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Nano Research 2019, 12(10): 2549-2553 https://doi.org/10.1007/s12274-019-2483-8
Research Article | Issue | Published: 29 July 2019

In situ TEM observation of neck formation during oriented attachment of PbSe nanocrystals

Show Author's Information Yu Wang1,2,  Xinxing Peng1,3,  Alex Abelson4,  Bing-Kai Zhang1,  Caroline Qian4,  Peter Ercius5,  Lin-Wang Wang1,  Matt Law4,  Haimei Zheng1,2( )
Materials Sciences Division,Lawrence Berkeley National Laboratory,Berkeley, California,94720,USA;
Department of Materials Science and Engineering,University of California,Berkeley, California,94720,USA;
State Key Lab of Physical Chemistry of Solid Surfaces,Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University,Xiamen,361005,China;
Department of Chemistry,University of California,Irvine, California,92697,USA;
National Center for Electron Microscopy, Molecular Foundry,Lawrence Berkeley National Laboratory,Berkeley, California,94720,USA;
Keywords:
liquid cell transmission electron microscopy (TEM), PbSe nanocrystals, quantum dots, superlattices, necking, oriented attachment
Topics:
Density functional theoryElectronic propertiesHigh resolution transmission electron microscopyIVLead compoundsNarrow band gap semiconductors Selenium compoundsSemiconductor quantum dotsSuperlatticesVI semiconductors
Cite this article:
Wang Y, Peng X, Abelson A, et al. In situ TEM observation of neck formation during oriented attachment of PbSe nanocrystals. Nano Research, 2019, 12(10): 2549-2553. https://doi.org/10.1007/s12274-019-2483-8
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Abstract Full text Electronic supplementary material About this article

Oriented attachment of nanocrystals is an important route to constructing epitaxially-connected nanocrystal superlattices for various applications. During oriented attachment of semiconductor nanocrystals, neck can be formed between nanocrystals and it strongly influences the properties of the resulting superlattice. However, the neck formation mechanism is poorly understood. Here, we use in situ liquid cell transmission electron microscopy (TEM) to directly observe the initiation and growth of homoepitaxial necks between PbSe nanocrystals with atomic details. We find that neck initiation occurs slowly (~ 10 s) when two nanocrystals approach to each other within an edge-to-edge distance of 0.6 nm. During neck initiation, Pb and Se atoms defuse from other facets into the gap, forming "dynamic reversible" filaments. Once the filament (neck) width is larger than a critical size of 0.9 nm, it gradually (15 s) widens into a 3-nm-wide neck. The atomic structure of the neck is further obtained using ex situ aberration-corrected scanning TEM imaging. Neck initiation and growth mechanisms are elucidated with density functional theory calculations. Our direct unveiling of the atomic pathways of neck formation during oriented attachment shed light into the fabrication of nanocrystal superlattices with improved structural order and electronic properties.


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Electronic supplementary material
About this article

In situ TEM observation of neck formation during oriented attachment of PbSe nanocrystals

Show Author's information Yu Wang1,2, Xinxing Peng1,3, Alex Abelson4, Bing-Kai Zhang1, Caroline Qian4, Peter Ercius5, Lin-Wang Wang1, Matt Law4, Haimei Zheng1,2( )
Materials Sciences Division,Lawrence Berkeley National Laboratory,Berkeley, California,94720,USA;
Department of Materials Science and Engineering,University of California,Berkeley, California,94720,USA;
State Key Lab of Physical Chemistry of Solid Surfaces,Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University,Xiamen,361005,China;
Department of Chemistry,University of California,Irvine, California,92697,USA;
National Center for Electron Microscopy, Molecular Foundry,Lawrence Berkeley National Laboratory,Berkeley, California,94720,USA;

Abstract

Oriented attachment of nanocrystals is an important route to constructing epitaxially-connected nanocrystal superlattices for various applications. During oriented attachment of semiconductor nanocrystals, neck can be formed between nanocrystals and it strongly influences the properties of the resulting superlattice. However, the neck formation mechanism is poorly understood. Here, we use in situ liquid cell transmission electron microscopy (TEM) to directly observe the initiation and growth of homoepitaxial necks between PbSe nanocrystals with atomic details. We find that neck initiation occurs slowly (~ 10 s) when two nanocrystals approach to each other within an edge-to-edge distance of 0.6 nm. During neck initiation, Pb and Se atoms defuse from other facets into the gap, forming "dynamic reversible" filaments. Once the filament (neck) width is larger than a critical size of 0.9 nm, it gradually (15 s) widens into a 3-nm-wide neck. The atomic structure of the neck is further obtained using ex situ aberration-corrected scanning TEM imaging. Neck initiation and growth mechanisms are elucidated with density functional theory calculations. Our direct unveiling of the atomic pathways of neck formation during oriented attachment shed light into the fabrication of nanocrystal superlattices with improved structural order and electronic properties.

Keywords: liquid cell transmission electron microscopy (TEM), PbSe nanocrystals, quantum dots, superlattices, necking, oriented attachment

References(39)

1

Zhang, X.; Shen, Z.; Liu, J.; Kerisit, S. N.; Bowden, M. E.; Sushko, M. L.; De Yoreo, J. J.; Rosso, K. M. Direction-specific interaction forces underlying zinc oxide crystal growth by oriented attachment. Nat. Commun. 2017, 8, 835.
DOI Google Scholar
2

Li, D. S.; Nielsen, M. H.; Lee, J. R. I.; Frandsen, C.; Banfield, J. F.; De Yoreo, J. J. Direction-specific interactions control crystal growth by oriented attachment. Science 2012, 336, 1014-1018.
DOI Google Scholar
3

Whitham, K.; Smilgies, D. M.; Hanrath, T. Entropic, enthalpic, and kinetic aspects of interfacial nanocrystal superlattice assembly and attachment. Chem. Mater. 2018, 30, 54-63.
DOI Google Scholar
4

Sandeep, C. S. S.; Azpiroz, J. M.; Evers, W. H.; Boehme, S. C.; Moreels, I.; Kinge, S.; Siebbeles, L. D. A.; Infante, I.; Houtepen, A. J. Epitaxially connected PbSe quantum-dot films: Controlled neck formation and optoelectronic properties. ACS Nano 2014, 8, 11499-11511.
DOI Google Scholar
5

Lim, T. H.; McCarthy, D.; Hendy, S. C.; Stevens, K. J.; Brown, S. A.; Tilley, R. D. Real-time TEM and kinetic Monte Carlo studies of the coalescence of decahedral gold nanoparticles. ACS Nano 2009, 3, 3809-3813.
DOI Google Scholar
6

Simon, P.; Bahrig, L.; Baburin, I. A.; Formanek, P.; Röder, F.; Sickmann, J.; Hickey, S. G.; Eychmuller, A.; Lichte, H.; Kniep, R. et al. Interconnection of nanoparticles within 2D superlattices of PbS/oleic acid thin films. Adv. Mater. 2014, 26, 3042-3049.
DOI Google Scholar
7

Whitham, K.; Hanrath, T. Formation of epitaxially connected quantum dot solids: Nucleation and coherent phase transition. J. Phys. Chem. Lett. 2017, 8, 2623-2628.
DOI Google Scholar
8

Xu, Y. H.; Wang, X. X.; Zhang, W. L.; Lv, F.; Guo, S. J. Recent progress in two-dimensional inorganic quantum dots. Chem. Soc. Rev. 2018, 47, 586-625.
DOI Google Scholar
9

Talapin, D. V.; Lee, J. S.; Kovalenko, M. V.; Shevchenko, E. V. Prospects of colloidal nanocrystals for electronic and optoelectronic applications. Chem. Rev. 2010, 110, 389-458.
DOI Google Scholar
10

Boles, M. A.; Engel, M.; Talapin, D. V. Self-assembly of colloidal nanocrystals: From intricate structures to functional materials. Chem. Rev. 2016, 116, 11220-11289.
DOI Google Scholar
11

Kagan, C. R.; Lifshitz, E.; Sargent, E. H.; Talapin, D. V. Building devices from colloidal quantum dots. Science 2016, 353, aac5523.
DOI Google Scholar
12

Boneschanscher, M. P.; Evers, W. H.; Geuchies, J. J.; Altantzis, T.; Goris, B.; Rabouw, F. T.; van Rossum, S. A. P.; van der Zant, H. S. J.; Siebbeles, L. D. A.; van Tendeloo, G. et al. Long-range orientation and atomic attachment of nanocrystals in 2D honeycomb superlattices. Science 2014, 344, 1377-1380.
DOI Google Scholar
13

Beugeling, W.; Kalesaki, E.; Delerue, C.; Niquet, Y. M.; Vanmaekelbergh, D.; Smith, C. M. Topological states in multi-orbital HgTe honeycomb lattices. Nat. Commun. 2015, 6, 6316.
DOI Google Scholar
14

Whitham, K.; Yang, J.; Savitzky, B. H.; Kourkoutis, L. F.; Wise, F.; Hanrath, T. Charge transport and localization in atomically coherent quantum dot solids. Nat. Mater. 2016, 15, 557-563.
DOI Google Scholar
15

Evers, W. H.; Schins, J. M.; Aerts, M.; Kulkarni, A.; Capiod, P.; Berthe, M.; Grandidier, B.; Delerue, C.; van der Zant, H. S. J.; van Overbeek, C. et al. High charge mobility in two-dimensional percolative networks of PbSe quantum dots connected by atomic bonds. Nat. Commun. 2015, 6, 8195.
DOI Google Scholar
16

Geuchies, J. J.; van Overbeek, C.; Evers, W. H.; Goris, B.; de Backer, A.; Gantapara, A. P.; Rabouw, F. T.; Hilhorst, J.; Peters, J. L.; Konovalov, O. et al. In situ study of the formation mechanism of two-dimensional superlattices from PbSe nanocrystals. Nat. Mater. 2016, 15, 1248-1254.
DOI Google Scholar
17

Weidman, M. C.; Smilgies, D. M.; Tisdale, W. A. Kinetics of the self-assembly of nanocrystal superlattices measured by real-time in situ X-ray scattering. Nat. Mater. 2016, 15, 775-781.
DOI Google Scholar
18

Zaluzhnyy, I. A.; Kurta, R. P.; Andre, A.; Gorobtsov, O. Y.; Rose, M.; Skopintsev, P.; Besedin, I.; Zozulya, A. V.; Sprung, M.; Schreiber, F. et al. Quantifying angular correlations between the atomic lattice and the superlattice of nanocrystals assembled with directional linking. Nano Lett. 2017, 17, 3511-3517.
DOI Google Scholar
19

Yalcin, A. O.; Fan, Z. C.; Goris, B.; Li, W. F.; Koster, R. S.; Fang, C. M.; van Blaaderen, A.; Casavola, M.; Tichelaar, F. D.; Bals, S. et al. Atomic resolution monitoring of cation exchange in CdSe-PbSe heteronanocrystals during epitaxial solid-solid-vapor growth. Nano Lett. 2014, 14, 3661-3667.
DOI Google Scholar
20

Cho, K. S.; Talapin, D. V.; Gaschler, W.; Murray, C. B. Designing PbSe nanowires and nanorings through oriented attachment of nanoparticles. J. Am. Chem. Soc. 2005, 127, 7140-7147.
DOI Google Scholar
21

Evers, W. H.; Goris, B.; Bals, S.; Casavola, M.; de Graaf, J.; van Roij, J.; Dijkstra, M.; Vanmaekelbergh, D. Low-dimensional semiconductor superlattices formed by geometric control over nanocrystal attachment. Nano Lett. 2013, 13, 2317-2323.
DOI Google Scholar
22

van Overbeek, C.; Peters, J. L.; van Rossum, S. A. P.; Smits, M.; van Huis, M. A.; Vanmaekelbergh, D. Interfacial self-assembly and oriented attachment in the family of PbX (X = S, Se, Te) nanocrystals. J. Phys. Chem. C 2018, 122, 12464-12473.
DOI Google Scholar
23

Tan, S. F.; Chee, S. W.; Lin, G. H.; Mirsaidov, U. Direct observation of interactions between nanoparticles and nanoparticle self-assembly in solution. Acc. Chem. Res. 2017, 50, 1303-1312.
DOI Google Scholar
24

Qi, K.; Wei, J. K.; Sun, M. H.; Huang, Q. M.; Li, X. M.; Xu, Z.; Wang, W. L.; Bai, X. D. Real-time observation of deep lithiation of tungsten oxide nanowires by in situ electron microscopy. Angew. Chem., Int. Ed. 2015, 127, 15437-15440.
DOI Google Scholar
25

Wu, S. Y.; Li, M. R.; Sun, Y. G. In situ synchrotron X-ray characterization shining light on the nucleation and growth kinetics of colloidal nanoparticles. Angew. Chem., Int. Ed. 2019, 58, 8987-8995.
DOI Google Scholar
26

Kim, J.; Ou, Z. H.; Jones, M. R.; Song, X. H.; Chen, Q. Imaging the polymerization of multivalent nanoparticles in solution. Nat. Commun. 2017, 8, 761.
DOI Google Scholar
27

de Yoreo, J. J.; Gilbert, P. U. P. A.; Sommerdijk, N. A. J. M.; Penn, R. L.; Whitelam, S.; Joester, D.; Zhang, H. Z.; Rimer, J. D.; Navrotsky, A.; Banfield, J. F. et al. Crystallization by particle attachment in synthetic, biogenic, and geologic environments. Science 2015, 349, aaa6760.
DOI Google Scholar
28

Urban, J. J. Prospects for thermoelectricity in quantum dot hybrid arrays. Nat. Nanotechnol. 2015, 10, 997-1001.
DOI Google Scholar
29

Liao, H. G.; Zheng, H. Liquid cell transmission electron microscopy. Annu. Rev. Phys. Chem. 2016, 67, 719-747.
DOI Google Scholar
30

Yuan, W. T.; Zhang, D. W.; Ou, Y.; Fang, K.; Zhu, B. E.; Yang, H. S.; Hansen, T. W.; Wagner, J. B.; Zhang, Z.; Gao, Y. et al. Direct in situ TEM visualization and insight into the facet-dependent sintering behaviors of gold on TiO2. Angew. Chem., Int. Ed. 2018, 57, 16827-16831.
DOI Google Scholar
31

Sutter, E.; Sutter, P.; Tkachenko, A. V.; Krahne, R.; de Graaf, J.; Arciniegas, M.; Manna, L. In situ microscopy of the self-assembly of branched nanocrystals in solution. Nat. Commun. 2016, 7, 11213.
DOI Google Scholar
32

Kim, B. H.; Yang, J.; Lee, D.; Choi, B. K.; Hyeon, T.; Park, J. Liquid-phase transmission electron microscopy for studying colloidal inorganic nanoparticles. Adv. Mater. 2018, 30, 1703316.
DOI Google Scholar
33

Wang, Y.; Peng, X. X.; Abelson, A.; Xiao, P. H.; Qian, C.; Yu, L.; Ophus, C.; Ercius, P.; Wang, L. W.; Law, M. et al. Dynamic deformability of individual PbSe nanocrystals during superlattice phase transitions. Sci. Adv. 2019, 5, eaaw5623.
DOI Google Scholar
34

Klokkenburg, M.; Houtepen, A. J.; Koole, R.; de Folter, J. W. J.; Erné, B. H.; van Faassen, E.; Vanmaekelbergh, D. Dipolar structures in colloidal dispersions of PbSe and CdSe quantum dots. Nano Lett. 2007, 7, 2931-2936.
DOI Google Scholar
35

Yuk, J. M.; Park, J.; Ercius, P.; Kim, K.; Hellebusch, D. J.; Crommie, M. F.; Lee, J. Y.; Zettl, A.; Alivisatos, A. P. High-resolution em of colloidal nanocrystal growth using graphene liquid cells. Science 2012, 336, 61-64.
DOI Google Scholar
36

Jin, B.; Sushko, M. L.; Liu, Z. M.; Jin, C. H.; Tang, R. K. In situ liquid cell tem reveals bridge-induced contact and fusion of Au nanocrystals in aqueous solution. Nano Lett. 2018, 18, 6551-6556.
DOI Google Scholar
37

Anand, U.; Lu, J. Y.; Loh, D.; Aabdin, Z.; Mirsaidov, U. Hydration layer-mediated pairwise interaction of nanoparticles. Nano Lett. 2016, 16, 786-790.
DOI Google Scholar
38

Zhu, C.; Liang, S. X.; Song, E. H.; Zhou, Y. J.; Wang, W.; Shan, F.; Shi, Y. T.; Hao, C.; Yin, K. B.; Zhang, T. et al. In-situ liquid cell transmission electron microscopy investigation on oriented attachment of gold nanoparticles. Nat. Commun. 2018, 9, 421.
DOI Google Scholar
39

Anderson, N. C.; Hendricks, M. P.; Choi, J. J.; Owen, J. S. Ligand exchange and the stoichiometry of metal chalcogenide nanocrystals: Spectroscopic observation of facile metal-carboxylate displacement and binding. J. Am. Chem. Soc. 2013, 135, 18536-18548.
DOI Google Scholar
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Publication history
Copyright
Acknowledgements

Publication history

Received: 16 May 2019
Revised: 11 July 2019
Accepted: 16 July 2019
Published: 29 July 2019
Issue date: October 2019

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2019

Acknowledgements

Acknowledgements

This work was supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES), Materials Sciences and Engineering Division under Contract No. DE-AC02- 05-CH11231 within the in-situ TEM (KC22ZH) program. Y. W., A. A., C. Q., and M. L. were supported by the UC Office of the President under the UC Laboratory Fees Research Program Collaborative Research and Training Award LFR-17-477148. X. P. acknowledges financial support from the China Scholarship Council. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.

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