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Marc Currie

Publications and source records attributed to Marc Currie.

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Effects of altermagnetic order, strain and doping in RuO$_2$

RuO$_2$, one of the most widely studied transition metal oxides, was recently predicted to host a novel form of collinear magnetic order referred to as altermagnetism. In this study we combine experiment (reflectance, transmittance, ellipsometry and Raman measurements) and first-principles calculations to elucidate the potential role of altermagnetic order, strain and doping on the optical and vibrational properties of RuO$_2$ grown on TiO$_2$ (001), (101) and (110) substrates. Our combined experimental and theoretical results point toward a nonmagnetic ground state as the most consistent description of the optical and vibrational properties of bulk RuO$_2$. RuO$_2$ strained to TiO$_2$ (001) remains nonmagnetic in our calculations. Straining to TiO$_2$ (110) stabilizes ferromagnetic and altermagnetic states that are nearly degenerate and both lower in energy than the nonmagnetic state. The relative energetic ordering of these states is highly sensitive to the level of strain and the choice of exchange-correlation approximation.

cond-mat.mtrl-sci

Measurement of the Crystallization and Phase Transition of Niobium Dioxide Thin-Films for Neuromorphic Computing Applications Using a Tube Furnace Optical Transmission System

Significant research has focused on low-power stochastic devices built from memristive materials. These devices foster neuromorphic approaches to computational efficiency enhancement in merged biomimetic and CMOS architectures due to their ability to phase transition from a dielectric to a metal at an increased temperature. Niobium dioxide has a volatile memristive phase change that occurs $\sim$800$^\circ$C~that makes it an ideal candidate for future neuromorphic electronics. A straightforward optical system has been developed on a horizontal tube furnace for \emph{in situ} spectral measurements as an as-grown \NbtOf\ film is annealed and ultimately crystallizes as \NbOt. The system measures the changing spectral transmissivity of \NbtOf\ as it undergoes both reduction and crystallization processes. We were also able to measure the transition from metallic-to-non-metallic \NbOt\ during the cooldown phase, which is shown to occur about 100$^\circ$C~ lower on a sapphire substrate than fused silica. After annealing, the material properties of the \NbtOf\ and \NbOt\ were assessed via X-ray photoelectron spectroscopy, X-ray diffraction, and 4-point resistivity, confirming that we have made crystalline \NbOt.

physics.app-ph

Increasing the Rate of Magnesium Intercalation Underneath Epitaxial Graphene on 6H-SiC(0001)

Magnesium intercalated 'quasi-freestanding' bilayer graphene on 6H-SiC(0001) (Mg-QFSBLG) has many favorable properties (e.g., highly n-type doped, relatively stable in ambient conditions). However, intercalation of Mg underneath monolayer graphene is challenging, requiring multiple intercalation steps. Here, we overcome these challenges and subsequently increase the rate of Mg intercalation by laser patterning (ablating) the graphene to form micron-sized discontinuities. We then use low energy electron diffraction to verify Mg-intercalation and conversion to Mg-QFSBLG, and X-ray photoelectron spectroscopy to determine the Mg intercalation rate for patterned and non-patterned samples. By modeling Mg intercalation with the Verhulst equation, we find that the intercalation rate increase for the patterned sample is 4.5$\pm$1.7. Since the edge length of the patterned sample is $\approx$5.2 times that of the non-patterned sample, the model implies that the increased intercalation rate is proportional to the increase in edge length. Moreover, Mg intercalation likely begins at graphene discontinuities in pristine samples (not step edges or flat terraces), where the 2D-like crystal growth of Mg-silicide proceeds. Our laser patterning technique may enable the rapid intercalation of other atomic or molecular species, thereby expanding upon the library of intercalants used to modify the characteristics of graphene, or other 2D materials and heterostructures.

cond-mat.mtrl-sci

Freestanding n-Doped Graphene via Intercalation of Calcium and Magnesium into the Buffer Layer - SiC(0001) Interface

The intercalation of epitaxial graphene on SiC(0001) with Ca has been studied extensively, yet precisely where the Ca resides remains elusive. Furthermore, the intercalation of Mg underneath epitaxial graphene on SiC(0001) has not been reported. Here, we use low energy electron diffraction, x-ray photoelectron spectroscopy, secondary electron cut-off photoemission and scanning tunneling microscopy to elucidate the physical and electronic structure of both Ca- and Mg-intercalated epitaxial graphene on 6H-SiC(0001). We find that Ca intercalates underneath the buffer layer and bonds to the Si-terminated SiC surface, breaking the C-Si bonds of the buffer layer i.e. 'freestanding' the buffer layer to form Ca-intercalated quasi-freestanding bilayer graphene (Ca-QFSBLG). The situation is similar for the Mg-intercalation of epitaxial graphene on SiC(0001), where an ordered Mg-terminated reconstruction at the SiC surface and Mg bonds to the Si-terminated SiC surface are formed, resulting in Mg-intercalated quasi-freestanding bilayer graphene (Mg-QFSBLG). Ca-intercalation underneath the buffer layer has not been considered in previous studies of Ca-intercalated epitaxial graphene. Furthermore, we find no evidence that either Ca or Mg intercalates between graphene layers. However, we do find that both Ca-QFSBLG and Mg-QFSBLG exhibit very low workfunctions of 3.68 and 3.78 eV, respectively, indicating high n-type doping. Upon exposure to ambient conditions, we find Ca-QFSBLG degrades rapidly, whereas Mg-QFSBLG remains remarkably stable.

cond-mat.mtrl-sci

Oxidation of Monolayer WS$_{2}$ in Ambient is a Photoinduced Process

We have studied the ambient air oxidation of chemical vapor deposition (CVD) grown monolayers of the semiconducting transition metal dichalcogenide (S-TMD) WS$_{2}$ using optical microscopy, laser scanning confocal microscopy (LSCM), photoluminescence (PL) spectroscopy, and atomic force microscopy (AFM). Monolayer WS$_{2}$ exposed to ambient conditions in the presence of light (typical laboratory ambient light for weeks, or typical PL spectroscopy map), exhibits damage due to oxidation which can be detected with the LSCM and AFM; though may not be evident in conventional optical microscopy due to poorer contrast and resolution. Additionally, this oxidation was not random, and correlated with 'high-symmetry' and red-shifted areas in the PL spectroscopy map - areas thought to contain a higher concentration of sulfur vacancies. In contrast, samples kept in ambient and darkness showed no signs of oxidation for up to 10 months. Low-irradiance/fluence experiments showed that samples subjected to excitation energies at or above the trion excitation energy (532 nm/2.33 eV and 660 nm/1.88 eV) oxidized in as little as 7 days, even for irradiances and fluences eight and four orders of magnitude lower (respectively) than previously reported. No significant oxidation was observed for 760 nm/1.63 eV light exposure, which lies below the trion excitation energy in WS$_{2}$. The strong wavelength dependence and apparent lack of irradiance dependence suggests that ambient oxidation of WS$_{2}$ is initiated by photon-mediated electronic band transitions, that is, photo-oxidation. These findings have important implications for prior, present and future studies concerning S-TMDs measured, stored or manipulated in ambient conditions.

physics.app-ph

Understanding Variations in Circularly Polarized Photoluminescence in Monolayer Transition Metal Dichalcogenides

Monolayer transition metal dichalcogenides are promising materials for valleytronic operations. They exhibit two inequivalent valleys in the Brillouin zone, and the valley populations can be directly controlled and determined using circularly polarized optical excitation and emission. The photoluminescence polarization reflects the ratio of the two valley populations. A wide range of values for the degree of circularly polarized emission, Pcirc, has been reported for monolayer WS2, although the reasons for the disparity are unclear. Here we optically populate one valley, and measure Pcirc to explore the valley population dynamics at room temperature in a large number of monolayer WS2 samples synthesized via chemical vapor deposition. Under resonant excitation, Pcirc ranges from 2% to 32%, and we observe a pronounced inverse relationship between photoluminescence (PL) intensity and Pcirc. High quality samples exhibiting strong PL and long exciton relaxation time exhibit a low degree of valley polarization, and vice versa. This behavior is also demonstrated in monolayer WSe2 samples and transferred WS2, indicating that this correlation may be more generally observed and account for the wide variations reported for Pcirc. Time resolved PL provides insight into the role of radiative and non-radiative contributions to the observed polarization. Short non-radiative lifetimes result in a higher measured polarization by limiting opportunity for depolarizing scattering events.

cond-mat.mes-hall

Optical polarization and intervalley scattering in single layers of MoS2 and MoSe2

Single layers of MoS2 and MoSe2 were optically pumped with circularly polarized light and an appreciable polarization was initialized as the pump energy was varied. The circular polarization of the emitted photoluminescence was monitored as function of the difference between the excitation energy and the A-exciton emission at the K-point of the Brillouin zone. Our results show a threshold of twice the LA phonon energy, specific to the material, above which phonon-assisted intervalley scattering causes depolarization. In both materials this lead to almost complete depolarization within ~100 meV above the threshold energy. We identify the extra kinetic energy of the exciton (independent of whether it is neutral or charged) as the key parameter for presenting a unifying picture of the depolarization process.

cond-mat.mtrl-sci

Anomalous temperature-dependent spin-valley polarization in monolayer WS$_{2}$

Single layers of transition metal dichalcogenides (TMDs) are direct gap semiconductors with nondegenerate valley indices. An intriguing possibility for these materials is the use of their valley index as an alternate state variable. Several limitations to such a utility include strong, phonon-enabled intervalley scattering, as well as multiparticle interactions leading to multiple emission channels. We prepare single-layer WS$_{2}$ such that the photoluminescence is from either the neutral or charged exciton (trion). After excitation with circularly polarized light, the neutral exciton emission has zero polarization, however, the trion emission has a large polarization (28%) at room temperature. The trion emission also has a unique, non-monotonic temperature dependence that we show is a consequence of the multiparticle nature of the trion. This temperature dependence enables us to determine that coulomb assisted intervalley scattering, electron-hole radiative recombination, and a 3-particle Auger process are the dominant mechanisms at work in this system. Because this dependence involves trion systems, one can use gate voltages to modulate the polarization (or intensity) emitted from TMD structures.

cond-mat.mtrl-sci