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Achieving high carrier mobility and low lattice thermal conductivity in gete-based alloys by cationic/anionic co-doping

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Rare Metals 2024年第6期43卷 2784-2795页

作者： Xiao-Qiang Wang Xiao-Quan Hu Jun-Yan Lin Chu-Bin Li Xiao-Tong Yu Qi-Yong Chen Li-Li Xi Qi-Shuo Yang Han Li Ji-Ye Zhang Shuan-Kui Li Kai Guo School of Physics and Materials Science Guangzhou University Research Center for Advanced Information Materials (CAIM) Huangpu Research & Graduate School of Guangzhou University School of Materials Science and Engineering Shanghai University Materials Genome Institute Shanghai University School of Mechanical and Mining Engineering University of Queensland Key Laboratory of Si-Based Information Materials & Devices and Integrated Circuits Design Department of Education of Guangdong Province

The Ⅳ-Ⅵ compound gete is considered as a promising alternative to the toxic PbTe for high-efficiency mid-temperature thermoelectric applications.However,pristine gete suffers from a high concentration of Ge vacancies,resulting in an excessively high hole concentration(> 1 × 1021cm-3),which greatly limits its thermoelectric enhancement.To address this issue,CuBiTe2alloying is introduced to increase the formation energy of Ge vacancies in gete,thereby inhibiting the high carrier concentration.The carrier scattering caused by the electronegativity difference between different elements is suppressed due to the similar electronegativity of Cu and Ge atoms.A relatively high hole mobility is obtained,which ultimately leads to a high power factor.Additionally,by introducing Se as an alloying element at the anionic site in gete,dense point defects with mass/strainfield fluctuations are induced.This contributes to the strengthening of phonon scattering,thereby reducing the lattice thermal conductivity from 1.44 W·m-1·K-1for pristine gete to 0.28 W·m-1·K-1for Ge0.95Cu0.05Bi0.05Te0.9Se0.15compound at 623 K.

关键词： gete Carrier mobility CuBiTe 2 alloying Lattice thermal conductivity Thermoelectric properties

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巧妙的稀掺杂策略实现高性能gete热电材料

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Science Bulletin 2024年第8期69卷 1037-1049页

作者：钟锦璇杨晓玉吕途梁格格张胜楠张朝华敖伟琴刘福生南鹏飞葛炳辉胡利鹏 College of Materials Science and Engineering Shenzhen Key Laboratory of Special Functional MaterialsGuangdong Research Center for Interfacial Engineering of Functional MaterialsGuangdong Provincial Key Laboratory of Deep Earth Sciences and Geothermal Energy Exploitation and UtilizationInstitute of Deep Earth Sciences and Green EnergyShenzhen UniversityShenzhen 518060China Information Materials and Intelligent Sensing Laboratory of Anhui Province Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationInstitutes of Physical Science and Information TechnologyAnhui UniversityHefei 230601China Superconducting Materials Research Center Northwest Institute for Nonferrous Metal ResearchXi’an 710016China

In thermoelectrics,doping is essential to augment the figure of merit.Traditional strategy,predomina ntly heavy doping,aims to optimize carrier concentration and restrain lattice thermal conductivity.However,this tactic can severely hamper carrier transport due to pronounced point defect scattering,particularly in materials with inherently low carrier mean-free-path.Conversely,dilute doping,although minimally affecting carrier mobility,frequently fails to optimize other vital thermoelectric parameters.Herein,we present a more nuanced dilute doping strategy in gete,leveraging the multifaceted roles of small-size metal atoms.A mere 4%CuPbSbTe_(3)introduction into gete swiftly suppresses rhombohedral distortion and optimizes carrier concentration through the aid of Cu interstitials.Additionally,the formation of multiscale microstructures,including zero-dimensional Cu interstitials,one-dimensional dislocations,two-dimensional planar defects,and three-dimensional nanoscale amorphous GeO_(2)and Cu_(2)gete_(3)precipitates,along with the ensuing lattice softening,contributes to an ultralow lattice thermal conductivity.Intriguingly,dilute CuPbSbTe_(3)doping incurs only a marginal decrease in carrier mobility.Subsequent trace Cd doping,employed to alleviate the bipolar effect and align the valence bands,yields an impressive figure-of-merit of 2.03 at 623 K in(Ge_(0.97)Cd_(0.03)Te)_(0.96)(CuPbSbTe_(3))_(0.04).This leads to a high energyconversion efficiency of 7.9%and a significant power density of 3.44 W cm^(-2)at a temperature difference of 500 K.These results underscore the invaluable insights gained into the constructive role of nuanced dilute doping in the concurrent tuning of carrier and phonon transport in gete and other thermoelectric materials.

关键词： Thermoelectric gete Dilute doping Interstitial atoms Lattice softening

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范德华铁磁体Fegete反常霍尔效应调控研究

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太原理工大学学报 2024年

作者：吴凯乐王峻山姜交林柴倩王钦桑胜波葛阳太原理工大学材料科学与工程学院能源革命创新研究院太原理工大学电子信息与光学工程学院微纳传感与人工智能感知山西省重点实验室

磁性材料的本征磁矩可以引发反常霍尔效应，显著降低霍尔电阻，从而改善微纳电子器件热损弊端。二维范德华磁性材料在原子级厚度上展现了出色的铁磁特性与输运性能，可用于制备下一代低维自旋电子器件，在低功耗自旋电子学、量子计算和... 详细信息

磁性材料的本征磁矩可以引发反常霍尔效应，显著降低霍尔电阻，从而改善微纳电子器件热损弊端。二维范德华磁性材料在原子级厚度上展现了出色的铁磁特性与输运性能，可用于制备下一代低维自旋电子器件，在低功耗自旋电子学、量子计算和光通信领域具有巨大的潜力。本文首先研究了块体Fe3gete2(FGT)的铁磁性和磁各向异性，结果表明，块体FGT在低于居里温度(Tc=165K)时，具有显著的面外磁易轴(H//c)。其次，制备了基于FGT的标准霍尔器件，并详细研究了不同温度和外加磁场方向下FGT纳米片的磁电输运性能。结果显示，零磁场时，存在0.764 Ω的反常霍尔电阻(20 K)，并且，在140 K时减小到 0.332 Ω，证明了FGT具有随温度调控的反常霍尔效应；随着外加磁场方向改变，磁滞回环由接近矩形逐渐转变为扁平菱形，表明FGT磁化方向已由面外转变为面内，进一步验证了FGT具有本征的面外磁各向异性。最后，我们还计算了大磁场下(-6 T～6 T)FGT的载流子浓度(20K时为2.5×1022cm-3)和迁移率(20 K时为13.3cm2/(V·s))。

关键词：范德华铁磁体 Fe gete 磁各向异性反常霍尔效应磁滞回线

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Enhanced near-room-temperature thermoelectric performance in gete

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Rare Metals 2022年第9期41卷 3027-3034页

作者： Xian Yi Tan Jin-Feng Dong Ning Jia Hong-Xia Zhang Rong Ji Ady Suwardi Zhi-Liang Li Qiang Zhu Jian-Wei Xu Qing-Yu Yan School of Materials Science and Engineering Nanyang Technological UniversitySingapore639798Singapore Institute of Materials Research and Engineering Agency for ScienceTechnology and ResearchSingapore138634Singapore Key Laboratory of High-Precision Computation and Application of Quantum Field Theory of Hebei Province College of Physics Science and TechnologyHebei UniversityBaoding071002China

gete is an excellent mid-temperature thermoelectric material with high dimensionless figure of merit(ZT)values at temperatures over 600 K.Its near-room-temperature performance is less studied due to the intrinsic high carrier concentration.Here,we successfully enhance the Seebeck coefficient of gete from~30 to 220μV·K^(−1) at 300 K,which is achieved by AgInSe2 alloying and Bi doping.It is demonstrated that Bi doping helps to optimize the Seebeck coefficient without deteriorating the intrinsic electrical transport properties of the matrix.A high room-temperature power factor(PF)of~11μW·cm^(−1)·K^(−2) is achieved for a wide range of Bi-doped samples.The simultaneously introduced abundant point defects cause mass and strain fluctuations,which decrease the lattice thermal conductivity(κ_(L))to a low value of 0.6 W·m^(−1)·K^(−1) at 300 K.Due to the synergetic effects of Bi doping in AgInSe2-alloyed gete,a high room-temperature ZT value of 0.46 is obtained together with a high ZT value of 1.1 at 523 K.

关键词： Thermoelectric gete Thermal conductivity Room-temperature ZT

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Se-alloying reducing lattice thermal conductivity of Ge_(0.95)Bi_(0.05)Te

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Journal of Materials Science & Technology 2022年第11期106卷 249-256页

作者： De-Zhuang Wang Wei-Di Liu Xiao-Lei Shi Han Gao Hao Wu Liang-Cao Yin Yuewen Zhang Yifeng Wang Xueping Wu Qingfeng Liu Zhi-Gang Chen State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing211800China Centre for Future Materials University of Southern QueenslandSpringfield CentralQLD 4300Australia School of Mechanical and Mining Engineering The University of QueenslandBrisbaneQLD 4072Australia Key Laboratory of Material Physics of Ministry of Education School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou450052China College of Materials science and engineering Nanjing Tech UniversityNanjing211800China School of Chemistry and Chemical Engineering Hefei University of TechnologyHefei230009China CAS Key Laboratory of Carbon Materials Institute of Coal ChemistryChinese Academy of SciencesTaiyuan030001China

High lattice thermal conductivity of intrinsic gete limits the wide application of gete-based thermoelectrics.Recently,the optimization of gete-based thermoelectric materials has been focusing on reducing lattice thermal conductivity via strengthening phonon scattering.In this study,we systematically studied thermoelectric properties of Se-alloyed Ge_(0.95) Bi_(0.05) Te via theoretical calculations,structural characterizations,and performance evaluations.Our results indicate that Se-alloying can induce dense point defects with mass/strain-field fluctuations and correspondingly enhance point defect phonon scattering of the Ge_(0.95) Bi_(0.05) Te matrix.Se-alloying might also change chemical bonding strength to introduce resonant states in the base frequency of Ge_(0.95) Bi_(0.05) Te matrix,which can strengthen Umklapp phonon scattering.Finally,a decreased lattice thermal conductivity from∼1.02 W m^(−1) K^(−1) to∼0.65 W m^(−1) K^(−1) at 723 K is obtained in Ge_(0.95) Bi_(0.05) Te_(1-x) Se_(x) pellets with increasing the Se content from 0 to 0.3.A peak figure of merit of∼1.6 at 723 K is achieved in Ge_(0.95) Bi_(0.05) Te_(0.7) Se_(0.3) pellet,which is∼77%higher than that of pristine gete.This study extends the understanding on the thermoelectric performance of gete.

关键词： Thermoelectric gete Se-alloying Lattice thermal conductivity

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gete热电材料的研究和进展

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材料导报 2022年第3期36卷 103-112页

作者：董源徐桂英北京科技大学材料科学与工程学院北京100083

当今,化石能源短缺和环境污染问题日益严峻,影响了人们的日常生活以及工业生产。世界各国都在寻找能够绿色高效地利用能源的新技术途径。在众多新技术途径中,热电转换技术因具有可以直接把热能转换成电能、不产生气体排放、不需要预先... 详细信息

当今,化石能源短缺和环境污染问题日益严峻,影响了人们的日常生活以及工业生产。世界各国都在寻找能够绿色高效地利用能源的新技术途径。在众多新技术途径中,热电转换技术因具有可以直接把热能转换成电能、不产生气体排放、不需要预先生产热能、仅靠工业生产和日常生活的废热即可发电等特点,受到工业界和学术界越来越广泛的关注。目前已经在深空探测、能源回收、空调制冷、芯片冷却等方面得到应用。半导体gete材料,是一种非常有前景的中温热电材料。在gete合成中,一般Ge不能完全参与反应而产生Ge空位,一个Ge空位会产生两个空穴,空穴作为载流子完成电导和电子热导,所以gete的热电性能与Ge的参与反应数量有关,受其制备工艺的影响很大。由于Ge不能完全参与反应,产生了大量的空穴载流子,载流子浓度高导致电导率高的同时,电子热导率也很大,限制了gete的热电应用。gete因为禁带比较窄,并且存在相转变过程,使其有着复杂的热电行为特征。采用不同的元素掺杂和烧结成型工艺会对gete的组成、晶体和能带结构及其热电性能产生巨大影响,为探索合适的组成、微观结构和制备工艺以提高gete基材料的热电优值提供了可能。此外gete基热电材料还具有较好的力学性能,满足高性能热电器件应用对力学性能的要求。这些特性使gete基合金成为目前为止在深空探测中得到实际应用的性能优良的p型中温热电半导体材料。本文主要从烧结工艺、元素掺杂、理论计算等方面,较详细地梳理总结了到目前为止对提高gete热电性能的探索和研究成果,以期为gete基热电材料的深入研究和广泛应用提供参考。

关键词：热电材料半导体 gete

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加热器顶置间接加热gete相变的四端口高速射频开关

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科学通报 2022年第17期67卷 1966-1974页

作者：刘元安穆冬梅肖烽于翠屏北京邮电大学电子工程学院北京100876

针对传统加热器中置间接加热相变开关的固有切换速度缓慢难题,本文提出一种加热器顶置的射频开关新结构,即加热器顶置的间接加热相变材料四端口开关(four-port indirect heating phase change switch with a top microheater,FIPCS-T),... 详细信息

针对传统加热器中置间接加热相变开关的固有切换速度缓慢难题,本文提出一种加热器顶置的射频开关新结构,即加热器顶置的间接加热相变材料四端口开关(four-port indirect heating phase change switch with a top microheater,FIPCS-T),通过热传导过程自上而下的定向性,建立了更加有效的焦耳热能量利用方法.新结构中不同射频参数的仿真表明,FIPCS-T结构对升温过程和淬火过程均能有效缩短相变材料达到临界温度的时间,升温过程比淬火过程的缩短更加显著.相比于传统中置间接加热相变开关,FIPCS-T的升温-淬火环节时间缩短20%以上,这不仅显著提高了切换速度,同时还降低了相变材料的重结晶风险,结合相变材料本身具有的高频低损耗特征及其器件结构设计的灵活性,从而可在微波、毫米波、太赫兹等超大范围频段内提供反射小、插损低和端口隔离度高的高速射频开关.尽管人们对gete相变材料在信息存储等方面的应用开展了多年研究,但其特殊相变特征能否解决未来射频开关面临的高性能需求,仍然存在诸多挑战.本文研究结果表明,gete热相变机理与PIN二极管、微机电系统(microelectromechanical systems,MEMS)等其他原理相比,新射频开关的速度更快、工作频率更高、插入损耗更低.在射频开关特性验证的基础上,我们构建了由5个FIPCS-T单元组成的缺陷地结构(defected ground structure,DGS)可重构滤波器,实现了滤波器频率和带宽的重构,证明了开关状态组合对滤波器媒质特性的调控能力;再通过5个单元FIPCS-T开关状态的组合与电致热控制,实现了低通、带通滤波特征的可重构,为未来大规模天线、大规模电路等先进可重构无线电系统的智慧调控提供了全新的射频开关机理和方法.同时,引入类似相变存储器多值方案的控制方法,可有效提升相变开关的调控和选择维度,增加可调控的性能范围和参数,实现其他类型开关不能实现的更深层次调控优势.

关键词：射频开关热相变材料 gete 间接加热可重构微波毫米波

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Phase and Defect Engineering of gete-based Alloys for High Thermoelectric Performance

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Chinese Journal of Structural Chemistry 2020年第5期39卷 821-830页

作者： ZHANG Chao-Hua WANG Yi-Bo LI Jun-Qin LIU Fu-Sheng College of Materials Science and Engineering Shenzhen Key Laboratory of Special Functional MaterialsShenzhen Engineering Laboratory for Advanced Technology of CeramicsGuangdong Research Center for Interfacial Engineering of Functional MaterialsInstitute of Deep Underground Sciences and Green EnergyShenzhen UniversityShenzhen 518060China

The widespread applications of thermoelectric(TE)materials in power generation and solid-state cooling require improving their TE figure of merit(ZT)significantly.Recently,gete-based alloys have shown great promise as mid-temperature TE materials with superhigh TE performance,mostly due to their relatively high-degeneracy band structures and low lattice thermal conductivity.In this perspective,we review the most recent progress of the gete-based TE alloys from the view of phase and defect engineering.These two strategies are the most widely-used and efficient approaches in gete-based alloys to optimize the transport properties of electrons and phonons for high ZT.The phase transition from rhombohedral to cubic structure is believed to improve the band convergence of gete-based alloys for higher electrical performance.Typical defects in gete-based alloys include the point defects from Ge vacancies and substitutional dopants,linear and planar defects from Ge vacancies.The defect engineering of gete-based alloys is important not only for optimizing the carrier density but also for tuning the band structure and phonon-scattering processes.The summarized strategies in this review can also be used as a reference for guiding the further development of gete-based alloys and also other TE materials.

关键词： gete thermoelectric phase defect Ge vacancies

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Pressure effects on the electrical transport and anharmonic lattice dynamics of r-gete:A first-principles study

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Journal of Materiomics 2021年第6期7卷 1190-1197页

作者： Juan Cui Shasha Li Chengliang Xia Yue Chen Jiaqing He Shenzhen Key Laboratory of Thermoelectric Materials Department of PhysicsSouthern University of Science and TechnologyShenzhen518055China Department of Mechanical Engineering The University of Hong KongPokfulam RoadSARHong KongChina School of Science Nanjing University of Posts and TelecommunicationsNanjing210023China HKU Zhejiang Institute of Research and Innovation 1623 Dayuan RoadLin A311305China Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Southern University of Science and TechnologyShenzhen518055China

Various strategies for thermoelectric material optimization have been widely studied and used for promoting electrical transport and suppressing thermal transport.As a nontraditional method,pressure has shown great potential,as it has been applied to obtain a high thermoelectric figure of merit,but the microscopic mechanisms involved have yet to be fully explored.In this study,we focus on r-gete,a lowtemperature phase of gete,and investigate the pressure effects on the electronic structure,electrical transport properties and anharmonic lattice dynamics based on density functional theory(DFT),the Boltzmann transport equations(BTEs)and perturbation theory.Electronic relaxation times are obtained based on the electron-phonon interaction and the constant relaxation time approximation.The corresponding electrical transport properties are compared with those obtained from previous experiments.Hydrostatic pressure is shown to increase valley degeneracy,decrease the band effective mass and enhance the electrical transport property.At the same time,the increase in the low-frequency phonon lifetime and phonon group velocity leads to an increase in lattice thermal conductivity under pressure.This study provides insight into r-gete under hydrostatic pressure and paves the way for a high-pressure strategy to optimize transport properties.

关键词： gete Pressure effect Electronic structure Transport properties

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gete薄膜欧姆接触研究及相变开关的制备

GeTe薄膜欧姆接触研究及相变开关的制备

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作者：王佳梅电子科技大学

学位级别：硕士

相变开关可用于实现信号的切换、信号中继以及其他网络重构活动等。在卫星系统、军事领域等有着广泛应用。本文从gete薄膜制备以及gete薄膜与金属欧姆接触的角度出发,设计了直接加热型相变开关结构,研制出gete相变开关并对其性能进行了... 详细信息

相变开关可用于实现信号的切换、信号中继以及其他网络重构活动等。在卫星系统、军事领域等有着广泛应用。本文从gete薄膜制备以及gete薄膜与金属欧姆接触的角度出发,设计了直接加热型相变开关结构,研制出gete相变开关并对其性能进行了测试。通过优化溅射参数得到gete薄膜的最佳溅射条件为160 W、1.6 Pa、80 sccm。实现非晶态与晶态电阻比超过10Ω。gete薄膜在220℃以上温度下退火可以发生相变,优先沿着(202)和(220)两晶面生长。退火后表面有氧化物Te O和GeO的生成。晶态gete薄膜有两种振动模式分别为Ge-Te和Te-Te。通过分峰拟合得到非晶态可能是五种结构的组合。利用传输线模型和圆形传输线模型的两种方法首次量化了gete薄膜与NiCr薄膜接触的比接触电阻率,分别为3.66×10Ω·cm和7.45×10Ω·cm。退火后gete/Ni Cr结构比接触电阻率降低,EDS结果显示退火后在界面处存在相互扩散现象,是比接触电阻率降低的主要原因。氨水溶液预处理gete薄膜表面可使其富Ge,有利于gete/Ni Cr接触的比接触电阻率减小。盐酸溶液预处理gete薄膜表面使其富Te,导致比接触电阻率增大。以NiCr为加热电极,设计了新型的两端口直接加热型相变开关,并完成器件的制备以及性能测试。开启脉冲电压最小为8 V,关闭脉冲最快为20 ns。在0-25GHz隔离度大于30 d B,插损小于1.7 d B。在此基础上设计了一种四端口直接加热型相变开关,该相变开关的关闭脉冲为14 V-30 ns,开启脉冲为10 V-7μs,均满足射频开关在射频前端应用要求。

关键词： gete 欧姆接触 CTLM TLM 相变开关

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