arXiv subjects

Chenhao Jin

Publications and source records attributed to Chenhao Jin.

34 records · Page 2Linked to original sources

arXiv2019

Resolving spin, valley, and moiré quasi-angular momentum of interlayer excitons in WSe2/WS2 heterostructures

Moiré superlattices provide a powerful way to engineer properties of electrons and excitons in two-dimensional van der Waals heterostructures. The moiré effect can be especially strong for interlayer excitons, where electrons and holes reside in different layers and can be addressed separately. In particular, it was recently proposed that the moiré superlattice potential not only localizes interlayer exciton states at different superlattice positions, but also hosts an emerging moiré quasi-angular momentum (QAM) that periodically switches the optical selection rules for interlayer excitons at different moiré sites. Here we report the observation of multiple interlayer exciton states coexisting in a WSe2/WS2 moiré superlattice and unambiguously determine their spin, valley, and moiré QAM through novel resonant optical pump-probe spectroscopy and photoluminescence excitation spectroscopy. We demonstrate that interlayer excitons localized at different moiré sites can exhibit opposite optical selection rules due to the spatially-varying moiré QAM. Our observation reveals new opportunities to engineer interlayer exciton states and valley physics with moiré superlattices for optoelectronic and valleytronic applications.

cond-mat.mes-hall↗

arXiv2018

Observation of Moiré Excitons in WSe2/WS2 Heterostructure Superlattices

Moiré superlattices provide a powerful tool to engineer novel quantum phenomena in two-dimensional (2D) heterostructures, where the interactions between the atomically thin layers qualitatively change the electronic band structure of the superlattice. For example, mini-Dirac points, tunable Mott insulator states, and the Hofstadter butterfly can emerge in different types of graphene/boron nitride moiré superlattices, while correlated insulating states and superconductivity have been reported in twisted bilayer graphene moiré superlattices. In addition to their dramatic effects on the single particle states, moiré superlattices were recently predicted to host novel excited states, such as moiré exciton bands. Here we report the first observation of moiré superlattice exciton states in nearly aligned WSe2/WS2 heterostructures. These moiré exciton states manifest as multiple emergent peaks around the original WSe2 A exciton resonance in the absorption spectra, and they exhibit gate dependences that are distinctly different from that of the A exciton in WSe2 monolayers and in large-twist-angle WSe2/WS2 heterostructures. The observed phenomena can be described by a theoretical model where the periodic moiré potential is much stronger than the exciton kinetic energy and creates multiple flat exciton minibands. The moiré exciton bands provide an attractive platform to explore and control novel excited state of matter, such as topological excitons and a correlated exciton Hubbard model, in transition metal dichalcogenides.

cond-mat.mes-hall↗

arXiv2018

Revealing the Biexciton and Trion-exciton Complexes in BN Encapsulated WSe2

Strong Coulomb interactions in single-layer transition metal dichalcogenides (TMDs) result in the emergence of strongly bound excitons, trions and biexcitons. These excitonic complexes possess the valley degree of freedom, which can be exploited for quantum optoelectronics. However, in contrast to the good understanding of the exciton and trion properties, the binding energy of the biexciton remains elusive, with theoretical calculations and experimental studies reporting discrepant results. In this work, we resolve the conflict by employing low-temperature photoluminescence spectroscopy to identify the biexciton state in BN encapsulated single-layer WSe2. The biexciton state only exists in charge neutral WSe2, which is realized through the control of efficient electrostatic gating. In the lightly electron-doped WSe2, one free electron binds to a biexciton and forms the trion-exciton complex. Improved understanding of the biexciton and trion-exciton complexes paves the way for exploiting the many-body physics in TMDs for novel optoelectronics applications.

cond-mat.mes-hall↗

arXiv2018

Predicting Webpage Aesthetics with Heatmap Entropy

Today, eye trackers are extensively used in user interface evaluations. However, it's still hard to analyze and interpret eye tracking data from the aesthetic point of view. To find quantitative links between eye movements and aesthetic experience, we tracked 30 observers' initial landings for 40 web pages (each displayed for 3 seconds). The web pages were also rated based on the observers' subjective aesthetic judgments. Shannon entropy was introduced to analyze the eye-tracking data. The result shows that the heatmap entropy (visual attention entropy, VAE) is highly correlated with the observers' aesthetic judgements of the web pages. Its improved version, relative VAE (rVAE), has a more significant correlation with the perceived aesthetics. (r=-0.65, F= 26.84, P$<$0.0001). This single metric alone can distinguish between good- and bad-looking pages with an approximate 85\% accuracy. Further investigation reveals that the performance of both VAE and rVAE became stable after 1 second. The curves indicate that their performances could be better, if the tracking time was extended beyond 3 seconds.

cs.HC↗

arXiv2016

Observation of Ultralong Valley Lifetime in WSe2/MoS2 Heterostructures

The valley degree of freedom in two-dimensional (2D) crystals recently emerged as a novel information carrier in addition to spin and charge. The intrinsic valley lifetime in 2D transition metal dichalcoginides (TMD) is expected to be remarkably long due to the unique spin-valley locking behavior, where the inter-valley scattering of electron requires simultaneously a large momentum transfer to the opposite valley and a flip of the electron spin. The experimentally observed valley lifetime in 2D TMDs, however, has been limited to tens of nanoseconds so far. Here we report efficient generation of microsecond-long lived valley polarization in WSe2/MoS2 heterostructures by exploiting the ultrafast charge transfer processes in the heterostructure that efficiently creates resident holes in the WSe2 layer. These valley-polarized holes exhibit near unity valley polarization and ultralong valley lifetime: we observe a valley-polarized hole population lifetime of over 1 us, and a valley depolarization lifetime (i.e. inter-valley scattering lifetime) over 40 us at 10 Kelvin. The near-perfect generation of valley-polarized holes in TMD heterostructures with ultralong valley lifetime, orders of magnitude longer than previous results, opens up new opportunities for novel valleytronics and spintronics applications.

cond-mat.mtrl-sci↗

arXiv2016

Electronic Structure, Surface Doping, and Optical Response in Epitaxial WSe2 Thin Films

High quality WSe2 films have been grown on bilayer graphene (BLG) with layer-by-layer control of thickness using molecular beam epitaxy (MBE). The combination of angle-resolved photoemission (ARPES), scanning tunneling microscopy/spectroscopy (STM/STS), and optical absorption measurements reveal the atomic and electronic structures evolution and optical response of WSe2/BLG. We observe that a bilayer of WSe2 is a direct bandgap semiconductor, when integrated in a BLG-based heterostructure, thus shifting the direct-indirect band gap crossover to trilayer WSe2. In the monolayer limit, WSe2 shows a spin-splitting of 475 meV in the valence band at the K point, the largest value observed among all the MX2 (M = Mo, W; X = S, Se) materials. The exciton binding energy of monolayer-WSe2/BLG is found to be 0.21 eV, a value that is orders of magnitude larger than that of conventional 3D semiconductors, yet small as compared to other 2D transition metal dichalcogennides (TMDCs) semiconductors. Finally, our finding regarding the overall modification of the electronic structure by an alkali metal surface electron doping opens a route to further control the electronic properties of TMDCs.

cond-mat.mtrl-sci↗

arXiv2016

Direct Observation of Layer-Dependent Electronic Structure in Phosphorene

Phosphorene, a single atomic layer of black phosphorus, has recently emerged as a new twodimensional (2D) material that holds promise for electronic and photonic technology. Here we experimentally demonstrate that the electronic structure of few-layer phosphorene varies significantly with the number of layers, in good agreement with theoretical predictions. The interband optical transitions cover a wide, technologically important spectrum range from visible to mid-infrared. In addition, we observe strong photoluminescence in few-layer phosphorene at energies that match well with the absorption edge, indicating they are direct bandgap semiconductors. The strongly layer-dependent electronic structure of phosphorene, in combination with its high electrical mobility, gives it distinct advantages over other twodimensional materials in electronic and opto-electronic applications.

cond-mat.mtrl-sci↗

arXiv2015

Amplitude- and phase-resolved nano-spectral imaging of phonon polaritons in hexagonal boron nitride

Phonon polaritons are quasiparticles resulting from strong coupling of photons with optical phonons. Excitation and control of these quasiparticles in 2D materials offer the opportunity to confine and transport light at the nanoscale. Here, we image the phonon polariton (PhP) spectral response in thin hexagonal boron nitride (hBN) crystals as a representative 2D material using amplitude- and phase-resolved near-field interferometry with broadband mid-IR synchrotron radiation. The large spectral bandwidth enables the simultaneous measurement of both out-of-plane (780 cm-1) and in-plane (1370 cm-1) hBN phonon modes. In contrast to the strong and dispersive in-plane mode, the out-of-plane mode PhP response is weak. Measurements of the PhP wavelength reveal a proportional dependence on sample thickness for thin hBN flakes, which can be understood by a general model describing two-dimensional polariton excitation in ultrathin materials.

cond-mat.mes-hall↗

arXiv2014

Ultrafast Charge Transfer in Atomically Thin MoS2/WS2 Heterostructures

Van der Waals heterostructures have recently emerged as a new class of materials, where quantum coupling between stacked atomically thin two-dimensional (2D) layers, including graphene, hexagonal-boron nitride, and transition metal dichalcogenides (MX2), give rise to fascinating new phenomena. MX2 heterostructures are particularly exciting for novel optoelectronic and photovoltaic applications, because 2D MX2 monolayers can have an optical bandgap in the near-infrared to visible spectral range and exhibit extremely strong light-matter interactions. Theory predicts that many stacked MX2 heterostructures form type-II semiconductor heterojunctions that facilitate efficient electron-hole separation for light detection and harvesting. Here we report the first experimental observation of ultrafast charge transfer in photo-excited MoS2/WS2 heterostructures using both photoluminescence mapping and femtosecond (fs) pump-probe spectroscopy. We show that hole transfer from the MoS2 layer to the WS2 layer takes place within 50 fs after optical excitation, a remarkable rate for van der Waals coupled 2D layers. Such ultrafast charge transfer in van der Waals heterostructures can enable novel 2D devices for optoelectronics and light harvesting.

cond-mat.mes-hall↗

arXiv2014

Ultrafast Generation of Pseudo-magnetic Field for Valley Excitons in WSe2 Monolayers

A new degree of freedom, the valley pseudospin, emerges in atomically thin two-dimensional transition metal dichalcogenides (MX2) and has attracted great scientific interest. The capability to manipulate the valley pseudospin, in analogy to the control of spin in spintronics, can open up exciting opportunities in valleytronics. Here we demonstrate that an ultrafast and ultrahigh valley pseudomagnetic field can be generated using circularly polarized femtosecond pulses to selectively control the valley degree of freedom in monolayer MX2. Employing ultrafast pump-probe spectroscopy, we observed a pure and valley-selective optical Stark effect in WSe2 monolayers from the non-resonant pump, which instantaneously lift the degeneracy of valley exciton transitions without any dissipation. The strength of the optical Stark effect scales linearly with both the pump intensity and the inverse of pump detuning. An energy splitting more than 10 meV between the K and K_prime valley transitions can be achieved, which corresponds to an effective pseudomagnetic field over 170 Tesla. Our study demonstrates efficient and ultrafast control of the valley excitons with optical light, and opens up the possibility to coherent manipulate the valley polarization for quantum information applications.

cond-mat.mes-hall↗

arXiv2014

Evolution of Interlayer Coupling in Twisted MoS2 Bilayers

Van der Waals (vdW) coupling is emerging as a powerful method to engineer and tailor physical properties of atomically thin two-dimensional (2D) materials. In graphene/graphene and graphene/boron-nitride structures it leads to interesting physical phenomena ranging from new van Hove singularities1-4 and Fermi velocity renormalization5, 6 to unconventional quantum Hall effects7 and Hofstadter's butterfly pattern8-12. 2D transition metal dichalcogenides (TMDCs), another system of predominantly vdW-coupled atomically thin layers13, 14, can also exhibit interesting but different coupling phenomena because TMDCs can be direct or indirect bandgap semiconductors15, 16. Here, we present the first study on the evolution of interlayer coupling with twist angles in as-grown MoS2 bilayers. We find that an indirect bandgap emerges in bilayers with any stacking configuration, but the bandgap size varies appreciably with the twist angle: it shows the largest redshift for AA- and AB-stacked bilayers, and a significantly smaller but constant redshift for all other twist angles. The vibration frequency of the out-of-plane phonon in MoS2 shows similar twist angle dependence. Our observations, together with ab initio calculations, reveal that this evolution of interlayer coupling originates from the repulsive steric effects, which leads to different interlayer separations between the two MoS2 layers in different stacking configurations.

cond-mat.mes-hall↗

arXiv2014

Gate-dependent Pseudospin Mixing in Graphene/Boron Nitride Moire Superlattices

Electrons in graphene are described by relativistic Dirac-Weyl spinors with a two-component pseudospin1-12. The unique pseudospin structure of Dirac electrons leads to emerging phenomena such as the massless Dirac cone2, anomalous quantum Hall effect2, 3, and Klein tunneling4, 5 in graphene. The capability to manipulate electron pseudospin is highly desirable for novel graphene electronics, and it requires precise control to differentiate the two graphene sub-lattices at atomic level. Graphene/boron nitride (graphene/BN) Moire superlattice, where a fast sub-lattice oscillation due to B-N atoms is superimposed on the slow Moire period, provides an attractive approach to engineer the electron pseudospin in graphene13-18. This unusual Moire superlattice leads to a spinor potential with unusual hybridization of electron pseudospins, which can be probed directly through infrared spectroscopy because optical transitions are very sensitive to excited state wavefunctions. Here, we perform micro-infrared spectroscopy on graphene/BN heterostructure and demonstrate that the Moire superlattice potential is dominated by a pseudospin-mixing component analogous to a spatially varying pseudomagnetic field. In addition, we show that the spinor potential depends sensitively on the gate-induced carrier concentration in graphene, indicating a strong renormalization of the spinor potential from electron-electron interactions. Our study offers deeper understanding of graphene pseudospin structure under spinor Moire potential, as well as exciting opportunities to control pseudospin in two-dimensional heterostructures for novel electronic and photonic nanodevices.

cond-mat.mes-hall↗

arXiv2014

Quasi-1D graphene superlattices formed on high index surfaces

We report preparation of large area quasi-1D monolayer graphene superlattices on a prototypical high index surface Cu(410)-O and characterization by Raman spectroscopy, Auger electron spectroscopy (AES), low energy electron diffraction (LEED), scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). The periodically stepped substrate gives a 1D modulation to graphene, forming a superlattice of the same super-periodicity. Consequently the moire pattern is also quasi-1D, with a different periodicity. Scanning tunneling spectroscopy measurements revealed new Dirac points formed at the superlattice Brillouin zone boundary as predicted by theories.

cond-mat.mtrl-sci↗

arXiv2013

Systematic Determination of Absolute Absorption Cross-section of Individual Carbon Nanotubes

Determination of optical absorption cross-section is always among the central importance of understanding a material. However its realization on individual nanostructures, such as carbon nanotubes, is experimentally challenging due to the small extinction signal using conventional transmission measurements. Here we develop a technique based on polarization manipulation to enhance the sensitivity of single-nanotube absorption spectroscopy by two-orders of magnitude. We systematically determine absorption cross-section over broad spectral range at single-tube level for more than 50 chirality-defined single-walled nanotubes. Our data reveals chirality-dependent one-dimensional photo-physics through the behaviours of exciton oscillator strength and lifetime. We also establish an empirical formula to predict absorption spectrum of any nanotube, which provides the foundation to determine quantum efficiencies in important photoluminescence and photovoltaic processes.

cond-mat.mes-hall↗

arXiv2013

High-throughput Imaging and Spectroscopy of Individual Carbon Nanotubes in Devices with Light Microscopy

Two paramount challenges in carbon nanotube research are achieving chirality-controlled synthesis and understanding chirality-dependent device physics. High-throughput and in-situ chirality and electronic structural characterization of individual carbon nanotubes is crucial for addressing these challenges. Optical imaging and spectroscopy has unparalleled throughput and specificity, but its realization for single nanotubes on substrates or in devices has long been an outstanding challenge. Here we demonstrate video-rate imaging and in-situ spectroscopy of individual carbon nanotubes on various substrates and in functional devices using a novel high-contrast polarization-based optical microscopy. Our technique enables the complete chirality profiling of hundreds of as-grown carbon nanotubes. In addition, we in-situ monitor nanotube electronic structure in active field-effect devices, and observe that high-order nanotube optical resonances are dramatically broadened by electrostatic doping. This unexpected behaviour points to strong interband electron-electron scattering processes that can dominate ultrafast dynamics of excited states in carbon nanotubes.

cond-mat.mes-hall↗

arXiv2012

Opposite Changes in Gap Width of Opposite Spin States Induced by Rashba Effect in Anti-ferromagnetic Graphene on Ni(111)

Graphene is a promising candidate for applications in spintronics. In this paper, Density Functional Theory method is used to calculate the band structure and magnetic properties of graphene on Ni(111). Our results show that once there is antiferromagnetic order in graphene, an external electric field at the order of 10^9 V/m can induce a gap width difference of tens of meV for opposite spin states near the Fermi surface.

cond-mat.mtrl-sci↗