arXiv subjects

Yongqing Cai

Publications and source records attributed to Yongqing Cai.

At least 55 records · Page 3Linked to original sources

arXiv2022

Activation of Phosphorene-like Two-dimensional GeSe for Efficient Electrocatalytic Nitrogen Reduction via States Filtering of Ru

Nitrogen reduction reaction (NRR) which converts nitrogen (N2) to ammonia (NH3) normally requires harsh conditions to break the bound nitrogen bond. Herein, via first-principles calculation we reveal that a superior NRR catalytic activity could be obtained through anchoring atomic catalyst above a phosphorene-like puckering surface of germanium selenide (GeSe). Through examining the single- and double- atoms (B, Fe, W, Mo and Ru) decorated on GeSe, we find that its rippled structure allows an intimate contact between the deposited species and the GeSe which significantly promotes the states hybridization. Amongst the various atomic catalyst, we predict that the Ru dimer decorated GeSe monolayer (Ru2@GeSe) has superior catalytic activity for the N2 fixation and reduction. Through examining the three NRR pathways (distal, alternating and enzymatic), the distal and enzymatic pathway is both the thermodynamically favorable with the maximum Gibbs free energy change (ΔGMAX) of 0.25 and 0.26 eV, respectively. Such a superior activity could be attributed to the filtered states of GeSe by Ru dimer which leads to the effective activation of the adsorbed N2 bond. As an efficient near-infrared absorber of GeSe, the Ru mediated hybridization of GeSe-Ru-N2 complex enables an in-gap state which further broadens the absorbing window, rendering for a broadband solar absorption and possible photocatalysis.

cond-mat.mtrl-sci↗

arXiv2022

Oxygen Deficient α-MoO3 with Promoted Adsorption and State-Quenching of H2O for Gas Sensor: A DFT Study

Semiconducting oxides with reducible cations are ideal platforms for various functional applications in nanoelectronics and catalysts. Here we report an ultrathin monolayer alpha-MoO3 where tunable electronic properties and different gas adsorbing behaviors upon introducing the oxygen vacancies (VO). The unique property of alpha-MoO3 is that it contains three different types of oxygen atoms occupying three Wyckoff sites that are absent in other low-dimensional oxides and provides rich electronic hybridized states. The presence of VO triggers intermediate state in the gap at ~0.59 eV below the conduction band minimum and reduces the work function dramatically, together with new excitations at near infrared. The realigned Fermi level associated with the dangling state of VO reduces the neighboring Mo atoms and affects the gas adsorption thereafter. The binding energy of H2O molecules above VO is 2.5 times up to -0.75 eV compared with that of perfect lattice site and trends of transfer of electrons also reverse. The latter is related with the shallow localized state in the band gap due to H2O adsorbed above perfect MoO3 which becomes quenched upon adsorbing at the VO site. Those rich in-gap defective states in oxygen deficient MoO3, broadening the light absorption and promoting the uptake of water, are conductive to the application of alpha-MoO3 for optoelectronics, photothermal therapy, and sensor of moisture.

cond-mat.mtrl-sci↗

arXiv2022

Squeezed metallic droplet with tunable Kubo gap and charge injection in transition metal dichalcogenides

Shrinking the size of a bulk metal into nanoscale leads to the discreteness of electronic energy levels, the so-called Kubo gap. Renormalization of the electronic properties with a tunable and size-dependent Kubo gap renders fascinating photon emission and electron tunneling. In contrast with usual three-dimensional (3D) metal clusters, here we demonstrate that Kubo gap can be achieved with a two-dimensional (2D) metallic transition metal dichalcogenide (i.e., 1T'-phase MoTe2) nanocluster embedded in a semiconducting polymorph (i.e., 1H-phase MoTe2). Such a 1T'-1H MoTe2 nanodomain resembles a 3D metallic droplet squeezed in a 2D space which shows a strong polarization catastrophe while simultaneously maintains its bond integrity which is absent in traditional delta-gapped 3D clusters. The weak screening of the host 2D MoTe2 leads to photon emission of such pseudo-metallic systems and a ballistic injection of carriers in the 1T'-1H-1T' homojunctions which may find applications in sensors and 2D reconfigurable devices.

cond-mat.mtrl-sci↗

arXiv2022

Ubiquitous Coexisting Electron-Mode Couplings in High Temperature Cuprate Superconductors

In conventional superconductors, the electron-phonon coupling plays a dominant role in pairing the electrons and generating superconductivity. In high temperature cuprate superconductors, the existence of the electron coupling with phonons and other boson modes and its role in producing high temperature superconductivity remain unclear. The evidence of the electron-boson coupling mainly comes from the angle-resolved photoemission (ARPES) observations of the ~70meV nodal dispersion kink and the ~40meV antinodal kink. However, the reported results are sporadic and the nature of the involved bosons are still under debate. Here we report new findings of ubiquitous two coexisting electron-mode couplings in cuprate superconductors. By taking ultra-high resolution laser-based ARPES measurements, combined with the improved second derivative analysis method, we discovered that the electrons are coupled simultaneously with two sharp phonon modes with energies of ~70meV and ~40meV in different superconductors with different doping levels, over the entire momentum space and at different temperatures above and below the superconducting transition temperature. The observed electron-phonon couplings are unusual because the associated energy scales do not exhibit an obvious change across the superconducting transition. We further find that the well-known "peak-dip-hump" structure, which has long been considered as a hallmark of superconductivity, is also omnipresent and consists of finer structures that originates from electron coupling with two sharp phonon modes. These comprehensive results provide a unified picture to reconcile all the reported observations and pinpoint the origin of the electron-mode couplings in cuprate superconductors. They provide key information to understand the role of the electron-phonon coupling in generating high temperature superconductivity.

cond-mat.supr-con↗

arXiv2021

Protected valley states and generation of valley- and spin-polarized current in monolayer MA2Z4

The optical selection rules obeyed by two-dimensional materials with spin-valley coupling enable the selective excitation of carriers. We show that six members of the monolayer MA2Z4 (M = Mo and W; A = C, Si, and Ge; Z = N, P, and As) family are direct band-gap semiconductors with protected valley states and that circularly polarized infrared light can induce valley-selective inter-band transitions. Our optovalleytronic device demonstrates a close to 100% valley- and spin-polarized current under in-plane bias and circularly polarized infrared light, which can be exploited to encode, process, and store information.

cond-mat.mtrl-sci↗

arXiv2021

Dirac Nodal Lines and Nodal Loops in a Topological Kagome Superconductor CsV$_3$Sb$_5$

The intertwining of charge order, superconductivity and band topology has promoted the AV$_3$Sb$_5$ (A=K, Rb, Cs) family of materials to the center of attention in condensed matter physics. Underlying those mysterious macroscopic properties such as giant anomalous Hall conductivity (AHC) and chiral charge density wave is their nontrivial band topology. While there have been numerous experimental and theoretical works investigating the nontrivial band structure and especially the van Hove singularities, the exact topological phase of this family remains to be clarified. In this work, we identify CsV$_3$Sb$_5$ as a Dirac nodal line semimetal based on the observation of multiple Dirac nodal lines and loops close to the Fermi level. Combining photoemission spectroscopy and density functional theory, we identify two groups of Dirac nodal lines along $k_z$ direction and one group of Dirac nodal loops in the A-H-L plane. These nodal loops are located at the Fermi level within the instrumental resolution limit. Importantly, our first-principle analyses indicate that these nodal loops may be a crucial source of the mysterious giant AHC observed. Our results not only provide a clear picture to categorize the band structure topology of this family of materials, but also suggest the dominant role of topological nodal loops in shaping their transport behavior.

cond-mat.str-el↗

arXiv2021

Doping evolution of superconductivity, charge order and band topology in hole-doped topological kagome superconductors Cs(V$_{1-x}$Ti$_x$)$_3$Sb$_5$

The newly discovered Kagome superconductors $A$V$_3$Sb$_5$ ($A$ = K, Rb, Cs) exhibit superconductivity, charge order, and band topology simultaneously. To explore the intricate interplay between the superconducting and charge orders, we investigate the doping evolution of superconductivity, charge-density-wave (CDW) order, and band topology in doped topological kagome superconductors Cs(V$_{1-x}$Ti$_x$)$_3$Sb$_5$ where the Ti-dopant introduces hole-like charge carriers. Despite the absence of the CDW phase transition in doped compounds even for the lowest doping level of $x=0.047$, the superconductivity survives in all doped samples with enhanced critical temperatures. The high-resolution angle-resolved photoemission spectroscopy (ARPES) measurements reveal that the Ti-dopant in the kagome plane lowers the chemical potential, pushing the van Hove singularity (VHS) at $M$ point above the Fermi level. First-principle simulations corroborate the doping evolution of the band structure observed in ARPES, and affirm that the CDW instability does not occur once the VHS is pushed above the Fermi level, explaining the absence of the CDW ordering in our doped samples Cs(V$_{1-x}$Ti$_x$)$_3$Sb$_5$. Our results demonstrate a competition between the CDW and superconducting orders in the kagome-metal superconductor CsV$_3$Sb$_5$, although the superconductivity is likely inconsequential of the CDW order.

cond-mat.supr-con↗

arXiv2021

Emergence of Quantum Confinement in Topological Kagome Superconductor CsV$_3$Sb$_5$ family

Quantum confinement is a restriction on the motion of electrons in a material to specific region, resulting in discrete energy levels rather than continuous energy bands. In certain materials quantum confinement could dramatically reshape the electronic structure and properties of the surface with respect to the bulk. Here, in the recently discovered kagome superconductor CsV$_3$Sb$_5$ (A=K, Rb, Cs) family of materials, we unveil the dominant role of quantum confinement in determining their surface electronic structure. Combining angle-resolved photoemission spectroscopy (ARPES) measurement and density-functional theory simulation, we report the observations of two-dimensional quantum well states due to the confinement of bulk electron pocket and Dirac cone to the nearly isolated surface layer. The theoretical calculations on the slab model also suggest that the ARPES observed spectra are almost entirely contributed by the top two layers. Our results not only explain the disagreement of band structures between the recent experiments and calculations, but also suggest an equally important role played by quantum confinement, together with strong correlation and band topology, in shaping the electronic properties of this family of materials.

cond-mat.str-el↗

arXiv2021

Electronic Self-passivation of Single Vacancy in Black Phosphorus via a Controlled Ionization

We report that mono-elemental black phosphorus presents a new electronic self-passivation scheme of single vacancy (SV). By means of low-temperature scanning tunneling microscopy and bond-resolved non-contact atomic force microscopy, we demonstrate that the local reconstruction and ionization of SV into negatively charged $\mathrm{SV}^-$ leads to the passivation of dangling bonds and thus the quenching of in-gap states, which can be achieved by mild thermal annealing or STM tip manipulation. SV exhibits a strong and symmetric Friedel oscillation (FO) pattern, while $\mathrm{SV}^-$ shows an asymmetric FO pattern with local perturbation amplitude reduced by one order of magnitude and a faster decay rate. The enhanced passivation by forming $\mathrm{SV}^-$ can be attributed to its weak dipole-like perturbation, consistent with density-functional theory and numerical calculations. Therefore, self-passivated $\mathrm{SV}^-$ is electronically benign and acts as a much weaker scattering center, which may hold the key to further enhance the charge mobility of BP and its analogs.

cond-mat.mtrl-sci↗

arXiv2021

Unusual Electronic Structure of Dirac Material BaMnSb$_2$ Revealed by Angle-Resolved Photoemission Spectroscopy

High resolution angle resolved photoemission measurements and band structure calculations are carried out to study the electronic structure of BaMnSb$_2$. All the observed bands are nearly linear that extend to a wide energy range. The measured Fermi surface mainly consists of one hole pocket around $Γ$ and a strong spot at Y which are formed from the crossing points of the linear bands. The measured electronic structure of BaMnSb$_2$ is unusual and deviates strongly from the band structure calculations. These results will stimulate further efforts to theoretically understand the electronic structure of BaMnSb$_2$ and search for novel properties in this Dirac material.

cond-mat.mtrl-sci↗

arXiv2021

Electronic Structure Examination on the Topological Properties of CaMnSb$_{2}$ by Angle-Resolved Photoemission Spectroscopy

We have carried out detailed high resolution ARPES measurements and band structure calculations to study the electronic structure of CaMnSb$_{2}$. The observed Fermi surface mainly consists of one hole pocket around $Γ$ point and one tiny hole pocket at Y point. Strong spectral weight accumulation along the $Γ$-X direction is observed on the hole-like Fermi surface around $Γ$ point, suggesting strong anisotropy of the density of states along the Fermi surface. The tiny hole pocket at Y point originates from an anisotropic Dirac-like band with the crossing point of the linear bands lying $\sim$ 10 meV above the Fermi level. These observations are in a good agreement with the band structure calculations. In addition, we observe additional features along the $Γ$-Y line that cannot be accounted for by the band structure calculations. Our results provide important information in understanding and exploration of novel properties in CaMnSb$_{2}$ and related materials.

cond-mat.mtrl-sci↗

arXiv2021

Common ($π$,$π$) Band Folding and Surface Reconstruction in FeAs-Based Superconductors

High resolution angle-resolved photoemission spectroscopy (ARPES) measurements are carried out on CaKFe$_4$As$_4$, KCa$_2$Fe$_4$As$_4$F$_2$ and (Ba$_{0.6}$K$_{0.4}$)Fe$_2$As$_2$ superconductors. Clear evidence of band folding between the Brillouin zone center and corners with a ($π$,$π$) wave vector has been found from the measured Fermi surface and band structures in all the three kinds of superconductors. A dominant $\sqrt{2}\,\times\,\sqrt{2}$ surface reconstruction is observed on the cleaved surface of CaKFe$_4$As$_4$ by scanning tunneling microscopy (STM) measurements. We propose that the commonly observed $\sqrt{2}\,\times\,\sqrt{2}$ reconstruction in the FeAs-based superconductors provides a general scenario to understand the origin of the ($π$,$π$) band folding. Our observations provide new insights in understanding the electronic structure and superconductivity mechanism in iron-based superconductors.

cond-mat.supr-con↗

arXiv2021

Genuine Electronic Structure and Superconducting Gap Structure in (Ba$_{0.6}$K$_{0.4}$)Fe$_{2}$As$_{2}$ Superconductor

The electronic structure and superconducting gap structure are prerequisites to establish microscopic theories in understanding the superconductivity mechanism of iron-based superconductors. However, even for the most extensively studied optimally-doped (Ba$_{0.6}$K$_{0.4}$)Fe$_2$As$_2$, there remain outstanding controversies on its electronic structure and superconducting gap structure. Here we resolve these issues by carrying out high-resolution angle-resolved photoemission spectroscopy (ARPES) measurements on the optimally-doped (Ba$_{0.6}$K$_{0.4}$)Fe$_2$As$_2$ superconductor using both Helium lamp and laser light sources. Our results indicate the "flat band" feature observed around the Brillouin zone center in the superconducting state originates from the combined effect of the superconductivity-induced band back-bending and the folding of a band from the zone corner to the center. We found direct evidence of the band folding between the zone corner and the center in both the normal and superconducting state. Our resolution of the origin of the flat band makes it possible to assign the three hole-like bands around the zone center and determine their superconducting gap correctly. Around the zone corner, we observe a tiny electron-like band and an M-shaped band simultaneously in both the normal and superconducting states. The obtained gap size for the bands around the zone corner ($\sim$5.5 meV) is significantly smaller than all the previous ARPES measurements. Our results establish a new superconducting gap structure around the zone corner and resolve a number of prominent controversies concerning the electronic structure and superconducting gap structure in the optimally-doped (Ba$_{0.6}$K$_{0.4}$)Fe$_2$As$_2$. They provide new insights in examining and establishing theories in understanding superconductivity mechanism in iron-based superconductors.

cond-mat.supr-con↗

arXiv2021

Momentum-Resolved Visualization of Electronic Evolution in Doping a Mott Insulator

High temperature superconductivity in cuprates arises from doping a parent Mott insulator by electrons or holes. A central issue is how the Mott gap evolves and the low-energy states emerge with doping. Here we report angle-resolved photoemission spectroscopy measurements on a cuprate parent compound by sequential in situ electron doping. The chemical potential jumps to the bottom of the upper Hubbard band upon a slight electron doping, making it possible to directly visualize the charge transfer band and the full Mott gap region. With increasing doping, the Mott gap rapidly collapses due to the spectral weight transfer from the charge transfer band to the gapped region and the induced low-energy states emerge in a wide energy range inside the Mott gap. These results provide key information on the electronic evolution in doping a Mott insulator and establish a basis for developing microscopic theories for cuprate superconductivity.

cond-mat.str-el↗

arXiv2021

Spectroscopic Evidence on Realization of a Genuine Topological Nodal Line Semimetal in LaSbTe

The nodal line semimetals have attracted much attention due to their unique topological electronic structure and exotic physical properties. A genuine nodal line semimetal is qualified by the presence of Dirac nodes along a line in the momentum space that are protected against the spin-orbit coupling. In addition, it requires that the Dirac points lie close to the Fermi level allowing to dictate the macroscopic physical properties. Although the material realization of nodal line semimetals have been theoretically predicted in numerous compounds, only a few of them have been experimentally verified and the realization of a genuine nodal line semimetal is particularly rare. Here we report the realization of a genuine nodal line semimetal in LaSbTe. We investigated the electronic structure of LaSbTe by band structure calculations and angle-resolved photoemission (ARPES) measurements. Taking spin-orbit coupling into account, our band structure calculations predict that a nodal line is formed in the boundary surface of the Brillouin zone which is robust and lies close to the Fermi level. The Dirac nodes along the X-R line in momentum space are directly observed in our ARPES measurements and the energies of these Dirac nodes are all close to the Fermi level. These results constitute clear evidence that LaSbTe is a genuine nodal line semimetal,providing a new platform to explore for novel phenomena and possible applications associated with the nodal line semimetals.

cond-mat.mtrl-sci↗

arXiv2021

Theoretical analysis of thermal boundary conductance of MoS2-SiO2 and WS2-SiO2 interface

Understanding the physical processes involved in interfacial heat transfer is critical for the interpretation of thermometric measurements and the optimization of heat dissipation in nanoelectronic devices that are based on transition metal dichalcogenide (TMD) semiconductors. We model the phononic and electronic contributions to the thermal boundary conductance (TBC) variability for the MoS$_{2}$-SiO$_{2}$ and WS$_{2}$-SiO$_{2}$ interface. A phenomenological theory to model diffuse phonon transport at disordered interfaces is introduced and yields $G$=13.5 and 12.4 MW/K/m$^{2}$ at 300 K for the MoS$_{2}$-SiO$_{2}$ and WS$_{2}$-SiO$_{2} $ interface, respectively. We compare its predictions to those of the coherent phonon model and find that the former fits the MoS$_{2}$-SiO$_{2}$ data from experiments and simulations significantly better. Our analysis suggests that heat dissipation at the TMD-SiO$_{2}$ interface is dominated by phonons scattered diffusely by the rough interface although the electronic TBC contribution can be significant even at low electron densities ($n\leq10^{12}$ cm$^{-2}$) and may explain some of the variation in the experimental TBC data from the literature. The physical insights from our study can be useful for the development of thermally aware designs in TMD-based nanoelectronics.

cond-mat.mes-hall↗

arXiv2020

Spectroscopic Evidence of Superconductivity Pairing at 83 K in Single-Layer FeSe/SrTiO3 Films

Single-layer FeSe films grown on the SrTiO3 substrate (FeSe/STO) have attracted much attention because of their possible record-high superconducting critical temperature Tc and distinct electronic structures in iron-based superconductors. However, it has been under debate on how high its Tc can really reach due to the inconsistency of the results obtained from the transport, magnetic and spectroscopic measurements. Here we report spectroscopic evidence of superconductivity pairing at 83 K in single-layer FeSe/STO films. By preparing high-quality single-layer FeSe/STO films, we observe for the first time strong superconductivity-induced Bogoliubov back-bending bands that extend to rather high binding energy ~100 meV by high-resolution angle-resolved photoemission measurements. The Bogoliubov back-bending band provides a new definitive benchmark of superconductivity pairing that is directly observed up to 83 K in the single-layer FeSe/STO films. Moreover, we find that the superconductivity pairing state can be further divided into two temperature regions of 64-83 K and below 64 K. We propose the 64-83 K region may be attributed to superconductivity fluctuation while the region below 64 K corresponds to the realization of long-range superconducting phase coherence. These results indicate that either Tc as high as 83 K is achievable in iron-based superconductors, or there is a pseudogap formation from superconductivity fluctuation in single-layer FeSe/STO films.

cond-mat.supr-con↗

arXiv2020

Evidence for bosonic mode coupling in electron dynamics of LiFeAs superconductor

Super-high resolution laser-based angle-resolved photoemission measurements are carried out on LiFeAs superconductor to investigate its electron dynamics. Three energy scales at $\sim$20 meV, $\sim$34 meV and $\sim$55 meV are revealed for the first time in the electron self-energy both in the superconducting state and normal state. The $\sim$20 meV and $\sim$34 meV scales can be attributed to the coupling of electrons with sharp bosonic modes which are most likely phonons. These observations provide definitive evidence on the existence of mode coupling in iron-based superconductors.

cond-mat.supr-con↗