arXiv subjects

Jill A. Miwa

Publications and source records attributed to Jill A. Miwa.

50 records · Page 3Linked to original sources

arXiv2017

Quasi one-dimensional metallic band dispersion in the commensurate charge density wave of $1T$-TaS$_2$

The commensurate charge density wave (CDW) in the layered compound $1T$-TaS$_2$ has hitherto mostly been treated as a quasi two-dimensional phenomenon. Recent band structure calculations have, however, predicted that the CDW coexists with a nearly one-dimensional metallic dispersion perpendicular to the crystal planes. Using synchrotron radiation based angle-resolved photoemission spectroscopy, we show that this metallic band does in fact exist. Its occupied band width is in excellent agreement with predictions for a simple $τ_c$ stacking order of the CDW between adjacent layers and its periodicity in the $c$ direction is $2 π/ c$.

cond-mat.str-el↗

arXiv2016

Spin and Valley Control of Free Carriers in Single-Layer WS$_2$

The semiconducting single-layer transition metal dichalcogenides have been identified as ideal materials for accessing and manipulating spin- and valley-quantum numbers due to a set of favorable optical selection rules in these materials. Here, we apply time- and angle-resolved photoemission spectroscopy to directly probe optically excited free carriers in the electronic band structure of a high quality single layer of WS$_2$. We observe that the optically generated free hole density in a single valley can be increased by a factor of 2 using a circularly polarized optical excitation. Moreover, we find that by varying the photon energy of the excitation we can tune the free carrier density in a given spin-split state around the valence band maximum of the material. The control of the photon energy and polarization of the excitation thus permits us to selectively excite free electron-hole pairs with a given spin and within a single valley.

cond-mat.mes-hall↗

arXiv2016

Crystalline and electronic structure of single-layer TaS$_2$

Single-layer TaS$_2$ is epitaxially grown on Au(111) substrates. The resulting two-dimensional crystals adopt the 1H polymorph. The electronic structure is determined by angle-resolved photoemission spectroscopy and found to be in excellent agreement with density functional theory calculations. The single layer TaS$_2$ is found to be strongly n-doped, with a carrier concentration of 0.3(1) extra electrons per unit cell. No superconducting or charge density wave state is observed by scanning tunneling microscopy at temperatures down to 4.7 K.

cond-mat.str-el↗

arXiv2016

Ultrafast Band Structure Control of a Two-Dimensional Heterostructure

The electronic structure of two-dimensional (2D) semiconductors can be significantly altered by screening effects, either from free charge carriers in the material itself, or by environmental screening from the surrounding medium. The physical properties of 2D semiconductors placed in a heterostructure with other 2D materials are therefore governed by a complex interplay of both intra- and inter-layer interactions. Here, using time- and angle-resolved photoemission, we are able to isolate both the layer-resolved band structure and, more importantly, the transient band structure evolution of a model 2D heterostructure formed of a single layer of MoS$_2$ on graphene. Our results reveal a pronounced renormalization of the quasiparticle gap of the MoS$_2$ layer. Following optical excitation, the band gap is reduced by up to $\sim\!$400 meV on femtosecond timescales due to a persistence of strong electronic interactions despite the environmental screening by the $n$-doped graphene. This points to a large degree of tuneability of both the electronic structure and electron dynamics for 2D semiconductors embedded in a van der Waals-bonded heterostructure.

cond-mat.mtrl-sci↗

arXiv2016

Tunable Carrier Multiplication and Cooling in Graphene

Time- and angle-resolved photoemission measurements on two doped graphene samples displaying different doping levels reveal remarkable differences in the ultrafast dynamics of the hot carriers in the Dirac cone. In the more strongly ($n$-)doped graphene, we observe larger carrier multiplication factors ($>$ 3) and a significantly faster phonon-mediated cooling of the carriers back to equilibrium compared to in the less ($p$-)doped graphene. These results suggest that a careful tuning of the doping level allows for an effective manipulation of graphene's dynamical response to a photoexcitation.

cond-mat.mtrl-sci↗

arXiv2016

Single-layer MoS$_2$ on Au(111): band gap renormalization and substrate interaction

The electronic structure of epitaxial single-layer MoS$_2$ on Au(111) is investigated by angle-resolved photoemission spectroscopy, scanning tunnelling spectroscopy, and first principles calculations. While the band dispersion of the supported single-layer is close to a free-standing layer in the vicinity of the valence band maximum at $\bar{K}$ and the calculated electronic band gap on Au(111) is similar to that calculated for the free-standing layer, significant modifications to the band structure are observed at other points of the two-dimensional Brillouin zone: At $\barΓ$, the valence band maximum has a significantly higher binding energy than in the free MoS$_2$ layer and the expected spin-degeneracy of the uppermost valence band at the $\bar{M}$ point cannot be observed. These band structure changes are reproduced by the calculations and can be explained by the detailed interaction of the out-of-plane MoS$_2$ orbitals with the substrate.

cond-mat.str-el↗

arXiv2015

Synthesis of Epitaxial Single-Layer MoS$_2$ on Au(111)

We present a method for synthesizing large area epitaxial single-layer MoS$_2$ on the Au(111) surface in ultrahigh vacuum. Using scanning tunneling microscopy and low energy electron diffraction, the evolution of the growth is followed from nanoscale single-layer MoS$_2$ islands to a continuous MoS$_2$ layer. An exceptionally good control over the MoS$_2$ coverage is maintained using an approach based on cycles of Mo evaporation and sulfurization to first nucleate the MoS$_2$ nano-islands and then gradually increase their size. During this growth process the native herringbone reconstruction of Au(111) is lifted as shown by low energy electron diffraction measurements. Within these MoS$_2$ islands, we identify domains rotated by 60$^{\circ}$ that lead to atomically sharp line defects at domain boundaries. As the MoS$_2$ coverage approaches the limit of a complete single-layer, the formation of bilayer MoS$_2$ islands is initiated. Angle-resolved photoemission spectroscopy measurements of both single and bilayer MoS$_2$ samples show a dramatic change in their band structure around the center of the Brillouin zone. Brief exposure to air after removing the MoS$_2$ layer from vacuum is not found to affect its quality.

cond-mat.mtrl-sci↗

arXiv2015

Growth and electronic structure of epitaxial single-layer WS$_2$ on Au(111)

Large-area single-layer WS$_2$ is grown epitaxially on Au(111) using evaporation of W atoms in a low pressure H$_2$S atmosphere. It is characterized by means of scanning tunneling microscopy, low-energy electron diffraction and core-level spectroscopy. Its electronic band structure is determined by angle-resolved photoemission spectroscopy. The valence band maximum at $\bar{K}$ is found to be significantly higher than at $\barΓ$. The observed dispersion around $\bar{K}$ is in good agreement with density functional theory calculations for a free-standing monolayer, whereas the bands at $\barΓ$ are found to be hybridized with states originating from the Au substrate. Strong spin-orbit coupling leads to a large spin-splitting of the bands in the neighborhood of the $\bar{K}$ points, with a maximum splitting of 419(11)~meV. The valence band dispersion around $\bar{K}$ is found to be highly anisotropic with spin-branch dependent effective hole masses of $0.40(02)m_e$ and $0.57(09)m_e$ for the upper and lower split valence band, respectively. The large size of the spin-splitting and the low effective mass of the valence band maximum make single-layer WS$_2$ a promising alternative to the widely studied MoS$_2$ for applications in electronics, spintronics and valleytronics.

cond-mat.str-el↗

arXiv2015

Observation of Ultrafast Free Carrier Dynamics in Single Layer MoS$_2$

The dynamics of excited electrons and holes in single layer (SL) MoS$_2$ have so far been difficult to disentangle from the excitons that dominate the optical response of this material. Here, we use time- and angle-resolved photoemission spectroscopy for a SL of MoS$_2$ on a metallic substrate to directly measure the excited free carriers. This allows us to ascertain a direct quasiparticle band gap of 1.95 eV and determine an ultrafast (50 fs) extraction of excited free carriers via the metal in contact with the SL MoS$_2$. This process is of key importance for optoelectronic applications that rely on separated free carriers rather than excitons.

cond-mat.mtrl-sci↗

arXiv2015

Ramifications of Optical Pumping on the Interpretation of Time-Resolved Photoemission Experiments on Graphene

In pump-probe time and angle-resolved photoemission spectroscopy (TR-ARPES) experiments the presence of the pump pulse adds a new level of complexity to the photoemission process in comparison to conventional ARPES. This is evidenced by pump-induced vacuum space-charge effects and surface photovoltages, as well as multiple pump excitations due to internal reflections in the sample-substrate system. These processes can severely affect a correct interpretation of the data by masking the out-of-equilibrium electron dynamics intrinsic to the sample. In this study, we show that such effects indeed influence TR-ARPES data of graphene on a silicon carbide (SiC) substrate. In particular, we find a time- and laser fluence-dependent spectral shift and broadening of the acquired spectra, and unambiguously show the presence of a double pump excitation. The dynamics of these effects is slower than the electron dynamics in the graphene sample, thereby permitting us to deconvolve the signals in the time domain. Our results demonstrate that complex pump-related processes should always be considered in the experimental setup and data analysis.

cond-mat.str-el↗

arXiv2014

Electronic Structure of Epitaxial Single-Layer MoS$_2$

The electronic structure of epitaxial single-layer MoS$_2$ on Au(111) is investigated by angle-resolved photoemission spectroscopy. Pristine and potassium-doped layers are studied in order to gain access to the conduction band. The potassium-doped layer is found to have a (1.39$\pm$0.05)~eV direct band gap at $\bar{K}$ with the valence band top at $\barΓ$ having a significantly higher binding energy than at $\bar{K}$. The moiré superstructure of the epitaxial system does not lead to the presence of observable replica bands or minigaps. The degeneracy of the upper valence band at $\bar{K}$ is found to be lifted by the spin-orbit interaction, leading to a splitting of (145$\pm$4)~meV. This splitting is anisotropic and in excellent agreement with recent calculations. Finally, it is shown that the strength of the potassium doping is $k$-dependent, leading to the possibility of band structure engineering in single-layers of transition metal dichalcogenides.

cond-mat.mtrl-sci↗

arXiv2014

Ultrafast Dynamics of Massive Dirac Fermions in Bilayer Graphene

Bilayer graphene is a highly promising material for electronic and optoelectronic applications since it is supporting massive Dirac fermions with a tuneable band gap. However, no consistent picture of the gap's effect on the optical and transport behavior has emerged so far, and it has been proposed that the insulating nature of the gap could be compromised by unavoidable structural defects, by topological in-gap states, or that the electronic structure could be altogether changed by many-body effects. Here we directly follow the excited carriers in bilayer graphene on a femtosecond time scale, using ultrafast time- and angle-resolved photoemission. We find a behavior consistent with a single-particle band gap. Compared to monolayer graphene, the existence of this band gap leads to an increased carrier lifetime in the minimum of the lowest conduction band. This is in sharp contrast to the second sub-state of the conduction band, in which the excited electrons decay through fast, phonon-assisted inter-band transitions.

cond-mat.mes-hall↗

arXiv2013

Electron-phonon coupling-induced kinks in the sigma band of graphene

Angle-resolved photoemission spectroscopy reveals pronounced kinks in the dispersion of the sigma band of graphene. Such kinks are usually caused by the combination of a strong electron-boson interaction and the cut-off in the Fermi-Dirac distribution. They are therefore not expected for the $σ$ band of graphene that has a binding energy of more than 3.5 eV. We argue that the observed kinks are indeed caused by the electron-phonon interaction, but the role of the Fermi-Dirac distribution cutoff is assumed by a cut-off in the density of $σ$ states. The existence of the effect suggests a very weak coupling of holes in the $σ$ band not only to the $π$ electrons of graphene but also to the substrate electronic states. This is confirmed by the presence of such kinks for graphene on several different substrates that all show a strong coupling constant of lambda=1.

cond-mat.mes-hall↗

arXiv2012

Direct band structure measurement of a buried two-dimensional electron gas

Buried two dimensional electron gasses (2DEGs) have recently attracted considerable attention as a testing ground for both fundamental physics and quantum computation applications. Such 2DEGs can be created by phosphorus delta (δ) doping of silicon, a technique in which a dense and narrow dopant profile is buried beneath the Si surface. Phosphorous δ-doping is a particularly attractive platform for fabricating scalable spin quantum bit architectures, compatible with current semiconductor technology. The band structure of the δ-layers that underpin these devices has been studied intensely using different theoretical methods, but it has hitherto not been possible to directly compare these predictions with experimental data. Here we report the first measurement of the electronic band structure of a δ-doped layer below the Si(001) surface by angle resolved photoemission spectroscopy (ARPES). Our measurements confirm the layer to be metallic and give direct access to the Fermi level position. Surprisingly, the direct observation of the states is possible despite them being buried far below the surface. Using this experimental approach, buried states in a wide range of other material systems, including metallic oxide interfaces, could become accessible to direct spectroscopic investigations.

cond-mat.mtrl-sci↗