arXiv subjects

Shiyou Chen

Publications and source records attributed to Shiyou Chen.

At least 37 records · Page 2Linked to original sources

arXiv2023

Defect Regulation by Palladium Incorporation towards Grain Boundaries of Kesterite solar cells

Kesterite Cu2ZnSn(S, Se)4 (CZTSSe) solar cell has emerged as one of the most promising candidates for thin-film photovoltaics. However, severe charge losses occurring at the grain boundaries (GBs) of Kesterite polycrystalline absorbers has hindered the improvement of cell performance. Herein, we report a redox reaction strategy involving palladium (Pd) to eliminate atomic vacancy defects such as VSn and VSe in GBs of the Kesterite absorbers. We demonstrate that PdSex compounds could form during the selenization process and distribute at the GBs and the absorber surfaces; thereby aid in the suppression of Sn and Se volatilization loss and inhibiting the formation of VSn and VSe defects. Furthermore, Pd(II)/Pd(IV) serves as a redox shuttle, i.e., on one hand, Pd(II) captures Se vapor from the reaction environment to produce PdSe2, on the other hand, PdSe2 provides Se atoms to the Kesterite absorber by being reduced to PdSe, thus contributing to the elimination of pre-existing VSe defects within GBs. These effects collectively reduce defects and enhance the p-type characteristics of the Kesterite absorber, leading to a significant reduction in charge recombination loss within the cell. As a result, high-performance Kesterite solar cells with a total-area efficiency of 14.5% have been achieved. This remarkable efficiency increase benefited from the redox reaction strategy offers a promising avenue for the precise regulation of defects in Kesterite solar cells and holds generally significant implications for the exploration of various other photovoltaic devices.

cond-mat.mtrl-sci↗

arXiv2023

Transferable Machine Learning Approach for Predicting Electronic Structures of Charged Defects

The study of the electronic properties of charged defects is crucial for our understanding of various electrical properties of materials. However, the high computational cost of density functional theory (DFT) hinders the research on large defect models. In this study, we present an E(3) equivariant graph neural network framework (HamGNN-Q), which can predict the tight-binding Hamiltonian matrices for various defect types with different charges using only one set of network parameters. By incorporating features of background charge into the element representation, HamGNN-Q enables a direct mapping from structure and background charge to the electronic Hamiltonian matrix of charged defect systems without DFT calculation. We demonstrate the model's high precision and transferability through testing on GaAs systems with various charged defect configurations. Our approach provides a practical solution for accelerating charged defect electronic structure calculations and advancing the design of materials with tailored electronic properties.

physics.comp-ph↗

arXiv2023

Vibration and jitter of free-flowing thin liquid sheets as target for high-repetition-rate laser-ion acceleration

Very thin free-flowing liquid sheets are promising targets for high-repetition-rate laser-ion acceleration. In this work, we report the generation of micrometer-thin free-flowing liquid sheets from the collision of two liquid jets, and study the vibration and jitter in their surface normal direction. The dependence of their motion amplitudes on the generation parameters is studied in detail. The origins of the vibration and jitter are discussed. Our results indicate that when the generation parameters are optimized, the motion amplitudes in the stable region can be stabilized below 3.7 μm to meet the stringent requirement of sheet position stability for a tight-focusing setup in laser-ion acceleration experiments.

physics.plasm-ph↗

arXiv2022

Synchronous post-acceleration of laser-driven protons in helical coil targets by controlling the current dispersion

Post-acceleration of protons in helical coil targets driven by intense, ultrashort laser pulses can enhance the ion energy by utilizing the transient current originating from the self-discharging of the targets. The acceleration length of the protons can exceed a few millimeters, and the accelerating gradient is in the order of GeV/m. How to ensure the synchronization of the accelerating electric field with the protons is a crucial problem for an efficient post-acceleration. In this paper, we study how the electric field mismatch induced by the current dispersion affects the synchronous acceleration of the protons. We propose a scheme using a two-stage helical coil to control the current dispersion. With optimized parameters, the energy gain of protons is enhanced by 4 times. And it is expected that the proton energy would reach 45 MeV using a hundreds-terawatt laser, or over 100 MeV using a petawatt laser, by controlling the current dispersion.

physics.plasm-ph↗

arXiv2022

Capturing long-range interaction with reciprocal space neural network

Machine Learning (ML) interatomic models and potentials have been widely employed in simulations of materials. Long-range interactions often dominate in some ionic systems whose dynamics behavior is significantly influenced. However, the long-range effect such as Coulomb and Van der Wales potential is not considered in most ML interatomic potentials. To address this issue, we put forward a method that can take long-range effects into account for most ML local interatomic models with the reciprocal space neural network. The structure information in real space is firstly transformed into reciprocal space and then encoded into a reciprocal space potential or a global descriptor with full atomic interactions. The reciprocal space potential and descriptor keep full invariance of Euclidean symmetry and choice of the cell. Benefiting from the reciprocal-space information, ML interatomic models can be extended to describe the long-range potential including not only Coulomb but any other long-range interaction. A model NaCl system considering Coulomb interaction and the GaxNy system with defects are applied to illustrate the advantage of our approach. At the same time, our approach helps to improve the prediction accuracy of some global properties such as the band gap where the full atomic interaction beyond local atomic environments plays a very important role. In summary, our work has expanded the ability of current ML interatomic models and potentials when dealing with the long-range effect, hence paving a new way for accurate prediction of global properties and large-scale dynamic simulations of systems with defects.

cond-mat.mtrl-sci↗

arXiv2022

Alpha-particle generation from H-11B fusion initiated by laser-accelerated boron ions

Here we report the generation of MeV alpha-particles from H-11B fusion initiated by laser-accelerated boron ions. Boron ions with maximum energy of 6MeV and fluence of 10^9/MeV/sr@5MeV were generated from 60-nm-thick self-supporting boron nanofoils irradiated by 1J femtosecond pulses at an intensity of 10^19W/cm^2. By bombarding secondary hydrogenous targets with the boron ions, 3*10^5/sr alpha-particles from H-11B fusion were registered, which is consistent with the theoretical yield calculated from the measured boron energy spectra. Our results demonstrate an alternative way toward ultrashort MeV alpha-particle sources employing compact femtosecond lasers. The ion acceleration and product measurement scheme are referential for the studies on the ion stopping power and cross-section of the H-11B reaction in solid or plasma.

physics.plasm-ph↗

arXiv2022

Two-Dimensional Organic-Inorganic Room-Temperature Multiferroic

Organic-inorganic multiferroics are promising for the next generation of electronic devices. To date, dozens of organic-inorganic multiferroics have been reported; however, most of them show magnetic Curie temperature much lower than room temperature, which drastically hampers their application. Here, by performing first-principle calculations and building effective model Hamiltonians, we reveal a molecular orbital-mediated magnetic coupling mechanism in two-dimensional Cr(pyz)2 (pyz=pyrazine), and the role that the valence state of the molecule plays in determining the magnetic coupling type between metal ions. Based on these, we demonstrate that a two-dimensional organic-inorganic room-temperature multiferroic, Cr(h-fpyz)2 (h-fpyz= half-fluoropyrazine), can be rationally designed by introducing ferroelectricity in Cr(pyz)2 while keeping the valence state of the molecule unchanged. Our work not only reveals the origin of magnetic coupling in 2D organic-inorganic systems, but also provides a way to design room temperature multiferroic materials rationally.

cond-mat.mtrl-sci↗

arXiv2022

Effective Lifetime of Non-Equilibrium Carriers in Semiconductors from Non-Adiabatic Molecular Dynamics Simulations

The lifetime of non-equilibrium electrons and holes in semiconductors is crucial for solar cell and optoelectronic applications. Non-adiabatic molecular dynamics (NAMD) simulations based on time-dependent density functional theory (TDDFT) are widely used to study excited-state carrier dynamics. However, the calculated carrier lifetimes are often different from experimental results by orders of magnitude. In this work, by revisiting the definition of carrier lifetime and considering different recombination mechanisms, we report a systematic procedure for calculating the effective carrier lifetime in realistic semiconductor crystals that can be compared directly to experimental measurements. The procedure shows that considering all recombination mechanisms and using reasonable densities of carriers and defects are crucial in calculating the effective lifetime. When NAMD simulations consider only Shockey-Read-Hall (SRH) defect-assisted and band-to-band non-radiative recombination while neglect band-to-band radiative recombination, and the densities of non-equilibrium carriers and defects in supercell simulations are much higher than those in realistic semiconductors under solar illumination, the calculated lifetimes are ineffective and thus differ from experiments. Using our procedure, the calculated effective lifetime of the halide perovskite CH3NH3PbI3 agrees with experiments. It is mainly determined by band-to-band radiative and defect-assisted non-radiative recombination, while band-to-band non-radiative recombination is negligible. These results indicate that it is possible to calculate carrier lifetimes accurately based on NAMD simulations, but the directly calculated values should be converted to effective lifetimes for comparison to experiments. The revised procedure can be widely applied in future carrier lifetime simulations.

cond-mat.mtrl-sci↗

arXiv2022

DASP: Defect and Dopant ab-initio Simulation Package

In order to perform automated calculations of defect and dopant properties in semiconductors and insulators, we developed a software package, Defect and Dopant ab-initio Simulation Package (DASP), which is composed of four modules for calculating: (i) elemental chemical potentials, (ii) defect (dopant) formation energies and transition energy levels, (iii) defect and carrier densities and (iv) carrier dynamics properties of high-density defects. DASP uses the materials genome database for quick determination of competing secondary phases and calculation of the energy above convex hull when calculating the elemental chemical potential that stabilizes compound semiconductors, so it can perform high-throughput prediction of thermodynamic stability of multinary compounds. DASP calls the ab-initio softwares to perform the total energy, structural relaxation and electronic structure calculations of the defect supercells with different structure configurations and charge states, based on which the defect formation energies and transition energy levels are calculated and the corrections for electrostatic potential alignment and image charge interaction can be included. Then DASP can calculate the equilibrium densities of defects and electron and hole carriers as well as the Fermi level in semiconductors under different chemical potential conditions and different growth/working temperature. For high-density defects, DASP can calculate the carrier dynamics properties such as the photoluminescence (PL) spectrum, defect-related radiative and non-radiative carrier capture cross sections, and recombination lifetime of non-equilibrium carriers.

cond-mat.mtrl-sci↗

arXiv2021

A Generalized Tunneling Current Formula for Metal/Insulator Heterojunctions under Large Bias and Finite Temperature

The Fowler-Nordheim tunneling current formula has been widely used in the design of devices based on metal/insulator (metal/semiconductor) heterojunctions with triangle potential barriers, such as the flash memory. Here we adopt the model that was used to derive the Landauer formula at finite temperature, the nearly-free electron approximation to describe the electronic states in semi-infinite metal electrode and the Wentzel-Kramers-Brillouin (WKB) approximation to describe the transmission coefficient, and derive a tunneling current formula for metal/insulator heterojunctions under large bias and electric field. In contrast to the Fowler-Nordheim formula which is the limit at zero temperature, our formula is generalized to the finite temperature (with the thermal excitation of electrons in metal electrode considered) and the potential barriers beyond triangle ones, which may be used for the design of more complicated heterojunction devices based on the carrier tunneling.

cond-mat.mes-hall↗

arXiv2020

High-efficiency water-window x-ray generation from nanowire array targets irradiated with femtosecond laser pulses

We demonstrate the high-efficiency generation of water-window soft x-ray emissions from polyethylene nanowire array targets irradiated by femtosecond laser pulses at the intensity of 4*10^19 W/cm^2. The experimental results indicate more than one order of magnitude enhancement of the water-window x-ray emissions from the nanowire array targets compared to the planar targets. The highest energy conversion efficiency from laser to water-window x-rays is measured as 0.5%/sr, which comes from the targets with the longest nanowires. Supported by particle-in-cell simulations and atomic kinetic codes, the physics that leads to the high conversion efficiency is discussed.

physics.plasm-ph↗

arXiv2020

Laser-induced damage thresholds of ultrathin targets and their constrain on laser contrast in laser-driven ion acceleration experiments

Single-shot laser-induced damage threshold (LIDT) measurements of multi-type free-standing ultrathin foils were performed in vacuum environment for 800 nm laser pulses with durations τ ranging from 50 fs to 200 ps. Results show that the laser damage threshold fluences (DTFs) of the ultrathin foils are significantly lower than those of corresponding bulk materials. Wide band gap dielectric targets such as SiN and formvar have larger DTFs than those of semiconductive and conductive targets by 1-3 orders of magnitude depending on the pulse duration. The damage mechanisms for different types of targets are studied. Based on the measurement, the constrain of the LIDTs on the laser contrast is discussed.

physics.plasm-ph↗

arXiv2020

Simultaneous measurements on the electron and X-ray spectra from laser-irradiated near-critical-density double-layer targets at relativistic intensity

We report the experimental results of simultaneous measurements on the electron and X-ray spectra from near-critical-density (NCD) double-layer targets irradiated by relativistic femtosecond pulses at the intensity of 5E19 W/cm^2. The dependence of the electron and X-ray spectra on the density and thickness of the NCD layer was studied. For the optimal targets, electrons with temperature of 5.5 MeV and X-rays with critical energy of 5 keV were obtained. 2D particle-in-cell simulations based on the experimental parameters confirm the electrons are accelerated in the plasma channel through direct laser acceleration, resulting in temperature significantly higher than the pondermotive temperature. Bright X-rays are generated from betatron emission and Thomson backscattering before the electrons leave the double-layer targets.

physics.plasm-ph↗

arXiv2020

First-Principles Exploration of Defect-Pairs in GaN

Using first-principles calculations, we explored all the 21 defect-pairs in GaN and considered 6 configurations with different defect-defect distances for each defect-pair. 15 defect-pairs with short defect-defect distances are found to be stable during structural relaxation, so they can exist in the GaN lattice once formed during the irradiation of high-energy particles. 9 defect-pairs have formation energies lower than 10 eV in the neutral state. The vacancy-pair VN-VN is found to have very low formation energies, as low as 0 eV in p-type and Ga-rich GaN, and act as efficient donors producing two deep donor levels, which can limit the p-type doping and minority carrier lifetime in GaN. VN-VN has been overlooked in the previous study of defects in GaN. Most of these defect-pairs act as donors and produce a large number of defect levels in the band gap. Their formation energies and concentrations are sensitive to the chemical potentials of Ga and N, so their influences on the electrical and optical properties of Ga-rich and N-rich GaN after irradiation should differ significantly. These results about the defect-pairs provide fundamental data for understanding the radiation damage mechanism in GaN and simulating the defect formation and diffusion behavior under irradiation.

cond-mat.mtrl-sci↗

arXiv2019

Impact of Metal ns2 Lone Pair on Luminescence Efficiency in Low-Dimensional Halide Perovskites

Based on first-principles calculations, we show that chemically active metal ns2 lone pairs play an important role in exciton relaxation and dissociation in low-dimensional halide perovskites. We studied excited-state properties of several recently discovered luminescent all-inorganic and hybrid organic-inorganic zero-dimensional (0D) Sn and Pb halides. The results show that, despite the similarity in ground-state electronic structure between Sn and Pb halide perovskites, the chemically more active Sn2+ lone pair leads to stronger excited-state structural distortion and larger Stokes shift in Sn halides. The enhanced Stokes shift hinders excitation energy transport, which reduces energy loss to defects and increases the photoluminescence quantum efficiency (PLQE). The presence of the ns2 metal cations in the 0D halide perovskites also promotes the exciton dissociation into electron and hole polarons especially in all-inorganic compounds, in which the coupling between metal-halide clusters is significant.

cond-mat.mtrl-sci↗

arXiv2018

Biocompatible Two-dimensional Titanium Nanosheets for Efficient Plasmonic Photothermal Cancer Therapy

Photothermal therapy (PTT) has shown significant potential in cancer treatment. However, developing nanomaterial-based photothermal agents with good biocompatibility and high photothermal conversion efficiency (PTCE) remains a key challenge. Titanium has been widely employed as biomedical materials based on their excellent biocompatibility. In this work, the titanium based plasmonic photothermal therapy (Ti-PPTT) is demonstrated. Using the liquid-phase exfoliation (LPE), the metallic Ti can be fabricated into the two-dimensional (2D) nanosheets (NSs), similar to exfoliating other layered 2D materials. The 2D Ti NSs exhibited good biocompatibility, high extinction coefficient of 20.8 Lg-1cm1 and high PTCE of 73.4%, owing to localized surface plasmon resonances (LSPR); which is significantly higher than other photothermal agents, including Au (21%), MoS2 (24.4%), BP (28.4%) and Ti3C2 MXene (30.6%). Consequently, 2D Ti-PPTT exhibited a notable therapeutic effect in a human hepatocellular carcinoma model without side effects. Our study could pave a new avenue for PTT using metal Ti and arouse a wide interest in the potential efficient PTT for other elemental transition metals owing to their LSPR. Furthermore, the efficient photothermal effect and environmental friendliness of Ti NSs make them deserve more research toward other application, such as solar energy harvesting and sea water desalination.

physics.app-ph↗

arXiv2015

Giant biquadratic interaction induced magnetic anisotropy in the iron-based superconductor AxFe2-ySe2

The emergence of the electron-pocket only iron-based superconductor AxFe2-ySe2 (A = alkali metal) challenges the Fermi-surface nesting picture established in iron-pnictides. It was widely believed that magnetism is correlated with the superconductivity in AxFe2-ySe2. Unfortunately, the highly anisotropic exchange parameters and the disagreement between theoretical calculations and experimental results triggered a fierce debate on the nature of magnetism in AxFe2-ySe2. Here we find that the strong magnetic anisotropy is from the anisotropic biquadratic interaction. In order to accurately obtain the magnetic interaction parameters, we propose a universal method, which does not need including other high energy configurations as did in conventional energy mapping method. We show that our model successfully captures the magnetic interactions in AxFe2-ySe2 and correctly predicts the spin wave spectrum, in quantitative agreement with the experimental observation. These results suggest that the local moment picture, including the biquadratic term, can describe accurately the magnetic properties and spin excitations in AxFe2-ySe2, which sheds new light on the future study of the high-Tc iron-based superconductors.

cond-mat.supr-con↗

arXiv2015

Intrinsic Instability of the Hybrid Halide Perovskite Semiconductor CH3NH3PbI3

The organic-inorganic hybrid perovskite CH3NH3PbI3 has attracted significant interest for its high performance in converting solar light into electrical power with an efficiency exceeding 20%. Unfortunately, chemical stability is one major challenge in the development of the CH3NH3PbI3 solar cells. It was commonly assumed that moisture or oxygen in the environment causes the poor stability of hybrid halide perovskites, however, here we show from the first-principles calculations that the room-temperature tetragonal phase of CH3NH3PbI3 is thermodynamically unstable with respect to the phase separation into CH3NH3I + PbI2, i.e., the disproportionation is exothermic, independent of the humidity or oxygen in the atmosphere. When the structure is distorted to the low-temperature orthorhombic phase, the energetic cost of separation increases, but remains small. Contributions from vibrational and configurational entropy at room temperature have been considered, but the instability of CH3NH3PbI3 is unchanged. When I is replaced by Br or Cl, Pb by Sn, or the organic cation CH3NH3 by inorganic Cs, the perovskites become more stable and do not phase-separate spontaneously. Our study highlights that the poor chemical stability is intrinsic to CH3NH3PbI3 and suggests that element-substitution may solve the chemical stability problem in hybrid halide perovskite solar cells.

cond-mat.mtrl-sci↗