skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Charge density wave activated excitons in TiSe2–MoSe2 heterostructures
Layered materials enable the assembly of a new class of heterostructures where lattice-matching is no longer a requirement. Interfaces in these heterostructures therefore become a fertile ground for unexplored physics as dissimilar phenomena can be coupled via proximity effects. In this article, we identify an unexpected photoluminescence (PL) peak when MoSe2 interacts with TiSe2. A series of temperature-dependent and spatially resolved PL measurements reveal that this peak is unique to the TiSe2–MoSe2 interface, is higher in energy compared to the neutral exciton, and exhibits exciton-like characteristics. The feature disappears at the TiSe2 charge density wave transition, suggesting that the density wave plays an important role in the formation of this new exciton. We present several plausible scenarios regarding the origin of this peak that individually capture some aspects of our observations but cannot fully explain this feature. These results therefore represent a fresh challenge for the theoretical community and provide a fascinating way to engineer excitons through interactions with charge density waves.  more » « less
Award ID(s):
1847782
PAR ID:
10595053
Author(s) / Creator(s):
; ; ; ; ; ; ; ;
Publisher / Repository:
American Institute of Physics
Date Published:
Journal Name:
APL Materials
Volume:
10
Issue:
1
ISSN:
2166-532X
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. 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
  2. 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
  3. Abstract Coupled two-dimensional electron-hole bilayers provide a unique platform to study strongly correlated Bose-Fermi mixtures in condensed matter. Electrons and holes in spatially separated layers can bind to form interlayer excitons, composite Bosons expected to support high-temperature exciton condensates. The interlayer excitons can also interact strongly with excess charge carriers when electron and hole densities are unequal. Here, we use optical spectroscopy to quantitatively probe the local thermodynamic properties of strongly correlated electron-hole fluids in MoSe2/hBN/WSe2heterostructures. We observe a discontinuity in the electron and hole chemical potentials at matched electron and hole densities, a definitive signature of an excitonic insulator ground state. The excitonic insulator is stable up to a Mott density of ~0.8 × 1012cm−2and has a thermal ionization temperature of ~70 K. The density dependence of the electron, hole, and exciton chemical potentials reveals strong correlation effects across the phase diagram. Compared with a non-interacting uniform charge distribution, the correlation effects lead to significant attractive exciton-exciton and exciton-charge interactions in the electron-hole fluid. Our work highlights the unique quantum behavior that can emerge in strongly correlated electron-hole systems. 
    more » « less
  4. We investigated the pressure-dependent exciton absorption and photoluminescence (PL) properties of colloidal InAs/ZnSe core/shell quantum dots (QDs) emitting near-infrared (NIR) photons, an environmentally friendly alternative to heavy-metal-containing NIR QDs. A detailed analysis of exciton absorption and emission spectra was conducted in the pressure range of 0–10 GPa, focusing on the energy shifts, PL intensity, and lineshape changes with pressure. The pressure coefficients for exciton absorption and PL peaks were ∼70% of the bulk InAs value, with enhanced bandgap nonlinearity tentatively attributed to the higher bulk modulus of QDs compared to bulk material. The pressure-induced shifts in exciton absorption and PL peaks were reversible upon compression and decompression, with no indication of the semiconductor-to-metallic phase transition observed in bulk InAs around 7 GPa. However, PL intensity exhibited partial irreversibility, suggesting defect formation at the core/shell interface under pressure. From the findings of this study, along with previous high-pressure studies on molecular beam epitaxy-grown InAs QDs on GaAs, we infer the importance of the shell in determining the pressure response of exciton absorption and PL in core/shell QD structures with non-negligible interfacial strain and wave function spill into the shell. 
    more » « less
  5. Transition metal dichalcogenides (TMDCs) have garnered considerable interest over the past decade as a class of semiconducting layered materials. Most studies on the carrier dynamics in these materials have focused on the monolayer due to its direct bandgap, strong photoluminescence, and strongly bound excitons. However, a comparative understanding of the carrier dynamics in multilayer (e.g., >10 layers) flakes is still absent. Recent computational studies have suggested that excitons in bulk TMDCs are confined to individual layers, leading to room-temperature stable exciton populations. Using this new context, we explore the carrier dynamics in MoSe2 flakes that are between ∼16 and ∼125 layers thick. We assign the kinetics to exciton–exciton annihilation (EEA) and Shockley–Read–Hall recombination of free carriers. Interestingly, the average observed EEA rate constant (0.003 cm2/s) is nearly independent of flake thickness and 2 orders of magnitude smaller than that of an unencapsulated monolayer (0.33 cm2/s) but very similar to values observed in encapsulated monolayers. Thus, we posit that strong intralayer interactions minimize the effect of layer thickness on recombination dynamics, causing the multilayer to behave like the monolayer and exhibit an apparent EEA rate intrinsic to MoSe2. 
    more » « less