SearcharxivSearch

arXiv subjects

Marcio D. Teodoro

Publications and source records attributed to Marcio D. Teodoro.

4 recordsLinked to original sources

Vanadium doping induced valley asymmetries in WS$_2$ monolayers

Transition metal dichalcogenide (TMD) monolayers offer an innovative platform for encoding and manipulating information through the valley degree of freedom. While unique valley-related physical phenomena have been reported so far, practical applications still require advanced control over the valley polarization efficiency and the valley Zeeman effect. Recently, the introduction of spin-polarized metal atoms as substitutional defects was reported to break the time-reversal symmetry in TMD monolayers, consequently inducing a room-temperature ferromagnetic ordering and enhancing the valley-dependent optical responses. Here, we report valley asymmetries for vanadium-doped WS$_2$ monolayers. With a given magnetic polarization, one valley exhibits larger Zeeman slope and degree of circular polarization than the other valley. Additionally, the overall degree of circular polarization in the doped samples is approximately twice that of the pristine WS$_2$ monolayer. Density functional theory calculations in the doped structure show that different energy shifts in conduction band edges due to spin-dependent hybridization lead to different exciton energies between valleys, which is consistent with the experimental observations. Our results pave the way for valleytronic technologies based on defect-engineered two-dimensional materials.

cond-mat.mes-hall

Anisotropic Dopant and Strain Architectures in WS$_2$ Nanocrystals Driven by Growth Kinetics

Dopant distribution in two-dimensional semiconductors is typically assumed to be stochastic, limiting deterministic defect engineering. Here, we show that non-equilibrium growth kinetics can be harnessed to define dopant-driven strain architectures in vanadium-doped WS$_2$ monolayers. Using synchrotron X-ray fluorescence, we identify preferential vanadium incorporation, anti-correlated with tungsten content, along crystallographic bisectors. An adsorption-growth-diffusion model with a single kinetic parameter quantitatively captures the dopant segregation arising from preferential corner adsorption and limited diffusion during chemical vapor deposition growth. Hyperspectral Raman imaging demonstrates mechanically induced vibrational responses, revealing localized tensile strain ($\varepsilon \approx0.70\%$) channels associated with the anisotropic dopant distribution. This regime is marked by the depletion of W-site-sensitive in-plane modes and the emergence of a localized $J2$ mode (210~cm$^{-1}$), which our ab-initio calculations attribute to antiphase V$-$V oscillations. These findings establish kinetic segregation as a route to deterministic chemical and strain architectures in 2D semiconductors, enabling programmable defect landscapes and strain engineering during synthesis.

cond-mat.mtrl-sci

Strong magneto-optical responses of an ensemble of defect-bound excitons in ambient exposed WS$_{2}$ and WSe$_{2}$ monolayers

Transition metal dichalcogenide (TMD) monolayers present a singular coupling in their spin and valley degrees of freedom. Moreover, by applying an external magnetic field it is possible to break the energy degeneracy between their K and $-$K valleys. This valley Zeeman effect opens the possibility of controlling and distinguishing the spin and valley characters of charge carriers in TMDs by their optical transition energies, making these materials promising for the next generation of spintronic and photonic devices. However, the free excitons of pristine TMD monolayers present a moderate valley Zeeman splitting of $\approx 0.23$ meV/T. Therefore, alternative excitonic states with higher magnetic responses are mandatory for application purposes. Here, we investigate the magneto-optical properties of ambient exposed WS$_2$ and WSe$_2$ monolayers by circularly polarized magneto-photoluminescence experiments at cryogenic temperatures. A broad lower energy photoluminescence emission related to an ensemble of defects is observed, presenting remarkable valley-related splittings of $\approx 1.45$ meV/T and $\approx 1.11$ meV/T for WS$_2$ and WSe$_2$ monolayers, respectively. In addition, we report a significant valley polarization of charge carriers in the defect mid-gap states induced by the external magnetic field. We explain this valley-polarized population and enhanced valley-related splitting in terms of imbalanced intervalley relaxations, leading to a magnetic field-dependent distribution of charge carriers in multiple defect levels. This effect, together with the individual Zeeman shiftings of the mid-gap states, explains the strong magneto-optical responses observed. Our work uncovers the singular potential of manipulating the light emission of ambient exposed TMD monolayers by an external magnetic field.

cond-mat.mes-hall

Optical memory in a MoSe$_2$/Clinochlore device

Two-dimensional heterostructures have been crucial in advancing optoelectronic devices utilizing van der Waals materials. Semiconducting transition metal dichalcogenide monolayers, known for their unique optical properties, offer extensive possibilities for light-emitting devices. Recently, a memory-driven optical device, termed a Mem-emitter, was proposed using these monolayers atop dielectric substrates. The successful realization of such devices heavily depends on selecting the optimal substrate. Here, we report a pronounced memory effect in a MoSe$_2$/clinochlore device, evidenced by electric hysteresis in the intensity and energy of MoSe$_2$ monolayer emissions. This demonstrates both population-driven and transition-rate-driven Mem-emitter abilities. Our theoretical approach correlates these memory effects with internal state variables of the substrate, emphasizing that clinochlore layered structure is crucial for a robust and rich memory response. This work introduces a novel two-dimensional device with promising applications in memory functionalities, highlighting the importance of alternative insulators in fabricating van der Waals heterostructures.

cond-mat.mtrl-sci