Ultrathin Shape Change Smart MaterialsClick to copy article linkArticle link copied!
Abstract

Conspectus
With the discovery of graphene, significant research has focused on the synthesis, characterization, and applications of ultrathin materials. Graphene has also brought into focus other ultrathin materials composed of organics, polymers, inorganics, and their hybrids. Together, these ultrathin materials have unique properties of broad significance. For example, ultrathin materials have a large surface area and high flexibility which can enhance conformal contact in wearables and sensors leading to improved sensitivity. When porous, the short transverse diffusion length in these materials allows rapid mass transport. Alternatively, when impermeable, these materials behave as an ultrathin barrier. Such controlled permeability is critical in the design of encapsulation and drug delivery systems. Finally, ultrathin materials often feature defect-free and single-crystal-like two-dimensional atomic structures resulting in superior mechanical, optical, and electrical properties.
A unique property of ultrathin materials is their low bending rigidity, which suggests that they could easily be bent, curved, or folded into 3D shapes. In this Account, we review the emerging field of 2D to 3D shape transformations of ultrathin materials. We broadly define ultrathin to include materials with a thickness below 100 nm and composed of a range of organic, inorganic, and hybrid compositions. This topic is important for both fundamental and applied reasons. Fundamentally, bending and curving of ultrathin films can cause atomistic and molecular strain which can alter their physical and chemical properties and lead to new 3D forms of matter which behave very differently from their planar precursors. Shape change can also lead to new 3D architectures with significantly smaller form factors. For example, 3D ultrathin materials would occupy a smaller space in on-chip devices or could permeate through tortuous media which is important for miniaturized robots and smart dust applications.
Our Account highlights several differences between ultrathin and traditional shape change materials. The latter is typically associated with hydrogels, liquid crystals, or shape memory elastomers. As compared to bulk materials, ultrathin materials can much more easily bend and fold due to the significantly reduced bending modulus. Consequently, it takes much less energy to alter the shape of ultrathin materials, and even small environmental stimuli can trigger a large response. Further, the energy barriers between different configurations are small which allow a variety of conformations and enhances programmability. Finally, due to their ultrathin nature, the shape changes are typically not slowed down by sluggish mass or thermal transport, and thus, responses can be much faster than those of bulk materials. The latter point is important in the design of high-speed actuators. Consequently, ultrathin materials could enable low-power, rapid, programmable, and complex shape transformations in response to a broad range of stimuli such as pH, temperature, electromagnetic fields, or chemical environments. The Account also includes a discussion of applications, important challenges, and future directions.
Cited By
Smart citations by scite.ai include citation statements extracted from the full text of the citing article. The number of the statements may be higher than the number of citations provided by ACS Publications if one paper cites another multiple times or lower if scite has not yet processed some of the citing articles.
This article is cited by 51 publications.
- Shan Liu, Muxuan Yang, Cade Smarr, Ge Zhang, Hazel Barton, Weinan Xu. Engineered Living Structures with Shape-Morphing Capability Enabled by 4D Printing with Functional Bacteria. ACS Applied Bio Materials 2024, 7
(5)
, 3247-3257. https://doi.org/10.1021/acsabm.4c00223
- Yuanyuan Liu, Xiyu Wang, Caihui Luo, Jie Cai, Yuting Li, Ying Cao, Yuanli Cai. l-Histidine Salt-Bridged Monomer Preassembly and Polymerization-Induced Electrostatic Self-Assembly. Macromolecules 2023, 56
(17)
, 6655-6666. https://doi.org/10.1021/acs.macromol.3c01143
- Dong Yan, Zhifang Wang, Zhenjie Zhang. Stimuli-Responsive Crystalline Smart Materials: From Rational Design and Fabrication to Applications. Accounts of Chemical Research 2022, 55
(7)
, 1047-1058. https://doi.org/10.1021/acs.accounts.2c00027
- Guang Yang, Jie Wang, Yangyang Yan, Zijuan Hai, Zan Hua, Guosong Chen. Multi-Stimuli-Triggered Shape Transformation of Polymeric Filaments Derived from Dynamic Covalent Block Copolymers. Biomacromolecules 2020, 21
(10)
, 4159-4168. https://doi.org/10.1021/acs.biomac.0c00956
- Jie Song, Xiaomei Xia, Jiatian Chen, Dan Xia, Qingzhong Xue, Qiang Li, Mingdong Dong. Folding 2D Graphene Nanoribbons into 3D Nanocages Induced by Platinum Nanoclusters. The Journal of Physical Chemistry C 2020, 124
(19)
, 10495-10501. https://doi.org/10.1021/acs.jpcc.0c00463
- Hongyu Guo, Qian Zhang, Wei Liu, Zhihong Nie. Light-Mediated Shape Transformation of a Self-Rolling Nanocomposite Hydrogel Tube. ACS Applied Materials & Interfaces 2020, 12
(11)
, 13521-13528. https://doi.org/10.1021/acsami.9b23195
- Mohammed AlAmer, Somayeh Zamani, Kristi Fok, Aishwarya Satish, Ae Ran Lim, Yong Lak Joo. Facile Production of Graphenic Microsheets and Their Assembly via Water-Based, Surfactant-Aided Mechanical Deformations. ACS Applied Materials & Interfaces 2020, 12
(7)
, 8944-8951. https://doi.org/10.1021/acsami.9b22824
- Weinan Xu, Tengfei Li, Zhao Qin, Qi Huang, Hui Gao, Kibum Kang, Jiwoong Park, Markus J. Buehler, Jacob B. Khurgin, David H. Gracias. Reversible MoS2 Origami with Spatially Resolved and Reconfigurable Photosensitivity. Nano Letters 2019, 19
(11)
, 7941-7949. https://doi.org/10.1021/acs.nanolett.9b03107
- Yigit Altay, Shoupeng Cao, Hailong Che, Loai K. E. A. Abdelmohsen, Jan C. M. van Hest. Adaptive Polymeric Assemblies for Applications in Biomimicry and Nanomedicine. Biomacromolecules 2019, 20
(11)
, 4053-4064. https://doi.org/10.1021/acs.biomac.9b01341
- Michael
F. Reynolds, Kathryn L. McGill, Maritha A. Wang, Hui Gao, Fauzia Mujid, Kibum Kang, Jiwoong Park, Marc Z. Miskin, Itai Cohen, Paul L. McEuen. Capillary Origami with Atomically Thin Membranes. Nano Letters 2019, 19
(9)
, 6221-6226. https://doi.org/10.1021/acs.nanolett.9b02281
- Weinan Xu, David H. Gracias. Soft Three-Dimensional Robots with Hard Two-Dimensional Materials. ACS Nano 2019, 13
(5)
, 4883-4892. https://doi.org/10.1021/acsnano.9b03051
- Kei Hashimoto, Yumi Kobayashi, Hisashi Kokubo, Takeshi Ueki, Koji Ohara, Kenta Fujii, Masayoshi Watanabe. Solvation Structure of Poly(benzyl methacrylate) in a Solvate Ionic Liquid: Preferential Solvation of Li–Glyme Complex Cation. The Journal of Physical Chemistry B 2019, 123
(18)
, 4098-4107. https://doi.org/10.1021/acs.jpcb.9b02458
- Weinan Xu, Santosh K. Paidi, Zhao Qin, Qi Huang, Chi-Hua Yu, Jayson V. Pagaduan, Markus J. Buehler, Ishan Barman, David H. Gracias. Self-Folding Hybrid Graphene Skin for 3D Biosensing. Nano Letters 2019, 19
(3)
, 1409-1417. https://doi.org/10.1021/acs.nanolett.8b03461
- Xin-Xin Jin, Zhen Shao, Peng-Xiang Fu, Yi-Fan Deng, Qi Sui, Yi-Han Wang, Jin Xiong, Bing-Wu Wang, Zhe-Ming Wang, Song Gao. Tuning photochromism and photomagnetism
via
diverse bimetallic cyanido viologen hybrid materials. Inorganic Chemistry Frontiers 2025, 12
(8)
, 3294-3304. https://doi.org/10.1039/D4QI03115F
- Veronika Kozlovskaya, Eugenia Kharlampieva. Synthesis and pH-responsive properties of bacteria mimicking hydrogel capsules. RSC Applied Polymers 2025, 3
(1)
, 125-136. https://doi.org/10.1039/D4LP00137K
- Vahid Moosabeiki, Ebrahim Yarali, Ava Ghalayaniesfahani, Sebastien J. P. Callens, Teunis van Manen, Angelo Accardo, Sepideh Ghodrat, José Bico, Mehdi Habibi, Mohammad J. Mirzaali, Amir A. Zadpoor. Curvature tuning through defect-based 4D printing. Communications Materials 2024, 5
(1)
https://doi.org/10.1038/s43246-024-00448-w
- Ruohong Shi, Qi Huang, Rebecca Schulman, David H. Gracias. Ultra-thin graphene oxide (GO)-DNA composite polymerization gels (CPGs). MRS Advances 2024, 9
(19)
, 1513-1519. https://doi.org/10.1557/s43580-024-00917-x
- Juncheng Guo, Yijun Yang, Yang Xiang, Shufang Zhang, Xueyi Guo. Application of smart hydrogel materials in cartilage injury repair: A systematic review and meta-analysis. Journal of Biomaterials Applications 2024, 39
(2)
, 96-116. https://doi.org/10.1177/08853282241248779
- Jie Zhang, Zhen Zhang, Xuemei Wang, Yuan Ma, Zheng Zhou, Xinzhen Du, Xiaoquan Lu. Ultra-thin FeCoNi-LDH hollow nanoflower as solid-phase microextraction coating for targeted capture of six pesticides by electrostatic adsorption. Talanta 2024, 276 , 126258. https://doi.org/10.1016/j.talanta.2024.126258
- Rezgar Hasanzadeh, Peyman Mihankhah, Taher Azdast, Asghar Rasouli, Mohadese Shamkhali, Chul B. Park. Biocompatible tissue-engineered scaffold polymers for 3D printing and its application for 4D printing. Chemical Engineering Journal 2023, 476 , 146616. https://doi.org/10.1016/j.cej.2023.146616
- Sheelbhadra Chatterjee, Sariful Molla, Jakir Ahmed, Subhajit Bandyopadhyay. Light-driven modulation of electrical conductance with photochromic switches: bridging photochemistry with optoelectronics. Chemical Communications 2023, 59
(85)
, 12685-12698. https://doi.org/10.1039/D3CC04269C
- Peiren Liu, Fang Fang, Haochen Wang, Niveen M. Khashab. Smart Materials Based on Synthetic Host Molecules: The Role of Host–Guest Chemistry in the Fabrication and Application. Angewandte Chemie 2023, 135
(32)
https://doi.org/10.1002/ange.202218706
- Peiren Liu, Fang Fang, Haochen Wang, Niveen M. Khashab. Smart Materials Based on Synthetic Host Molecules: The Role of Host–Guest Chemistry in the Fabrication and Application. Angewandte Chemie International Edition 2023, 62
(32)
https://doi.org/10.1002/anie.202218706
- Qi Huang, Tao Deng, Weinan Xu, ChangKyu Yoon, Zhao Qin, Yida Lin, Tengfei Li, Yuqian Yang, Michael Shen, Susanna M. Thon, Jacob B. Khurgin, David H. Gracias. Solvent Responsive Self‐Folding of 3D Photosensitive Graphene Architectures. Advanced Intelligent Systems 2023, 5
(4)
https://doi.org/10.1002/aisy.202000195
- Wenbo Wu, Kui Chen, Ting Wang, Na Wang, Xin Huang, Lina Zhou, Zhao Wang, Hongxun Hao. Stimuli-responsive flexible organic crystals. Journal of Materials Chemistry C 2023, 11
(6)
, 2026-2052. https://doi.org/10.1039/D2TC04642C
- Tiantian Li, Jonathan Luntz, Diann Brei, Paul Alexander, Wonhee Kim. Modeling and Design of Hinged Tile-Based Curling Air Surface for Morphing Windshield Cowling. ASME Open Journal of Engineering 2023, 2 https://doi.org/10.1115/1.4062220
- Fahad Alhashmi Alamer, Ghadah A. Almalki. Fabrication of Conductive Fabrics Based on SWCNTs, MWCNTs and Graphene and Their Applications: A Review. Polymers 2022, 14
(24)
, 5376. https://doi.org/10.3390/polym14245376
- Jongwook Kim, Sunghee Lee, Jisu Choi, Kyungnae Baek, Tae Soup Shim, Jerome Kartham Hyun, So‐Jung Park. Shape‐Changing DNA‐Linked Nanoparticle Films Dictated by Lateral and Vertical Patterns. Advanced Materials 2022, 34
(13)
https://doi.org/10.1002/adma.202109091
- Wenqiang Yan, Yun Ding, Run Zhang, Xinjie Luo, Pinghou Sheng, Ping Xue, Jimin He. Dual-functional polymer blends with rapid thermo-responsive shape memory and repeatable self-healing properties. Polymer 2022, 239 , 124436. https://doi.org/10.1016/j.polymer.2021.124436
- Veronika Kozlovskaya, Eugenia Kharlampieva. Anisotropic Particles through Multilayer Assembly. Macromolecular Bioscience 2022, 22
(1)
https://doi.org/10.1002/mabi.202100328
- Feng Zhou, Peiyang Gu, Zhipu Luo, Hari Krishna Bisoyi, Yujin Ji, Youyong Li, Qingfeng Xu, Quan Li, Jianmei Lu. Unexpected organic hydrate luminogens in the solid state. Nature Communications 2021, 12
(1)
https://doi.org/10.1038/s41467-021-22685-0
- Ziyang Zhang, Ziao Tian, Yongfeng Mei, Zengfeng Di. Shaping and structuring 2D materials via kirigami and origami. Materials Science and Engineering: R: Reports 2021, 145 , 100621. https://doi.org/10.1016/j.mser.2021.100621
- Minjeong Ha, Gilbert Santiago Cañón Bermúdez, Jessica A.‐C. Liu, Eduardo Sergio Oliveros Mata, Emily E. Evans, Joseph B. Tracy, Denys Makarov. Reconfigurable Magnetic Origami Actuators with On‐Board Sensing for Guided Assembly. Advanced Materials 2021, 33
(25)
https://doi.org/10.1002/adma.202008751
- Arash Ghoorchian, Tayyebeh Madrakian, Abbas Afkhami, Hasan Bagheri. Spectroelectrochemical and electrochromic behavior of poly(methylene blue) and poly(thionine)-modified multi-walled carbon nanotubes. Journal of Solid State Electrochemistry 2021, 25
(4)
, 1217-1229. https://doi.org/10.1007/s10008-021-04901-5
- Ziyang Zhang, Jigang Du, Jiaxu Li, Xiaodong Huang, Ting Kang, Chi Zhang, Song Wang, Olayemi Oluwatosin Ajao, Wen-Jun Wang, Pingwei Liu. Polymer nanocomposites with aligned two-dimensional materials. Progress in Polymer Science 2021, 114 , 101360. https://doi.org/10.1016/j.progpolymsci.2021.101360
- Yuntong Sun, Shan Ding, Chen Zhang, Jingjing Duan, Sheng Chen. A shape-memory V
3
O
7
·H
2
O electrocatalyst for foldable N
2
fixation. Journal of Materials Chemistry A 2021, 9
(3)
, 1603-1609. https://doi.org/10.1039/D0TA10510D
- Marc Z. Miskin. Atomic origami. Current Opinion in Solid State and Materials Science 2020, 24
(6)
, 100882. https://doi.org/10.1016/j.cossms.2020.100882
- Shan Liu, Pratik S. Kasbe, Muxuan Yang, Naifu Shen, Linrui Duan, Yimin Mao, Weinan Xu. Intimately bonded 2D materials and responsive polymer brushes for adaptive nanocomposites. Polymer 2020, 210 , 123033. https://doi.org/10.1016/j.polymer.2020.123033
- Kam Sang Kwok, Prabhjot K. Luthra, David H. Gracias. 3D Nanowire Arrays by Nanoimprint lithography and Mechanical Buckling. 2020, 207-208. https://doi.org/10.1109/NANO47656.2020.9183592
- Zhichao Fan, Yiyuan Yang, Fan Zhang, Zheng Xu, Hangbo Zhao, Taoyi Wang, Honglie Song, Yonggang Huang, John A. Rogers, Yihui Zhang. Inverse Design Strategies for 3D Surfaces Formed by Mechanically Guided Assembly. Advanced Materials 2020, 32
(14)
https://doi.org/10.1002/adma.201908424
- Kam Sang Kwok, Qi Huang, Massimo Mastrangeli, David H. Gracias. Self‐Folding Using Capillary Forces. Advanced Materials Interfaces 2020, 7
(5)
https://doi.org/10.1002/admi.201901677
- Run Zhang, Suwei Wang, Jing Tian, Ke Chen, Ping Xue, Yihui Wu, Weimin Chou. Effect of PEW and CS on the Thermal, Mechanical, and Shape Memory Properties of UHMWPE. Polymers 2020, 12
(2)
, 483. https://doi.org/10.3390/polym12020483
- L. K. Rivera-Tarazona, V. D. Bhat, H. Kim, Z. T. Campbell, T. H. Ware. Shape-morphing living composites. Science Advances 2020, 6
(3)
https://doi.org/10.1126/sciadv.aax8582
- Joel Berry, Simeon Ristić, Songsong Zhou, Jiwoong Park, David J. Srolovitz. The MoSeS dynamic omnigami paradigm for smart shape and composition programmable 2D materials. Nature Communications 2019, 10
(1)
https://doi.org/10.1038/s41467-019-12945-5
- Zhen Jiang, Broden Diggle, India C. G. Shackleford, Luke A. Connal. Tough, Self‐Healing Hydrogels Capable of Ultrafast Shape Changing. Advanced Materials 2019, 31
(48)
https://doi.org/10.1002/adma.201904956
- M. Manav, M. Ponga, A. Srikantha Phani. Stress in a polymer brush. Journal of the Mechanics and Physics of Solids 2019, 127 , 125-150. https://doi.org/10.1016/j.jmps.2019.03.009
- Shine K. Albert, Xiaole Hu, So‐Jung Park. Dynamic Nanostructures from DNA‐Coupled Molecules, Polymers, and Nanoparticles. Small 2019, 15
(26)
https://doi.org/10.1002/smll.201900504
- Zheng Xu, Zhichao Fan, Haoran Fu, Yuan Liu, Yanyang Zi, Yonggang Huang, Yihui Zhang. Optimization-Based Approach for the Inverse Design of Ribbon-Shaped Three-Dimensional Structures Assembled Through Compressive Buckling. Physical Review Applied 2019, 11
(5)
https://doi.org/10.1103/PhysRevApplied.11.054053
- Bhavana Gupta, Mariana C. Afonso, Lin Zhang, Cedric Ayela, Patrick Garrigue, Bertrand Goudeau, Alexander Kuhn. Wireless Coupling of Conducting Polymer Actuators with Light Emission. ChemPhysChem 2019, 20
(7)
, 941-945. https://doi.org/10.1002/cphc.201900116
- Conor M. Gomes, Chang Liu, Jeffrey A. Paten, Samuel M. Felton, Leila F. Deravi. Protein‐Based Hydrogels that Actuate Self‐Folding Systems. Advanced Functional Materials 2019, 29
(4)
, 1805777. https://doi.org/10.1002/adfm.201805777
- Vladimir A. Bolaños Quiñones, Hong Zhu, Alexander A. Solovev, Yongfeng Mei, David H. Gracias. Origami Biosystems: 3D Assembly Methods for Biomedical Applications. Advanced Biosystems 2018, 2
(12)
https://doi.org/10.1002/adbi.201800230
Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.
Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.
The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.