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Abstract The functionality of atomic quantum emitters is intrinsically linked to their host lattice coordination. Structural distortions that spontaneously break the lattice symmetry strongly impact their optical emission properties and spin-photon interface. Here we report on the direct imaging of charge state-dependent symmetry breaking of two prototypical atomic quantum emitters in mono- and bilayer MoS₂by scanning tunneling microscopy (STM) and non-contact atomic force microscopy (nc-AFM). By changing the built-in substrate chemical potential, different charge states of sulfur vacancies (Vac_S) and substitutional rhenium dopants (Re_Mo) can be stabilized.$${\mathrm{Vac}}_{{{{{{{{\rm{S}}}}}}}}}^{-1}$$ ${\mathrm{Vac}}_S^{-1}$as well as$${{\mathrm{Re}}}_{{{{{{{{\rm{Mo}}}}}}}}}^{0}$$ ${\mathrm{Re}}_{\mathrm{Mo}}^0$and$${\mathrm{Re}}_{{\rm{Mo}}}^{-1}$$ ${\mathrm{Re}}_{\mathrm{Mo}}^{-1}$exhibit local lattice distortions and symmetry-broken defect orbitals attributed to a Jahn-Teller effect (JTE) and pseudo-JTE, respectively. By mapping the electronic and geometric structure of single point defects, we disentangle the effects of spatial averaging, charge multistability, configurational dynamics, and external perturbations that often mask the presence of local symmetry breaking. 

Abstract Metamaterials and metasurfaces operating in the visible and near‐infrared (NIR) offer a promising route towards next‐generation photodetectors and devices for solar energy harvesting. While numerous metamaterials and metasurfaces using metals and semiconductors have been demonstrated, semimetals‐based metasurfaces in the vis‐NIR range are notably missing. This work experimentally demonstrates a broadband metasurface superabsorber based on large area, semimetallic, van der Waals platinum diselenide (PtSe₂) thin films in agreement with electromagnetic simulations. The results show that PtSe₂is an ultrathin and scalable semimetal that concurrently possesses high index and high extinction across the vis‐NIR range. Consequently, the thin‐film PtSe₂on a reflector separated by a dielectric spacer can absorb >85% for the unpatterned case and ≈97% for the optimized 2D metasurface in the 400–900 nm range making it one of the strongest and thinnest broadband perfect absorbers to date. The results present a scalable approach to photodetection and solar energy harvesting, demonstrating the practical utility of high index, high extinction semimetals for nanoscale optics. 

Abstract Scalable substitutional doping of 2D transition metal dichalcogenides is a prerequisite to developing next‐generation logic and memory devices based on 2D materials. To date, doping efforts are still nascent. Here, scalable growth and vanadium (V) doping of 2D WSe₂at front‐end‐of‐line and back‐end‐of‐line compatible temperatures of 800 and 400 °C, respectively, is reported. A combination of experimental and theoretical studies confirm that vanadium atoms substitutionally replace tungsten in WSe₂, which results inp‐type doping via the introduction of discrete defect levels that lie close to the valence band maxima. Thep‐type nature of the V dopants is further verified by constructed field‐effect transistors, where hole conduction becomes dominant with increasing vanadium concentration. Hence, this study presents a method to precisely control the density of intentionally introduced impurities, which is indispensable in the production of electronic‐grade wafer‐scale extrinsic 2D semiconductors. 

Abstract Reliable, controlled doping of 2D transition metal dichalcogenides will enable the realization of next‐generation electronic, logic‐memory, and magnetic devices based on these materials. However, to date, accurate control over dopant concentration and scalability of the process remains a challenge. Here, a systematic study of scalable in situ doping of fully coalesced 2D WSe₂films with Re atoms via metal–organic chemical vapor deposition is reported. Dopant concentrations are uniformly distributed over the substrate surface, with precisely controlled concentrations down to <0.001% Re achieved by tuning the precursor partial pressure. Moreover, the impact of doping on morphological, chemical, optical, and electronic properties of WSe₂is elucidated with detailed experimental and theoretical examinations, confirming that the substitutional doping of Re at the W site leads to n‐type behavior of WSe₂. Transport characteristics of fabricated back‐gated field‐effect‐transistors are directly correlated to the dopant concentration, with degrading device performances for doping concentrations exceeding 1% of Re. The study demonstrates a viable approach to introducing true dopant‐level impurities with high precision, which can be scaled up to batch production for applications beyond digital electronics. 

Abstract This work is a systematic experimental and theoretical study of the in‐plane dielectric functions of 2D gallium and indium films consisting of two or three atomic metal layers confined between silicon carbide and graphene with a corresponding bonding gradient from covalent to metallic to van der Waals type.k‐space resolved free electron and bound electron contributions to the optical response are identified, with the latter pointing towards the existence of thickness dependent quantum confinement phenomena. The resonance energies in the dielectric functions and the observed epsilon near‐zero behavior in the near infrared to visible spectral range, are dependent on the number of atomic metal layers and properties of the metal involved. A model‐based spectroscopic ellipsometry approach is used to estimate the number of atomic metal layers, providing a convenient route over expensive invasive characterization techniques. A strong thickness and metal choice dependence of the light–matter interaction makes these half van der Waals 2D polar metals attractive for quantum engineered metal films, tunable (quantum‐)plasmonics and nano‐photonics. 

Abstract Doping is a fundamental requirement for tuning and improving the properties of conventional semiconductors. Recent doping studies including niobium (Nb) doping of molybdenum disulfide (MoS₂) and tungsten (W) doping of molybdenum diselenide (MoSe₂) have suggested that substitutional doping may provide an efficient route to tune the doping type and suppress deep trap levels of 2D materials. To date, the impact of the doping on the structural, electronic, and photonic properties of in situ‐doped monolayers remains unanswered due to challenges including strong film substrate charge transfer, and difficulty achieving doping concentrations greater than 0.3 at%. Here, in situ rhenium (Re) doping of synthetic monolayer MoS₂with ≈1 at% Re is demonstrated. To limit substrate film charge transfer,r‐plane sapphire is used. Electronic measurements demonstrate that 1 at% Re doping achieves nearly degenerate n‐type doping, which agrees with density functional theory calculations. Moreover, low‐temperature photoluminescence indicates a significant quench of the defect‐bound emission when Re is introduced, which is attributed to the MoO bond and sulfur vacancies passivation and reduction in gap states due to the presence of Re. The work presented here demonstrates that Re doping of MoS₂is a promising route toward electronic and photonic engineering of 2D materials.