by exploring species evolution via the structural dynamics of polymer folding. Additionally, adaptive synthesis enables controlled, sequential folding of synthetic polymers, with the potential to mimic protein functions.

Actively tunable laser action in GeSn nanomechanical oscillators.

Mechanical forces induced by high-speed oscillations provide an elegant way to dynamically alter the fundamental properties of materials such as refractive index, absorption coefficient and gain dynamics. Although the precise control of mechanical oscillation has been well developed in the past decades, the notion of dynamic mechanical forces has not been harnessed for developing tunable lasers. Here we demonstrate actively tunable mid-infrared laser action in group-IV nanomechanical oscillators with a compact form factor. A suspended GeSn cantilever nanobeam on a Si substrate is resonantly driven by radio-frequency waves. Electrically controlled mechanical oscillation induces elastic strain that periodically varies with time in the GeSn nanobeam, enabling actively tunable lasing emission at >2 µm wavelengths. By utilizing mechanical resonances in the radio frequency as a driving mechanism, this work presents wide-range mid-infrared tunable lasers with ultralow tuning power consumption.

Enhanced second-harmonic generation in strained germanium-on-insulator microdisks for integrated quantum photonic technologies.

Quantum photonic circuits have recently attracted much attention owing to the potential to achieve exceptional performance improvements over conventional classical electronic circuits. Second-order χ(2) nonlinear processes play an important role in the realization of several key quantum photonic components. However, owing to their centrosymmetric nature, CMOS-compatible materials including silicon (Si) and germanium (Ge) traditionally do not possess the χ(2) response. Recently, second-harmonic generation (SHG) that requires the χ(2) response was reported in Ge, but no attempts at enhancing the SHG signal have been conducted and proven experimentally. Herein, we demonstrate the effect of strain on SHG from Ge by depositing a silicon nitride (Si3N4) stressor layer on Ge-on-insulator (GOI) microdisks. This approach allows the deformation of the centrosymmetric unit cell structure of Ge, which can further enhance the χ(2) nonlinear susceptibility for SHG emission. The experimental observation of SHG under femtosecond optical pumping indicates a clear trend of enhancement in SHG signals with increasing strain. Such improvements boost conversion efficiencies by 300% when compared to the control counterpart. This technique paves the way toward realizing a CMOS-compatible material with nonlinear characteristics, presenting unforeseen opportunities for its integration in the semiconductor industry.

Short-wave infrared cavity resonances in a single GeSn nanowire.

Nanowires are promising platforms for realizing ultra-compact light sources for photonic integrated circuits. In contrast to impressive progress on light confinement and stimulated emission in III-V and II-VI semiconductor nanowires, there has been no experimental demonstration showing the potential to achieve strong cavity effects in a bottom-up grown single group-IV nanowire, which is a prerequisite for realizing silicon-compatible infrared nanolasers. Herein, we address this limitation and present an experimental observation of cavity-enhanced strong photoluminescence from a single Ge/GeSn core/shell nanowire. A sufficiently large Sn content ( ~ 10 at%) in the GeSn shell leads to a direct bandgap gain medium, allowing a strong reduction in material loss upon optical pumping. Efficient optical confinement in a single nanowire enables many round trips of emitted photons between two facets of a nanowire, achieving a narrow width of 3.3 nm. Our demonstration opens new possibilities for ultrasmall on-chip light sources towards realizing photonic-integrated circuits in the underexplored range of short-wave infrared (SWIR).

High-Precision Wavelength Tuning of GeSn Nanobeam Lasers via Dynamically Controlled Strain Engineering.

The technology to develop a large number of identical coherent light sources on an integrated photonics platform holds the key to the realization of scalable optical and quantum photonic circuits. Herein, a scalable technique is presented to produce identical on-chip lasers by dynamically controlled strain engineering. By using localized laser annealing that can control the strain in the laser gain medium, the emission wavelengths of several GeSn one-dimensional photonic crystal nanobeam lasers are precisely matched whose initial emission wavelengths are significantly varied. The method changes the GeSn crystal structure in a region far away from the gain medium by inducing Sn segregation in a dynamically controllable manner, enabling the emission wavelength tuning of more than 10 nm without degrading the laser emission properties such as intensity and linewidth. The authors believe that the work presents a new possibility to scale up the number of identical light sources for the realization of large-scale photonic-integrated circuits.