arXiv subjects

Kaihui Liu

Publications and source records attributed to Kaihui Liu.

At least 73 records · Page 4Linked to original sources

arXiv2019

Atomic Imaging of Mechanically Induced Topological Transition of Ferroelectric Vortices

Ferroelectric vortices formed through complex lattice-charge interactions have great potential in applications for future nanoelectronics such as memories. For practical applications, it is crucial to manipulate these topological states under external stimuli. Here, we apply mechanical loads to locally manipulate the vortices in a PbTiO3-SrTiO3 superlattice via atomically resolved in situ scanning transmission electron microscopy. The vortices undergo a transition to the a-domain with in-plane polarization under external compressive stress and spontaneously recover after removal of the stress. We reveal the detailed transition process at the atomic scale and reproduce this numerically using phase-field simulations. These findings provide new pathways to control the exotic topological ferroelectric structures for future nanoelectronics and also valuable insights into understanding of lattice-charge interactions at nanoscale.

cond-mat.mtrl-sci↗

arXiv2019

Band Structure Engineering of Interfacial Semiconductors Based on Atomically Thin Lead Iodide Crystals

To explore new constituents in two-dimensional materials and to combine their best in van der Waals heterostructures, are in great demand as being unique platform to discover new physical phenomena and to design novel functionalities in interface-based devices. Herein, PbI2 crystals as thin as few-layers are first synthesized, particularly through a facile low-temperature solution approach with the crystals of large size, regular shape, different thicknesses and high-yields. As a prototypical demonstration of flexible band engineering of PbI2-based interfacial semiconductors, these PbI2 crystals are subsequently assembled with several transition metal dichalcogenide monolayers. The photoluminescence of MoS2 is strongly enhanced in MoS2/PbI2 stacks, while a dramatic photoluminescence quenching of WS2 and WSe2 is revealed in WS2/PbI2 and WSe2/PbI2 stacks. This is attributed to the effective heterojunction formation between PbI2 and these monolayers, but type I band alignment in MoS2/PbI2 stacks where fast-transferred charge carriers accumulate in MoS2 with high emission efficiency, and type II in WS2/PbI2 and WSe2/PbI2 stacks with separated electrons and holes suitable for light harvesting. Our results demonstrate that MoS2, WS2, WSe2 monolayers with very similar electronic structures themselves, show completely distinct light-matter interactions when interfacing with PbI2, providing unprecedent capabilities to engineer the device performance of two-dimensional heterostructures.

cond-mat.mes-hall↗

arXiv2018

Doping Induced Second Harmonic Generation in Centrosymmetric Graphene from Quadrupole Response

For centrosymmetric materials such as monolayer graphene, no optical second harmonic generation (SHG) is generally expected because it is forbidden under the electric-dipole approximation. Yet we observed a strong, doping induced SHG from graphene, with its highest strength comparable to the electric-dipole allowed SHG in non-centrosymmetric 2D materials. This novel SHG has the nature of an electric-quadrupole response, arising from the effective breaking of inversion symmetry by optical dressing with an in-plane photon wave vector. More remarkably, the SHG is widely tuned by carrier doping or chemical potential, being sharply enhanced at Fermi edge resonances, but vanishing at the charge neutral point that manifests the electron-hole symmetry of massless Dirac Fermions. The striking behavior in graphene, which should also arise in graphene-like Dirac materials, expands the scope of nonlinear optics, and holds the promise of novel optoelectronic and photonic applications.

cond-mat.mes-hall↗

arXiv2018

Study of electron emission from 1D nanomaterials under super high field

Photoemission driven by a strong electric field of near-infrared or visible light, referred to as strong-field photoemission, produces attosecond electron pulses that are synchronized to the waveform of the incident light, and this principle lies at the heart of current attosecond technologies. However, full access to strong-field photoemission regimes at near-infrared wavelengths based on solid-state materials is restricted by space-charge screening and material damage at high optical-field strengths, which significantly hampers the realization of predicted attosecond technologies, such as ultra-sensitive optical phase modulation. Here, we demonstrate a new type of strong-field photoemission behaviour with extreme nonlinearity -- photoemission current scales follow a 40th power law of the optical-field strength, making use of sub-nanometric carbon nanotubes and 800 nm pulses. As a result, the total photoemission current depends on the carrier-envelope phase with a greatly improved photoemission current modulation depth of up to 100%, which has not previously been achieved. Time-dependent density functional calculations reveal the completely new behaviour of the optical-field induced tunnelling emission process directly from the valence band of the carbon nanotubes, which is an indication of full access to a strong-field photoemission regime. Furthermore, the nonlinear dynamics are observed to be tunable by changing the binding energy of the valence-band-maximum, as confirmed by Simpleman model calculations. We believe that such extreme nonlinear photoemission from nanotips offers a new means of producing extreme temporal-spatial resolved electron pulses. These results additionally provide a new design philosophy for attosecond electronics and optics by making use of tunable band structures in nanomaterials.

physics.optics↗

arXiv2018

Towards the growth of single-crystal boron nitride monolayer on Cu

Atom-layered hexagonal boron nitride (hBN), with excellent stability, flat surface and large bandgap, has been reported to be the best 2D insulator to open up the great possibilities for exciting potential applications in electronics, optoelectronics and photovoltaics. The ability to grow high-quality large single crystals of hBN is at the heart for those applications, but the size of single-crystal 2D BN is less than a millimetre till now. Here, we report the first epitaxial growth of a 10*10 cm2 single-crystal hBN monolayer on a low symmetry Cu(110) "vicinal surface". The growth kinetics, unidirectional alignment and seamless stitching of hBN domains are unambiguously illustrated using centimetre- to the atomic-scale characterization techniques. The findings in this work are expected to significantly boost the massive applications of 2D materials-based devices, and also pave the way for the epitaxial growth of broad non-centrosymmetric 2D materials.

cond-mat.mtrl-sci↗

arXiv2018

Low-Rank Phase Retrieval via Variational Bayesian Learning

In this paper, we consider the problem of low-rank phase retrieval whose objective is to estimate a complex low-rank matrix from magnitude-only measurements. We propose a hierarchical prior model for low-rank phase retrieval, in which a Gaussian-Wishart hierarchical prior is placed on the underlying low-rank matrix to promote the low-rankness of the matrix. Based on the proposed hierarchical model, a variational expectation-maximization (EM) algorithm is developed. The proposed method is less sensitive to the choice of the initialization point and works well with random initialization. Simulation results are provided to illustrate the effectiveness of the proposed algorithm.

stat.ML↗

arXiv2018

Atomic Origin of Ti Deficient Dislocation in SrTiO3 Bicrystal and Their Electronic Structures

Dislocations in perovskite oxides have important impacts on their physical and chemical properties, which are determined by their unique atomic environments. In the present study, the structure of dislocations in a 10° low-angle grain boundary of SrTiO3 (STO) is characterized by spherical aberration corrected scanning transmission electron microscopy (Cs-STEM) and spectroscopy. In contrast to previous studies, the deficiency instead of enrichment of titanium (Ti) is observed at the dislocation cores mainly due to the Sr substitution and under occupancy of Ti. The presence of oxygen vacancies and partially reduced Ti are also detected at the Ti deficient dislocations cores. These findings indicate the atomic structure of dislocations can be very different even they have the same Burges vectors. Controllable elemental segregation in the dislocations and grain boundaries via bicrystal engineering should be very useful for design of devices with novel functions.

cond-mat.mtrl-sci↗

arXiv2017

Ultrafast, highly-sensitive infrared photodetectors based on two-dimensional oxyselenide crystals

Infrared detection and sensing is deeply embedded in modern technology and human society and its development has always been benefitting from the discovery of new photoelectric response materials. The rise of two-dimensional (2D) materials, thanks to their distinct electronic structure, extreme dimensional confinement and strong light-matter interactions, provides new material platform for next-generation infrared photodetection. Ideal infrared detectors should have fast respond, high sensitivity and air-stability, which is rare to meet at the same time for all existing 2D materials, either graphene, transition metal dichalcogenide or black phosphorous. Herein we demonstrate a new infrared photodetector based on 2D Bi2O2Se crystals, whose main characteristics are superb in the whole 2D family: high sensitivity of ~65 A/W at 1200 nm and ultrafast intrinsic photoresponse of ~1 ps at room temperature. Such great performance is attributed to the suitable electronic bandgap and high carrier mobility of 2D oxyselenide. With additional merits of mass production, excellent stability and flexibility, 2D oxyselenide detectors should open new avenues in highly-sensitive, high-speed, low-cost, flexible infrared photodetection and imaging.

cond-mat.mtrl-sci↗

arXiv2017

DOA and Polarization Estimation for Non-Circular Signals in 3-D Millimeter Wave Polarized Massive MIMO Systems

In this paper, an algorithm of multiple signal classification (MUSIC) is proposed for two-dimensional (2-D) direction of- arrival (DOA) and polarization estimation of non-circular signal in three-dimensional (3-D) millimeter wave polarized largescale/ massive multiple-input-multiple-output (MIMO) systems. The traditional MUSIC-based algorithms can estimate either the DOA and polarization for circular signal or the DOA for non-circular signal by using spectrum search. By contrast, in the proposed algorithm only the DOA estimation needs spectrum search, and the polarization estimation has a closedform expression. First, a novel dimension-reduced MUSIC (DRMUSIC) is proposed for DOA and polarization estimation of circular signal with low computational complexity. Next, based on the quaternion theory, a novel algorithm named quaternion non-circular MUSIC (QNC-MUSIC) is proposed for parameter estimation of non-circular signal with high estimation accuracy. Then based on the DOA estimation result using QNC-MUSIC, the polarization estimation of non-circular signal is acquired by using the closed-form expression of the polarization estimation in DR-MUSIC. In addition, the computational complexity analysis shows that compared with the conventional DOA and polarization estimation algorithms, our proposed QNC-MUSIC and DRMUSIC have much lower computational complexity, especially when the source number is large. The stochastic Cramer-Rao Bound (CRB) for the estimation of the 2-D DOA and polarization parameters of the non-circular signals is derived as well. Finally, numerical examples are provided to demonstrate that the proposed algorithms can improve the parameter estimation performance when the large-scale/massive MIMO systems are employed.

eess.SP↗

arXiv2017

Gate tunable third-order nonlinear optical response of massless Dirac fermions in graphene

Materials with massless Dirac fermions can possess exceptionally strong and widely tunable optical nonlinearities. Experiments on graphene monolayer have indeed found very large third-order nonlinear responses, but the reported variation of the nonlinear optical coefficient by orders of magnitude is not yet understood. A large part of the difficulty is the lack of information on how doping or chemical potential affects the different nonlinear optical processes. Here we report the first experimental study, in corroboration with theory, on third harmonic generation (THG) and four-wave mixing (FWM) in graphene that has its chemical potential tuned by ion-gel gating. THG was seen to have enhanced by ~30 times when pristine graphene was heavily doped, while difference-frequency FWM appeared just the opposite. The latter was found to have a strong divergence toward degenerate FWM in undoped graphene, leading to a giant third-order nonlinearity. These truly amazing characteristics of graphene come from the possibility to gate-control the chemical potential, which selectively switches on and off one- and multi-photon resonant transitions that coherently contribute to the optical nonlinearity, and therefore can be utilized to develop graphene-based nonlinear optoelectronic devices.

cond-mat.mes-hall↗

arXiv2017

Bayesian Compressive Sensing Using Normal Product Priors

In this paper, we introduce a new sparsity-promoting prior, namely, the "normal product" prior, and develop an efficient algorithm for sparse signal recovery under the Bayesian framework. The normal product distribution is the distribution of a product of two normally distributed variables with zero means and possibly different variances. Like other sparsity-encouraging distributions such as the Student's $t$-distribution, the normal product distribution has a sharp peak at origin, which makes it a suitable prior to encourage sparse solutions. A two-stage normal product-based hierarchical model is proposed. We resort to the variational Bayesian (VB) method to perform the inference. Simulations are conducted to illustrate the effectiveness of our proposed algorithm as compared with other state-of-the-art compressed sensing algorithms.

stat.ML↗

arXiv2017

Ultrafast Epitaxial Growth of Metre-Sized Single-Crystal Graphene on Industrial Cu Foil

A foundation of the modern technology that uses single-crystal silicon has been the growth of high-quality single-crystal Si ingots with diameters up to 12 inches or larger. For many applications of graphene, large-area high-quality (ideally of single-crystal) material will be enabling. Since the first growth on copper foil a decade ago, inch-sized single-crystal graphene has been achieved. We present here the growth, in 20 minutes, of a graphene film of 5 x 50 cm2 dimension with > 99% ultra-highly oriented grains. This growth was achieved by: (i) synthesis of sub-metre-sized single-crystal Cu(111) foil as substrate; (ii) epitaxial growth of graphene islands on the Cu(111) surface; (iii) seamless merging of such graphene islands into a graphene film with high single crystallinity and (iv) the ultrafast growth of graphene film. These achievements were realized by a temperature-driven annealing technique to produce single-crystal Cu(111) from industrial polycrystalline Cu foil and the marvellous effects of a continuous oxygen supply from an adjacent oxide. The as-synthesized graphene film, with very few misoriented grains (if any), has a mobility up to ~ 23,000 cm2V-1s-1 at 4 K and room temperature sheet resistance of ~ 230 ohm/square. It is very likely that this approach can be scaled up to achieve exceptionally large and high-quality graphene films with single crystallinity, and thus realize various industrial-level applications at a low cost.

cond-mat.mtrl-sci↗

arXiv2017

Ultrafast field-driven monochromatic photoemission from carbon nanotubes

Ultrafast electron pulses, combined with laser-pump and electron-probe technologies, allow for various forms of ultrafast microscopy and spectroscopy to elucidate otherwise challenging to observe physical and chemical transitions. However, the pursuit of simultaneous ultimate spatial and temporal resolution has been largely subdued by the low monochromaticity of the electron pulses and their poor phase synchronization to the optical excitation pulses. State-of-the-art photon-driven sources have good monochromaticity but poor phase synchronization. In contrast, field-driven photoemission has much higher light phase synchronization, due to the intrinsic sub-cycle emission dynamics, but poor monochromaticity. Such sources suffer from larger electron energy spreads (3 - 100 eV) attributed to the relatively low field enhancement of the conventional metal tips which necessitates long pump wavelengths (> 800 nm) in order to gain sufficient ponderomotive potential to access the field-driven regime. In this work, field-driven photoemission from ~1 nm radius carbon nanotubes excited by a femtosecond laser at a short wavelength of 410 nm has been realized. The energy spread of field-driven electrons is effectively compressed to 0.25 eV outperforming all conventional ultrafast electron sources. Our new nanotube-based ultrafast electron source opens exciting prospects for attosecond imaging and emerging light-wave electronics.

physics.optics↗

arXiv2016

High-resolution Collinear Chiral Sum Frequency Generation Microscopy by Using Vectorial Beam

In chiral sum frequency generation (C-SFG), the chiral nature of $χ^{(2)}$ requires the three involved electric fields to be pairwise non-parallel, leading to the traditional non-collinear configuration which is a hindrance for achieving diffraction limited resolution while utilizing it as a label-free imaging contrast mechanism . Here we propose a collinear C-SFG (CC-SFG) microscopy modality by using longitudinal z-polarized vectorial field. Label-free chiral imaging with enhanced spatial resolution (~1.4 times improvement in one lateral and the longitudinal directions over the traditional non-collinear scheme) is demonstrated, providing a new path for SFG microscopy with diffraction-limited resolution for mapping chirality.

physics.optics↗

arXiv2016

Monitoring Mechanical Motion of Carbon Nanotube based Nanomotor by Optical Absorption Spectrum

The optical absorption spectrums of nanomotors made from double-wall carbon nanotubes have been calculated with the time-dependent density functional based tight binding method. When the outer short tube of the nanomotor moves along or rotates around the inner long tube, the peaks in the spectrum will gradually evolve and may shift periodically, the amplitude of which can be as large as hundreds of meV. We show that the features and behaviors of the optical absorption spectrum could be used to monitor the mechanical motions of the double-wall carbon nanotube based nanomotor.

cond-mat.mes-hall↗

arXiv2016

Far-field nanoscale infrared spectroscopy of vibrational fingerprints of molecules with graphene plasmons

Infrared spectroscopy, especially for molecular vibrations in the fingerprint region between 600 and 1500 cm-1, is a powerful characterization method for bulk materials. However, molecular fingerprinting at the nanoscale level still remains a significant challenge, due to weak light-matter interaction between micron-wavelengthed infrared light and nano-sized molecules. Here, we demonstrate molecular fingerprinting at the nanoscale level using our specially designed graphene plasmonic structure on CaF2 nanofilm. This structure not only avoids the plasmon-phonon hybridization, but also provides in situ electrically-tunable graphene plasmon covering the entire infrared fingerprint region, which was previously unattainable. In addition, undisturbed and highly-confined graphene plasmon offers simultaneous detection of in-plane and out-of-plane vibrational modes with ultrahigh detection sensitivity down to the sub-monolayer level, significantly pushing the current detection limit of far-field mid-infrared spectroscopy. Our results provide a platform, fulfilling the long-awaited expectation of high sensitivity and selectivity far-field fingerprint detection of nano-scale molecules for numerous applications.

physics.optics↗

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↗

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↗