An official website of the United States government
Abstract Two distinct stacking orders in ReS2are identified without ambiguity and their influence on vibrational, optical properties and carrier dynamics are investigated. With atomic resolution scanning transmission electron microscopy (STEM), two stacking orders are determined as AA stacking with negligible displacement across layers, and AB stacking with about a one‐unit cell displacement along theaaxis. First‐principles calculations confirm that these two stacking orders correspond to two local energy minima. Raman spectra inform a consistent difference of modes I & III, about 13 cm−1for AA stacking, and 20 cm−1for AB stacking, making a simple tool for determining the stacking orders in ReS2. Polarized photoluminescence (PL) reveals that AB stacking possesses blueshifted PL peak positions, and broader peak widths, compared with AA stacking, indicating stronger interlayer interaction. Transient transmission measured with femtosecond pump–probe spectroscopy suggests exciton dynamics being more anisotropic in AB stacking, where excited state absorption related to Exc. III mode disappears when probe polarization aligns perpendicular tobaxis. The findings underscore the stacking‐order driven optical properties and carrier dynamics of ReS2, mediate many seemingly contradictory results in the literature, and open up an opportunity to engineer electronic devices with new functionalities by manipulating the stacking order.
more »
« less
This content will become publicly available on January 31, 2026
Harnessing in-plane optical anisotropy in WS 2 through ReS 2 crystal
Abstract In this work, we explore how the optical properties of isotropic materials can be modulated by adjacent anisotropic materials, providing new insights into anisotropic light-matter interactions in van der Waals heterostructures. Using a WS2/ReS2heterostructure, we systematically investigated the excitation angle-dependent photoluminescence (PL), differential reflectance, time-resolved PL, and power-dependent PL anisotropy of WS2. Our findings reveal that the anisotropic optical response of WS2, influenced by the crystallographically low symmetry and unique dielectric environment of ReS2, significantly impacts both the optical and temporal behavior of WS2. We observed that the emission anisotropy increases with optical power density, highlighting that anisotropic localization of photo-generated carriers and subsequent charge transfer dynamics are key contributors to the polarization-sensitive optical response. These findings provide a framework for leveraging optical density-sensitive anisotropy mirroring to design advanced anisotropic optoelectronic and photonic devices.
more »
« less
- PAR ID:
- 10573370
- Publisher / Repository:
- De Gruyter
- Date Published:
- Journal Name:
- Nanophotonics
- ISSN:
- 2192-8606
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract The field of photovoltaics is revolutionized in recent years by the development of two–dimensional (2D) type‐II heterostructures. These heterostructures are made up of two different materials with different electronic properties, which allows for the capture of a broader spectrum of solar energy than traditional photovoltaic devices. In this study, the potential of vanadium (V)‐doped WS2is investigated, hereafter labeled V‐WS2, in combination with air‐stable Bi2O2Se for use in high‐performance photovoltaic devices. Various techniques are used to confirm the charge transfer of these heterostructures, including photoluminescence (PL) and Raman spectroscopy, along with Kelvin probe force microscopy (KPFM). The results show that the PL is quenched by 40%, 95%, and 97% for WS2/Bi2O2Se, 0.4 at.% V‐WS2/Bi2O2Se, and 2 at.% V‐WS2/Bi2O2Se, respectively, indicating a superior charge transfer in V‐WS2/Bi2O2Se compared to pristine WS2/Bi2O2Se. The exciton binding energies for WS2/Bi2O2Se, 0.4 at.% V‐WS2/Bi2O2Se and 2 at.% V‐WS2/Bi2O2Se heterostructures are estimated to be ≈130, 100, and 80 meV, respectively, which is much lower than that for monolayer WS2. These findings confirm that by incorporating V‐doped WS2, charge transfer in WS2/Bi2O2Se heterostructures can be tuned, providing a novel light‐harvesting technique for the development of the next generation of photovoltaic devices based on V‐doped transition metal dichalcogenides (TMDCs)/Bi2O2Se.more » « less
-
Van der Waals (vdW) materials have recently attracted significant interest in the context of orientation-dependent linear and nonlinear optical properties. Recently, arsenic trisulfide (As2S3) or orpiment is identified as a new vdW layered material having anisotropic vibrational and optomechanical responses due to the reduced in-plane crystal symmetry, but its nonlinear optical response is still not well understood yet. Herein, the anisotropic third-harmonic generation (THG) response of mechanically exfoliated As2S3thin flakes is reported. The polarization-dependent evolution of THG emission from butterfly-shaped pattern to four-lobe pattern is comprehensively explored. Moreover, the third-order nonlinear susceptibility of As2S3crystal is extracted by analyzing the thickness-dependent THG emission. We anticipate that the discussed results will not only update the existing understanding on the nonlinear light-matter interaction in anisotropic vdW materials, but also promote future applications in integrated photonic circuits, on-chip nonlinear signal processing, and polarization-sensitive optical devices.more » « less
-
Abstract NaCl has widely been used as a seeding promoter for chemical vapor deposition of large-scale 2D transition metal dichalcogenides. In this work, we report a study of the influence of NaCl on the growth and optical properties of layered CVD-grown WS2using steady-state and time-resolved Kerr rotation measurements at room temperature. Strong photoluminescence (PL) signals from single flakes grown with a low NaCl content indicates direct band-gap emission, whereas flakes grown with higher amounts of NaCl exhibit red-shifted, weaker PL. Raman measurements from single flakes also indicate that WS2grown with higher NaCl amounts result in multilayered structures, while lower NaCl quantities yield monolayer WS2. Ultrafast carrier decay measurements from single flakes also indicate a NaCl-dependent on the valley exchange interaction component (<10 ps) and slower decay components (>50 ps), attributed to a combination of phenomena, such as the band gap transitioning from direct to indirect and defect-related localized states. Our study provides insight into the influence of seeding promoters in layered CVD-grown WS2in particular and 2D transition metal dichalcogenides in general.more » « less
-
Abstract 2D dilute magnetic semiconductors have been recently reported in transition metal dichalcogenides doped with spin‐polarized transition metal atoms, for example vanadium‐doped WS2monolayers, which exhibit room‐temperature ferromagnetic ordering. However, a broadband characterization of the electronic band structure of these doped WS2monolayers and its dependence on vanadium concentration is still lacking. Therefore, power‐dependent photoluminescence, resonant four‐wave mixing, and differential reflectance spectroscopies are performed here to study optical transitions close to the A exciton energy of vanadium‐doped WS2monolayers at three different doping levels. Instead of a single A exciton peak, vanadium‐doped samples exhibit two photoluminescence peaks associated with transitions from a donor‐like level and the conduction band minima. Moreover, resonant Raman and second‐harmonic generation experiments reveal a blueshift in the B exciton energy but no energy change in the C exciton after vanadium doping. Density functional theory calculations show that the band structure is sensitive to the HubbardUcorrection for vanadium, and several scenarios are proposed to explain the two photoluminescence peaks around the A exciton energy region. This work provides the first broadband optical characterization of these 2D dilute magnetic semiconductors, shedding light on the novel and tunable electronic features of V‐doped WS2 monolayers.more » « less
