多功能多元稀土六硼化物La1–x Srx B6光吸收及热电子发射机理

张红艳; 包黎红; 潮洛蒙; 赵凤岐; 刘子忠

doi:10.7498/aps.70.20211069

摘要

系统研究了多功能多元稀土六硼化物La_1–x Sr_x B₆纳米粉末的光吸收及多晶块体的热电子发射性能. 纳米粉体光吸收结果表明, 多元稀土六硼化物La_1–x Sr_xB₆透射光波长从591 nm至658 nm连续可调. 多晶块体热电子发射结果表明, 外加电压2000 V, 阴极温度为1773 K时, 热电子发射电流密度从2.3 A/cm²线性增大至19.36 A/cm², 表现出了热发射性能增强效果. 因此, 多元稀土六硼化物La_1–x Sr_x B₆为一种多功能材料, 在光吸收材料及热阴极材料领域具有潜在的应用前景. 此外, 为了揭示上述光吸收及热发射机理, 采用第一性原理系统计算体等离子共振频率能量和费米能级变化规律.

关键词:

Abstract

The optical absorption property of the nanocrystalline La_1–x Sr_x B₆ powder and thermionic emission property of the La_1–x Sr_x B₆ polycrystalline bulk are investigated. As a result, the transmission wavelength of LaB₆ is red-shifted from 591 nm to 658 nm with the increase of Sr doping content. The emission tests indicate that the thermionic emission current density of La_1–x Sr_x B₆ polycrystalline bulk increases from 2.3 A/cm² to 19.36 A/cm² with the increase of La doping content under an applied voltage of 2000 V. The first-principle calculation results reveal that Sr doping LaB₆ leads plasma frequency energy and Fermi level to decrease, resulting in the tunable characteristics of transmission wavelength and enhancement of thermionic emission. Therefore, the Sr-doped LaB₆ as a multifunctional ceramic has a potential application in the field of optical filter or becomes a promising cathode for microwave device.

Keywords:

作者及机构信息

1.
内蒙古师范大学物理与电子信息学院, 呼和浩特　010022

2.
内蒙古科技大学理学院, 包头　014010

3.
内蒙古师范大学化学与环境科学学院, 呼和浩特　010022

通信作者: 包黎红, baolihong@imnu.edu.cn

基金项目: 内蒙古自治区自然科学基金(批准号: 2019LH05001)和国家自然科学基金(批准号: 51662034)资助的课题

Authors and contacts

1.
College of Physics and Electronic Information, Inner Mongolia Normal University, Hohhot, 010022, China

2.
College of Science, Inner Mongolia University of Science Technology, Baotou 014010, China

3.
College of Chemistry and Environment Science, Inner Mongolia Normal University, Hohhot 010022, China

Corresponding author: Bao Li-Hong, baolihong@imnu.edu.cn

Funds: Project supported by the Natural Science Foundation of Inner Mongolia Autonomous Region, China (Grant No. 2019LH05001) and the National Natural Science Foundation of China (Grant No. 51662034).

[1]	Kirley M P, Novakovic B, Sule N, Weber M J, Knezevic I, Booske J H 2012 J. Appl. Phys. 111 063717 Google Scholar
[2]	Xu J Q, Hou G H, Li H Q, Zhai T Y, Dong B P, Yan H L, Wang Y R, Yu B H, Bando Y, Golberg D 2013 NPG Asia Mater. 5 547 Google Scholar
[3]	Kumari M, Gautam S, Shah P V, Pal S, Ojha U S, Kumar A, Naik A A, Rawat J S, Chaudhury P K, Harsh, Tandon R P 2012 Appl. Phys. Lett. 101 4995 Google Scholar
[4]	Yuan Y F, Zhang L, HuLJ, Wang W, Min G H 2011 J. Solid State Chem. 184 3364 Google Scholar
[5]	Tang H B, Su Y C, Tan J, Hu T, GongJY, Xiao L H 2014 Superattice Microst. 75 908 Google Scholar
[6]	Chao L M, Bao L H, Wei W, Tegus O, Zhang Z D 2016 J. Alloys. Compd. 672 419 Google Scholar
[7]	Mattox T M, Agrawal A, Milliron D J 2015 Chem. Mater. 27 6620 Google Scholar
[8]	Chen M C, Lin Z W, Ling M H 2016 Acs Nano 10 93 Google Scholar
[9]	Chen C J, Chen D H 2012 Chem. Eng. 180 337 Google Scholar
[10]	Tang S L, Huang W C, Gao Y, An N, Wu Y D, Yang B, Yan M, Cao J Y, Guo C S 2021 J. Mater. Chem. B 9 4380 Google Scholar
[11]	Takeda H, Kuno H, Adachi K 2008 J. Am. Ceram. Soc. 91 2897 Google Scholar
[12]	Schelm S, Smith G B 2003 Appl. Phys. Lett. 82 4346 Google Scholar
[13]	Adachi K, Miratsu M, Asahi T 2010 J. Mater. Res. 25 510 Google Scholar
[14]	Schelm S, Smith G B, Grrett P D, Fisher W K 2005 J. Appl. Phys. 97 124314 Google Scholar
[15]	Smith G B 2002 Mater. Forum. 26 20
[16]	Bao L H, Qi X P, Ta N, Chao L M, Tegus O 2016 Phys. Chem. Chem. Phys. 18 19165 Google Scholar
[17]	Bao L H, Chao L M, Wei W, Tegus O 2015 Mater. Lett. 139 187 Google Scholar
[18]	Bao L H, Qi X P, Bao T N, Tegus O 2018 J. Alloy. Compd. 731 332 Google Scholar
[19]	Zhou S L, Zhang J X, Bao L H, Yu X G, Hu Q L, Hu D Q 2014 J. Alloys. Compd. 611 130 Google Scholar
[20]	Hasan M M, Cuskelly D, Sugo H, Kisi E H 2015 J. Alloy. Compd. 636 37 Google Scholar
[21]	Hohenberg P, Kohn W 1964 Phys. Rev. 136 B864
[22]	Vanderbilt D 1990 Phys. Rev. B 41 7892 Google Scholar
[23]	Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[24]	Chao L M, Bao L H, Shi J J, Wei W, Tegus O, Zhang Z D 2015 J. Alloy. Compd. 622 618 Google Scholar
[25]	Liu H L, Zhang X, Ning S Y 2017 Vacuum 143 245 Google Scholar
[26]	Bao L H, Ming M, Tegus O 2015 J. Inorg. Mater. 30 1110 Google Scholar
[27]	Xiao L H, Su Y C, Zhou X Z, Chen H Y, Tan J, Hu T, Yan J, Peng P 2012 Appl. Phys. Lett. 101 041913 Google Scholar
[28]	Kimura S, Nanba T, Kunii S, Kasuya T 1990 Phys. Rev. B 59 3388 Google Scholar
[29]	Kauer E 1963 Phys. Lett. 7 171 Google Scholar
[30]	Kimura S, Nanba T, Kunii S, Suzuki T, Kasuya T 1990 Solid State Commun. 75 717 Google Scholar
[31]	Bao L H, Qi X P, Ta N, Chao L M, Tegus O 2016 Cryst. Eng. Comm. 18 1223 Google Scholar
[32]	Xin S W, Liu S C, Wang N, Han X Y, Wang L M, Xu B, Tian Y J, Liu Z Y, He J L, Yu D L 2011 J. Alloy. Compd. 509 7927 Google Scholar
[33]	Zheng S, Zou Z, Min G, Yu H S, Han J D, Wang W T 2002 J. Mater. Sci. Lett. 21 313 Google Scholar
[34]	Wang J, Zhu C, Meng F S, Liu G B, Gu Y, Wang H D, Gao S S, Wang K M 2018 Mod. Phys. Lett. B 32 1850007 Google Scholar
[35]	Futamoto M, Nakazawa M, Kawabe U 1980 Surf. Sci 100 470 Google Scholar
[36]	Swanson L W, Mcneely D R 1979 Surf. Sci 83 11 Google Scholar
[37]	周身林, 张久兴, 刘丹敏 2010 强激光与离子束 22 171 Google Scholar Zhou S L, Zhang J X, Liu D M 2010 High Power Laser and Particle Beams 22 171 Google Scholar

施引文献

图 1 La_0.825Sr_0.125B₆晶体结构示意图

Fig. 1. Schematic diagram of the La_0.825Sr_0.125B₆ crystal structure.

下载: 全尺寸图片幻灯片

图 2 (a)不同反应温度下制备的La_0.4Sr_0.6B₆纳米颗粒的XRD谱图; (b) 1150 ℃下制备的La_1–x Sr_x B₆纳米颗粒的XRD谱图

Fig. 2. (a) XRD pattern of La_0.4Sr_0.6B₆ nanoparticles prepared at different reaction temperatures; (b) XRD pattern of La_1–x Sr_x B₆ nanoparticles prepared at 1150 ℃.

下载: 全尺寸图片幻灯片

图 3 不同反应温度下所制备的纳米La_1–x Sr_x B₆ (x = 0.2, 0.4, 0.6, 0.8)粉末SEM照片　(a)—(d)反应温度为1150 ℃; (e)—(h)反应温度为1200℃. 最底层为纳米La_0.4Sr_0.6B₆粉末元素分布及EDS分析

Fig. 3. SEM image of La_1–x Sr_x B₆ (x = 0.2, 0.4, 0.6, 0.8) nanoparticles (a)−(d) prepared at 1150 ℃, (e)−(h) prepared at 1200 ℃. The lowest side shows the elements mapping and EDS analysis of La_0.4Sr_0.6B₆ nanoparticles.

下载: 全尺寸图片幻灯片

图 4 纳米La_0.4Sr_0.6B₆粉末的(a) TEM照片、(b)单颗粒形貌照片、(c) HRTEM照片; (d)图(c)的傅里叶(FFT)变换; (e)—(g)所选择的单晶颗粒的La, Sr, B元素分布图

Fig. 4. (a) TEM image of La_0.4Sr_0.6B₆ nanoparticles; (b) selected single crystal morphology; (c) HRTEM image for selected single crystal; (d) indexing FFT patterns from panel (c); (e)−(g) La , Sr , B element mapping for selected single crystal .

下载: 全尺寸图片幻灯片

图 5 纳米La_1–x Sr_x B₆ (x = 0 (a), 0.2 (b), 0.4 (c), 0.6 (d), 0.8 (e))粉末的光学吸收曲线

Fig. 5. Optical absorption spectrum of La_1–x Sr_x B₆ (x = 0 (a), 0.2 (b), 0.4 (c), 0.6 (d), 0.8 (e)) nanoparticles.

下载: 全尺寸图片幻灯片

图 6 La_0.875Sr_0.125B₆晶体的态密度的第一性原理计算结果

Fig. 6. First-principle calculation results of density of states of La_0.875Sr_0.125B₆ crystal.

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图 7 La_0.875Sr_0.125B₆晶体的(a)介电函数和(b)能量损失谱

Fig. 7. (a) Dielectric function and (b) loss function spectra of La_0.875Sr_0.125B₆ crystal.

下载: 全尺寸图片幻灯片

图 8 单晶SrB₆的(a) (100)面、(b) (110)面、(c) (111)面、(d) (210)面的结构示意图及逸出功计算结果; (e) SrB₆多晶块体的热电子发射电流密度随外加电压变化曲线; (f) SrB₆多晶块体的lgJ-U ^0.5曲线

Fig. 8. Schematic diagram of (a) (100) surface, (b) (110) surface, (c) (111) surface, (d) (210) surface of single crystal SrB₆ and the calculated results of escape work; (e) thermionic emission current density of SrB₆ polycrystalline bulk with applied voltage; (f) lgJ-U ^0.5 curves of SrB₆ polycrystalline bulk.

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图 9 La_1–x Sr_x B₆多晶块体的热电子发射电流密度　(a) x = 0.8; (b) x = 0.6; (c) x = 0.4; (d) x = 0.2

Fig. 9. Thermionic emission current density of La_1–x Sr_x B₆ bulks: (a) x = 0.8; (b) x = 0.6; (c) x = 0.4; (d) x = 0.2.

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图 10 La_1–x Sr_x B₆多晶块体肖特基外延曲线　(a) x = 0.8; (b) x = 0.6; (c) x = 0.4; (d) x = 0.2

Fig. 10. Typical Schottky plots for La_1–x Sr_x B₆ bulks: (a) x = 0.8; (b) x = 0.6; (c) x = 0.4; (d) x = 0.2.

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图 11 所提出的La_1–x Sr_x B₆增强热电子发射机理示意图

Fig. 11. Proposed mechanism of the La_1–x Sr_x B₆ enhanced thermionic emission.

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表 1 La_1–x Sr_x B₆ (x =1, 0.8, 0.6, 0.4, 0.2)多晶块体的零场发射电流密度J₀和有效逸出功φ_e

Table 1. Zero field emission current density J₀ and the effective escape work φ_e of the polycrystalline block La_1–x Sr_x B₆ (x = 1, 0.8, 0.6, 0.4, 0.2).

Compound 零场发射电流密度(J₀) 有效逸出功
φ_e/
eV
1673 K 1773 K

SrB₆ 0.97 1.79 2.845
La_0.2Sr_0.8B₆ 1.67 4.73 2.691
La_0.4Sr_0.6B₆ 3.5 8.7 2.585
La_0.6Sr_0.4B₆ 4.1 8.3 2.573
La_0.8Sr_0.2B₆ 5.39 10 2.552

下载: 导出CSV

map

[1]	Kirley M P, Novakovic B, Sule N, Weber M J, Knezevic I, Booske J H 2012 J. Appl. Phys. 111 063717 Google Scholar
[2]	Xu J Q, Hou G H, Li H Q, Zhai T Y, Dong B P, Yan H L, Wang Y R, Yu B H, Bando Y, Golberg D 2013 NPG Asia Mater. 5 547 Google Scholar
[3]	Kumari M, Gautam S, Shah P V, Pal S, Ojha U S, Kumar A, Naik A A, Rawat J S, Chaudhury P K, Harsh, Tandon R P 2012 Appl. Phys. Lett. 101 4995 Google Scholar
[4]	Yuan Y F, Zhang L, HuLJ, Wang W, Min G H 2011 J. Solid State Chem. 184 3364 Google Scholar
[5]	Tang H B, Su Y C, Tan J, Hu T, GongJY, Xiao L H 2014 Superattice Microst. 75 908 Google Scholar
[6]	Chao L M, Bao L H, Wei W, Tegus O, Zhang Z D 2016 J. Alloys. Compd. 672 419 Google Scholar
[7]	Mattox T M, Agrawal A, Milliron D J 2015 Chem. Mater. 27 6620 Google Scholar
[8]	Chen M C, Lin Z W, Ling M H 2016 Acs Nano 10 93 Google Scholar
[9]	Chen C J, Chen D H 2012 Chem. Eng. 180 337 Google Scholar
[10]	Tang S L, Huang W C, Gao Y, An N, Wu Y D, Yang B, Yan M, Cao J Y, Guo C S 2021 J. Mater. Chem. B 9 4380 Google Scholar
[11]	Takeda H, Kuno H, Adachi K 2008 J. Am. Ceram. Soc. 91 2897 Google Scholar
[12]	Schelm S, Smith G B 2003 Appl. Phys. Lett. 82 4346 Google Scholar
[13]	Adachi K, Miratsu M, Asahi T 2010 J. Mater. Res. 25 510 Google Scholar
[14]	Schelm S, Smith G B, Grrett P D, Fisher W K 2005 J. Appl. Phys. 97 124314 Google Scholar
[15]	Smith G B 2002 Mater. Forum. 26 20
[16]	Bao L H, Qi X P, Ta N, Chao L M, Tegus O 2016 Phys. Chem. Chem. Phys. 18 19165 Google Scholar
[17]	Bao L H, Chao L M, Wei W, Tegus O 2015 Mater. Lett. 139 187 Google Scholar
[18]	Bao L H, Qi X P, Bao T N, Tegus O 2018 J. Alloy. Compd. 731 332 Google Scholar
[19]	Zhou S L, Zhang J X, Bao L H, Yu X G, Hu Q L, Hu D Q 2014 J. Alloys. Compd. 611 130 Google Scholar
[20]	Hasan M M, Cuskelly D, Sugo H, Kisi E H 2015 J. Alloy. Compd. 636 37 Google Scholar
[21]	Hohenberg P, Kohn W 1964 Phys. Rev. 136 B864
[22]	Vanderbilt D 1990 Phys. Rev. B 41 7892 Google Scholar
[23]	Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[24]	Chao L M, Bao L H, Shi J J, Wei W, Tegus O, Zhang Z D 2015 J. Alloy. Compd. 622 618 Google Scholar
[25]	Liu H L, Zhang X, Ning S Y 2017 Vacuum 143 245 Google Scholar
[26]	Bao L H, Ming M, Tegus O 2015 J. Inorg. Mater. 30 1110 Google Scholar
[27]	Xiao L H, Su Y C, Zhou X Z, Chen H Y, Tan J, Hu T, Yan J, Peng P 2012 Appl. Phys. Lett. 101 041913 Google Scholar
[28]	Kimura S, Nanba T, Kunii S, Kasuya T 1990 Phys. Rev. B 59 3388 Google Scholar
[29]	Kauer E 1963 Phys. Lett. 7 171 Google Scholar
[30]	Kimura S, Nanba T, Kunii S, Suzuki T, Kasuya T 1990 Solid State Commun. 75 717 Google Scholar
[31]	Bao L H, Qi X P, Ta N, Chao L M, Tegus O 2016 Cryst. Eng. Comm. 18 1223 Google Scholar
[32]	Xin S W, Liu S C, Wang N, Han X Y, Wang L M, Xu B, Tian Y J, Liu Z Y, He J L, Yu D L 2011 J. Alloy. Compd. 509 7927 Google Scholar
[33]	Zheng S, Zou Z, Min G, Yu H S, Han J D, Wang W T 2002 J. Mater. Sci. Lett. 21 313 Google Scholar
[34]	Wang J, Zhu C, Meng F S, Liu G B, Gu Y, Wang H D, Gao S S, Wang K M 2018 Mod. Phys. Lett. B 32 1850007 Google Scholar
[35]	Futamoto M, Nakazawa M, Kawabe U 1980 Surf. Sci 100 470 Google Scholar
[36]	Swanson L W, Mcneely D R 1979 Surf. Sci 83 11 Google Scholar
[37]	周身林, 张久兴, 刘丹敏 2010 强激光与离子束 22 171 Google Scholar Zhou S L, Zhang J X, Liu D M 2010 High Power Laser and Particle Beams 22 171 Google Scholar

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多功能多元稀土六硼化物La_1–x Sr_x B₆光吸收及热电子发射机理

Optical absorption and thermionic emission mechanism of multi-functional La_1–x Sr_x B₆ hexaborides

摘要

Abstract

作者及机构信息

1.
内蒙古师范大学物理与电子信息学院, 呼和浩特　010022

2.
内蒙古科技大学理学院, 包头　014010

3.
内蒙古师范大学化学与环境科学学院, 呼和浩特　010022

通信作者: 包黎红, baolihong@imnu.edu.cn

Authors and contacts

Corresponding author: Bao Li-Hong, baolihong@imnu.edu.cn

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Compound	零场发射电流密度(J₀)		有效逸出功 φ_e/ eV
Compound	1673 K	1773 K	有效逸出功 φ_e/ eV
SrB₆	0.97	1.79	2.845
La_0.2Sr_0.8B₆	1.67	4.73	2.691
La_0.4Sr_0.6B₆	3.5	8.7	2.585
La_0.6Sr_0.4B₆	4.1	8.3	2.573
La_0.8Sr_0.2B₆	5.39	10	2.552

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