Publications by authors named "Sufei Shi"

The pursuit of two-dimensional (2D) magnetism is promising for energy-efficient electronic devices, including magnetoelectric random access memory and radio frequency/microwave magnonics, and it is gaining fundamental insights into quantum sensing technology. The key challenge resides in overseeing magnetic exchange interactions through a precise chemical reduction process, wherein manipulation of the arrangement of atoms and electrons is essential for achieving room-temperature 2D magnetism tailoring in a manner compatible with device architectures. Here, we report an electrochemically crafted CrI layered magnet─a van der Waals material─with precisely tailored lithiation and delithiation degrees.

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The enhanced Coulomb interaction in two-dimensional semiconductors leads to tightly bound electron-hole pairs known as excitons. The large binding energy of excitons enables the formation of Rydberg excitons with high principal quantum numbers (n), analogous to Rydberg atoms. Rydberg excitons possess strong interactions among themselves as well as sensitive responses to external stimuli.

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The enhanced Coulomb interaction in two dimensions leads to not only tightly bound excitons but also many-particle excitonic complexes: excitons interacting with other quasiparticles, which results in improved and even new exciton properties with better controls. Here, we summarize studies of excitonic complexes in monolayer transition metal dichalcogenides and their moiré heterojunctions, envisioning how to utilize them for exploring quantum many-body physics.

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Moiré superlattices of semiconducting transition metal dichalcogenides enable unprecedented spatial control of electron wavefunctions, leading to emerging quantum states. The breaking of translational symmetry further introduces a new degree of freedom: high symmetry moiré sites of energy minima behaving as spatially separated quantum dots. We demonstrate the superposition between two moiré sites by constructing a trilayer WSe/monolayer WS moiré heterojunction.

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Transition metal dichalcogenide (TMDC) moiré superlattices, owing to the moiré flatbands and strong correlation, can host periodic electron crystals and fascinating correlated physics. The TMDC heterojunctions in the type-II alignment also enable long-lived interlayer excitons that are promising for correlated bosonic states, while the interaction is dictated by the asymmetry of the heterojunction. Here we demonstrate a new excitonic state, quadrupolar exciton, in a symmetric WSe-WS-WSe trilayer moiré superlattice.

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The non-toxic and stable chalcogenide perovskite BaZrS fulfills many key optoelectronic properties for a high-efficiency photovoltaic material. It has been shown to possess a direct band gap with a large absorption coefficient and good carrier mobility values. With a reported band gap of 1.

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In the archetypal monolayer semiconductor WSe_{2}, the distinct ordering of spin-polarized valleys (low-energy pockets) in the conduction band allows for studies of not only simple neutral excitons and charged excitons (i.e., trions), but also more complex many-body states that are predicted at higher electron densities.

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Moiré coupling in transition metal dichalcogenides (TMDCs) superlattices introduces flat minibands that enable strong electronic correlation and fascinating correlated states, and it also modifies the strong Coulomb-interaction-driven excitons and gives rise to moiré excitons. Here, we introduce the layer degree of freedom to the WSe/WS moiré superlattice by changing WSe from monolayer to bilayer and trilayer. We observe systematic changes of optical spectra of the moiré excitons, which directly confirm the highly interfacial nature of moiré coupling at the WSe/WS interface.

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Lead iodide (PbI) as a layered material has emerged as an excellent candidate for optoelectronics in the visible and ultraviolet regime. Micrometer-sized flakes synthesized by mechanical exfoliation from bulk crystals or by physical vapor deposition have shown a plethora of applications from low-threshold lasing at room temperature to high-performance photodetectors with large responsivity and faster response. However, large-area centimeter-sized growth of epitaxial thin films of PbI with well-controlled orientation has been challenging.

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Heterobilayers of transition metal dichalcogenides (TMDCs) can form a moiré superlattice with flat minibands, which enables strong electron interaction and leads to various fascinating correlated states. These heterobilayers also host interlayer excitons in a type-II band alignment, in which optically excited electrons and holes reside on different layers but remain bound by the Coulomb interaction. Here we explore the unique setting of interlayer excitons interacting with strongly correlated electrons, and we show that the photoluminescence (PL) of interlayer excitons sensitively signals the onset of various correlated insulating states as the band filling is varied.

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Despite the broadband response, limited optical absorption at a particular wavelength hinders the development of optoelectronics based on Dirac fermions. Heterostructures of graphene and various semiconductors have been explored for this purpose, while non-ideal interfaces often limit the performance. The topological insulator (TI) is a natural hybrid system, with the surface states hosting high-mobility Dirac fermions and the small-bandgap semiconducting bulk state strongly absorbing light.

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Metal chalcogenide nanoparticles offer vast control over their optoelectronic properties via size, shape, composition, and morphology which has led to their use across fields including optoelectronics, energy storage, and catalysis. While cadmium and lead-based nanocrystals are prevalent in applications, concerns over their toxicity have motivated researchers to explore alternate classes of nanomaterials based on environmentally benign metals such as zinc and tin. The goal of this research is to identify material systems that offer comparable performance to existing metal chalcogenide systems from abundant, recyclable, and environmentally benign materials.

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Electrets are dielectric materials that have a quasi-permanent dipole polarization. A single-molecule electret is a long-sought-after nanoscale component because it can lead to miniaturized non-volatile memory storage devices. The signature of a single-molecule electret is the switching between two electric dipole states by an external electric field.

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Accurate classification of burn severities is of vital importance for proper burn treatments. A recent article reported that using the combination of Raman spectroscopy and optical coherence tomography (OCT) classifies different degrees of burns with an overall accuracy of 85% [1]. In this study, we demonstrate the feasibility of using Raman spectroscopy alone to classify burn severities on ex vivo porcine skin tissues.

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A strong Coulomb interaction could lead to a strongly bound exciton with high-order excited states, similar to the Rydberg atom. The interaction of giant Rydberg excitons can be engineered for a correlated ordered exciton array with a Rydberg blockade, which is promising for realizing quantum simulation. Monolayer transition metal dichalcogenides, with their greatly enhanced Coulomb interaction, are an ideal platform to host the Rydberg excitons in two dimensions.

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Strong many-body interaction in two-dimensional transitional metal dichalcogenides provides a unique platform to study the interplay between different quasiparticles, such as prominent phonon replica emission and modified valley-selection rules. A large out-of-plane magnetic field is expected to modify the exciton-phonon interactions by quantizing excitons into discrete Landau levels, which is largely unexplored. Here, we observe the Landau levels originating from phonon-exciton complexes and directly probe exciton-phonon interaction under a quantizing magnetic field.

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Monolayer transition-metal dichalcogenides (TMDs) are the first truly two-dimensional (2D) semiconductor, providing an excellent platform to investigate light-matter interaction in the 2D limit. The inherently strong excitonic response in monolayer TMDs can be further enhanced by exploiting the temporal confinement of light in nanophotonic structures. Here, we demonstrate a 2D exciton-polariton system by strongly coupling atomically thin tungsten diselenide (WSe) monolayer to a silicon nitride (SiN) metasurface.

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The heterostructure of monolayer transition metal dichalcogenides (TMDCs) provides a unique platform to manipulate exciton dynamics. The ultrafast carrier transfer across the van der Waals interface of the TMDC hetero-bilayer can efficiently separate electrons and holes in the intralayer excitons with a type II alignment, but it will funnel excitons into one layer with a type I alignment. In this work, we demonstrate the reversible switch from exciton dissociation to exciton funneling in a MoSe/WS heterostructure, which manifests itself as the photoluminescence (PL) quenching to PL enhancement transition.

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Heterostructures of two-dimensional transition metal dichalcogenides (TMDs) can offer a plethora of opportunities in condensed matter physics, materials science, and device engineering. However, despite state-of-the-art demonstrations, most current methods lack enough degrees of freedom for the synthesis of heterostructures with engineerable properties. Here, we demonstrate that combining a postgrowth chalcogen-swapping procedure with the standard lithography enables the realization of lateral TMD heterostructures with controllable dimensions and spatial profiles in predefined locations on a substrate.

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Transition metal dichalcogenides (TMDCs) heterostructure with a type II alignment hosts unique interlayer excitons with the possibility of spin-triplet and spin-singlet states. However, the associated spectroscopy signatures remain elusive, strongly hindering the understanding of the Moiré potential modulation of the interlayer exciton. In this work, we unambiguously identify the spin-singlet and spin-triplet interlayer excitons in the WSe/MoSe heterobilayer with a 60° twist angle through the gate- and magnetic field-dependent photoluminescence spectroscopy.

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This study utilizes Raman spectroscopy to analyze the burn-induced collagen conformational changes in ex vivo porcine skin tissue. Raman spectra of wavenumbers 500-2000 cm were measured for unburnt skin as well as four different burn conditions: (i) 200 °F for 10 s, (ii) 200 °F for the 30 s, (iii) 450 °F for 10 s and (iv) 450 °F for 30 s. The overall spectra reveal that protein and amino acids-related bands have manifested structural changes including the destruction of protein-related functional groups, and transformation from α-helical to disordered structures which are correlated with increasing burn severity.

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Inversion symmetry breaking and 3-fold rotation symmetry grant the valley degree of freedom to the robust exciton in monolayer transition-metal dichalcogenides, which can be exploited for valleytronics applications. However, the short lifetime of the exciton significantly constrains the possible applications. In contrast, the dark exciton could be long-lived but does not necessarily possess the valley degree of freedom.

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Article Synopsis
  • Spin-forbidden dark excitons in tungsten-based TMDCs have long lifetimes and unique spin textures, making them a focus of research in material science.
  • Researchers demonstrated the ability to control these dark excitons by combining them with free electrons or holes, creating what are known as dark trions.
  • The study revealed distinct differences in photon valley polarization due to the intervalley scattering mechanisms of electrons and holes, and highlighted the ability to tune the lifetime of dark trions by adjusting gate voltage, opening new avenues for applications in excitonic optoelectronics and valleytronics.
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Tungsten-based monolayer transition metal dichalcogenides host a long-lived "dark" exciton, an electron-hole pair in a spin-triplet configuration. The long lifetime and unique spin properties of the dark exciton provide exciting opportunities to explore light-matter interactions beyond electric dipole transitions. Here we demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe.

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