arXiv subjects

Xiaodong Xu

Publications and source records attributed to Xiaodong Xu.

At least 325 records · Page 18Linked to original sources

arXiv2016

Multiple Hot-Carrier Collection in Photo-Excited Graphene Moire Superlattices

In conventional light harvesting devices, the absorption of a single photon only excites one electron, which sets the standard limit of power-conversion efficiency, such as the Shockley-Queisser limit. In principle, generating and harnessing multiple carriers per absorbed photon can improve the efficiency and possibly overcome this limit. Here, we report the observation of multiple hot carrier collection in graphene-boron-nitride Moire superlattice structures. A record-high zero-bias photoresponsivity of 0.3 ampere per watt, equivalently, an external quantum efficiency exceeding 50 percent, is achieved utilizing graphene photo-Nernst effect, which demonstrates a collection of at least 5 carriers per absorbed photon. We reveal that this effect arises from the enhanced Nernst coefficient through Lifshtiz transition at low energy Van Hove singularities, which is an emergent phenomenon due to the formation of Moire minibands. Our observation points to a new means for extremely efficient and flexible optoelectronics based on van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2016

Exciton Dynamics in Monolayer Transition Metal Dichalcogenides

Since the discovery of semiconducting monolayer transition metal dichalcogenides, a variety of experimental and theoretical studies have been carried out seeking to understand the intrinsic exciton population decay and valley relaxation dynamics. Reports of the exciton decay time range from hundreds of femtoseconds to ten nanoseconds, while the valley depolarization time can exceed one nanosecond. At present, however, a consensus on the microscopic mechanisms governing exciton radiative and non-radiative recombination is lacking. The strong exciton oscillator strength resulting in up to 20% absorption for a single monolayer points to ultrafast radiative recombination. However, the low quantum yield and large variance in the reported lifetimes suggest that non-radiative Auger-type processes obscure the intrinsic exciton radiative lifetime. In either case, the electron-hole exchange interaction plays an important role in the exciton spin and valley dynamics. In this article, we review the experiments and theory that have led to these conclusions and comment on future experiments that could complement our current understanding.

cond-mat.mes-hall↗

arXiv2016

Band parameters and hybridization in 2D semiconductor heterostructures from photoemission spectroscopy

Combining monolayers of different two-dimensional (2D) semiconductors into heterostructures opens up a wealth of possibilities for novel electronic and optical functionalities. Exploiting them hinges on accurate measurements of the band parameters and orbital hybridization in separate and stacked monolayers, many of which are only available as small samples. The recently introduced technique of angle-resolved photoemission spectroscopy with submicron spatial resolution (μ-ARPES) offers the capability to measure small samples, but the energy resolution obtained for such exfoliated samples to date (~0.5 eV) has been inadequate. Here, we show that by suitable heterostructure sample design the full potential of μ-ARPES can be realized. We focus on MoSe2/WSe2 van der Waals heterostructures, which are 2D analogs of 3D semiconductor heterostructures. We find that in a MoSe2/WSe2 heterobilayer the bands in the K valleys are weakly hybridized, with the conduction and valence band edges originating in the MoSe2 and WSe2 respectively. There is stronger hybridization at the Γ point, but the valence band edge remains at the K points. This is consistent with the recent observation of interlayer excitons where the electron and hole are valley polarized but in opposite layers. We determine the valence band offset to be 300 meV, which combined with photoluminescence measurements implies that the binding energy of interlayer excitons is at least 200 meV, comparable with that of intralayer excitons.

cond-mat.mes-hall↗

arXiv2016

Expansion of a Valley-Polarized Exciton Cloud in a 2D Heterostructure

Heterostructures comprising different monolayer semiconductors provide a new system for fundamental science and device technologies, such as in the emerging field of valleytronics. Here, we realize valley-specific interlayer excitons in monolayer WSe2-MoSe2 vertical heterostructures. We create interlayer exciton spin-valley polarization by circularly polarized optical pumping and determine a valley lifetime of 40 nanoseconds. This long-lived polarization enables the visualization of the expansion of a valley-polarized exciton cloud over several microns. The spatial pattern of the polarization evolves into a ring with increasing exciton density, a manifestation of valley exciton exchange interactions. Our work lays a foundation for quantum optoelectronics and valleytronics based on interlayer excitons in van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2016

Hybrid tip-enhanced nano-spectroscopy and -imaging of monolayer WSe2 with local strain control

Many classes of two-dimensional (2D) materials have emerged as potential platforms for novel electronic and optical devices. However, the physical properties are strongly influenced by nanoscale heterogeneities in the form of edges, grain boundaries, and nucleation sites. Using combined tip-enhanced Raman scattering (TERS) and photoluminescence (TEPL) nano-spectroscopy and -imaging, we study the associated effects on the excitonic properties in monolayer WSe2 grown by physical vapor deposition (PVD). With <15 nm spatial resolution we resolve nonlocal nanoscale correlations of PL spectral intensity and shifts with crystal edges and internal twin boundaries associated with the expected exciton diffusion length. Through an active atomic force tip interaction we can control the crystal strain on the nanoscale, and tune the local bandgap in reversible (up to 24 meV shift) and irreversible (up to 48 meV shift) fashion. This allows us to distinguish the effect of strain from the dominant influence of defects on the PL modification at the different structural heterogeneities. Hybrid nano-optical and nano-mechanical imaging and spectroscopy thus enables the systematic study of the coupling of structural and mechanical degrees of freedom to the nanoscale electronic and optical properties in layered 2D materials.

physics.optics↗

arXiv2015

Generation of 30-fs pulses from a diode-pumped graphene mode-locked Yb:CaYAlO4 laser

Stable 30 fs pulses centered at 1068 nm (less than 10 optical cycles) are demonstrated in a diode pumped Yb:CaYAlO4 laser by using high-quality chemical vapor deposited monolayer graphene as the saturable absorber. The mode locked 8.43 optical-cycle pulses have a spectral bandwidth of ~ 50 nm and a pulse repetition frequency of ~ 113.5 MHz. To our knowledge, this is the shortest pulse ever reported for graphene mode-locked lasers and mode-locked Yb-doped bulk lasers. Our experimental results demonstrate that graphene mode locking is a very promising practical technique to generate few-cycle optical pulses directly from a laser oscillator.

physics.optics↗

arXiv2015

Trion Formation Dynamics in Monolayer Transition Metal Dichalcogenides

We report charged exciton (trion) formation dynamics in doped monolayer transition metal dichalcogenides (TMDs), specifically molybdenum diselenide (MoSe2), using resonant two-color pump-probe spectroscopy. When resonantly pumping the exciton transition, trions are generated on a picosecond timescale through exciton-electron interaction. As the pump energy is tuned from the high energy to low energy side of the inhomogeneously broadened exciton resonance, the trion formation time increases by ~ 50%. This feature can be explained by the existence of both localized and delocalized excitons in a disordered potential and suggests the existence of an exciton mobility edge in TMDs. The quasiparticle formation and conversion processes are important for interpreting photoluminescence and photoconductivity in TMDs.

cond-mat.mes-hall↗

arXiv2015

Electronic structures and theoretical modelling of two-dimensional group-VIB transition metal dichalcogenides

Atomically thin group-VIB transition metal dichalcogenides (TMDs) have recently emerged as a new class of two-dimensional (2D) semiconductors with extraordinary properties including the direct band gap in the visible frequency range, the pronounced spin-orbit coupling, the ultra-strong Coulomb interaction, and the rich physics associated with the valley degree of freedom. These 2D TMDs exhibit great potentials for device applications and have attracted vast interest for the exploration of new physics. 2D TMDs have complex electronic structures which underlie their physical properties. Here we review the bulk electronic structures in these new 2D materials as well as the theoretical models developed at different levels, along which we sort out the understandings on the origins of a variety of properties observed or predicted.

cond-mat.mes-hall↗

arXiv2015

Anomalous light cones and valley optical selection rules of interlayer excitons in twisted heterobilayers

We show that, because of the inevitable twist and lattice mismatch in heterobilayers of transition metal dichalcogenides, interlayer excitons have six-fold degenerate light cones anomalously located at finite velocities on the parabolic energy dispersion. The photon emissions at each light cone are elliptically polarized, with major axis locked to the direction of exciton velocity, and helicity specified by the valley indices of the electron and the hole. These finite-velocity light cones allow unprecedented possibilities to optically inject valley polarization and valley current, and the observation of both direct and inverse valley Hall effects, by exciting interlayer excitons. Our findings suggest potential excitonic circuits with valley functionalities, and unique opportunities to study exciton dynamics and condensation phenomena in semiconducting 2D heterostructures.

cond-mat.mes-hall↗

arXiv2015

Photo-Nernst current in graphene

Photocurrent measurements provide a powerful means of studying the spatially resolved optoelectronic and electrical properties of a material or device. Generally speaking there are two classes of mechanism for photocurrent generation: those involving separation of electrons and holes, and thermoelectric effects driven by electron temperature gradients. Here we introduce a new member in the latter class: the photo-Nernst effect. In graphene devices in a perpendicular magnetic field we observe photocurrent generated uniformly along the free edges, with opposite sign at opposite edges. The signal is antisymmetric in field, shows a peak versus gate voltage at the neutrality point flanked by wings of opposite sign at low fields, and exhibits quantum oscillations at higher fields. These features are all explained by the Nernst effect associated with laser-induced electron heating. This photo-Nernst current provides a simple and clear demonstration of the Shockley-Ramo nature of long-range photocurrent generation in a gapless material.

cond-mat.mes-hall↗

arXiv2015

Valley excitons in two-dimensional semiconductors

Monolayer group-VIB transition metal dichalcogenides have recently emerged as a new class of semiconductors in the two-dimensional limit. The attractive properties include: the visible range direct band gap ideal for exploring optoelectronic applications; the intriguing physics associated with spin and valley pseudospin of carriers which implies potentials for novel electronics based on these internal degrees of freedom; the exceptionally strong Coulomb interaction due to the two-dimensional geometry and the large effective masses. The physics of excitons, the bound states of electrons and holes, has been one of the most actively studied topics on these two-dimensional semiconductors, where the excitons exhibit remarkably new features due to the strong Coulomb binding, the valley degeneracy of the band edges, and the valley dependent optical selection rules for interband transitions. Here we give a brief overview of the experimental and theoretical findings on excitons in two-dimensional transition metal dichalcogenides, with focus on the novel properties associated with their valley degrees of freedom.

cond-mat.mes-hall↗

arXiv2015

A step forwards on the Erdős-Sós problem concerning the Ramsey numbers $R(3,k)$

Let $Δ_s=R(K_3,K_s)-R(K_3,K_{s-1})$, where $R(G,H)$ is the Ramsey number of graphs $G$ and $H$ defined as the smallest $n$ such that any edge coloring of $K_n$ with two colors contains $G$ in the first color or $H$ in the second color. In 1980, Erdős and Sós posed some questions about the growth of $Δ_s$. The best known concrete bounds on $Δ_s$ are $3 \le Δ_s \le s$, and they have not improved since the stating of the problem. In this paper we present some constructions, which imply in particular that $R(K_3,K_s) \ge R(K_3,K_{s-1}-e) + 4$. This does not improve the lower bound of 3 on $Δ_s$, but we still consider it a step towards to understanding its growth. We discuss some related questions and state two conjectures involving $Δ_s$, including the following: for some constant $d$ and all $s$ it holds that $Δ_s - Δ_{s+1} \leq d$. We also prove that if the latter is true, then $\lim_{s \rightarrow \infty} Δ_s/s=0$.

math.CO↗

arXiv2015

Electrical Control of Second-Harmonic Generation in a WSe2 Monolayer Transistor

Nonlinear optical frequency conversion, in which optical fields interact with a nonlinear medium to produce new field frequencies, is ubiquitous in modern photonic systems. However, the nonlinear electric susceptibilities that give rise to such phenomena are often challenging to tune in a given material, and so far, dynamical control of optical nonlinearities remains confined to research labs as a spectroscopic tool. Here, we report a mechanism to electrically control second-order optical nonlinearities in monolayer WSe2, an atomically thin semiconductor. We show that the intensity of second-harmonic generation at the A-exciton resonance is tunable by over an order of magnitude at low temperature and nearly a factor of 4 at room temperature through electrostatic doping in a field-effect transistor. Such tunability arises from the strong exciton charging effects in monolayer semiconductors, which allow for exceptional control over the oscillator strengths at the exciton and trion resonances. The exciton-enhanced second-harmonic generation is counter-circularly polarized to the excitation laser, arising from the combination of the two-photon and one-photon valley selection rules that have opposite helicity in the monolayer. Our study paves the way towards a new platform for chip-scale, electrically tunable nonlinear optical devices based on two-dimensional semiconductors.

cond-mat.mes-hall↗

arXiv2015

Population pulsation resonances of excitons in monolayer MoSe2 with sub 1 μeV linewidth

Monolayer transition metal dichalcogenides, a new class of atomically thin semiconductors, possess optically coupled 2D valley excitons. The nature of exciton relaxation in these systems is currently poorly understood. Here, we investigate exciton relaxation in monolayer MoSe2 using polarization-resolved coherent nonlinear optical spectroscopy with high spectral resolution. We report strikingly narrow population pulsation resonances with two different characteristic linewidths of 1 μeV and <0.2 μeV at low-temperature. These linewidths are more than three orders of magnitude narrower than the photoluminescence and absorption linewidth, and indicate that a component of the exciton relaxation dynamics occurs on timescales longer than 1 ns. The ultra-narrow resonance (<0.2 μeV) emerges with increasing excitation intensity, and implies the existence of a long-lived state whose lifetime exceeds 6 ns.

cond-mat.mes-hall↗

arXiv2015

Ultra-Low Threshold Monolayer Semiconductor Nanocavity Lasers

Engineering the electromagnetic environment of a nanoscale light emitter by a photonic cavity can significantly enhance its spontaneous emission rate through cavity quantum electrodynamics in the Purcell regime. This effect can greatly reduce the lasing threshold of the emitter, providing the ultimate low-threshold laser system with small footprint, low power consumption and ultrafast modulation. A state-of-the-art ultra-low threshold nanolaser has been successfully developed though embedding quantum dots into photonic crystal cavity (PhCC). However, several core challenges impede the practical applications of this architecture, including the random positions and compositional fluctuations of the dots, extreme difficulty in current injection, and lack of compatibility with electronic circuits. Here, we report a new strategy to lase, where atomically thin crystalline semiconductor, i.e., a tungsten-diselenide (WSe2) monolayer, is nondestructively and deterministically introduced as a gain medium at the surface of a pre-fabricated PhCC. A new type of continuous-wave nanolaser operating in the visible regime is achieved with an optical pumping threshold as low as 27 nW at 130 K, similar to the value achieved in quantum dot PhCC lasers. The key to the lasing action lies in the monolayer nature of the gain medium, which confines direct-gap excitons to within 1 nm of the PhCC surface. The surface-gain geometry allows unprecedented accessibilities to multi-functionalize the gain, enabling electrically pumped operation. Our scheme is scalable and compatible with integrated photonics for on-chip optical communication technologies.

cond-mat.mes-hall↗

arXiv2015

Theory of low power ultra-broadband terahertz sideband generation in bi-layer graphene

In a semiconductor illuminated by a strong terahertz field, optically excited electron-hole pairs can recombine to emit light in a broad frequency comb evenly spaced by twice the terahertz frequency. Such high-order terahertz sideband generation is of interest both as an example of extreme nonlinear optics and also as a method for ultrafast electro-optical modulation. So far, this phenomenon has only been observed with large field strengths (~10 kVcm-1), an obstacle for technological applications. Here we predict that bi-layer graphene generates high-order sidebands at much weaker terahertz fields. We find that a terahertz field of strength 1 kVcm-1 can produce a high-sideband spectrum of about 30 THz, 100 times broader than in GaAs. The sidebands are generated despite the absence of classical collisions, with the quantum coherence of the electron-hole pairs enabling recombination. These remarkable features lower the barrier to desktop electro-optical modulation at terahertz frequencies, facilitating ultrafast optical communications.

cond-mat.mes-hall↗

arXiv2014

Single Quantum Emitters in Monolayer Semiconductors

Single quantum emitters (SQEs) are at the heart of quantum optics and photonic quantum information technologies. To date, all demonstrated solid-state single-photon sources are confined in three-dimensional materials. Here, we report a new class of SQEs based on excitons that are spatially localized by defects in two-dimensional tungsten-diselenide monolayers. The optical emission from these SQEs shows narrow linewidths of ~0.13 meV, about two orders of magnitude smaller than that of delocalized valley excitons. Second-order correlation measurements reveal strong photon anti-bunching, unambiguously establishing the single photon nature of the emission. The SQE emission shows two non-degenerate transitions, which are cross-linearly polarized. We assign this fine structure to two excitonic eigen-modes whose degeneracy is lifted by a large ~0.71 meV coupling, likely due to the electron-hole exchange interaction in presence of anisotropy. Magneto-optical measurements also reveal an exciton g-factor of ~8.7, several times larger than that of delocalized valley excitons. In addition to their fundamental importance, establishing new SQEs in 2D quantum materials could give rise to practical advantages in quantum information processing, such as efficient photon extraction and high integratability and scalability.

cond-mat.mes-hall↗

arXiv2014

Highly Anisotropic and Robust Excitons in Monolayer Black Phosphorus

Semi-metallic graphene and semiconducting monolayer transition metal dichalcogenides (TMDCs) are the two-dimensional (2D) materials most intensively studied in recent years. Recently, black phosphorus emerged as a promising new 2D material due to its widely tunable and direct bandgap, high carrier mobility and remarkable in-plane anisotropic electrical, optical and phonon properties. However, current progress is primarily limited to its thin-film form, and its unique properties at the truly 2D quantum confinement have yet to be demonstrated. Here, we reveal highly anisotropic and tightly bound excitons in monolayer black phosphorus using polarization-resolved photoluminescence measurements at room temperature. We show that regardless of the excitation laser polarization, the emitted light from the monolayer is linearly polarized along the light effective mass direction and centers around 1.3 eV, a clear signature of emission from highly anisotropic bright excitons. In addition, photoluminescence excitation spectroscopy suggests a quasiparticle bandgap of 2.2 eV, from which we estimate an exciton binding energy of around 0.9 eV, consistent with theoretical results based on first-principles. The experimental observation of highly anisotropic, bright excitons with exceedingly large binding energy not only opens avenues for the future explorations of many-electron effects in this unusual 2D material, but also suggests a promising future in optoelectronic devices such as on-chip infrared light sources.

cond-mat.mes-hall↗