Facet-selective etching trajectories of individual semiconductor nanocrystals

Yan, Chang; Byrne, Dana; Ondry, Justin C.; Kahnt, Axel; Moreno-Hernandez, Ivan A.; Kamat, Gaurav A.; Liu, Zi-Jie; Laube, Christian; Crook, Michelle F.; Zhang, Ye; Ercius, Peter; Alivisatos, A. Paul

doi:10.1126/sciadv.abq1700

Title: Facet-selective etching trajectories of individual semiconductor nanocrystals

Journal Article · Wed Aug 10 00:00:00 EDT 2022 · Science Advances

DOI:https://doi.org/10.1126/sciadv.abq1700· OSTI ID:1884786

^[1]; Byrne, Dana ^[2];

^[2];

^[3];

^[2];

^[2]; Liu, Zi-Jie ^[2];

^[4];

^[2];

^[5];

^[6]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Leibniz Inst. of Surface Engineering (IOM), Leipzig (Germany)
Univ. of California, Berkeley, CA (United States); Leibniz Inst. of Surface Engineering (IOM), Leipzig (Germany)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of Chicago, IL (United States)

The size and shape of semiconductor nanocrystals govern their optical and electronic properties. Liquid cell transmission electron microscopy (LCTEM) is an emerging tool that can directly visualize nanoscale chemical transformations and therefore inform the precise synthesis of nanostructures with desired functions. However, it remains difficult to controllably investigate the reactions of semiconductor nanocrystals with LCTEM, because of the highly reactive environment formed by radiolysis of liquid. Here, we harness the radiolysis processes and report the single-particle etching trajectories of prototypical semiconductor nanomaterials with well-defined crystalline facets. Lead selenide nanocubes represent an isotropic structure that retains the cubic shape during etching via a layer-by-layer mechanism. The anisotropic arrow-shaped cadmium selenide nanorods have polar facets terminated by either cadmium or selenium atoms, and the transformation trajectory is driven by etching the selenium-terminated facets. LCTEM trajectories reveal how nanoscale shape transformations of semiconductors are governed by the reactivity of specific facets in liquid environments.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1884786

Journal Information:: Science Advances, Vol. 8, Issue 32; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

References (51)

Synthesis and characterization of nearly monodisperse CdE (E = sulfur, selenium, tellurium) semiconductor nanocrystallites Murray, C. B.; Norris, D. J.; Bawendi, M. G. Journal of the American Chemical Society, Vol. 115, Issue 19, p. 8706-8715 https://doi.org/10.1021/ja00072a025	journal	September 1993
Atomic Imaging of Phase Transitions and Morphology Transformations in Nanocrystals van Huis, Marijn A.; Young, Neil P.; Pandraud, Grégory Advanced Materials, Vol. 21, Issue 48 https://doi.org/10.1002/adma.200902561	journal	October 2009
Unraveling Kinetically-Driven Mechanisms of Gold Nanocrystal Shape Transformations Using Graphene Liquid Cell Electron Microscopy Hauwiller, Matthew R.; Frechette, Layne B.; Jones, Matthew R. Nano Letters, Vol. 18, Issue 9 https://doi.org/10.1021/acs.nanolett.8b02337	journal	August 2018
Quantum Dots as Cellular Probes Alivisatos, A. Paul; Gu, Weiwei; Larabell, Carolyn Annual Review of Biomedical Engineering, Vol. 7, Issue 1 https://doi.org/10.1146/annurev.bioeng.7.060804.100432	journal	August 2005
Experimental Determination of the Extinction Coefficient of CdTe, CdSe, and CdS Nanocrystals Yu, W. William; Qu, Lianhua; Guo, Wenzhuo Chemistry of Materials, Vol. 15, Issue 14, p. 2854-2860 https://doi.org/10.1021/cm034081k	journal	July 2003
Compact high-quality CdSe–CdS core–shell nanocrystals with narrow emission linewidths and suppressed blinking Chen, Ou; Zhao, Jing; Chauhan, Vikash P. Nature Materials, Vol. 12, Issue 5 https://doi.org/10.1038/nmat3539	journal	February 2013
Amine-Assisted Facetted Etching of CdSe Nanocrystals Li, Rongfu; Lee, Jeunghoon; Yang, Baocheng Journal of the American Chemical Society, Vol. 127, Issue 8 https://doi.org/10.1021/ja0465404	journal	March 2005
Defining the radiation chemistry during liquid cell electron microscopy to enable visualization of nanomaterial growth and degradation dynamics: DEFINING THE RADIATION CHEMISTRY DURING LCEM Woehl, T. J.; Abellan, P. Journal of Microscopy, Vol. 265, Issue 2 https://doi.org/10.1111/jmi.12508	journal	December 2016
Design and synthesis of multigrain nanocrystals via geometric misfit strain Oh, Myoung Hwan; Cho, Min Gee; Chung, Dong Young Nature, Vol. 577, Issue 7790 https://doi.org/10.1038/s41586-019-1899-3	journal	January 2020
Reversible disorder-order transitions in atomic crystal nucleation Jeon, Sungho; Heo, Taeyeong; Hwang, Sang-Yeon Science, Vol. 371, Issue 6528 https://doi.org/10.1126/science.aaz7555	journal	January 2021
Kinetic pathways of crystallization at the nanoscale Ou, Zihao; Wang, Ziwei; Luo, Binbin Nature Materials, Vol. 19, Issue 4 https://doi.org/10.1038/s41563-019-0514-1	journal	October 2019
Size- and shape-controlled synthesis of PbSe and PbS nanocrystalsvia a facile method Li, Hongbo; Chen, Dong; Li, Linlin CrystEngComm, Vol. 12, Issue 4 https://doi.org/10.1039/B917833C	journal	January 2010
Resilient Pathways to Atomic Attachment of Quantum Dot Dimers and Artificial Solids from Faceted CdSe Quantum Dot Building Blocks Ondry, Justin C.; Philbin, John P.; Lostica, Michael ACS Nano, Vol. 13, Issue 11 https://doi.org/10.1021/acsnano.9b03052	journal	June 2019
Drastic Structural Transformation of Cadmium Chalcogenide Nanoparticles Using Chloride Ions and Surfactants Saruyama, Masaki; Kanehara, Masayuki; Teranishi, Toshiharu Journal of the American Chemical Society, Vol. 132, Issue 10 https://doi.org/10.1021/ja9095285	journal	February 2010
Competition Reactions of H ₂ O ^•+ Radical in Concentrated Cl ^– Aqueous Solutions: Picosecond Pulse Radiolysis Study El Omar, Abdel Karim; Schmidhammer, Uli; Rousseau, Bernard The Journal of Physical Chemistry A, Vol. 116, Issue 47 https://doi.org/10.1021/jp309381z	journal	November 2012
Redefining near-unity luminescence in quantum dots with photothermal threshold quantum yield Hanifi, David A.; Bronstein, Noah D.; Koscher, Brent A. Science, Vol. 363, Issue 6432 https://doi.org/10.1126/science.aat3803	journal	March 2019
Electron–Water Interactions and Implications for Liquid Cell Electron Microscopy Schneider, Nicholas M.; Norton, Michael M.; Mendel, Brian J. The Journal of Physical Chemistry C, Vol. 118, Issue 38 https://doi.org/10.1021/jp507400n	journal	September 2014
Reduction Potentials of One‐Electron Couples Involving Free Radicals in Aqueous Solution Wardman, Peter Journal of Physical and Chemical Reference Data, Vol. 18, Issue 4 https://doi.org/10.1063/1.555843	journal	October 1989
Electron–electron and electron‐hole interactions in small semiconductor crystallites: The size dependence of the lowest excited electronic state Brus, L. E. The Journal of Chemical Physics, Vol. 80, Issue 9 https://doi.org/10.1063/1.447218	journal	May 1984
Highly efficient and stable InP/ZnSe/ZnS quantum dot light-emitting diodes Won, Yu-Ho; Cho, Oul; Kim, Taehyung Nature, Vol. 575, Issue 7784 https://doi.org/10.1038/s41586-019-1771-5	journal	November 2019
Dynamic microscopy of nanoscale cluster growth at the solid–liquid interface Williamson, M. J.; Tromp, R. M.; Vereecken, P. M. Nature Materials, Vol. 2, Issue 8 https://doi.org/10.1038/nmat944	journal	July 2003
Understanding Reactivity Patterns of Radical Cations Schmittel, Michael; Burghart, Armin Angewandte Chemie International Edition in English, Vol. 36, Issue 23 https://doi.org/10.1002/anie.199725501	journal	December 1997
Nanoheterostructure Cation Exchange: Anionic Framework Conservation Jain, Prashant K.; Amirav, Lilac; Aloni, Shaul Journal of the American Chemical Society, Vol. 132, Issue 29 https://doi.org/10.1021/ja104126u	journal	July 2010
Equilibrium shape of Si Eaglesham, D. J.; White, A. E.; Feldman, L. C. Physical Review Letters, Vol. 70, Issue 11 https://doi.org/10.1103/PhysRevLett.70.1643	journal	March 1993
Critical Review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (⋅OH/⋅O ⁻ in Aqueous Solution Buxton, George V.; Greenstock, Clive L.; Helman, W. Phillips Journal of Physical and Chemical Reference Data, Vol. 17, Issue 2 https://doi.org/10.1063/1.555805	journal	April 1988
Shape-Controlled Synthesis of Colloidal Metal Nanocrystals: Thermodynamic versus Kinetic Products Xia, Younan; Xia, Xiaohu; Peng, Hsin-Chieh Journal of the American Chemical Society, Vol. 137, Issue 25 https://doi.org/10.1021/jacs.5b04641	journal	June 2015
Some simple, highly reactive, inorganic chlorine derivatives in aqueous solution. Their formation using pulses of radiation and their role in the mechanism of the Fricke dosimeter Jayson, G. G.; Parsons, B. J.; Swallow, A. J. Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 69, Issue 0 https://doi.org/10.1039/f19736901597	journal	January 1973
Tracking the Effects of Ligands on Oxidative Etching of Gold Nanorods in Graphene Liquid Cell Electron Microscopy Hauwiller, Matthew R.; Ye, Xingchen; Jones, Matthew R. ACS Nano, Vol. 14, Issue 8 https://doi.org/10.1021/acsnano.0c03601	journal	July 2020
The surface science of nanocrystals Boles, Michael A.; Ling, Daishun; Hyeon, Taeghwan Nature Materials, Vol. 15, Issue 2 https://doi.org/10.1038/nmat4526	journal	January 2016
Electronic spectra, photochemistry, and autoxidation mechanism of the sulfite-bisulfite-pyrosulfite systems. SO2-, SO3-, SO4-, and SO5- radicals Hayon, E.; Treinin, A.; Wilf, J. Journal of the American Chemical Society, Vol. 94, Issue 1 https://doi.org/10.1021/ja00756a009	journal	January 1972
The role of organic ligand shell structures in colloidal nanocrystal synthesis Calvin, Jason J.; Brewer, Amanda S.; Alivisatos, A. Paul Nature Synthesis, Vol. 1, Issue 2 https://doi.org/10.1038/s44160-022-00025-4	journal	February 2022
Single-particle mapping of nonequilibrium nanocrystal transformations Ye, Xingchen; Jones, Matthew R.; Frechette, Layne B. Science, Vol. 354, Issue 6314 https://doi.org/10.1126/science.aah4434	journal	November 2016
Gold Nanocrystal Etching as a Means of Probing the Dynamic Chemical Environment in Graphene Liquid Cell Electron Microscopy Hauwiller, Matthew R.; Ondry, Justin C.; Chan, Cindy M. Journal of the American Chemical Society, Vol. 141, Issue 10 https://doi.org/10.1021/jacs.9b00082	journal	February 2019
Thermodynamic Oxidation and Reduction Potentials of Photocatalytic Semiconductors in Aqueous Solution Chen, Shiyou; Wang, Lin-Wang Chemistry of Materials, Vol. 24, Issue 18 https://doi.org/10.1021/cm302533s	journal	September 2012
Redox Mediated Control of Electrochemical Potential in Liquid Cell Electron Microscopy Moreno-Hernandez, Ivan A.; Crook, Michelle F.; Ondry, Justin C. Journal of the American Chemical Society, Vol. 143, Issue 31 https://doi.org/10.1021/jacs.1c03906	journal	July 2021
Application of Dislocation Theory to Minimize Defects in Artificial Solids Built with Nanocrystal Building Blocks Ondry, Justin C.; Alivisatos, A. Paul Accounts of Chemical Research, Vol. 54, Issue 6 https://doi.org/10.1021/acs.accounts.0c00719	journal	February 2021
Critical Review of Aqueous Solution Reaction Rate Constants for Hydrogen Atoms Madden, Keith P.; Mezyk, Stephen P. Journal of Physical and Chemical Reference Data, Vol. 40, Issue 2 https://doi.org/10.1063/1.3578343	journal	June 2011
Shape control of CdSe nanocrystals Peng, Xiaogang; Manna, Liberato; Yang, Weidong Nature, Vol. 404, Issue 6773, p. 59-61 https://doi.org/10.1038/35003535	journal	March 2000
Shape Control of Colloidal Metal Nanocrystals Tao, Andrea R.; Habas, Susan; Yang, Peidong Small, Vol. 4, Issue 3 https://doi.org/10.1002/smll.200701295	journal	March 2008
Shape control and applications of nanocrystals Scher, Erik C.; Manna, Liberato; Alivisatos, A. Paul Philosophical Transactions of the Royal Society of London. Series A: Mathematical, Physical and Engineering Sciences, Vol. 361, Issue 1803 https://doi.org/10.1098/rsta.2002.1126	journal	December 2002
Sub–single-exciton lasing using charged quantum dots coupled to a distributed feedback cavity Kozlov, Oleg V.; Park, Young-Shin; Roh, Jeongkyun Science, Vol. 365, Issue 6454 https://doi.org/10.1126/science.aax3489	journal	August 2019
Reactivity of HO ₂ /O ⁻ ₂ Radicals in Aqueous Solution Bielski, Benon H. J.; Cabelli, Diane E.; Arudi, Ravindra L. Journal of Physical and Chemical Reference Data, Vol. 14, Issue 4 https://doi.org/10.1063/1.555739	journal	October 1985
Pulse radiolysis study of concentrated sulfuric acid solutions. Formation mechanism, yield and reactivity of sulfate radicals Jiang, Pei-Yun; Katsumura, Yosuke; Nagaishi, Ryuji Journal of the Chemical Society, Faraday Transactions, Vol. 88, Issue 12 https://doi.org/10.1039/ft9928801653	journal	January 1992
The surface energy of Si, GaAs, and GaP Messmer, C.; Bilello, J. C. Journal of Applied Physics, Vol. 52, Issue 7 https://doi.org/10.1063/1.329342	journal	July 1981
In Situ Transmission Electron Microscopy of Cadmium Selenide Nanorod Sublimation Hellebusch, Daniel J.; Manthiram, Karthish; Beberwyck, Brandon J. The Journal of Physical Chemistry Letters, Vol. 6, Issue 4 https://doi.org/10.1021/jz502566m	journal	January 2015
Redox and Acidity Properties of Alkyl- and Arylamine Radical Cations and the Corresponding Aminyl Radicals ¹ Jonsson, Mats; Wayner, Danial D. M.; Lusztyk, Janusz The Journal of Physical Chemistry, Vol. 100, Issue 44 https://doi.org/10.1021/jp961286q	journal	January 1996
Elucidating the Role of Halides and Iron during Radiolysis-Driven Oxidative Etching of Gold Nanocrystals Using Liquid Cell Transmission Electron Microscopy and Pulse Radiolysis Crook, Michelle F.; Laube, Christian; Moreno-Hernandez, Ivan A. Journal of the American Chemical Society, Vol. 143, Issue 30 https://doi.org/10.1021/jacs.1c05099	journal	July 2021
Reaction between hydroperoxo radicals and chlorine in aqueous solution Bjergbakke, E.; Navaratnam, S.; Parsons, B. J. Journal of the American Chemical Society, Vol. 103, Issue 19 https://doi.org/10.1021/ja00409a059	journal	September 1981
Semiconductor Clusters, Nanocrystals, and Quantum Dots Alivisatos, A. P. Science, Vol. 271, Issue 5251, p. 933-937 https://doi.org/10.1126/science.271.5251.933	journal	February 1996
Anomalous nanoparticle surface diffusion in LCTEM is revealed by deep learning-assisted analysis Jamali, Vida; Hargus, Cory; Ben-Moshe, Assaf Proceedings of the National Academy of Sciences, Vol. 118, Issue 10 https://doi.org/10.1073/pnas.2017616118	journal	March 2021
Computer modelling of the radiolysis in an aqueous lithium salt blanket: Suppression of radiolysis by addition of hydrogen Elliot, A. John; McCracken, David R. Fusion Engineering and Design, Vol. 13, Issue 1 https://doi.org/10.1016/0920-3796(90)90028-5	journal	August 1990

Similar Records

Using Graphene Liquid Cell Transmission Electron Microscopy to Study in Situ Nanocrystal Etching

Journal Article · Thu May 17 00:00:00 EDT 2018 · Journal of Visualized Experiments · OSTI ID:1884786

Hauwiller, Matthew R.; Ondry, Justin C.; Alivisatos, A. Paul

Unraveling Anisotropic and Pulsating Etching of ZnO Nanorods in Hydrochloric Acid via Correlative Electron Microscopy

Journal Article · Fri Jun 23 00:00:00 EDT 2023 · ACS Nano · OSTI ID:1884786

Liu, Fangyuan; Lu, Xingxu; Zhu, Chunxiang; +14 more

Elucidating the Role of Halides and Iron during Radiolysis-Driven Oxidative Etching of Gold Nanocrystals Using Liquid Cell Transmission Electron Microscopy and Pulse Radiolysis

Journal Article · Thu Jul 22 00:00:00 EDT 2021 · Journal of the American Chemical Society · OSTI ID:1884786

Crook, Michelle F.; Laube, Christian; Moreno-Hernandez, Ivan A.; +5 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Facet-selective etching trajectories of individual semiconductor nanocrystals

Citation Formats

References (51)

Similar Records

Related Subjects