The in-plane piezoelectricity or ferroelectricity of two-dimensional (2D) materials can vanish due to the appearance of inversion symmetry with increasing flake thickness, which drastically limits the development of their energy-harvesting application. Although the inversion symmetry breaking in spiral structure of 2D material may solve this problem, the control of spiral growth remains immature. Here, a novel technique to achieve high percentage of spiral SnS flakes with superior control of nucleation position is demonstrated. By introducing atomic steps on substrates, the screw dislocation can be easily formed when SnS partially grows across these steps and leads to over 90% of spiral SnS flakes grown by physical vapor deposition (PVD). Furthermore, the preference for SnS to nucleate at steps can introduce remarkable nucleation site control of spiral growth even on substrates with artificially transferred graphene atomic steps. Interestingly, it turns out that the spiral SnS structure exhibits centrosymmetric characteristic, indicating that single-spiral 2D materials with monolayer step height do not guarantee an inversion symmetry breaking structure. The high spiral flake percentage and precise control of nucleation sites in this study will facilitate future development of spiral 2D materials.

We report on the first demonstration of metal−insulator−semiconductor-type plasmonic lasers at the telecom wavelength (∼1.3 μm) using top-down fabricated semiconductor waveguides on single-crystalline metallic platforms formed using epitaxially grown Ag films. The critical role of the Ag film thickness in sustaining plasmonic lasing at the telecom wavelength is investigated systematically. Low-threshold (0.2 MW/cm 2 ) and continuous-wave operation of plasmonic lasing at cryogenic temperatures can be achieved on a 150 nm Ag platform with minimum radiation leakage into the substrate. Plasmonic lasing occurs preferentially through higher-order surface-plasmon-polariton modes, which exhibit a higher mode confinement factor, lower propagation loss, and better field−gain coupling. We observed plasmonic lasing up to ∼200 K under pulsed excitations. The plasmonic lasers on large-area epitaxial Ag films open up a scalable platform for on-chip integrations of plasmonics and optoelectronics at the telecom wavelength.

Single‐layered MoS2 is a naturally stable material. Integrating spin, valley, and circularly polarized photons is an interesting endeavor to achieve advanced spin‐valleytronics. In this study, room‐temperature ferromagnetism in MoS2 induced by the magnetic proximity effect (MPE) of yttrium iron garnet (YIG) and the antiferromagnetic coupling at the interface is demonstrated. Insulating YIG without charge carriers is an excellent magnetic candidate featuring a long spin diffusion length and remarkable surface flatness, enabling long‐range magnetic interactions with MoS2. Spin‐resolved photoluminescence spectroscopy and magnetic circular dichroism (MCD) reveal that the spin‐polarized valleys of MoS2 can achieve sustained ferromagnetism even at room temperature. The bandgap‐sensitivity of MCD further demonstrates the extent of antiferromagnetic coupling between the MPE‐induced moments of MoS2 and YIG. This work provides a layer‐selected approach to study magnetic interactions/configurations in the YIG/MoS2 bilayer and highlights the role of MoS2 in achieving the MPE toward high temperature.

Single crystalline Ag films on dielectric substrates have received tremendous attention recently due to their technological potentials as low loss plasmonic materials. Two different growth approaches have been used to produce single crystalline Ag films previously. One approach is based on repetitive cycles of a two-step process (low temperature deposition followed by RT annealing) using molecular beam epitaxy (MBE), which is extremely timeconsuming due to the need for repeat growth cycles. Another approach is based on rapid e-beam deposition which is capable of growing thick single crystalline Ag films (>300 nm) but lacks the precision in thickness control of thin epitaxial films. Here, we report a universal approach to grow atomically smooth epitaxial Ag films by eliminating the repetitive cycles used in the previous two-step MBE method while maintaining the precise thickness control from a few monolayers to the optically thick regime, thus overcoming the limitations of the two aforementioned methods. In addition, we develop an in situ growth of aluminum oxide as the capping layer to protect the epitaxial Ag films. The quality of the epitaxial Ag films was evaluated using a variety of techniques, and the superior optical performance of the films is demonstrated by measuring the propagation length of surface plasmon polaritons (∼80 μm at 632 nm) as well as their capability to support a plasmonic nanolaser in infrared incorporating an InGaAsP quantum well as the gain media.

Transition-metal dichalcogenide (TMDC) homoand heterostacks hold tantalizing prospects for being integrated as active components in future van der Waals (vdW) electronics and optoelectronics. However, most TMDC homo-and heterostacks are created by onerous mechanical exfoliation, followed by a mixing-and-matching process. While versatile enough for pilot demonstrations, these strategies are clearly not scalable for practical technologies and widespread implementations. Here, we report a two-step epitaxy strategy that promotes the growth of second-layer TMDCs on the basal plane of the first TMDCs epilayer. The first-layer TMDCs are grown on substrates where the tensile strength can be tuned by the control of chemical environments. The succeeding epilayers then prefer to grow layer-by-layer on the highly tensile-strained first layers. The result is the growth of high-density TMDC homo (WSe 2 ) bilayers and hetero (WSe 2 −MoS 2 ) bilayers with an exceedingly high yield (>99% bilayers) and uniformity. A density functional theory simulation further sheds light on how strain engineering shifts the subsequent layer growth preference. Second-harmonic generation and high-angle annular dark-field scanning transmission electron microscopy collectively attest to the AB and AA′ stacking between the TMDC epi-and overlayers. The proposed strategy could be a versatile platform for synthesizing diverse arrays of vdW homo-and heterostacks, thus providing prospects for realizing largescale and layer-controllable two-dimensional electronics.