Menglin Huang, Shanshan Wang, Shiyou Chen
Strong nonradiative recombination has been observed in quasi-one-dimensional antimony selenide, which runs counter to the simple intuition that claims high defect tolerance exists in semiconductors with antibonding state in the valence band and bonding state in the conduction band. Here we reveal such a defect intolerance actually stems from the richness of structural metastability and vibrational anharmonicity owing to the low-symmetry atomic structure. Taking the deep defect V$_{\rm Se}$ as a benchmark, we show the defect with its ground-state configuration alone does not act as a recombination center. Instead, we identify three different configurations with different formation energies, such richness of metastability offers a higher probability to accomplish a rapid recombination cycle. Another contributing factor is the anharmonicity in the potential energy surfaces that is caused by the large atomic relaxation, which elevates the total capture coefficient by 2-3 orders of magnitude compared with harmonic approximation. Therefore, the unique properties from both crystals and phonons in quasi-one-dimensional system enhance the nonradiative recombination, making the traditional intuition of defect tolerance invalid. These results highlight the importance of the correct identification of metastable defects and phonon anharmonicity in the nonradiative recombination in low-symmetry semiconductors.
Menglin Huang, Zhengneng Zheng, Zhenxing Dai, Xinjing Guo, Shanshan Wang, Lilai Jiang, Jinchen Wei, Shiyou Chen
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.
He Li, Menglin Huang, Shiyou Chen
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.
Siyuan Chen, Heng Xu, Yanjun Guo, Bojun Wang, R. Nicolas Caballero, Jinchen Jiang, Jiangwei Xu, Zihan Xue, Kejia Lee, Jianping Yuan, Yonghua Xu, Jingbo Wang, Longfei Hao, Jintao Luo, Jinlin Han, Peng Jiang, Zhiqiang Shen, Min Wang, Na Wang, Renxin Xu, Xiangping Wu, Lei Qian, Xin Guan, Menglin Huang, Chun Sun, Yan Zhu
The Chinese Pulsar Timing Array (CPTA) has collected observations from 57 millisecond pulsars using the Five-hundred-meter Aperture Spherical Radio Telescope (FAST) for close to three years, for the purpose of searching for gravitational waves (GWs). To robustly search for ultra-low-frequency GWs, pulsar timing arrays (PTAs) need to use models to describe the noise from the individual pulsars. We report on the results from the single pulsar noise analysis of the CPTA data release I (DR1). Conventionally, power laws in the frequency domain are used to describe pulsar red noise and dispersion measurement (DM) variations over time. Employing Bayesian methods, we found the choice of number and range of frequency bins with the highest evidence for each pulsar individually. A comparison between a dataset using DM piecewise measured (DMX) values and a power-law Gaussian process to describe the DM variations shows strong Bayesian evidence in favour of the power-law model. Furthermore, we demonstrate that the constraints obtained from four independent software packages are very consistent with each other. The short time span of the CPTA DR1, paired with the large sensitivity of FAST, has proved to be a challenge for the conventional noise model using a power law. This mainly shows in the difficulty to separate different noise terms due to their covariances with each other. Nineteen pulsars are found to display covariances between the short-term white noise and long-term red and DM noise. With future CPTA datasets, we expect that the degeneracy can be broken. Finally, we compared the CPTA DR1 results against the noise properties found by other PTA collaborations. While we can see broad agreement, there is some tension between different PTA datasets for some of the overlapping pulsars. This could be due to the differences in the methods and frequency range compared to the other PTAs.
Junjie Zhou, Xinpeng Li, Menglin Huang, Shiyou Chen
Atomic vibrations play a critical role in phonon-assisted electron transitions at defects in solids. However, accurate phonon calculations in defect systems are often hindered by the high computational cost of large-supercell first-principles calculations. Recently, foundation models, such as universal machine learning interatomic potentials (MLIPs), emerge as a promising alternative for rapid phonon calculations, but the quantitatively low accuracy restricts its fundamental applicability for high-level defect phonon calculations, such as nonradiative carrier capture rates. In this paper, we propose a "one defect, one potential" strategy in which an MLIP is trained on a limited set of perturbed supercells. We demonstrate that this strategy yields phonons with accuracy comparable to density functional theory (DFT), regardless of the supercell size. The predicted accuracy of defect phonons is validated by phonon frequencies, Huang-Rhys factors, and phonon dispersions. Further calculations of photoluminescence (PL) spectra and nonradiative capture rates based on this defect-specific model also show good agreements with DFT results, meanwhile reducing the computational expenses by more than an order of magnitude. Our approach provides a practical pathway for studying defect phonons in 10$^4$-atom large supercell with high accuracy and efficiency.
Wenze Li, Zhichen Pan, Lei Qian, Liyun Zhang, Yujie Chen, Dejiang Yin, Baoda Li, Yinfeng Dai, Yaowei Li, Dongyue Jiang, Qiaoli Hao, Menglin Huang, Xingyi Wang, Xianghua Niu, Minglei Guo, Jinyou Song, Shuangyuan Chen
As most of the companions in the double neutron star systems should be normal pulsars, the Fast Folding Algorithm (FFA), which is suitable for finding these long spin period pulsars, was used to search their possible radio signals. A time domain resampling code PYSOLATOR was used to maximize the available data length by removing the orbital modulation. We collected and processed 272.2 hours observational data taken by the Five-hundred-meter Aperture Spherical radio Telescope (FAST) for the 13 double neutron star systems in its sky. The signal-to-noise ratios of known pulsar signals are obviously improved by this search method, including the detection of a faint pulsar signal which only saw by folding the data. Unfortunately, no companion signals were found among all the 197962 candidates. Geodetic precession of the orbit could enhance detectability in future observations.
Weiwei Zhu, Di Li, Rui Luo, Chenchen Miao, Bing Zhang, Laura Spitler, Duncan Lorimer, Michael Kramer, David Champion, Youling Yue, Andrew Cameron, Marilyn Cruces, Ran Duan, Yi Feng, Jun Han, George Hobbs, Chenhui Niu, Jiarui Niu, Zhichen Pan, Lei Qian, Dai Shi, Ningyu Tang, Pei Wang, Hongfeng Wang, Mao Yuan, Lei Zhang, Xinxin Zhang, Shuyun Cao, Li Feng, Hengqian Gan, Long Gao, Xuedong Gu, Minglei Guo, Qiaoli Hao, Lin Huang, Menglin Huang, Peng Jiang, Chengjin Jin, Hui Li, Qi Li, Qisheng Li, Hongfei Liu, Gaofeng Pan, Bo Peng, Hui Qian, Xiangwei Shi, Jinyuo Song, Liqiang Song, Caihong Sun, Jinghai Sun, Hong Wang, Qiming Wang, Yi Wang, Xiaoyao Xie, Jun Yan, Li Yang, Shimo Yang, Rui Yao, Dongjun Yu, Jinglong Yu, Chengmin Zhang, Haiyan Zhang, Shuxin Zhang, Xiaonian Zheng, Aiying Zhou, Boqin Zhu, Lichun Zhu, Ming Zhu, Wenbai Zhu, Yan Zhu
Apr 29, 2020·astro-ph.HE·PDF We report the discovery of a highly dispersed fast radio burst, FRB~181123, from an analysis of $\sim$1500~hr of drift-scan survey data taken using the Five-hundred-meter Aperture Spherical radio Telescope (FAST). The pulse has three distinct emission components, which vary with frequency across our 1.0--1.5~GHz observing band. We measure the peak flux density to be $>0.065$~Jy and the corresponding fluence $>0.2$~Jy~ms. Based on the observed dispersion measure of 1812~cm$^{-3}$~pc, we infer a redshift of $\sim 1.9$. From this, we estimate the peak luminosity and isotropic energy to be $\lesssim 2\times10^{43}$~erg~s$^{-1}$ and $\lesssim 2\times10^{40}$~erg, respectively. With only one FRB from the survey detected so far, our constraints on the event rate are limited. We derive a 95\% confidence lower limit for the event rate of 900 FRBs per day for FRBs with fluences $>0.025$~Jy~ms. We performed follow-up observations of the source with FAST for four hours and have not found a repeated burst. We discuss the implications of this discovery for our understanding of the physical mechanisms of FRBs.
Shanshan Wang, Menglin Huang, Su-Huai Wei, Xin-Gao Gong, Shiyou Chen
The ABC model has been widely used to describe the carrier recombination rate, in which the rate of non-radiative recombination assisted by deep-level defects is assumed to depend linearly on excess carrier density $Δn$, leading to a constant recombination coefficient A. However, for multi-level defects that are prevalent in semiconductors, we demonstrate here that the rate should depend nonlinearly on $Δn$. When $Δn$ varies, the carrier capture and emission of defects can change the defect density distribution in different charge states, which can further change the carrier capture and emission rates of the defects and thus make the recombination rate depend non-linearly on $Δn$, leading to an $A(n)$ function. However, in many recent calculation studies on carrier recombination rate of multi-level defects, only carrier capture was considered while carrier emission from defect levels was neglected, causing incorrect charge-state distribution and misleading linear dependence of the rate on $Δn$. For $\text{V}_{\text{Ga}}$-$\text{O}_{\text{N}}$ in GaN and $\text{Pb}_\text{I}$ in CsPbI$_3$, our calculations showed that neglecting the carrier emission can cause the recombination rate underestimation by more than 8 orders of magnitude when $Δn$ is $10^{15}$ cm$^{-3}$. Our findings suggest that the recent studies on carrier recombination assisted by multi-level defects should be revisited with carrier emission considered, and the widely-used $ABC$ model should be reformed into the $A(n)BC$ model.
Jiangwei Xu, Jinchen Jiang, Heng Xu, Bojun Wang, Zihan Xue, Siyuan Chen, Yanjun Guo, R. Nicolas Caballero, Kejia Lee, Jianping Yuan, Yonghua Xu, Jingbo Wang, Longfei Hao, Zhixuan Li, Yuxiang Huang, Zezhong Xu, Jintao Luo, Jinlin Han, Peng Jiang, Zhiqiang Shen, Min Wang, Na Wang, Renxin Xu, Xiangping Wu, Lei Qian, Youling Yue, Xin Guan, Menglin Huang, Chun Sun, Yan Zhu
Feb 28, 2025·astro-ph.HE·PDF We present polarization pulse profiles for 56 millisecond pulsars (MSPs) monitored by the Chinese Pulsar Timing Array (CPTA) collaboration using the Five-hundred-meter Aperture Spherical radio Telescope (FAST). The observations centered at 1.25 GHz with a raw bandwidth of 500 MHz. Due to the high sensitivity ($\sim$16 K/Jy) of the FAST telescope and our long integration time, the high signal-to-noise ratio polarization profiles show features hardly detected before. Among 56 pulsars, the polarization profiles of PSRs J0406$+$3039, J1327$+$3423, and J2022$+$2534 were not previously reported. 80\% of MSPs in the sample show weak components below 3\% of peak flux, 25\% of pulsars show interpulse-like structures, and most pulsars show linear polarization position angle jumps. Six pulsars seem to be emitting for full rotation phase, with another thirteen pulsars being good candidates for such a 360$^\circ$ radiator. We find that the distribution of the polarization percentage in our sample is compatible with the normal pulsar distribution. Our detailed evaluation of the MSP polarization properties suggests that the wave propagation effects in the pulsar magnetosphere are important in shaping the MSP polarization pulse profiles.
Dongyue Jiang, Lei Qian, Minglei Guo, Qiaoli Hao, Menglin Huang, Peng Jiang, Hongfei Liu, Chun Sun, Xingyi Wang, Qingliang Yang, Naiping Yu, Lei Zhao, Yutao Zhao, Liyun Zhang, Yichi Zhang, Tongjie Zhang, Zhichen Pan
Dec 26, 2025·astro-ph.EP·PDF We observed comet C/2025 A6 with the Five-hundred-meter Aperture Spherical radio Telescope (FAST) equipped with the ultra-wideband receiver from 2025 October 23 to November 8, and it was the first detection for this comet with FAST.Through trapezoidal fitting of the OH line profiles, we derived the expansion velocities of the water which showed an increase from 1.5$\pm$0.3 km s$^{-1}$ at the heliocentric distance of 0.65 AU to 3.0$\pm$0.9 km s$^{-1}$ at 0.54 AU. Based on these results, we estimated the OH production rates of C/2025 A6 for October 23, October 26, November 4 and November 5 which were (1.0$\pm$0.1)$\times$10$^{29}$, (1.2$\pm$0.1)$\times$10$^{29}$, (1.4$\pm$0.3)$\times$10$^{29}$, and (1.5$\pm$0.4)$\times$10$^{29}$ s$^{-1}$ respectively. The results show a significant upward trend.
Arun Mannodi-Kanakkithodi, Menglin Huang, Prashun Gorai, Seán R. Kavanagh
Point defects in solid-state materials are now routinely simulated using large supercell structures, requiring efficient quantum mechanical solutions. Data-driven and machine learning (ML) models trained on computational data can enable rapid defect property predictions and high-throughput screening. In this article, we provide an overview of prominent efforts to accelerate defect simulations using these approaches. We begin by discussing the motivations for data-driven techniques in defect modeling, and describe efforts over the past decade to use descriptor-based models for rapid screening of defect properties -- most notably in oxides. In particular, we discuss case studies where surrogate models and interatomic potentials were trained on density functional theory (DFT) data, leading to predictions with quantum-mechanical accuracies at a fraction of the cost. In addition to geometry relaxation and formation energy predictions, these interatomic potentials are capable of predicting phonon modes and vibrational free energies to yield defect energetics at finite temperatures -- representing a key frontier for computational defect research. We finish with a discussion on how to connect these approaches and their outputs with experimental data, and provide an outlook on this burgeoning sub-field.
Heng Xu, Siyuan Chen, Yanjun Guo, Jinchen Jiang, Bojun Wang, Jiangwei Xu, Zihan Xue, R. Nicolas Caballero, Jianping Yuan, Yonghua Xu, Jingbo Wang, Longfei Hao, Jingtao Luo, Kejia Lee, Jinlin Han, Peng Jiang, Zhiqiang Shen, Min Wang, Na Wang, Renxin Xu, Xiangping Wu, Richard Manchester, Lei Qian, Xin Guan, Menglin Huang, Chun Sun, Yan Zhu
Jun 28, 2023·astro-ph.HE·PDF Observing and timing a group of millisecond pulsars (MSPs) with high rotational stability enables the direct detection of gravitational waves (GWs). The GW signals can be identified from the spatial correlations encoded in the times-of-arrival of widely spaced pulsar-pairs. The Chinese Pulsar Timing Array (CPTA) is a collaboration aiming at the direct GW detection with observations carried out using Chinese radio telescopes. This short article serves as a `table of contents' for a forthcoming series of papers related to the CPTA Data Release 1 (CPTA DR1) which uses observations from the Five-hundred-meter Aperture Spherical radio Telescope (FAST). Here, after summarizing the time span and accuracy of CPTA DR1, we report the key results of our statistical inference finding a correlated signal with amplitude $\log A_{\rm c}= -14.4 \,^{+1.0}_{-2.8}$ for spectral index in the range of $α\in [-1.8, 1.5]$ assuming a GW background (GWB) induced quadrupolar correlation. The search for the Hellings-Downs (HD) correlation curve is also presented, where some evidence for the HD correlation has been found that a 4.6-$σ$ statistical significance is achieved using the discrete frequency method around the frequency of 14 nHz. We expect that the future International Pulsar Timing Array data analysis and the next CPTA data release will be more sensitive to the nHz GWB, which could verify the current results.
Xinjing Guo, Menglin Huang, Shiyou Chen
As implemented in the commercialized device modeling software, the four-state nonradiative multi-phonon model has attracted intensive attention in the past decade for describing the physics in negative bias temperature instability (NBTI) and other reliability issues of Si/SiO$_\text{2}$ MOSFET devices. It was proposed initially based on the assumption that the oxygen vacancy defects (V$_\text{O}$) in SiO$_\text{2}$ dielectric layer are bistable in the Si-dimer and back-projected structures during carrier capture and emission. Through high-throughput first-principles structural search, we found V$_\text{O}$ on non-equivalent O sites in amorphous SiO$_\text{2}$ can take 4 types of structural configurations in neutral state and 7 types of configurations in +1 charged state after capturing holes, which produce a wide range of charge-state transition levels for trapping holes. The finding contrasts the structural-bistability assumption and makes the four-state model invalid for most of O sites. To describe the reliability physics accurately, we propose an all-state model to consider all these structural configurations as well as all the carrier capture/emission transitions and thermal transitions between them. With the all-state model, we show that the V$_\text{O}$ defects play important roles in causing NBTI, which challenges the recent studies that discarded V$_\text{O}$ as a possible hole trap in NBTI. Our systematical calculations on the diversified V$_\text{O}$ properties and the all-state model provide the microscopic foundation for describing the reliability physics of MOSFETs and other transistors accurately.
Ruirong Bai, Menglin Huang, Shanshan Wang, Shiyou Chen, Yu-Ning Wu
As the electroluminescence (EL) of NV color centers in diamond has been realized in p-i-n diodes,the underlying mechanism remains a puzzle for longer than a decade. In this study,using first-principles approaches,the electronic configurations and the possible transitions are comprehensively investigated. Based on the calculated carrier cross sections and transition rates,the mechanism of the EL of NV centers and the charge-state dynamics are revealed. The continuous EL is maintained by the cycle of NV0 ground (GNV0),NV+ metastable (MNV+) and NV0 excited state (ENV0). The weaker EL intensity compared to photoluminescence (PL) is explained by the bottleneck transition from MNV+ to ENV0 and another non-luminescent transition cycle. Additionally,our results also explain the disappearance of the luminescence of NV- as a result of unbalanced transitions between NV- and NV0. This study not only reveal the mechanism of electroluminescence of NV centers and explain experimental observations,but also provide first-principles insights to understand the charge-dynamics of other color centers under electric and optical field.
Chen-Min Dai, Feifan Bian, Yafeng Zhang, Jiaqi Chen, Zenghua Cai, Menglin Huang, Chunlan Ma
As a newly identified single-crystalline van der Waals dielectric with a high dielectric constant, Bi2SeO5 plays a pivotal role in advancing 2D electronic devices. In this work, we systematically investigate the defect properties of Bi2SeO5 using first-principles calculations based on a hybrid functional. Although Bi2SeO5 is a chemically ternary compound, each constituent element occupies several crystallographically nonequivalent sites, rendering its defect chemistry highly complex. Due to the anomalous +4 cationic valence state of Se, the defect formation energies of same main group anion antisite defects (SeO and OSe) are prohibitively high, and their concentrations can therefore be neglected. In contrast, the extraordinary cation-cation antisite defects BiSe and SeBi emerge as the dominant defects. The pronounced variability in the formation energies of the six types of VO defects demonstrates that identical defect types located on nonequivalent atomic sites can exhibit markedly different properties. Under O-rich and Se/Bi-poor conditions, Bi2SeO5 shows relatively robust p-type behavior. Conversely, under O-poor and Se/Bi-rich conditions, or at intermediate O, Se, and Bi partial pressures, Bi2SeO5 behaves as an intrinsic semiconductor or displays very weak n-type conductivity due to strong donor-acceptor compensation. This study provides theoretical insights to guide the design and development of high-performance Bi2SeO5-based electronic devices.
Xinjing Guo, Menglin Huang, Shiyou Chen
As transistors continue to scale down, device reliability has become a critical concern. In order to accurately simulate defect-induced reliability degradation in MOSFET based logic, memory and power devices, we develop RASP (Reliability Ab initio Simulation Package), which implements the all-state model for reliability simulation. Unlike conventional two-state and four-state models that consider only two and four defect configurations respectively, the all-state model systematically considers all possible defect configurations in amorphous gate dielectrics and all nonradiative multiphonon (NMP) and thermal transition pathways among them. With defect parameters obtained from ab initio calculations as input, RASP enables accurate simulation of threshold voltage shifts caused by defects. Using RASP to simulate oxygen vacancies in a-SiO$_2$, we find that they are a non-negligible source of negative bias temperature instability (NBTI).
Zenghua Cai, Menglin Huang, Peng Zhou, Shiyou Chen
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.
Jiale Zhang, Hui Tian, Stefano Bellotti, Tianqi Cang, Joseph R. Callingham, Harish K. Vedantham, Bin Chen, Sijie Yu, Philippe Zarka, Corentin K. Louis, Peng Jiang, Hongpeng Lu, Yang Gao, Jinghai Sun, Hengqian Gan, Hui Li, Chun Sun, Zheng Lei, Menglin Huang
Oct 20, 2025·astro-ph.SR·PDF Detecting coherent radio bursts from nearby M dwarfs provides opportunities for exploring their magnetic activity and interaction with orbiting exoplanets. However, it remains uncertain if the emission is related to flare-like activity similar to the Sun or magnetospheric process akin to magnetized planets. Using observations (1.0 - 1.5 GHz) taken by the Five-hundred-meter Aperture Spherical radio Telescope, we found a type of millisecond-scale radio bursts with exceptionally high frequency drift rates ($\sim 8\;\rm{GHz\;s^{-1}}$) from an active M dwarf, AD Leo. The ultrafast drift rates point to a source region with a notably low magnetic scale height ($<0.15\; r_\star$, $r_\star$ as the stellar radius), a feature not expected in a commonly assumed dipole-like global field but highly possible in localized strong-field structures, i.e. starspots. Our findings suggest that a concentrated magnetic field above starspots could be responsible for some of the most intense radio bursts from M dwarfs, supporting a solar-like electron acceleration mechanism.
Zhenxing Dai, Zhong Yang, Mingjue Ni, Menglin Huang, Hongjun Xiang, Xin-Gao Gong, Shiyou Chen
Point defects critically influence the properties of materials and devices, yet density functional theory (DFT) remains computationally demanding for defect supercell calculations. Machine learning interatomic potentials (MLIPs) offer high efficiency but require extensive datasets. MLIPs trained only on defect configurations in small supercells exhibit systematic energy errors in larger supercells, demonstrating limited transferability. Here, we present a machine learning Hamiltonian (MLH) model-based method for calculating total energies and atomic forces in defect supercells with linear-scaling computational cost, enabling efficient structural relaxation and accurate formation energy predictions. We take oxygen vacancies in amorphous SiO$_2$ as an example and train the MLH model on defect configurations in 95-atom supercells, with the training data derived from 120 self-consistent field calculations and 12 structural relaxations. The MLH model enables efficient structural relaxations for host (defect-free) and defect systems in larger supercells, avoiding the systematic energy errors observed in MLIPs. The cancellation of energy errors between host and defect systems yields accurate formation energy predictions, with deviations from DFT below 50 meV. The proposed method holds significant potential for defect simulations in complex materials.
Shanshan Wang, Menglin Huang, Yu-Ning Wu, Weibin Chu, Jin Zhao, Aron Walsh, Xin-Gao Gong, Su-Huai Wei, Shiyou Chen
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.