Morphologies of self-assembled gold nanorod-surfactant-lipid complexes at molecular level

Yang Ying; Song Jun-Jie; Wan Ming-Wei; Gao Liang-Hui; Fang Wei-Hai

doi:10.7498/aps.69.20200979

Abstract

Gold nanorods (GNRs) have aroused the extensive interest of many researchers in recent years due to their unique physicochemical properties. However, the toxic cetyltrimethylammonium bromide (CTAB) is often introduced into the process of synthesizing GNRs, which hinders the wide-range applications of GNRs in clinical practice. To reduce the toxicity, the CTAB molecules coated on the surface of GNRs should be replaced by nontoxic and biocompatible agents such as phospholipid. Thus the component and morphology of the mixed coating agents on the surface of GNRs affect the physicochemical properties of GNRs. To study the morphology and properties of the coated GNRs at a molecular level, we investigate the self-assembly of GNRs, CTAB, and dimyristoyl phosphatidylcholine (DMPC) by using solvent-free dissipative particle dynamics simulations. Our results show that the morphology of the assembled complex mainly depends on the CTAB/DMPC molar ratio, while neither of the interaction strength between GNRs and the coating agents nor the diameter of GNRs has significant effect on the morphology. At a certain combination of GNRs-coating agent interaction strength with GNRs diameter, the mixture of CTAB and DMPC on the surface of GNRs undergoes a gradual change in morphology as the CTAB/DMPC molar ratio increases, including the forming of intact bilayer membrane, cracked bilayer membrane, long patches of micelles, and short wormlike micelles winding GNRs in spiral shape. The morphology of intact bilayer membrane verifies the experimental guess, while the other three morphologies are brand-new discoveries. We also find that when the GNR’s diameter becomes smaller, or the CTAB/DMPC molar ratio is larger, or the interaction strength is greater, the agents cap the ends of GNRs, meanwhile the membrane thickness becomes thinner. The multiple morphologies of the assembled complexes can be qualitatively explained by the shape energy of a membrane adsorbed on a solid surface. When the surface tension of the membrane (which is proportional to the spontaneous curvature of the membrane) exceeds a critical value (which is equal to the adhesion energy density of the membrane), the membrane dissociates from the solid surface and its shape changes. The change trend is related to the spontaneous curvature of the free membrane. As a result of the synergy and competition among the inherent curvatures of GNRs, the spontaneous curvature of CTAB/DMPC membrane or micelle, as well as the adhesion energy, various interesting morphologies are produced. Our simulations and analyses directly characterize the morphological structures of CTAB and lipid coated GNRs, which allow us to in depth understand the self-assembling behaviors of GNRs at a molecular level. This is also conductive to achieving the controlled assemblies of GNRs.

Keywords:

Authors and contacts

1.
Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875, China
2.
Institution of Theoretical and Computational Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China

Corresponding author: Wan Ming-Wei, wmwbnu@foxmail.com ; Gao Liang-Hui, lhgao@bnu.edu.cn ;

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 21673021, 21421003)

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References

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Cited By

图 1 粗粒化模型　(a) GNRs; (b) CTAB; (c) DMPC

Figure 1. Coarse-grained model of (a) GNRs, (b) CTAB, and (c) DMPC

DownLoad: Full-Size Img PowerPoint

图 2 CTAB和DMPC混合物的形貌图(CTAB的头部H和尾巴T珠子分别用蓝色和黄色表示, 而DMPC的H和M/T珠子分别用红色和绿色表示)

Figure 2. Morphology of a mixture of CTAB and DMPC. The H and T beads of CTAB are colored in blue and yellow, while the H and M/T beads of DMPC are in red and green, respectively.

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图 3 GNRs-CTAB-DMPC复合体在d = 4 nm, D = 4k_BT时的组装形貌, 其中CTAB/DMPC摩尔比分别为(a) 1∶1, (b) 3∶2, (c) 4∶1, (d) 8∶1, (e) 16∶1, (f) 1∶0

Figure 3. Morphology of assembled GNRs-CTAB-DMPC complex with d = 4 nm and D = 4k_BT. The CTAB/DMPC molar ratio is (a) 1∶1, (b) 3∶2, (c) 4∶1, (d) 8∶1, (e) 16∶1, (f) 1∶0, respectively.

DownLoad: Full-Size Img PowerPoint

图 D1 d = 4 nm和D = 4 k_BT时GNRs表面修饰剂的投影展开分布图, 其中摩尔比分别为(a) 1∶1, (b) 3∶2, (c) 4∶1, (d) 8∶1, (e) 16∶1, (f) 1∶0

Figure D1. Projected expansion map of coating agents distributing on the surface of GNRs. Data is obtained at d = 4 nm and D = 4 k_BT. The CTAB/DMPC molar ratio is (a) 1∶1, (b) 3∶2, (c) 4∶1, (d) 8∶1, (e) 16∶1, (f) 1∶0.

DownLoad: Full-Size Img PowerPoint

图 4 (a) 当金纳米棒直径d = 4 nm时, GNRs-CTAB-DMPC复合体在不同CTAB/DMPC摩尔比及D下的组装形貌; (b) 当Morse势参数D = 4k_BT时, GNRs-CTAB-DMPC复合体在不同CTAB/DMPC摩尔比及d下的组装形貌

Figure 4. (a) Morphology of assembled GNRs-CTAB-DMPC complex at various CTAB/DMPC molar ratio and D with given GNR diameter d = 4 nm; (b) morphology of assembled GNRs-CTAB-DMPC complex at various CTAB/DMPC molar ratio and d with given Morse potential parameter D = 4k_BT.

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图 5 (a) CTAB和(b) DMPC的$ \alpha $角的定义示意图

Figure 5. Schematic diagram of definition of $ \alpha $ for (a) CTAB and (b) DMPC.

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图 6 (a) 修饰剂的蠕虫系数F_worm与D的关系图; (b) F_worm与d的关系图; (c) GNRs的覆盖率F_cap与D的关系图; (d) F_cap与d的关系图; 不同颜色的直线代表不同的摩尔比

Figure 6. (a) Worming coefficient F_worm of coating agents as a function of D; (b) F_worm as a function of d; (c) capping rate F_cap of GNRs as a function of D; (d) F_cap as a function of d. Results are obtained at various CTAB/DMPC molar ratios, shown in different colors.

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图 7 CTAB与DMPC的H₁珠子和金珠子在不同D及CTAB/DMPC摩尔比下的RDF, 其中摩尔比分别为(a) 1∶1, (b) 3∶2, (c) 4∶1, (d) 8∶1, (e) 16∶1, (f) 1∶0

Figure 7. RDF between H₁ bead of CTAB and DMPC and gold bead at various D and CTAB/DMPC molar ratios. The molar ratio is (a) 1∶1, (b) 3∶2, (c) 4∶1, (d) 8∶1, (e) 16∶1, (f) 1∶0, respectively.

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图 8 不同CTAB/DMPC摩尔比下得到的膜厚度L_mem与D的关系图.

Figure 8. Membrane thickness L_mem as a function of D. Results are obtained at various CTAB/DMPC molar ratios.

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图 9 不同D下得到的GNRs表面修饰剂的投影展开分布图(GNRs直径d = 4 nm), 其中, 线性拟合斜率代表螺旋程度; 左图是CTAB/DMPC摩尔比为16∶1的结果, (a) D = 1k_BT, (b) D = 2k_BT, (c) D = 3k_BT, (d) D = 4k_BT; 右图是CTAB/DMPC摩尔比为1∶0的结果, (e) D = 1k_BT, (f) D = 2k_BT, (g) D = 3k_BT, (h) D = 4k_BT

Figure 9. Projected expansion map of coating agent distributing on the surface of GNRs with d = 4 nm. The slope of the linear fitting represents the spiral degree. The left panels are results at CTAB/DMPC molar ratio of 16∶1 with (a) D = 1k_BT, (b) D = 2k_BT, (c) D = 3k_BT, (d) D = 4k_BT. The right panels are results at CTAB/DMPC molar ratio of 1∶0 with (e) D = 1k_BT, (f) D = 2k_BT, (g) D = 3k_BT, (h) D = 4k_BT.

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图 C1 纯DMPC和d = 4 nm, D = 4k_BT时GNRs-DMPC的组装形貌　(a) DMPC的形貌及(b)切面图; (c) GNRs-DMPC的形貌及(d)切面图

Figure C1. Morphology of the pure DMPC lipids and assembled GNRs-DMPC complex with d = 4 nm and D = 4k_BT: (a) Morpohology and (b) cross-sectional view of DMPC; (c) morpohology and (d) cross-sectional view of GNRs-DMPC

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图 E1 RDF峰的位置示意图, 其中金珠子用黄色表示, CTAB和DMPC的H₁珠子用红色表示

Figure E1. Schematic diagram of RDF. The GN bead is shown in yellow, the H₁ head beads of CTAB and DMPC were shown in red.

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表 A1 DPD力场中a_ij参数的取值(ION, H₁, H₂, M, T珠子分别和文献[43]中的W, Q₀, Q_a, N_a, C珠子一一对应)

Table A1. Values of parameters a_ij in DPD Force field. The ION, H₁, H₂, M, and T beads correspond to the W, Q₀, Q_a, N_a, and C beads in Ref [43], respectively.

a_ij	ION	H₁	H₂	M	T
ION	100	98	98	102	130
H₁	98	110	100	102	130
H₂	98	100	110	102	130
M	102	102	102	100	110
T	130	130	130	110	100

DownLoad: CSV

表 A2 Im-DPD力场中c, σ和s参数的值

Table A2. Values of c, σ, s in Im-DPD Force field.

	ION	H₁	H₂	M	T
c	0	19.37	19.37	20.02	24.56
σ	0.5385	0.536	0.536	0.541	0.566
s	0.625	0.625	0.625	0.7135	0.7135

DownLoad: CSV

表 A3 Im-DPD力场中的键长、键角和对应的力参数(d是以纳米为单位的金纳米棒的直径)

Table A3. Equilibrium bonds, angles, and corresponding force constants in Im-DPD Force field. d is the diameter of GNRs in unit of nanometer.

bond	L₀/r₀	K₂/k_BT·r₀^–2	angle	θ₀/(º)	K₃/k_BT
GN—GN	d/0.71	512	GN—GN—GN	180	600
H₁—T	0.47	512	H₂—M—M	120	6
H₁—H₂	0.47	512	H₂—M—T	180	6
H₂—M	0.47	512	M—T—T	180	6
M—M	0.31	512	T—T—T	180	6
M—T	0.59	512
T—T	0.59	512

DownLoad: CSV

表 E1 不同D及CTAB/DMPC摩尔比下的r₁, r₂, r₃和L_mem

Table E1. r₁, r₂, r₃ and L_mem at different combinations of D and CTAB/DMPC molar ratio.

Molar ratio	D = 1k_BT			D = 2k_BT			D = 3k_BT				D = 4k_BT
Molar ratio	r₂	r₃	L_mem	r₂	r₃	L_mem	r₁	r₂	r₃	L_mem	r₁	r₂	r₃	L_mem
1∶1	2.88	6.33	3.45	2.72	6.11	3.39		2.62	5.82	3.2	2.24	2.68	5.78	3.1
3∶2	2.93	6.42	3.49	2.72	5.95	3.23		2.64	5.71	3.07	2.25	2.66	5.63	2.97
4∶1	2.89	6.1	3.21	2.8	5.75	2.95	2.32	2.73	5.62	2.89	2.29	2.67	5.36	2.69
8∶1	2.75	6.06	3.31	2.74	5.71	2.97	2.3	2.74	5.52	2.78	2.24	2.70	5.36	2.66
16∶1	2.87	6.09	3.22	2.71	5.74	3.03	2.23	2.70	5.58	2.88	2.26	2.74	5.46	2.72
1∶0	2.75	5.89	3.14	2.79	5.60	2.81	2.29	2.67	5.42	2.75	2.29	2.77	5.36	2.59

DownLoad: CSV

表 B1 单个CTAB胶束的模拟结果, 其中, D是胶束的直径, e是离心率, α是CTAB分子的电离度(更多细节详见文献[50]), 表格中的前3行数据来自文献[50], 用作对比分析

Table B1. Simulations results of the single CTAB micelle. D is the diameter of the micelle, e is the eccentricity, and α is the degree of ionization of CTAB molecules (see Ref. [50] for details). The data in the first three lines are taken from Ref. [50] for comparison.

Force Field	D/nm	e	α
All-atomic	4.79	0.29	0.63
Martini	4.54	0.14	0.78
Dry Martini	4.42	0.12	0.73
Im-DPD	5.13	0.16	0.68

DownLoad: CSV

[1]	Cioffi N, Torsi L, Ditaranto N, Tantillo G, Ghibelli L, Sabbatini L, Bleve-Zacheo T, D'Alessio M, Zambonin P G, Traversa E 2005 Chem. Mater. 17 5255 Google Scholar
[2]	Jin R C, Cao Y W, Mirkin C A, Kelly K L, Schatz G C, Zheng J G 2001 Science 294 1901 Google Scholar
[3]	Levard C, Hotze E M, Lowry G V, Jr Brown G E 2012 Environ. Sci. Technol. 46 6900 Google Scholar
[4]	Elahi N, Kamali M, Baghersad M H 2018 Talanta 184 537 Google Scholar
[5]	黄运欢, 李璞 2015 物理学报 64 207301 Google Scholar Huang Y H, Li P 2015 Acta Phys. Sin. 64 207301 Google Scholar
[6]	柯善林阚彩侠莫博从博朱杰君 2012 物理化学学报 28 1275 Google Scholar Ke S L, Kan C X, Mo B, Cong B, Zhu J J 2012 Acta Phys.-Chim. Sin. 28 1275 Google Scholar
[7]	Singh N, Charan S, Sanjiv K, Huang S H, Hsiao Y C, Kuo C W, Chien F C, Lee T C, Chen P 2012 Bioconjugate Chem. 23 421 Google Scholar
[8]	von Maltzahn G, Centrone A, Park J H, Ramanathan R, Sailor M J, Hatton T A, Bhatia S N 2009 Adv. Mater. 21 3175 Google Scholar
[9]	Zhang Y, Qian J, Wang D, Wang Y, He S 2013 Angew. Chem. Int. Ed. 52 1148 Google Scholar
[10]	Cao J, Galbraith E K, Sun T, Grattan K T V 2012 Sens. Actuators, B 169 360 Google Scholar
[11]	Li X, Qian J, He S 2008 Nanotechnology 19 355501 Google Scholar
[12]	Mayer K M, Hafner J H 2011 Chem. Rev. 111 3828 Google Scholar
[13]	Joshi P P, Yoon S J, Hardin W G, Emelianov S, Sokolov K V 2013 Bioconjugate Chem. 24 878 Google Scholar
[14]	Luo T, Huang P, Gao G, Shen G X, Fu S, Cui D X, Zhou C Q, Ren Q S 2011 Opt. Express 19 17030 Google Scholar
[15]	Zhang J B, Balla N K, Gao C, Sheppard C J R, Yung L Y L, Rehman S, Teo J Y, Kulkarni S R, Fu Y H, Yin S J 2012 Aust. J. Chem. 65 290 Google Scholar
[16]	Troiber C, Kasper J C, Milani S, Scheible M, Martin I, Schaubhut F, Kuchler S, Radler J, Simmel F C, Friess W, Wagner E 2013 Eur. J. Pharmacol. 84 255 Google Scholar
[17]	Xue H Y, Wong H L 2011 ACS Nano 5 7034 Google Scholar
[18]	Martin C R 1994 Science 266 1961 Google Scholar
[19]	Raj M A, John S A 2014 Electrochem. Commun. 45 27 Google Scholar
[20]	Abdelrasoul G N, Cingolani R, Diaspro A, Athanassiou A, Pignatelli F 2014 J. Photochem. Photobiol., A 275 7 Google Scholar
[21]	Johnson C J, Dujardin E, Davis S A, Murphy C J, Mann S 2002 J. Mater. Chem. 12 1765 Google Scholar
[22]	Takahashi H, Niidome Y, Niidome T, Kaneko K, Kawasaki H, Yamada S 2006 Langmuir 22 2 Google Scholar
[23]	Lyubartsev A P, Rabinovich A L 2011 Soft Matter 7 25 Google Scholar
[24]	Orendorff C J, Alam T M, Sasaki D Y, Bunker B C, Voigt J A 2009 ACS Nano 3 971 Google Scholar
[25]	Galati E, Tebbe M, Querejeta-Fernandez A, Xin H L, Gang O, Zhulina E B, Kumacheva E 2017 ACS Nano 11 4995 Google Scholar
[26]	Galati E, Tao H, Tebbe M, Ansari R, Rubinstein M, Zhulina E B, Kumacheva E 2019 Angew. Chem. Int. Ed. 58 3123 Google Scholar
[27]	Tao H, Chen L, Galati E, Manion J G, Seferos D S, Zhulina E B, Kumacheva E 2019 Langmuir 35 15872 Google Scholar
[28]	Wang R Y, Wang H, Wu X, Ji Y, Wang P, Qu Y, Chung T S 2011 Soft Matter 7 8370 Google Scholar
[29]	Matthews J R, Payne C M, Hafner J H 2015 Langmuir 31 9893 Google Scholar
[30]	Nakashima H, Furukawa K, Kashimura Y, Torimitsu K 2008 Langmuir 24 5654 Google Scholar
[31]	Yang J A, Murphy C J 2012 Langmuir 28 5404 Google Scholar
[32]	Sreeprasad T S, Pradeep T 2011 Langmuir 27 3381 Google Scholar
[33]	闫昭, 赵文静, 王荣瑶 2016 物理学报 65 126101 Google Scholar Yan Z, ZhaoW J, Wang R Y 2016 Acta Phys. Sin. 65 126101 Google Scholar
[34]	Zhu Y, Qu C, Kuang H, Xu L, Liu L, Hua Y, Wang L, Xu C 2011 Biosens. Bioelectron. 26 4387 Google Scholar
[35]	Wang Y T, Dellago C 2003 J. Phys. Chem. B 107 9214 Google Scholar
[36]	da Silva J, Dias R, da Hora G, Soares T, Meneghetti M 2018 J. Braz. Chem. Soc. 29 191 Google Scholar
[37]	Schmid N, Eichenberger A P, Choutko A, Riniker S, Winger M, Mark A E, van Gunsteren W F 2011 Eur. Biophys. J. 40 843 Google Scholar
[38]	da Silva J A, Meneghetti M R 2018 Langmuir 34 366 Google Scholar
[39]	da Silva J A, Netz P A, Meneghetti M R 2020 Langmuir 36 257 Google Scholar
[40]	Oroskar P A, Jameson C J, Murad S 2016 Mol. Phys. 115 1122 Google Scholar
[41]	Horsch M A, Zhang Z, Glotzer S C 2005 Phys. Rev. Lett. 95 056105 Google Scholar
[42]	Wan M W, Li X X, Gao L H, Fang W H 2016 Nanotechnology 27 465704 Google Scholar
[43]	Li X X, Gao L H, Fang W H 2016 PLoS One 11 e0154568 Google Scholar
[44]	Sevink G J A, Charlaganov M, Fraaije J G E M 2013 Soft Matter 9 2816 Google Scholar
[45]	Sevink G J A, Fraaije J 2014 Soft Matter 10 5129 Google Scholar
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Vol. 69, Issue 24 - 2020-12-20

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