arXiv subjects

Xiaodong Xu

Publications and source records attributed to Xiaodong Xu.

At least 343 records · Page 19Linked to original sources

arXiv2014

Intrinsic Exciton Linewidth in Monolayer Transition Metal Dichalcogenides

Monolayer transition metal dichalcogenides feature Coulomb-bound electron-hole pairs (excitons) with exceptionally large binding energy and coupled spin and valley degrees of freedom. These unique attributes have been leveraged for electrical and optical control of excitons for atomically-thin optoelectronics and valleytronics. The development of such technologies relies on understanding and quantifying the fundamental properties of the exciton. A key parameter is the intrinsic exciton homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath (vacuum and other quasiparticles) interactions. Using optical coherent two-dimensional spectroscopy, we provide the first experimental determination of the exciton homogeneous linewidth in monolayer transition metal dichalcogenides, specifically tungsten diselenide (WSe2). The role of exciton-exciton and exciton-phonon interactions in quantum decoherence is revealed through excitation density and temperature dependent linewidth measurements. The residual homogeneous linewidth extrapolated to zero density and temperature is ~1.5 meV, placing a lower bound of approximately 0.2 ps on the exciton radiative lifetime. The exciton quantum decoherence mechanisms presented in this work are expected to be ubiquitous in atomically-thin semiconductors.

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arXiv2014

Valley Contrasting Magnetoluminescence in Monolayer MoS$_{2}$ Quantum Hall Systems

The valley dependent optical selection rules in recently discovered monolayer group-VI transition metal dichalcogenides (TMDs) make possible optical control of valley polarization, a crucial step towards valleytronic applications. However, in presence of Landaul level(LL) quantization such selection rules are taken over by selection rules between the LLs, which are not necessarily valley contrasting. Using MoS$_{2}$ as an example we show that the spatial inversion-symmetry breaking results in unusual valley dependent inter-LL selection rules, which directly locks polarization to valley. We find a systematic valley splitting for all Landau levels (LLs) in the quantum Hall regime, whose magnitude is linearly proportional to the magnetic field and in comparable with the LL spacing. Consequently, unique plateau structures are found in the optical Hall conductivity, which can be measured by the magneto-optical Faraday rotations.

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arXiv2014

Magnetic Control of Valley Pseudospin in Monolayer WSe2

Local energy extrema of the bands in momentum space, or valleys, can endow electrons in solids with pseudo-spin in addition to real spin. In transition metal dichalcogenides this valley pseudo-spin, like real spin, is associated with a magnetic moment which underlies the valley-dependent circular dichroism that allows optical generation of valley polarization, intervalley quantum coherence, and the valley Hall effect. However, magnetic manipulation of valley pseudospin via this magnetic moment, analogous to what is possible with real spin, has not been shown before. Here we report observation of the valley Zeeman splitting and magnetic tuning of polarization and coherence of the excitonic valley pseudospin, by performing polarization-resolved magneto-photoluminescence on monolayer WSe2. Our measurements reveal both the atomic orbital and lattice contributions to the valley orbital magnetic moment; demonstrate the deviation of the band edges in the valleys from an exact massive Dirac fermion model; and reveal a striking difference between the magnetic responses of neutral and charged valley excitons which is explained by renormalization of the excitonic spectrum due to strong exchange interactions.

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arXiv2014

Lateral heterojunctions within monolayer semiconductors

Heterojunctions between three-dimensional (3D) semiconductors with different bandgaps are the basis of modern light-emitting diodes, diode lasers, and high-speed transistors. Creating analogous heterojunctions between different two-dimensional (2D) semiconductors would enable band engineering within the 2D plane and open up new realms in materials science, device physics and engineering. Here we demonstrate that seamless high-quality in-plane heterojunctions can be grown between the 2D monolayer semiconductors MoSe2 and WSe2. The junctions, grown by lateral hetero-epitaxy using physical vapor transport, are visible in an optical microscope and show enhanced photoluminescence. Atomically resolved transmission electron microscopy reveals that their structure is an undistorted honeycomb lattice in which substitution of one transition metal by another occurs across the interface. The growth of such lateral junctions will allow new device functionalities, such as in-plane transistors and diodes, to be integrated within a single atomically thin layer.

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arXiv2014

Nonlinear valley and spin currents from Fermi pocket anisotropy in 2D crystals

Controlled flow of spin and valley pseudospin is key to future electronics exploiting these internal degrees of freedom of carriers. Here we discover a universal possibility for generating spin and valley currents by electric bias or temperature gradient only, which arises from the anisotropy of Fermi pockets in crystalline solids. We find spin and valley currents to the second order in the electric field, as well as their thermoelectric counterparts, i.e. the nonlinear spin and valley Seebeck effects. These second-order nonlinear responses allow two unprecedented possibilities to generate pure spin and valley flows without net charge current: (i) by an AC bias; or (ii) by an arbitrary inhomogeneous temperature distribution. As examples, we predict appreciable nonlinear spin and valley currents in two-dimensional (2D) crystals including graphene, monolayer and trilayer transition metal dichalcogenides, and monolayer gallium selenide. Our finding points to a new route towards electrical and thermal generations of spin and valley currents for spintronic and valleytronic applications based on 2D quantum materials.

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arXiv2014

Observation of Long-Lived Interlayer Excitons in Monolayer MoSe2-WSe2 Heterostructures

Two-dimensional (2D) materials, such as graphene1, boron nitride2, and transition metal dichalcogenides (TMDs)3-5, have sparked wide interest in both device physics and technological applications at the atomic monolayer limit. These 2D monolayers can be stacked together with precise control to form novel van der Waals heterostructures for new functionalities2,6-9. One highly coveted but yet to be realized heterostructure is that of differing monolayer TMDs with type II band alignment10-12. Their application potential hinges on the fabrication, understanding, and control of bonded monolayers, with bound electrons and holes localized in individual monolayers, i.e. interlayer excitons. Here, we report the first observation of interlayer excitons in monolayer MoSe2-WSe2 heterostructures by both photoluminescence and photoluminescence excitation spectroscopy. The energy and luminescence intensity of interlayer excitons are highly tunable by an applied vertical gate voltage, implying electrical control of the heterojunction band-alignment. Using time resolved photoluminescence, we find that the interlayer exciton is long-lived with a lifetime of about 1.8 ns, an order of magnitude longer than intralayer excitons13-16. Our work demonstrates the ability to optically pump interlayer electric polarization and provokes the immediate exploration of interlayer excitons for condensation phenomena, as well as new applications in 2D light-emitting diodes, lasers, and photovoltaic devices.

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arXiv2014

Electrically Tunable Excitonic Light Emitting Diodes based on Monolayer WSe2 p-n Junctions

Light-emitting diodes are of importance for lighting, displays, optical interconnects, logic and sensors. Hence the development of new systems that allow improvements in their efficiency, spectral properties, compactness and integrability could have significant ramifications. Monolayer transition metal dichalcogenides have recently emerged as interesting candidates for optoelectronic applications due to their unique optical properties. Electroluminescence has already been observed from monolayer MoS2 devices. However, the electroluminescence efficiency was low and the linewidth broad due both to the poor optical quality of MoS2 and to ineffective contacts. Here, we report electroluminescence from lateral p-n junctions in monolayer WSe2 induced electrostatically using a thin boron nitride support as a dielectric layer with multiple metal gates beneath. This structure allows effective injection of electrons and holes, and combined with the high optical quality of WSe2 it yields bright electroluminescence with 1000 times smaller injection current and 10 times smaller linewidth than in MoS2. Furthermore, by increasing the injection bias we can tune the electroluminescence between regimes of impurity-bound, charged, and neutral excitons. This system has the required ingredients for new kinds of optoelectronic devices such as spin- and valley-polarized light-emitting diodes, on-chip lasers, and two-dimensional electro-optic modulators.

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arXiv2014

Coherent Electronic Coupling in Atomically Thin MoSe2

We report the first direct spectroscopic evidence for coherent electronic coupling between excitons and trions in atomically thin transition metal dichalcogenides, specifically monolayer MoSe2. Signatures of coupling appear as isolated cross-peaks in two-color pump-probe spectra, and the lineshape of the peaks reveals that the coupling originates from many-body interactions. Excellent agreement between the experiment and density matrix calculations suggests the formation of a correlated exciton-trion state due to their coupling.

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arXiv2014

Bright excitons in monolayer transition metal dichalcogenides: from Dirac cones to Dirac saddle points

In monolayer transition metal dichalcogenides, tightly bound excitons have been discovered with a valley pseudospin that can be optically addressed through polarization selection rules. Here, we show that this valley pseudospin is strongly coupled to the exciton center-of-mass motion through electron-hole exchange. This coupling realizes a massless Dirac cone with chirality index I=2 for excitons inside the light cone, i.e. bright excitons. Under moderate strain, the I=2 Dirac cone splits into two degenerate I=1 Dirac cones, and saddle points with a linear Dirac spectrum emerge in the bright exciton dispersion. Interestingly, after binding an extra electron, the charged exciton becomes a massive Dirac particle associated with a large valley Hall effect protected from intervalley scattering. Our results point to unique opportunities to study Dirac physics, with exciton's optical addressability at specifiable momentum, energy and pseudospin. The strain-tunable valley-orbit coupling also implies new structures of exciton condensates, new functionalities of excitonic circuits, and possibilities for mechanical control of valley pseudospin.

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arXiv2013

Spin-Layer Locking Effects in Optical Orientation of Exciton Spin in Bilayer WSe2

Coupling degrees of freedom of distinct nature plays a critical role in numerous physical phenomena. The recent emergence of layered materials provides a laboratory for studying the interplay between internal quantum degrees of freedom of electrons. Here, we report experimental signatures of new coupling phenomena connecting real spin with layer pseudospins in bilayer WSe2. In polarization-resolved photoluminescence measurements, we observe large spin orientation of neutral and charged excitons generated by both circularly and linearly polarized light, with a splitting of the trion spectrum into a doublet at large vertical electrical field. These observations can be explained by locking of spin and layer pseudospin in a given valley. Because up and down spin states are localized in opposite layers, spin relaxation is substantially suppressed, while the doublet emerges as a manifestation of electrically induced spin splitting resulting from the interlayer bias. The observed distinctive behavior of the trion doublet under circularly and linearly polarized light excitation further provides spectroscopic evidence of interlayer and intralayer trion species, a promising step toward optical manipulation in van der Waals heterostructures through the control of interlayer excitons.

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arXiv2013

Control of Two-Dimensional Excitonic Light Emission via Photonic Crystal

Monolayers of transition metal dichalcogenides (TMDCs) have emerged as new optoelectronic materials in the two dimensional (2D) limit, exhibiting rich spin-valley interplays, tunable excitonic effects, and strong light-matter interactions. An essential yet undeveloped ingredient for many photonic applications is the manipulation of its light emission. Here we demonstrate the control of excitonic light emission from monolayer tungsten diselenide (WSe2) in an integrated photonic structure, achieved by transferring one monolayer onto a photonic crystal (PhC) with a cavity. In addition to the observation of greatly enhanced (~60 times) photoluminescence of WSe2 and an effectively coupled cavity-mode emission, we are able to redistribute the emitted photons both polarly and azimuthally in the far field through designing PhC structures, as revealed by momentum-resolved microscopy. A 2D optical antenna is thus constructed. Our work suggests a new way of manipulating photons in hybrid 2D photonics, important for future energy efficient optoelectronics and 2D nano-lasers.

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arXiv2013

Majorana Fermions on Zigzag Edge of Monolayer Transition Metal Dichalcogenides

Majorana fermions, quantum particles with non-Abelian exchange statistics, are not only of fundamental importance, but also building blocks for fault-tolerant quantum computation. Although certain experimental breakthroughs for observing Majorana fermions have been made recently, their conclusive dection is still challenging due to the lack of proper material properties of the underlined experimental systems. Here we propose a new platform for Majorana fermions based on edge states of certain non-topological two-dimensional semiconductors with strong spin-orbit coupling, such as monolayer group-VI transition metal dichalcogenides (TMD). Using first-principles calculations and tight-binding modeling, we show that zigzag edges of monolayer TMD can host well isolated single edge band with strong spin-orbit coupling energy. Combining with proximity induced s-wave superconductivity and in-plane magnetic fields, the zigzag edge supports robust topological Majorana bound states at the edge ends, although the two-dimensional bulk itself is non-topological. Our findings points to a controllable and integrable platform for searching and manipulating Majorana fermions.

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arXiv2013

Giant Faraday rotation induced by Berry phase in bilayer graphene under strong terahertz fields

High-order terahertz (THz) sideband generation (HSG) in semiconductors is a phenomenon with physics similar to high-order harmonic generation but in a much lower frequency regime. It was found that the electron-hole pairs excited by a weak optical laser can accumulate Berry phases along a cyclic path under the driving of a strong THz field. The Berry phases appear as the Faraday rotation angles of the emission signal under short-pulse excitation in monolayer MoS$_2$. In this paper, the theory of Berry phase in THz extreme nonlinear optics is applied to biased bilayer graphene with Bernal stacking, which has similar Bloch band features and optical properties to the monolayer MoS$_2$, such as time-reversal related valleys and valley contrasting optical selection rules. The bilayer graphene has much larger Berry curvature than monolayer MoS$_2$, which leads to a giant Faraday rotation of the optical emission ($\sim$ 1 rad for a THz field with frequency 1 THz and strength 8 kV/cm). This provides opportunities to use bilayer graphene and low-power THz lasers for ultrafast electro-optical devices.

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arXiv2013

Optical Generation of Excitonic Valley Coherence in Monolayer WSe2

Due to degeneracies arising from crystal symmetries, it is possible for electron states at band edges ("valleys") to have additional spin-like quantum numbers. An important question is whether coherent manipulation can be performed on such valley pseudospins, analogous to that routinely implemented using true spin, in the quest for quantum technologies. Here we show for the first time that SU(2) valley coherence can indeed be generated and detected. Using monolayer semiconductor WSe2 devices, we first establish the circularly polarized optical selection rules for addressing individual valley excitons and trions. We then reveal coherence between valley excitons through the observation of linearly polarized luminescence, whose orientation always coincides with that of any linearly polarized excitation. Since excitons in a single valley emit circularly polarized photons, linear polarization can only be generated through recombination of an exciton in a coherent superposition of the two valleys. In contrast, the corresponding photoluminescence from trions is not linearly polarized, consistent with the expectation that the emitted photon polarization is entangled with valley pseudospin. The ability to address coherence, in addition to valley polarization, adds a critical dimension to the quantum manipulation of valley index necessary for coherent valleytronics.

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arXiv2013

Use of MAX-CUT for Ramsey Arrowing of Triangles

In 1967, Erdős and Hajnal asked the question: Does there exist a $K_4$-free graph that is not the union of two triangle-free graphs? Finding such a graph involves solving a special case of the classical Ramsey arrowing operation. Folkman proved the existence of these graphs in 1970, and they are now called Folkman graphs. Erdős offered \$100 for deciding if one exists with less than $10^{10}$ vertices. This problem remained open until 1988 when Spencer, in a seminal paper using probabilistic techniques, proved the existence of a Folkman graph of order $3\times 10^9$ (after an erratum), without explicitly constructing it. In 2008, Dudek and Rödl developed a strategy to construct new Folkman graphs by approximating the maximum cut of a related graph, and used it to improve the upper bound to 941. We improve this bound first to 860 using their approximation technique and then further to 786 with the MAX-CUT semidefinite programming relaxation as used in the Goemans-Williamson algorithm.

math.CO↗

arXiv2013

Magnetoelectric effects and valley controlled spin quantum gates in transition metal dichalcogenide bilayers

In monolayer group-VI transition metal dichalcogenides (TMDC), charge carriers have spin and valley degrees of freedom, both associated with magnetic moments. On the other hand, the layer degree of freedom in multilayers is associated with electrical polarization. Here, we show that TMDC bilayers offer an unprecedented platform to realize a strong coupling between the spin, layer pseudospin, and valley degrees of freedom of holes. Such coupling not only gives rise to the spin Hall effect and spin circular dichroism in inversion symmetric bilayer, but also leads to a variety of magnetoelectric effects permitting quantum manipulation of these electronic degrees of freedom. Oscillating electric and magnetic fields can both drive the hole spin resonance where the two fields have valley-dependent interference, making possible a prototype interplay between the spin and valley as information carriers for potential valley-spintronic applications. We show how to realize quantum gates on the spin qubit controlled by the valley bit.

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arXiv2013

Vapor-Solid Growth of High Optical Quality MoS2 Monolayers With Near-Unity Valley Polarization

Monolayers of transition metal dichalcogenides (TMDCs) are atomically thin direct-gap semiconductors with potential applications in nanoelectronics, optoelectronics, and electrochemical sensing. Recent theoretical and experimental efforts suggest that they are ideal systems for exploiting the valley degrees of freedom of Bloch electrons. For example, Dirac valley polarization has been demonstrated in mechanically exfoliated monolayer MoS2 samples by polarization-resolved photoluminescence, although polarization has rarely been seen at room temperature. Here we report a new method for synthesizing high optical quality monolayer MoS2 single crystals up to 25 microns in size on a variety of standard insulating substrates (SiO2, sapphire and glass) using a catalyst-free vapor-solid growth mechanism. The technique is simple and reliable, and the optical quality of the crystals is extremely high, as demonstrated by the fact that the valley polarization approaches unity at 30 K and persists at 35% even at room temperature, suggesting a virtual absence of defects. This will allow greatly improved optoelectronic TMDC monolayer devices to be fabricated and studied routinely.

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arXiv2013

Electrical Control of Two-Dimensional Neutral and Charged Excitons in a Monolayer Semiconductor

Monolayer group VI transition metal dichalcogenides have recently emerged as semiconducting alternatives to graphene in which the true two-dimensionality (2D) is expected to illuminate new semiconducting physics. Here we investigate excitons and trions (their singly charged counterparts) which have thus far been challenging to generate and control in the ultimate 2D limit. Utilizing high quality monolayer molybdenum diselenide (MoSe2), we report the unambiguous observation and electrostatic tunability of charging effects in positively charged (X+), neutral (Xo), and negatively charged (X-) excitons in field effect transistors via photoluminescence. The trion charging energy is large (30 meV), enhanced by strong confinement and heavy effective masses, while the linewidth is narrow (5 meV) at temperatures below 55 K. This is greater spectral contrast than in any known quasi-2D system. We also find the charging energies for X+ and X- to be nearly identical implying the same effective mass for electrons and holes.

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