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Qingkai Yu

Publications and source records attributed to Qingkai Yu.

13 recordsLinked to original sources

Self-formed 2D/3D Heterostructure on the Edge of 2D Ruddlesden-Popper Hybrid Perovskites Responsible for Intriguing Optoelectronic Properties and Higher Cell Efficiency

The observation of low energy edge photoluminescence and its beneficial effect on the solar cell efficiency of Ruddlesden-Popper perovskites has unleashed an intensive research effort to reveal its origin. This effort, however, has been met with more challenges as the underlying material structure has still not been identified; new modellings and observations also do not seem to converge. Using 2D (BA)2(MA)2Pb3Br10 as an example, we show that 3D MAPbBr3 is formed due to the loss of BA on the edge. This self-formed MAPbBr3 can explain the reported edge emission under various conditions, while the reported intriguing optoelectronic properties such as fast exciton trapping from the interior 2D perovskite, rapid exciton dissociation and long carrier lifetime can be understood via the self-formed 2D/3D lateral perovskite heterostructure. The 3D perovskite is identified by submicron infrared spectroscopy, the emergence of XRD signature from freezer-milled nanometer-sized 2D perovskite and its photoluminescence response to external hydrostatic pressure. The revelation of this edge emission mystery and the identification of a self-formed 2D/3D heterostructure provide a new approach to engineering 2D perovskites for high-performance optoelectronic devices.

physics.app-ph

Revealing the Origin of Luminescence Center in 0D Cs4PbBr6 Perovskite

Zero dimensional perovskite Cs4PbBr6 has attracted considerable attention recently not only because of its highly efficient green photoluminescence (PL), but also its two highly debated opposing mechanisms of the luminescence: embedded CsPbBr3 nanocrystals versus intrinsic Br vacancy states. After a brief discussion on the root cause of the controversy, we provide sensitive but non-invasive methods that can not only directly correlate luminescence with the underlying structure, but also distinguish point defects from embedded nanostructures. We first synthesized both emissive and non-emissive Cs4PbBr6 crystals, obtained the complete Raman spectrum of Cs4PbBr6 and assigned all Raman bands based on density functional theory simulations. We then used correlated Raman-PL as a passive structure-property method to identify the difference between emissive and non-emissive Cs4PbBr6 crystals and revealed the existence of CsPbBr3 nanocrystals in emissive Cs4PbBr6. We finally employed a diamond anvil cell to probe the response of luminescence centers to hydrostatic pressure. The observations of fast red-shifting, diminishing and eventual disappearance of both green emission and Raman below Cs4PbBr6 phase transition pressure of ~3 GPa is compatible with CsPbBr3 nanocrystal inclusions as green PL emitters and cannot be explained by Br vacancies. The resolution of this long-lasting controversy paves the way for further device applications of low dimensional perovskites, and our comprehensive optical technique integrating structure-property with dynamic pressure response is generic and can be applied to other emerging optical materials to understand the nature of their luminescent centers.

cond-mat.mtrl-sci

New strategy for black phosphorus crystal growth through ternary clathrate

We are reporting a new synthetic strategy to grow large size black phosphorus (Black-P) crystals through a ternary clathrate Sn$_{24}$P$_{22-x}$I$_8$, under lower synthetic temperature and pressure. The Black-P crystals are found grown in situ at the site where the solid clathrate originally resides, which suggests chemical vapor mineralizer does not play a critical role for the Black-P formation. More detailed systematical studies has indicated the P vacancies in the framework of ternary clathrate Sn$_{24}$P$_{22-x}$I$_8$ is important for the subsequent Black-P from phosphorus vapors, and a likely Vapor-Solid-Solid (VSS) model is responsible for the Black-P crystal growth. The obtained room temperature mobility {\mu} is ~ 350 $cm^2/Vs$ from Hall measurements at mechanically-cleaved flake, where noticeable micro-cracks are visible. The obtained high mobility value further suggest the high quality of the Black-P crystals synthesized through this route.

cond-mat.mtrl-sci

Synthetic Graphene Grown by Chemical Vapor Deposition on Copper Foils

The discovery of graphene, a single layer of covalently bonded carbon atoms, has attracted intense interests. Initial studies using mechanically exfoliated graphene unveiled its remarkable electronic, mechanical and thermal properties. There has been a growing need and rapid development in large-area deposition of graphene film and its applications. Chemical vapour deposition on copper has emerged as one of the most promising methods in obtaining large-scale graphene films with quality comparable to exfoliated graphene. In this chapter, we review the synthesis and characterizations of graphene grown on copper foil substrates by atmospheric pressure chemical vapour deposition. We also discuss potential applications of such large scale synthetic graphene.

cond-mat.mtrl-sci

Graphene Induced Surface Reconstruction of Cu

An atomic-scale study utilizing scanning tunneling microscopy (STM) in ultrahigh vacuum (UHV) is performed on large single crystalline graphene grains synthesized on Cu foil by a chemical vapor deposition (CVD) method. After thermal annealing, we observe the presence of periodic surface depressions (stripe patterns) that exhibit long-range order formed in the area of Cu covered by graphene. We suggest that the observed stripe pattern is a Cu surface reconstruction formed by partial dislocations (which appeared to be stair-rod-like) resulting from the strain induced by the graphene overlayer. In addition, these graphene grains are shown to be more decoupled from the Cu substrate compared to previously studied grains that exhibited Moir\'e patterns.

cond-mat.mes-hall

Growth from Below: Bilayer Graphene on Copper by Chemical Vapor Deposition

We evaluate how a second graphene layer forms and grows on Cu foils during chemical vapor deposition (CVD). Low-energy electron diffraction and microscopy is used to reveal that the second layer nucleates and grows next to the substrate, i.e., under a graphene layer. This underlayer mechanism can facilitate the synthesis of uniform single-layer films but presents challenges for growing uniform bilayer films by CVD. We also show that the buried and overlying layers have the same edge termination.

cond-mat.mtrl-sci

Quantum Hall effect on centimeter scale chemical vapor deposited graphene films

We report observations of well developed half integer quantum Hall effect (QHE) on mono layer graphene films of 7 mm \times 7 mm in size. The graphene films are grown by chemical vapor deposition (CVD) on copper, then transferred to SiO_{2} /Si substrates, with typical carrier mobilities \approx 4000 cm^{2} /Vs. The large size graphene with excellent quality and electronic homogeneity demonstrated in this work is promising for graphene-based quantum Hall resistance standards, and can also facilitate a wide range of experiments on quantum Hall physics of graphene and practical applications exploiting the exceptional properties of graphene.

cond-mat.mes-hall

Direct Imaging of Graphene Edges: Atomic Structure and Electronic Scattering

We report an atomically-resolved scanning tunneling microscopy (STM) investigation of the edges of graphene grains synthesized on Cu foils by chemical vapor deposition (CVD). Most of the edges are macroscopically parallel to the zigzag directions of graphene lattice. These edges have microscopic roughness that is found to also follow zigzag directions at atomic scale, displaying many ~120 degree turns. A prominent standing wave pattern with periodicity ~3a/4 (a being the graphene lattice constant) is observed near a rare-occurring armchair-oriented edge. Observed features of this wave pattern are consistent with the electronic intervalley backscattering predicted to occur at armchair edges but not at zigzag edges.

cond-mat.mes-hall

Control and Characterization of Individual Grains and Grain Boundaries in Graphene Grown by Chemical Vapor Deposition

The strong interest in graphene has motivated the scalable production of high quality graphene and graphene devices. Since large-scale graphene films synthesized to date are typically polycrystalline, it is important to characterize and control grain boundaries, generally believed to degrade graphene quality. Here we study single-crystal graphene grains synthesized by ambient CVD on polycrystalline Cu, and show how individual boundaries between coalescing grains affect graphene's electronic properties. The graphene grains show no definite epitaxial relationship with the Cu substrate, and can cross Cu grain boundaries. The edges of these grains are found to be predominantly parallel to zigzag directions. We show that grain boundaries give a significant Raman "D" peak, impede electrical transport, and induce prominent weak localization indicative of intervalley scattering in graphene. Finally, we demonstrate an approach using pre-patterned growth seeds to control graphene nucleation, opening a route towards scalable fabrication of single-crystal graphene devices without grain boundaries.

cond-mat.mes-hall

Room-temperature Tunable Fano Resonance by Chemical Doping in Few-layer Graphene Synthesized by Chemical Vapor Deposition

A Fano-like phonon resonance is observed in few-layer (~3) graphene at room temperature using infrared Fourier transform spectroscopy. This Fano resonance is the manifestation of a strong electron-phonon interaction between the discrete in-plane lattice vibrational mode and continuum electronic excitations in graphene. By employing ammonia chemical doping, we have obtained different Fano line shapes ranging from anti-resonance in hole-doped graphene to phonon-dominated in n-type graphene. The Fano resonance shows the strongest interference feature when the Fermi level is located near the Dirac point. The charged phonon exhibits much-enhanced oscillator strength and experiences a continuous red shift in frequency as electron density increases. It is suggested that the phonon couples to different electronic transitions as Fermi level is tuned by chemical doping.

cond-mat.mes-hall

Electronic Transport in Chemical Vapor Deposited Graphene Synthesized on Cu: Quantum Hall Effect and Weak Localization

We report on electronic properties of graphene synthesized by chemical vapor deposition (CVD) on copper then transferred to SiO2/Si. Wafer-scale (up to 4 inches) graphene films have been synthesized, consisting dominantly of monolayer graphene as indicated by spectroscopic Raman mapping. Low temperature transport measurements are performed on micro devices fabricated from such CVD graphene, displaying ambipolar field effect (with on/off ratio ~5 and carrier mobilities up to ~3000 cm^2/Vs) and "half-integer" quantum Hall effect, a hall-mark of intrinsic electronic properties of monolayer graphene. We also observe weak localization and extract information about phase coherence and scattering of carriers.

cond-mat.mes-hall

Large-scale Graphitic Thin Films Synthesized on Ni and Transferred to Insulators: Structural and Electronic Properties

We present a comprehensive study of the structural and electronic properties of ultrathin films containing graphene layers synthesized by chemical vapor deposition (CVD) based surface segregation on polycrystalline Ni foils then transferred onto insulating SiO2/Si substrates. Films of size up to several mm's have been synthesized. Structural characterizations by atomic force microscopy (AFM), scanning tunneling microscopy (STM), cross-sectional transmission electron microscopy (XTEM) and Raman spectroscopy confirm that such large scale graphitic thin films (GTF) contain both thick graphite regions and thin regions of few layer graphene. The films also contain many wrinkles, with sharply-bent tips and dislocations revealed by XTEM, yielding insights on the growth and buckling processes of the GTF. Measurements on mm-scale back-gated transistor devices fabricated from the transferred GTF show ambipolar field effect with resistance modulation ~50% and carrier mobilities reaching ~2000 cm^2/Vs. We also demonstrate quantum transport of carriers with phase coherence length over 0.2 $μ$m from the observation of 2D weak localization in low temperature magneto-transport measurements. Our results show that despite the non-uniformity and surface roughness, such large-scale, flexible thin films can have electronic properties promising for device applications.

cond-mat.mtrl-sci

Graphene Segregated on Ni surfaces and Transferred to Insulators

We report an approach to synthesize high quality graphene by surface segregation and substrate transfer. Graphene was segregated from Ni surface under the ambient pressure by dissolving carbon in Ni at high temperatures followed by cooling down with various rates. Different cooling rates led to different segregation behaviors, strongly affecting the thickness and quality of the graphene films. Electron microscopy and Raman spectroscopy indicated that the graphene films synthesized with medium cooling rates have high quality crystalline structure and well-controlled thicknesses. The graphene films were transferred to insulating substrates by wet etching and found to maintain their high quality.

cond-mat.mtrl-sci