arXiv subjects

D. Rhodes

Publications and source records attributed to D. Rhodes.

32 records · Page 2Linked to original sources

arXiv2018

Hundredfold Enhancement of Light Emission via Defect Control in Monolayer Transition-Metal Dichalcogenides

Two dimensional (2D) transition-metal dichalcogenide (TMD) based semiconductors have generated intense recent interest due to their novel optical and electronic properties, and potential for applications. In this work, we characterize the atomic and electronic nature of intrinsic point defects found in single crystals of these materials synthesized by two different methods - chemical vapor transport and self-flux growth. Using a combination of scanning tunneling microscopy (STM) and scanning transmission electron microscopy (STEM), we show that the two major intrinsic defects in these materials are metal vacancies and chalcogen antisites. We show that by control of the synthetic conditions, we can reduce the defect concentration from above $10^{13} /cm^2$ to below $10^{11} /cm^2$. Because these point defects act as centers for non-radiative recombination of excitons, this improvement in material quality leads to a hundred-fold increase in the radiative recombination efficiency.

cond-mat.mtrl-sci↗

arXiv2018

Detailed study on the Fermi surfaces of the type-II Dirac semimetallic candidates PdTe2 and PtTe2

We present a detailed quantum oscillatory study on the Dirac type-II semimetallic candidates PdTe$_{2}$ and PtTe$_{2}$ \emph{via} the temperature and the angular dependence of the de Haas-van Alphen (dHvA) and Shubnikov-de Haas (SdH) effects. In high quality single crystals of both compounds, i.e. displaying carrier mobilities between $10^3$ and $10^4$ cm$^2$/Vs, we observed a large non-saturating magnetoresistivity (MR) which in PtTe$_2$ at a temperature $T = 1.3$ K, leads to an increase in the resistivity up to $5 \times 10^{4}$ % under a magnetic field $μ_0 H = 62$ T. These high mobilities correlate with their light effective masses in the range of 0.04 to 1 bare electron mass according to our measurements. For PdTe$_{2}$ the experimentally determined Fermi surface cross-sectional areas show an excellent agreement with those resulting from band-structure calculations. Surprisingly, this is not the case for PtTe$_{2}$ whose agreement between calculations and experiments is relatively poor even when electronic correlations are included in the calculations. Therefore, our study provides a strong support for the existence of a Dirac type-II node in PdTe$_2$ and probably also for PtTe$_2$. Band structure calculations indicate that the topologically non-trivial bands of PtTe$_2$ do not cross the Fermi-level ($\varepsilon_F$). In contrast, for PdTe$_2$ the Dirac type-II cone does intersect $\varepsilon_F$, although our calculations also indicate that the associated cyclotron orbit on the Fermi surface is located in a distinct $k_z$ plane with respect to the one of the Dirac type-II node. Therefore it should yield a trivial Berry-phase.

cond-mat.str-el↗

arXiv2017

Bulk Fermi-surface of the Weyl type-II semi-metallic candidate MoTe2

The electronic structure of WTe$_2$ and orthorhombic $γ-$MoTe$_2$, are claimed to contain pairs of Weyl type-II points. A series of ARPES experiments claim a broad agreement with these predictions. We synthesized single-crystals of MoTe$_2$ through a Te flux method to validate these predictions through measurements of its bulk Fermi surface (FS) \emph{via} quantum oscillatory phenomena. We find that the superconducting transition temperature of $γ-$MoTe$_2$ depends on disorder as quantified by the ratio between the room- and low-temperature resistivities, suggesting the possibility of an unconventional superconducting pairing symmetry. Similarly to WTe$_2$, the magnetoresistivity of $γ-$MoTe$_2$ does not saturate at high magnetic fields and can easily surpass $10^{6}$ \%. Remarkably, the analysis of the de Haas-van Alphen (dHvA) signal superimposed onto the magnetic torque, indicates that the geometry of its FS is markedly distinct from the calculated one. The dHvA signal also reveals that the FS is affected by the Zeeman-effect precluding the extraction of the Berry-phase. A direct comparison between the previous ARPES studies and density-functional-theory (DFT) calculations reveals a disagreement in the position of the valence bands relative to the Fermi level $\varepsilon_F$. Here, we show that a shift of the DFT valence bands relative to $\varepsilon_F$, in order to match the ARPES observations, and of the DFT electron bands to explain some of the observed dHvA frequencies, leads to a good agreement between the calculations and the angular dependence of the FS cross-sectional areas observed experimentally. However, this relative displacement between electron- and hole-bands eliminates their crossings and, therefore, the Weyl type-II points predicted for $γ-$MoTe$_2$.

cond-mat.mes-hall↗

arXiv2016

Engineering the structural and electronic phases of MoTe2 through W substitution

MoTe$_2$ is an exfoliable transition metal dichalcogenide (TMD) which crystallizes in three symmetries, the semiconducting trigonal-prismatic $2H-$phase, the semimetallic $1T^{\prime}$ monoclinic phase, and the semimetallic orthorhombic $T_d$ structure. The $2H-$phase displays a band gap of $\sim 1$ eV making it appealing for flexible and transparent optoelectronics. The $T_d-$phase is predicted to possess unique topological properties which might lead to topologically protected non-dissipative transport channels. Recently, it was argued that it is possible to locally induce phase-transformations in TMDs, through chemical doping, local heating, or electric-field to achieve ohmic contacts or to induce useful functionalities such as electronic phase-change memory elements. The combination of semiconducting and topological elements based upon the same compound, might produce a new generation of high performance, low dissipation optoelectronic elements. Here, we show that it is possible to engineer the phases of MoTe$_2$ through W substitution by unveiling the phase-diagram of the Mo$_{1-x}$W$_x$Te$_2$ solid solution which displays a semiconducting to semimetallic transition as a function of $x$. We find that only $\sim 8$ \% of W stabilizes the $T_d-$phase at room temperature. Photoemission spectroscopy, indicates that this phase possesses a Fermi surface akin to that of WTe$_2$.

cond-mat.mes-hall↗

arXiv2016

Hall-effect within the colossal magnetoresistive semi-metallic state of MoTe2

Here, we report a systematic study on the Hall-effect of the semi-metallic state of bulk MoTe$_2$, which was recently claimed to be a candidate for a novel type of Weyl semi-metallic state. The temperature ($T$) dependence of the carrier densities and of their mobilities, as estimated from a numerical analysis based on the isotropic two-carrier model, indicates that its exceedingly large and non-saturating magnetoresistance may be attributed to a near perfect compensation between the densities of electrons and holes at low temperatures. A sudden increase in hole density, with a concomitant rapid increase in the electron mobility below $T \sim 40$ K, leads to comparable densities of electrons and holes at low temperatures suggesting a possible electronic phase-transition around this temperature.

cond-mat.supr-con↗

arXiv2016

Two-dimensional superconductivity in a bulk single-crystal

Both Nb$_3$Pd$_x$Se$_7$ and Ta$_4$Pd$_3$Te$_{16}$ crystallize in a monoclinic point group while exhibiting superconducting transition temperatures as high as $T_c\sim 3.5$ and $\sim 4.7 $ K, respectively. Disorder was claimed to lead to the extremely large upper critical fields ($H_{c2}$) observed in related compounds. Despite the presence of disorder and heavier elements, $H_{c2}$s in Ta$_4$Pd$_3$Te$_{16}$ are found to be considerably smaller than those of Nb$_3$Pd$_x$Se$_7$ while displaying an anomalous, non-saturating linear dependence on temperature $T$ for fields along all three crystallographic axes. In contrast, crystals of the latter compound displaying the highest $T_c$s display $H_{c2}\propto (1-T/T_c)^{1/2}$, which in monolayers of transition metal dichalcogenides is claimed to be evidence for an Ising paired superconducting state resulting from strong spin-orbit coupling. This anomalous $T$-dependence indicates that the superconducting state of Nb$_3$Pd$_x$Se$_7$ is quasi-two-dimensional in nature. This is further supported by a nearly divergent anisotropy in upper-critical fields, i.e. $γ= H_{c2}^{b}/H_{c2}^{a^{\prime}}$, upon approaching $T_c$. Hence, in Nb$_3$Pd$_x$Se$_7$ the increase of $T_c$ correlates with a marked reduction in electronic dimensionality as observed, for example, in intercalated FeSe. For the Nb compound, Density functional theory (DFT) calculations indicate that an increase in the external field produces an anisotropic orbital response, with especially strong polarization at the Pd sites when the field is perpendicular to their square planar environment. Therefore, DFT suggests the field-induced pinning of the spin to the lattice as a possible mechanism for decoupling the superconducting planes. Overall, our observations represent further evidence for unconventional superconductivity in the Pd chalcogenides.

cond-mat.supr-con↗

arXiv2016

Uncovering the behavior of Hf2Te2P and the candidate Dirac metal Zr2Te2P

Results are reported for single crystal specimens of Hf$_2$Te$_2$P and compared to its structural analogue Zr$_2$Te$_2$P, which was recently proposed to be a potential reservoir for Dirac physics.[1] Both materials are produced using the iodine vapor transport method and the resulting crystals are exfoliable. The bulk electrical transport and thermodynamic properties indicate Fermi liquid behavior at low temperature for both compounds. Quantum oscillations are observed in magnetization measurements for fields applied parallel but not perpendicular to the $c$-axis, suggesting that the Fermi surfaces are quasi-two dimensional. Frequencies are determined from quantum oscillations for several parts of the Fermi surfaces. Lifshitz-Kosevich fits to the temperature dependent amplitudes of the oscillations reveal small effective masses, with a particularly small value $m^*$ $=$ 0.046$m_0$ for the α branch of Zr$_2$Te$_2$P. Electronic structure calculations are in good agreement with quantum oscillation results and illustrate the effect of a stronger spin-orbit interaction going from Zr to Hf. These results suggest that by using appropriate tuning parameters this class of materials may deepen the pool of novel Dirac phenomena.

cond-mat.mtrl-sci↗

arXiv2015

Role of spin-orbit coupling and evolution of the electronic structure of WTe$_2$ under an external magnetic field

Here, we present a detailed study on the temperature and angular dependence of the Shubnikov-de-Haas (SdH) effect in the semi-metal WTe$_2$. This compound was recently shown to display a very large non-saturating magnetoresistance which was attributed to nearly perfectly compensated densities of electrons and holes. We observe four fundamental SdH frequencies and attribute them to spin-orbit split, electron- and hole-like, Fermi surface (FS) cross-sectional areas. Their angular dependence seems consistent with ellipsoidal FSs with volumes suggesting a modest excess in the density of electrons with respect to that of the holes. We show that density functional theory (DFT) calculations fail to correctly describe the FSs of WTe$_2$. When their cross-sectional areas are adjusted to reflect the experimental data, the resulting volumes of the electron/hole FSs obtained from the DFT calculations would imply a pronounced imbalance between the densities of electrons and holes. We find evidence for field-dependent Fermi surface cross-sectional areas by fitting the oscillatory component superimposed onto the magnetoresistivity signal to several Lifshitz-Kosevich components. We also observe a pronounced field-induced renormalization of the effective masses. Taken together, our observations suggest that the electronic structure of WTe$_2$ evolves with the magnetic field. This evolution might be a factor contributing to its pronounced magnetoresistivity.

cond-mat.mtrl-sci↗

arXiv2015

Hall and field-effect mobilities in few layered $p$-WSe$_2$ field-effect transistors

Here, we present a temperature ($T$) dependent comparison between field-effect and Hall mobilities in field-effect transistors based on few-layered WSe$_2$ exfoliated onto SiO$_2$. Without dielectric engineering and beyond a $T$-dependent threshold gate-voltage, we observe maximum hole mobilities approaching 350 cm$^2$/Vs at $T$=300 K. The hole Hall mobility reaches a maximum value of 650 cm$^2$/Vs as $T$ is lowered below $\sim$ 150 K, indicating that insofar WSe$_2$-based field-effect transistors (FETs) display the largest Hall mobilities among the transition metal dichalcogenides. The gate capacitance, as extracted from the Hall-effect, reveals the presence of spurious charges in the channel, while the two-terminal sheet resistivity displays two-dimensional variable-range hopping behavior, indicating carrier localization induced by disorder at the interface between WSe$_2$ and SiO$_2$. We argue that improvements in the fabrication protocols as, for example, the use of a substrate free of dangling bonds are likely to produce WSe$_2$-based FETs displaying higher room temperature mobilities, i.e. approaching those of $p$-doped Si, which would make it a suitable candidate for high performance opto-electronics.

cond-mat.mes-hall↗

arXiv2014

CeCu_2Ge_2: Challenging our Understanding of Quantum Criticality

Here, we unveil evidence for a quantum phase-transition in CeCu_2Ge_2 which displays both an incommensurate spin-density wave (SDW) ground-state, and a strong renormalization of the quasiparticle effective masses (mu) due to the Kondo-effect. For all angles theta between an external magnetic field (H) and the crystallographic c-axis, the application of H leads to the suppression of the SDW-state through a 2^nd-order phase-transition at a theta-dependent critical-field H_p(theta) leading to the observation of small Fermi surfaces (FSs) in the paramagnetic (PM) state. For H || c-axis, these FSs are characterized by light mu's pointing also to the suppression of the Kondo-effect at H_p with surprisingly, no experimental evidence for quantum-criticality (QC). But as $H$ is rotated towards the a-axis, these mu's increase considerably becoming undetectable for θ> 56^0 between H and the c-axis. Around H_p^a~ 30 T the resistivity becomes proportional T which, coupled to the divergence of mu, indicates the existence of a field-induced QC-point at H_p^a(T=0 K). This observation, suggesting FS hot-spots associated with the SDW nesting-vector, is at odds with current QC scenarios for which the continuous suppression of all relevant energy scales at H_p(theta,T) should lead to a line of quantum-critical points in the H-theta plane. Finally, we show that the complexity of its magnetic phase-diagram(s) makes CeCu_2Ge_2 an ideal system to explore field-induced quantum tricritical and QC end-points.

cond-mat.str-el↗

arXiv2013

Bulk evidence for a time reversal symmetry broken superconducting state in URu2Si2

URu$_2$Si$_2$ is claimed to be a chiral \emph{d}-wave superconductor with a $k_z (k_x \pm ik_y)$ time-reversal symmetry broken orbital component for the Cooper pair wave-function, which contains both nodal points and lines of nodes \cite{kasahara, kasahara2}. To study the magnetic response of such an unconventional state through a bulk, thermodynamic probe, we measured the magnetic torque $τ$ in very high-quality, well-characterized URu$_2$Si$_2$ single-crystals \cite{altarawneh,altarawneh2} at high magnetic-fields $H$ and at very low temperatures $T$. The magnetization $M(H) \propto τ(H) /H$ of URu$_2$Si$_2$, in its superconducting state and for angles within $15^{\circ}$ from the \emph{ab}-plane, reveals a change in its sign for $H$ approaching $H_{c2}$: from a clear diamagnetic response dominated by the pinning of vortices to a state with a smaller but "paramagnetic-like" hysteretic response which \emph{disappears} at $H_{c2}$, thus implying that it is intrinsically related to the superconducting state. We argue that this anomalous, angular-dependent behavior is evidence for a time-reversal symmetry broken superconducting state in URu$_2$Si$_2$, although not necessarily for the $k_z (k_x \pm ik_y)$ state.

cond-mat.supr-con↗

arXiv2013

Anomalous metallic state and anisotropic multiband superconductivity in Nb3Pd0.7Se7

We report the discovery of superconductivity in Nb$_3$Pd$_{x}$Se$_7$ with a $x$-dependent superconducting transition-temperature as high as $T_c \simeq 2.1 $ K for $x \simeq0.7$ (middle point of the resistive transition). Needle-like single crystals display anisotropic upper-critical fields with an anisotropy $γ= H^{b}_{c2}/H^{a}_{c2}$ as large as 6 between fields applied along their needle axis (or $b-$axis) or along the $a-$axis. As for the Fe based superconductors $γ$ is temperature-dependent suggesting that Nb$_3$Pd$_{0.7}$Se$_7$ is a multi-band superconductor. This is supported by band structure calculations which reveal a Fermi surface composed of quasi-one-dimensional and quasi-two-dimensional sheets of hole character, as well as three-dimensional sheets of both hole- and electron-character. Remarkably, $H^{b}_{c2}$ is observed to saturate at $H^{b}_{c2}(T \rightarrow 0 \text{K}) \simeq 14.1$ T which is $4.26 \times H_p$ where $H_p$ is the Pauli-limiting field in the weak-coupling regime. The synthesis procedure yields additional crystals belonging to the Nb$_2$Pd$_{x}$Se$_5$ phase which also becomes superconducting when the fraction of Pd is varied. For both phases we find that superconductivity condenses out of an anomalous metallic state, i.e. displaying $\partial ρ/ \partial T < 0$ above $T_c$ similarly to what is observed in the pseudogap-phase of the underdoped cuprates. An anomalous metallic state, low-dimensionality, multi-band character, extremely high and anisotropic $H_{c2}$s, are all ingredients for unconventional superconductivity.

cond-mat.supr-con↗

arXiv2013

Intrinsic carrier mobility of multi-layered MoS$_2$ field-effect transistors on SiO$_2$

By fabricating and characterizing multi-layered MoS$_2$-based field-effect transistors (FETs) in a four terminal configuration, we demonstrate that the two terminal-configurations tend to underestimate the carrier mobility $μ$ due to the Schottky barriers at the contacts. For a back-gated two-terminal configuration we observe mobilities as high as 125 cm$^2$V$^{-1}$s$^{-1}$ which is considerably smaller than 306.5 cm$^2$V$^{-1}$s$^{-1}$ as extracted from the same device when using a four-terminal configuration. This indicates that the intrinsic mobility of MoS$_2$ on SiO$_2$ is significantly larger than the values previously reported, and provides a quantitative method to evaluate the charge transport through the contacts.

cond-mat.mes-hall↗

arXiv2013

Superconductivity with extremely large upper critical fields in Nb2Pd0.81S5

Here, we report the discovery of superconductivity in a new transition metal-chalcogenide compound, i.e. Nb2Pd0.81S5, with a transition temperature Tc > 6.6 K. Despite its relatively low Tc, it displays remarkably high and anisotropic superconducting upper critical fields, e.g. mu_0 H_{c2} (T approaching 0 K). 37 T for fields applied along the crystallographic b-axis. For a field applied perpendicularly to the b-axis, mu_0 H_{c2} shows a linear dependence in temperature which coupled to a temperature-dependent anisotropy of the upper critical fields, suggests that Nb2Pd0.81S5 is a multi-band superconductor. This is consistent with band structure calculations which reveal nearly cylindrical and quasi-one-dimensional Fermi surface sheets having hole and electron character, respectively. The static spin susceptibility as calculated through the random phase approximation, reveals strong peaks suggesting proximity to a magnetic state and therefore the possibility of unconventional superconductivity.

cond-mat.supr-con↗