arXiv subjects

Qihua Xiong

Publications and source records attributed to Qihua Xiong.

52 records · Page 3Linked to original sources

arXiv2018

Optical spin pumping induced pseudo-magnetic field in two dimensional heterostructures

Two dimensional heterostructures are likely to provide new avenues for the manipulation of magnetization that is crucial for spintronics or magnetoelectronics. Here, we demonstrate that optical spin pumping can generate a large effective magnetic field in two dimensional MoSe2/WSe2 heterostructures. We determine the strength of the generated field by polarization-resolved measurement of the interlayer exciton photoluminescence spectrum: the measured splitting exceeding 10 milli-electron volts (meV) between the emission originating from the two valleys corresponds to an effective magnetic field of ~ 30 T. The strength of this optically induced field can be controlled by the excitation light polarization. Our finding opens up new possibilities for optically controlled spintronic devices based on van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2018

Highly efficient visible colloidal lead-halide perovskite nanocrystal light-emitting diodes

Lead-halide perovskites have been attracting attention for potential use in solid-state lighting. Following the footsteps of solar cells, the field of perovskite light-emitting diodes (PeLEDs) has been growing rapidly. Their application prospects in lighting, however, remain still uncertain due to a variety of shortcomings in device performance including their limited levels of luminous efficiency achievable thus far. Here we show high-efficiency PeLEDs based on colloidal perovskite nanocrystals (PeNCs) synthesized at room temperature possessing dominant first-order excitonic radiation (enabling a photoluminescence quantum yield of 71% in solid film), unlike in the case of bulk perovskites with slow electron-hole bimolecular radiative recombination (a second-order process). In these PeLEDs, by reaching charge balance in the recombination zone, we find that the Auger nonradiative recombination, with its significant role in emission quenching, is effectively suppressed in low driving current density range. In consequence, these devices reach a record high maximum external quantum efficiency of 12.9% reported to date and an unprecedentedly high power efficiency of 30.3 lm W-1 at luminance levels above 1000 cd m-2 as required for various applications. These findings suggest that, with feasible levels of device performance, the PeNCs hold great promise for their use in LED lighting and displays.

physics.app-ph↗

arXiv2017

Surface Plasmon Enhanced Strong Exciton-Photon Coupling in Hybrid Inorganic-Organic Perovskites Nanowires

Manipulating strong light-matter interaction in semiconductor microcavities is crucial for developing high-performance exciton polariton devices with great potentials in next-generation all-solid state quantum technologies. In this work, we report surface plasmon enhanced strong exciton-photon interaction in CH3NH3PbBr3 perovskite nanowires. Characteristic anti-crossing behaviors, indicating Rabi splitting energy up to ~ 560 meV, are observed near exciton resonance in hybrid semiconductor-insulator-metallic waveguide cavity at room temperature. An exciton-photon coupling strength enhancement factor of ~ 1.4 times is evaluated, which is mainly attributed to surface plasmon induced localized excitation field redistribution. Further, systematic studies on nanowires and insulator dimension dependence of exciton-photon interaction are presented. These results provide new avenues to achieve extremely high coupling strengths and push forward the development of electrically pumped and ultra-low threshold small lasers.

cond-mat.mes-hall↗

arXiv2017

Room Temperature Polariton Lasing in All-Inorganic Perovskites

Polariton lasing is the coherent emission arising from a macroscopic polariton condensate first proposed in 1996. Over the past two decades, polariton lasing has been demonstrated in a few inorganic and organic semiconductors in both low and room temperatures. Polariton lasing in inorganic materials significantly relies on sophisticated epitaxial growth of crystalline gain medium layers sandwiched by two distributed Bragg reflectors in which combating the built-in strain and mismatched thermal properties is nontrivial. On the other hand, organic active media usually suffer from large threshold density and weak nonlinearity due to the Frenkel exciton nature. Further development of polariton lasing towards technologically significant applications demand more accessible materials, ease of device fabrication and broadly tunable emission at room temperature. Herein, we report the experimental realization of room-temperature polariton lasing based on an epitaxy-free all-inorganic cesium lead chloride perovskite microcavity. Polariton lasing is unambiguously evidenced by a superlinear power dependence, macroscopic ground state occupation, blueshift of ground state emission, narrowing of the linewidth and the build-up of long-range spatial coherence. Our work suggests considerable promise of lead halide perovskites towards large-area, low-cost, high performance room temperature polariton devices and coherent light sources extending from the ultraviolet to near infrared range.

cond-mat.mtrl-sci↗

arXiv2017

Observation of forbidden phonons and dark excitons by resonance Raman scattering in few-layer WS$_2$

The optical properties of the two-dimensional (2D) crystals are dominated by tightly bound electron-hole pairs (excitons) and lattice vibration modes (phonons). The exciton-phonon interaction is fundamentally important to understand the optical properties of 2D materials and thus help develop emerging 2D crystal based optoelectronic devices. Here, we presented the excitonic resonant Raman scattering (RRS) spectra of few-layer WS$_2$ excited by 11 lasers lines covered all of A, B and C exciton transition energies at different sample temperatures from 4 to 300 K. As a result, we are not only able to probe the forbidden phonon modes unobserved in ordinary Raman scattering, but also can determine the bright and dark state fine structures of 1s A exciton. In particular, we also observed the quantum interference between low-energy discrete phonon and exciton continuum under resonant excitation. Our works pave a way to understand the exciton-phonon coupling and many-body effects in 2D materials.

cond-mat.mtrl-sci↗

arXiv2017

Microsecond dark-exciton valley polarization memory in 2D heterostructures

Transition metal dichalcogenides (TMDs) have valley degree of freedom, which features optical selection rule and spin-valley locking, making them promising for valleytronics devices and quantum computation. For either application, a long valley polarization lifetime is crucial. Previous results showed that it is around picosecond in monolayer excitons, nanosecond for electrons, holes or local excitons and tens of nanosecond for interlayer excitons. Here we show that dark excitons in 2D heterostructures provide a microsecond valley polarization memory thanks to the magnetic field induced suppression of valley mixing. The lifetime of the dark excitons shows magnetic field and temperature dependence which is consistent with the theoretical prediction. The long dark exciton lifetime and valley polarization lifetime in 2D heterostructures make them promising for long-distance exciton transport and macroscopic quantum state generations.

cond-mat.mes-hall↗

arXiv2017

Coherent control of a strongly driven silicon vacancy optical transition in diamond

The ability to prepare, optically read out and coherently control single quantum states is a key requirement for quantum information processing. Optically active solid state emitters have emerged as promising candidates with their prospects for on chip integration as quantum nodes and sources of coherent photons for connecting these nodes. Under strongly driving resonant laser field, such quantum emitter can exhibit quantum behavior such as Autler-Townes splitting and Mollow triplet spectrum. Here we demonstrate coherent control of a strongly driven optical transition in silicon vacancy (SiV) center in diamond. Rapid optical detection of photons enabled the observation of time resolved coherent Rabi oscillations and the Mollow triplet from an optical transition of a single SiV defect. Detection with a probing transition further confirmed Autler-Townes splitting generated by a strong laser field. Coherence time of the emitted photons is shown to be comparable to its lifetime and robust under very strong driving laser field, which is promising for generation of indistinguishable photons.

quant-ph↗

arXiv2015

Broadband tunable hybrid photonic crystal-nanowire light emitter

We integrate about 100 single Cadmium Selenide semiconductor nanowires in self-standing Silicon Nitride photonic crystal cavities in a single processing run. Room temperature measurements reveal a single narrow emission linewidth, corresponding to a Q-factor as large as 5000. By varying the structural parameters of the photonic crystal, the peak wavelength is tuned, thereby covering the entire emission spectral range of the active material. A very large spectral range could be covered by heterogeneous integration of different active materials.

physics.optics↗

arXiv2015

Large Frequency Change with Thickness in Interlayer Breathing Mode - Significant Interlayer Interactions in Few Layer Black Phosphorus

Bulk black phosphorus (BP) consists of puckered layers of phosphorus atoms. Few-layer BP, obtained from bulk BP by exfoliation, is an emerging candidate as a channel material in post-silicon electronics. A deep understanding of its physical properties and its full range of applications are still being uncovered. In this paper, we present a theoretical and experimental investigation of phonon properties in few-layer BP, focusing on the low-frequency regime corresponding to interlayer vibrational modes. We show that the interlayer breathing mode A3g shows a large redshift with increasing thickness; the experimental and theoretical results agreeing well. This thickness dependence is two times larger than that in the chalcogenide materials such as few-layer MoS2 and WSe2, because of the significantly larger interlayer force constant and smaller atomic mass in BP. The derived interlayer out-of-plane force constant is about 50% larger than that in graphene and MoS2. We show that this large interlayer force constant arises from the sizable covalent interaction between phosphorus atoms in adjacent layers, and that interlayer interactions are not merely of the weak van der Waals type. These significant interlayer interactions are consistent with the known surface reactivity of BP, and have been shown to be important for electric-field induced formation of Dirac cones in thin film BP.

cond-mat.mtrl-sci↗

arXiv2015

Stacking sequence determines Raman intensities of observed interlayer shear modes in 2D layered materials - A general bond polarizability model

2D layered materials have recently attracted tremendous interest due to their fascinating properties and potential applications. The interlayer interactions are much weaker than the intralayer bonds, allowing the as-synthesized materials to exhibit different stacking sequences (e.g. ABAB, ABCABC), leading to different physical properties. Here, we show that regardless of the space group of the 2D material, the Raman frequencies of the interlayer shear modes observed under the typical configuration blue shift for AB stacked materials, and red shift for ABC stacked materials, as the number of layers increases. Our predictions are made using an intuitive bond polarizability model which shows that stacking sequence plays a key role in determining which interlayer shear modes lead to the largest change in polarizability (Raman intensity); the modes with the largest Raman intensity determining the frequency trends. We present direct evidence for these conclusions by studying the Raman modes in few layer graphene, MoS2, MoSe2, WSe2 and Bi2Se3, using both first principles calculations and Raman spectroscopy. This study sheds light on the influence of stacking sequence on the Raman intensities of intrinsic interlayer modes in 2D layered materials in general, and leads to a practical way of identifying the stacking sequence in these materials.

cond-mat.mtrl-sci↗

arXiv2014

Effects of Lower Symmetry and Dimensionality on Raman Spectra in 2D WSe2

We report the observation and interpretation of new Raman peaks in few-layer tungsten diselenide (WSe2), induced by the reduction of symmetry going from 3D to 2D. In general, Raman frequencies in 2D materials follow quite closely the frequencies of corresponding eigenmodes in the bulk. However, while the modes that are Raman active in the bulk are also Raman active in the thin films, the reverse is not always true due to the reduced symmetry in thin films. Here, we predict from group theory and density functional calculations that two intra-layer vibrational modes which are Raman inactive in bulk WSe2 in our experimental configuration become Raman active in thin film WSe2, due to reduced symmetry in thin films. This phenomenon explains the Raman peaks we observe experimentally at ~310 cm-1 and 176 cm-1 in thin film WSe2. Interestingly, the bulk mode at ~310 cm-1 that is Raman inactive can in fact be detected in Raman measurements under specific wavelengths of irradiation, suggesting that in this case, crystal symmetry selection rules may be broken due to resonant scattering. Both theory and experiment indicate that the and modes blue-shift with decreasing thickness, which we attribute to surface effects. Our results shed light on a general understanding of the Raman/IR activities of the phonon modes in layered transition metal dichalcogenide materials and their evolution behavior from 3D to 2D.

cond-mat.mtrl-sci↗

arXiv2013

Rapid and reliable thickness identification of two-dimensional nanosheets using optical microscopy

The physical and electronic properties of ultrathin two-dimensional (2D) layered nanomaterials are highly related to their thickness. Therefore, the rapid and accurate identification of single- and few- to multi-layer nanosheets is essential to their fundamental study and practical applications. Here, a universal optical method has been developed for simple, rapid and reliable identification of single- to quindecuple-layer (1L-15L) 2D nanosheets, including graphene, MoS2, WSe2 and TaS2, on Si substrates coated with 90 nm or 300 nm SiO2. The optical contrast differences between the substrates and 2D nanosheets with different layer numbers were collected and tabulated, serving as a standard reference, from which the layer number of a given nanosheet can be readily and reliably determined without using complex calculation nor expensive instrument. Our general optical identification method will facilitate the thickness-dependent study of various 2D nanomaterials, and expedite their research toward practical applications.

cond-mat.mtrl-sci↗

arXiv2013

Anomalous Frequency Trends in MoS2 Thin Films Attributed to Surface Effects

The layered dichalcogenide MoS2 has many unique physical properties in low dimensions. Recent experimental Raman spectroscopies report an anomalous blue shift of the in-plane E2g1 mode with decreasing thickness, a trend that is not understood. Here, we combine experimental Raman scattering and theoretical studies to clarify and explain this trend. Special attention is given to understanding the surface effect on Raman frequencies by using a force constants model based on first-principles calculations. Surface effects refer to the larger Mo-S force constants at the surface of thin film MoS2, which results from a loss of neighbours in adjacent MoS2 layers. Without surface effects, the frequencies of both out-of-plane A1g and in-plane E2g1 modes decrease with decreasing thickness. However, the E2g1 mode blue shifts while the A1g mode red shifts once the surface effect is included, in agreement with the experiment. Our results show that competition between the thickness effect and the surface effect determines the mechanical properties of two-dimensional MoS2, which we believe applies to other layered materials.

cond-mat.mtrl-sci↗

arXiv2013

Tailoring Plasmonic Metamaterials for DNA Molecular Logic Gates

Structural and functional information encoded in DNA combined with unique properties of nanomaterials could be of use for the construction of novel biocomputational circuits and intelligent biomedical nanodevices. However, at present their practical applications are still limited by either low reproducibility of fabrication, modest sensitivity, or complicated handling procedures. Here, we demonstrate the construction of label-free and switchable molecular logic gates that use specific conformation modulation of a guanine- and thymine- rich DNA, while the optical readout is enabled by the tunable alphabetical metamaterials, which serve as a substrate for surface enhanced Raman spectroscopy (MetaSERS). By computational and experimental investigations, we present a comprehensive solution to tailor the plasmonic responses of MetaSERS with respect to the metamaterial geometry, excitation energy, and polarization. Our tunable MetaSERS-based DNA logic is simple to operate, highly reproducible, and can be stimulated by ultra-low concentration of the external inputs, enabling an extremely sensitive detection of mercury ions.

cond-mat.mtrl-sci↗

arXiv2013

Interlayer breathing and shear modes in few-trilayer MoS2 and WSe2

Two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have recently attracted tremendous interest as potential valleytronic and nano-electronic materials, in addition to being well-known as excellent lubricants in the bulk. The interlayer van der Waals (vdW) coupling and low frequency phonon modes, and how they evolve with the number of layers, are important for both the mechanical and electrical properties of 2D TMDs. Here we uncover the ultra-low frequency interlayer breathing and shear modes in few-layer MoS2 and WSe2, prototypical layered TMDs, using both Raman spectroscopy and first principles calculations. Remarkably, the frequencies of these modes can be perfectly described using a simple linear chain model with only nearest-neighbour interactions. We show that the derived in-plane (shear) and out-of-plane (breathing) force constants from experiment remain the same from two-layer 2D crystals to the bulk materials, suggesting that the nanoscale interlayer frictional characteristics of these excellent lubricants should be independent of the number of layers.

cond-mat.mtrl-sci↗

arXiv2012

Direct Observation of Inner and Outer G' Band Double-resonance Raman Scattering in Free Standing Graphene

In contrary to the widely reported single and symmetric peak feature of G' (or 2D) band in Raman spectrum of graphene, we herein report the observation of splitting in G' band in free standing graphene. Our experimental findings provide a direct and strong support for the previous theoretical prediction that the coexistence of the outer and inner processes in the doubleresonance Raman scattering would cause the splitting of G' mode. Our investigation of the influence of trigonal warping effect on the spectral features of G' subbands further verified the theoretical interpretation established on the anisotropic electronic structure of graphene.

cond-mat.mtrl-sci↗