Optical absorption and thermionic emission mechanism of multi-functional La1–x Srx B6 hexaborides

Zhang Hong-Yan; Bao Li-Hong; Chao Luo-Meng; Zhao Feng-Qi; Liu Zi-Zhong

doi:10.7498/aps.70.20211069

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:

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
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[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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图 1 La_0.825Sr_0.125B₆晶体结构示意图

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

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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

Figure 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 ℃.

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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

Figure 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.

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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

Figure 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 .

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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

Figure 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.

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

Figure 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

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

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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

Figure 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

Figure 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

Figure 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

Figure 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

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

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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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