Theoretical design and study of two-dimensional organic ferroelectric monolayer based on cyclobutene-1,2-dicarboxylic acid

Tong Jian; Ma Liang

doi:10.7498/aps.71.20211759

Abstract

Compared with traditional inorganic ferroelectric materials, organic molecular ferroelectric materials possess many advantages, such as light weight, flexibility, no heavy metal atoms and low cost, and have received extensive attention for a long time. In recent years, atomic-thick two-dimensional (2D) inorganic ferroelectric materials have achieved breakthrough and attracted much attention. However, there are few reports on the design and research of two-dimensional organic ferroelectric materials. In this paper, we theoretically propose a 2D monolayer organic ferroelectric molecular crystal with the cyclobutene-1,2-dicarboxylic acid (CBDC) molecules as the building block based on density functional theory calculations. The bulk of CBDC molecular crystals clearly shows layered structure due to the chain-like arrangement of hydrogen bonds in crystal. It is found that the internal hydrogen bond chains give rise to the anisotropic cleavage energy values along different crystal planes of the CBDC molecular crystal bulk. Theoretical calculation suggests that the CBDC based 2D monolayer organic ferroelectric molecular crystal can be achieved by the mechanical/chemical peeling along the (102) crystal plane because of the lowest cleavage energy. It is predicted that the in-plane spontaneous polarization of the CBDC (102) molecular crystal monolayer is ～0.39 × 10^–6 μC/cm, which is comparable to those of some inorganic counterparts. Calculations also indicate that the CBDC (102) molecular crystal monolayer shows a high polarization reversal barrier and is sensitive to the external uniaxial stress. The CBDC (102) monolayer organic ferroelectric molecular crystal reveals high in-plane spontaneous polarization with polarization reversal barrier easily modulated by the interface strain engineering, thereby rendering it great potential in lightweight, metal-free and flexible ferroelectric devices.

Keywords:

Authors and contacts

Tong Jian,
Ma Liang

School of Physics, Southeast University, Nanjing 211189, China

Corresponding author: Ma Liang, liang.ma@seu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 21903014) and the Basic Research Program of Jiangsu Province, China (Grant No. BK20190328).

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References

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[6]	Bertolazzi S, Brivio J, Kis A 2011 ACS Nano 5 9703 Google Scholar
[7]	Cai Y, Lan J, Zhang G, Zhang Y W 2014 Phys. Rev. B 89 035438 Google Scholar
[8]	Profeta G, Calandra M, Mauri F 2012 Nat. Phys. 8 131 Google Scholar
[9]	Zhou J J, Feng W, Liu C C, Guan S, Yao Y 2014 Nano Lett. 14 4767 Google Scholar
[10]	Li X, Yang J 2014 J. Mater. Chem. C 8 8098 Google Scholar
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[18]	Wang H, Liu Z R, Yoong H Y, Paudel T R, Xiao J X, Guo R, Lin W N, Yang P, Wang J, Chow G M, Venkatesan T, Tsymbal E Y, Tian H, Chen J S 2018 Nat. Commun. 9 3319 Google Scholar
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[23]	Liu C, Wan W, Ma J, Guo W, Yao Y 2018 Nanoscale 10 7984 Google Scholar
[24]	Liu F, You L, Seyler K L, Li X, Yu P, Lin J, Wang X, Zhou J, Wang H, He H, Pantelides S T, Zhou W, Sharma P, Xu X, Ajayan P M, Wang J, Liu Z 2016 Nat. Commun. 7 12357 Google Scholar
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[26]	Reimers J R, Tawfik S A, Ford M J 2018 Chem. Sci. 9 7620 Google Scholar
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[37]	Tang Y Y, Li P F, Zhang W Y, Ye H Y, You Y M, Xiong R G 2017 J. Am. Chem. Soc. 139 13903 Google Scholar
[38]	Yang Q, Xiong W, Zhu L, Gao G, Wu M 2017 J. Am. Chem. Soc. 139 11506 Google Scholar
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[41]	Ma L, Jia Y, Ducharme S, Wang J, Zeng X C 2019 J. Am. Chem. Soc. 141 1452 Google Scholar
[42]	Kresse G, Furthmuller J 1996 Phys. Rev. B 54 11169 Google Scholar
[43]	Perdew J P, Yue W 1986 Phys. Rev. B 33 8800 Google Scholar
[44]	Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[45]	Blochl P E 1994 Phys. Rev. B 50 17953 Google Scholar
[46]	Grimme S, Antony J, Ehrlich S, Krieg H 2010 J. Chem. Phys. 132 154104 Google Scholar
[47]	Monkhorst H J, Pack J D 1976 Phys. Rev. B 13 5188 Google Scholar
[48]	King-Smith R D, Vanderbilt D 1993 Phys. Rev. B. 47 1651 Google Scholar
[49]	Horiuchi S, Tokunaga Y, Giovannetti G, Picozzi S, Itoh H, Shimano R, Kumai R, Tokura Y 2010 Nature 463 789 Google Scholar
[50]	Horiuchi S, Kumai R, Tokura Y 2011 Adv. Mater. 23 2098 Google Scholar
[51]	Horiuchi S, Kagawa F, Hatahara K, Kobayashi K, Kumai R, Murakami Y, Tokura Y 2012 Nat. Commun. 3 1308 Google Scholar
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Cited By

图 1 优化后的CBDC分子晶体结构图示　(a) CBDC块体的斜视图; (b)—(d)分别为晶胞沿a, b, c基矢方向的视图. 图中灰色、白色和红色小球分别指代碳原子、氢原子和氧原子

Figure 1. Optimized structure of bulk of CBDC molecular crystal: (a) Perspective view of bulk CBDC; (b)–(d) view of bulk CBDC along a, b and c axis, respectively. The gray, white and red balls denote C, H and O atoms, respectively.

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图 2 优化后的块体3-HPLN分子沿晶胞不同基矢方向的晶体结构视图　(a) 基矢a方向; (b) 基矢b方向; (c) 基矢c方向. 图中灰色、乳白色和红色小球分别指代碳原子、氢原子和氧原子

Figure 2. View of optimized structure of bulk 3-HPLN molecular crystal along different axes: (a) Along a axis; (b) along b axis; (c) along c axis. The gray, milk white and red balls denote C, H and O atoms, respectively.

DownLoad: Full-Size Img PowerPoint

图 3 优化后的块体PhMDA分子沿晶胞不同基矢方向的晶体结构视图　(a) 基矢a方向; (b) 基矢b方向; (c) 基矢c方向. 图中灰色、乳白色和红色小球分别指代碳原子、氢原子和氧原子

Figure 3. View of optimized structure of bulk PhMDA molecular crystal along different axes:. (a) Along a axis; (b) along b axis; (c) along c axis. The gray, milk white and red balls denote C, H and O atoms respectively.

DownLoad: Full-Size Img PowerPoint

图 4 CBDC晶体的铁电机制. 图中绿色圆圈标注了氢键的位置, 其中质子的集体迁移导致了铁电极化由晶格$[20\bar{1}]$方向转为$ [\bar{2}01] $方向; 灰色、乳白色和红色小球分别指代碳原子、氢原子和氧原子

Figure 4. Ferroelectric mechanism of CBDC crystal. Green circles mark the collective transfer of protons within the hydrogen bonds, leading to the orientation of polarity being reversed from $ [20\bar{1}] $ direction to $ [\bar{2}01] $ direction. The gray, milk white and red balls denote C, H and O atoms, respectively.

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图 5 CBDC分子晶体块体沿(102)晶面的剥离示意图. 其中左图中黄色平面代表(102)密勒晶面, 右图为(102)单层的顶视图. 灰色乳白色和红色小球分别指代碳原子、氢原子和氧原子.

Figure 5. Exfoliation of CBDC bulk crystal along the (102) Millar plane. The yellow plane in left panel denotes the (102) plane. The right panel is the top view of the single-unit-thick (102) plane. The gray, white and red balls denote C, H and O atoms respectively.

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图 6 CBDC块体沿着(100), (010), (010)和(102)晶面的剥离能, 图中横坐标为相邻两单层之间相对于初始结构所拉开的距离

Figure 6. Energy required to cleave the bulk of CBDC molecular crystal along (100), (010), (001) and (102) plane. The x axis denotes the interlayer distance of the two fractured sections compared with the original bulk crystal.

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图 7 (a) 顺电相下的CBDC (102), 绿色圆圈中质子处于相邻两个氧原子中间处; (b) 顺电相下的CBDC (102)中的CBDC分子结构示意图, 黄色平面为分子的对称面

Figure 7. (a) Paraelectric phase of CBDC (102) monolayer crystal, the protons in green circles are located at the center of the adjacent oxygen atoms; (b) CBDC molecular in paraelectric phase, the yellow plane denotes symmetry plane of the molecular.

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图 8 CBDC (102)分子单层从顺电参考相(λ = 0)转变至铁电相(λ = 1)的过程中极化值的演变曲线

Figure 8. Evolution curves of ferroelectric polarization for CBDC (102) monolayer crystal from the referenced paraelectric phase (λ = 0) to ferroelectric phase (λ = 1).

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图 9 CBDC (102)铁电极化反转路径的能量变化曲线

Figure 9. Energy profile along the polarity reverse path of the CBDC (102) monolayer crystal.

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图 10 平行于极化方向的单轴压缩应力下单层CBDC (102)的极化反转能量曲线

Figure 10. Potential energy curve for the polarity reversal of the CBDC (102) monolayer crystal under uniaxial compressive strain range of 1%–5%.

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图 11 平行于极化方向的单轴拉伸应力下CBDC (102)单层分子晶体的极化反转能量曲线

Figure 11. Potential energy curve for the polarity reversal of the CBDC (102) monolayer crystal under uniaxial tensile strain range of 1%–5%.

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图 12 二维CBDC (102)单层分子晶体在–5%—5%单轴应力下的极化反转势垒变化曲线

Figure 12. Ferroelectric reversing barrier of two-dimensional CBDC (102) monolayer molecular crystal under uniaxial strain from –5% to 5%.

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图 13 单层CBDC (102)的能带结构(带隙值为3.4 eV)

Figure 13. Band structure of CBDC (102) monolayer crystal.

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图 14 石墨烯基底上的CBDC (102)单层分子晶体经过5 ps从头算分子动力学模拟后的结构图(NPT系综, 温度300 K, 时间步长1 fs)　(a) 正视图; (b) 侧视图. 图(a)中绿色曲线指示了多条有序排列的氢键链, 为清晰起见, 图(a)中的石墨烯衬底已被隐去

Figure 14. (a) Top and (b) side views of snapshot of the two-dimensional CBDC (102) monolayer supported on a graphene sheet, after 5 ps of AIMD simulation. The substrate in panel (a) is removed for clarity.

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表 1 铁电相CBDC分子晶体的自发极化

Table 1. Spontaneous polarization of ferroelectric phase of CBDC molecular crystal.

Polarization/(μC·cm^–2)
a b c

Exp. 8.6 0 10
DFT (Horiuchi^[52]) 11.7 0 9.6
DFT (Our work) 11.7 0 9.5

DownLoad: CSV

表 2 CBDC (102)的晶格参数以及自发铁电极化值

Table 2. Lattice parameters and spontaneous ferroelectric polarization of CBDC (102).

a/Å b/Å γ/(°) P_s/(10^–6μC·cm^–1)

CBDC (102) 14.92 13.56 90 0.39

DownLoad: CSV

[1]	Novoselov K S, Geim A K, Morozov S V, Jiang D, Zhang Y, Dubonos S V, Grigorieva I V, Firsov A A 2004 Science 306 666 Google Scholar
[2]	Radisavljevic B, Radenovic A, Brivio J, Giacometti V, Kis A 2011 Nat. Nanotechnol. 6 147 Google Scholar
[3]	Lopez-Sanchez O, Lembke D, Kayci M, Radenovic A, Kis A 2013 Nat. Nanotechnol. 8 497 Google Scholar
[4]	Zeng H, Dai J, Yao W, Xiao D, Cui X 2012 Nat. Nanotechnol. 7 490 Google Scholar
[5]	Cong C, Shang J, Wu X, Cao B, Peimyoo N, Qiu C, Sun L, Yu T 2014 Adv. Opt. Mater. 2 131 Google Scholar
[6]	Bertolazzi S, Brivio J, Kis A 2011 ACS Nano 5 9703 Google Scholar
[7]	Cai Y, Lan J, Zhang G, Zhang Y W 2014 Phys. Rev. B 89 035438 Google Scholar
[8]	Profeta G, Calandra M, Mauri F 2012 Nat. Phys. 8 131 Google Scholar
[9]	Zhou J J, Feng W, Liu C C, Guan S, Yao Y 2014 Nano Lett. 14 4767 Google Scholar
[10]	Li X, Yang J 2014 J. Mater. Chem. C 8 8098 Google Scholar
[11]	Belianinov A, He Q, Dziaugys A, Maksymovych P, Eliseev E, Borisevich A, Morozovska A, Banys J, Vysochanskii Y, Kalinin S V 2015 Nano Lett. 15 3808 Google Scholar
[12]	Bune A V, Fridkin V M, Ducharme S, Blinov L M, Palto S P, Sorokin A V, Yudin S G, Zlatkin A 1998 Nature 391 874 Google Scholar
[13]	Blinov L M, Fridkin V M, Palto S P, Bune A V, Dowben P A, Ducharme S 2000 Phys. Usp. 43 243 Google Scholar
[14]	Mehta R R, Silverman B D, Jacobs J T 1973 J. Appl. Phys. 44 3379 Google Scholar
[15]	Fong D D, Stephenson G B, Streiffer S K, Eastman J A, Auciello O, Fuoss P H, Thompson C 2004 Science 304 1650 Google Scholar
[16]	Gruverman A, Wu D, Lu H, Wang Y, Jang H W, Folkman C M, Zhuravlev M Y, Felker D, Rzchowski M, Eom C B, Tsymbal E Y 2009 Nano Lett. 9 3539 Google Scholar
[17]	Jin Hu W, Wang Z, Yu W, Wu T 2016 Nat. Commun. 7 10808 Google Scholar
[18]	Wang H, Liu Z R, Yoong H Y, Paudel T R, Xiao J X, Guo R, Lin W N, Yang P, Wang J, Chow G M, Venkatesan T, Tsymbal E Y, Tian H, Chen J S 2018 Nat. Commun. 9 3319 Google Scholar
[19]	Chang K, Liu J, Lin H, Wang N, Zhao K, Zhang A, Jin F, Zhong Y, Hu X, Duan W, Zhang Q, Fu L, Xue Q K, Chen X, Ji S H 2016 Science 353 274 Google Scholar
[20]	Yang Q, Wu M, Li J 2018 J. Phys. Chem. Lett. 9 7160 Google Scholar
[21]	Fei R, Kang W, Yang L 2016 Phys. Rev. Lett. 117 097601 Google Scholar
[22]	Wu M, Zeng X C 2016 Nano Lett. 16 3236 Google Scholar
[23]	Liu C, Wan W, Ma J, Guo W, Yao Y 2018 Nanoscale 10 7984 Google Scholar
[24]	Liu F, You L, Seyler K L, Li X, Yu P, Lin J, Wang X, Zhou J, Wang H, He H, Pantelides S T, Zhou W, Sharma P, Xu X, Ajayan P M, Wang J, Liu Z 2016 Nat. Commun. 7 12357 Google Scholar
[25]	Xu B, Xiang H, Xia Y, Jiang K, Wan X, He J, Yin J, Liu Z 2017 Nanoscale 9 8427 Google Scholar
[26]	Reimers J R, Tawfik S A, Ford M J 2018 Chem. Sci. 9 7620 Google Scholar
[27]	Lai Y, Song Z, Wan Y, Xue M, Wang C, Ye Y, Dai L, Zhang Z, Yang W, Du H, Yang J 2019 Nanoscale 11 5163 Google Scholar
[28]	Ding W, Zhu J, Wang Z, Gao Y, Xiao D, Gu Y, Zhang Z, Zhu W 2017 Nat. Commun. 8 14956 Google Scholar
[29]	Cui C, Hu W J, Yan X, Addiego C, Gao W, Wang Y, Wang Z, Li L, Cheng Y, Li P, Zhang X, Alshareef H N, Wu T, Zhu W, Pan X, Li L J 2018 Nano Lett. 18 1253 Google Scholar
[30]	Wu M, Zeng X C 2017 Nano Lett. 17 6309 Google Scholar
[31]	Ren Y, Dong S, Wu M 2018 ACS Appl. Mater. Interfaces 10 35361 Google Scholar
[32]	Wu M, Duan T, Lu C, Fu H, Dong S, Liu J 2018 Nanoscale 10 9509 Google Scholar
[33]	Valasek J 1921 Phys. Rev. 17 475 Google Scholar
[34]	Furukawa T 1989 Phase Transitions 18 143 Google Scholar
[35]	Naber R C, Asadi K, Blom P W, de Leeuw D M, de Boer B 2010 Adv. Mater. 22 933 Google Scholar
[36]	Heremans P, Gelinck G H, Muller R, Baeg K J, Kim D Y, Noh Y Y 2011 Chem. Mater. 23 341 Google Scholar
[37]	Tang Y Y, Li P F, Zhang W Y, Ye H Y, You Y M, Xiong R G 2017 J. Am. Chem. Soc. 139 13903 Google Scholar
[38]	Yang Q, Xiong W, Zhu L, Gao G, Wu M 2017 J. Am. Chem. Soc. 139 11506 Google Scholar
[39]	Yang C K, Chen W N, Ding Y T, Wang J, Rao Y, Liao W Q, Tang Y Y, Li P F, Wang Z X, Xiong R G 2019 Adv. Mater. 3 1 Google Scholar
[40]	Shi P P, Lu S Q, Song X J, Chen X G, Liao W Q, Li P F, Tang Y Y, Xiong R G 2019 J. Am. Chem. Soc. 141 18334 Google Scholar
[41]	Ma L, Jia Y, Ducharme S, Wang J, Zeng X C 2019 J. Am. Chem. Soc. 141 1452 Google Scholar
[42]	Kresse G, Furthmuller J 1996 Phys. Rev. B 54 11169 Google Scholar
[43]	Perdew J P, Yue W 1986 Phys. Rev. B 33 8800 Google Scholar
[44]	Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[45]	Blochl P E 1994 Phys. Rev. B 50 17953 Google Scholar
[46]	Grimme S, Antony J, Ehrlich S, Krieg H 2010 J. Chem. Phys. 132 154104 Google Scholar
[47]	Monkhorst H J, Pack J D 1976 Phys. Rev. B 13 5188 Google Scholar
[48]	King-Smith R D, Vanderbilt D 1993 Phys. Rev. B. 47 1651 Google Scholar
[49]	Horiuchi S, Tokunaga Y, Giovannetti G, Picozzi S, Itoh H, Shimano R, Kumai R, Tokura Y 2010 Nature 463 789 Google Scholar
[50]	Horiuchi S, Kumai R, Tokura Y 2011 Adv. Mater. 23 2098 Google Scholar
[51]	Horiuchi S, Kagawa F, Hatahara K, Kobayashi K, Kumai R, Murakami Y, Tokura Y 2012 Nat. Commun. 3 1308 Google Scholar
[52]	Horiuchi S, Kobayashi K, Kumai R, Ishibashi S 2017 Nat. Commun. 8 14426 Google Scholar

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Vol. 71, Issue 6 - 2022-03-20

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