High-density stable glasses formed on soft substrates

Luo, Peng; Wolf, Sarah E.; Govind, Shivajee; Stephens, Richard B.; Kim, Dong Hyup; Chen, Cindy Y.; Nguyen, Truc; Wąsik, Patryk; Zhernenkov, Mikhail; Mcclimon, Brandon; Fakhraai, Zahra

doi:10.1038/s41563-024-01828-w

Title: High-density stable glasses formed on soft substrates

Journal Article · 27 February 2024 · Nature Materials

DOI: https://doi.org/10.1038/s41563-024-01828-w · OSTI ID:2440568

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Univ. of Pennsylvania, Philadelphia, PA (United States)
State Univ. of New York (SUNY), Cortland, NY (United States)
Univ. of Pennsylvania, Philadelphia, PA (United States); Seoul National Univ. (Korea, Republic of)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Enabled by surface-mediated equilibration, physical vapour deposition can create high-density stable glasses comparable with liquid-quenched glasses aged for millions of years. Deposition is often performed at various rates and temperatures on rigid substrates to control the glass properties. Here, in this work, we demonstrate that on soft, rubbery substrates, surface-mediated equilibration is enhanced up to 170 nm away from the interface, forming stable glasses with densities up to 2.5% higher than liquid-quenched glasses within 2.5 h of deposition. Gaining similar properties on rigid substrates would require 10 million times slower deposition, taking ~3,000 years. Controlling the modulus of the rubbery substrate provides control over the glass structure and density at constant deposition conditions. These results underscore the significance of substrate elasticity in manipulating the properties of the mobile surface layer and thus the glass structure and properties, allowing access to deeper states of the energy landscape without prohibitively slow deposition rates.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2440568

Report Number(s):: BNL--226009-2024-JAAM

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 5 Vol. 23; ISSN 1476-1122

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

References (53)

High-Modulus Organic Glasses Prepared by Physical Vapor Deposition Kearns, Kenneth L.; Still, Tim; Fytas, George Advanced Materials, Vol. 22, Issue 1 https://doi.org/10.1002/adma.200901673	journal	January 2010
Quantitative evaluation of orientation in cellulose fibres from the X-ray fibre diagram Hermans, J. J.; Hermans, P. H.; Vermaas, D. Recueil des Travaux Chimiques des Pays-Bas, Vol. 65, Issue 6 https://doi.org/10.1002/recl.19460650605	journal	January 1946
A comparison of JKR-based methods to analyze quasi-static and dynamic indentation force curves Ebenstein, Donna M.; Wahl, Kathryn J. Journal of Colloid and Interface Science, Vol. 298, Issue 2 https://doi.org/10.1016/j.jcis.2005.12.062	journal	June 2006
Raman, mid-infrared, near-infrared and ultraviolet–visible spectroscopy of PDMS silicone rubber for characterization of polymer optical waveguide materials Cai, Dengke; Neyer, Andreas; Kuckuk, Rüdiger Journal of Molecular Structure, Vol. 976, Issue 1-3 https://doi.org/10.1016/j.molstruc.2010.03.054	journal	July 2010
Process and material properties of polydimethylsiloxane (PDMS) for Optical MEMS Schneider, Florian; Draheim, Jan; Kamberger, Robert Sensors and Actuators A: Physical, Vol. 151, Issue 2 https://doi.org/10.1016/j.sna.2009.01.026	journal	April 2009
Structural Characterization of Vapor-Deposited Glasses of an Organic Hole Transport Material with X-ray Scattering Gujral, Ankit; O’Hara, Kathryn A.; Toney, Michael F. Chemistry of Materials, Vol. 27, Issue 9 https://doi.org/10.1021/acs.chemmater.5b00583	journal	April 2015
Exploring the Importance of Surface Diffusion in Stability of Vapor-Deposited Organic Glasses Samanta, Subarna; Huang, Georgia; Gao, Gui The Journal of Physical Chemistry B, Vol. 123, Issue 18 https://doi.org/10.1021/acs.jpcb.9b01012	journal	April 2019
Origin of Anisotropic Molecular Packing in Vapor-Deposited Alq3 Glasses Bagchi, Kushal; Jackson, Nicholas E.; Gujral, Ankit The Journal of Physical Chemistry Letters, Vol. 10, Issue 2 https://doi.org/10.1021/acs.jpclett.8b03582	journal	December 2018
Vapor-Deposited Ethylbenzene Glasses Approach “Ideal Glass” Density Beasley, M. S.; Bishop, C.; Kasting, B. J. The Journal of Physical Chemistry Letters, Vol. 10, Issue 14 https://doi.org/10.1021/acs.jpclett.9b01508	journal	July 2019
Over What Length Scale Does an Inorganic Substrate Perturb the Structure of a Glassy Organic Semiconductor? Bagchi, Kushal; Deng, Chuting; Bishop, Camille ACS Applied Materials & Interfaces, Vol. 12, Issue 23 https://doi.org/10.1021/acsami.0c06428	journal	May 2020
Microscopic Structural Evolution during Ultrastable Metallic Glass Formation Luo, Peng; Zhu, Fan; Lv, Yu-Miao ACS Applied Materials & Interfaces, Vol. 13, Issue 33 https://doi.org/10.1021/acsami.1c10716	journal	August 2021
Local Glass Transition Temperature T _g ( z ) Within Polystyrene Is Strongly Impacted by the Modulus of the Neighboring PDMS Domain Gagnon, Yannic J.; Roth, Connie B. ACS Macro Letters, Vol. 9, Issue 11 https://doi.org/10.1021/acsmacrolett.0c00659	journal	October 2020
Direct Measurement of Molecular Motion in Freestanding Polystyrene Thin Films Paeng, Keewook; Swallen, Stephen F.; Ediger, M. D. Journal of the American Chemical Society, Vol. 133, Issue 22 https://doi.org/10.1021/ja2022834	journal	June 2011
High-Throughput Ellipsometric Characterization of Vapor-Deposited Indomethacin Glasses Dalal, Shakeel S.; Fakhraai, Zahra; Ediger, M. D. The Journal of Physical Chemistry B, Vol. 117, Issue 49 https://doi.org/10.1021/jp405005n	journal	August 2013
Hiking down the Energy Landscape: Progress Toward the Kauzmann Temperature via Vapor Deposition Kearns, Kenneth L.; Swallen, Stephen F.; Ediger, M. D. The Journal of Physical Chemistry B, Vol. 112, Issue 16 https://doi.org/10.1021/jp7113384	journal	April 2008
Structural Variations of an Organic Glassformer Vapor-Deposited onto a Temperature Gradient Stage Fakhraai, Zahra; Still, Tim; Fytas, George The Journal of Physical Chemistry Letters, Vol. 2, Issue 5 https://doi.org/10.1021/jz101723d	journal	February 2011
Physical Aging of Polymer Films Quenched and Measured Free-Standing via Ellipsometry: Controlling Stress Imparted by Thermal Expansion Mismatch between Film and Support Pye, Justin E.; Roth, Connie B. Macromolecules, Vol. 46, Issue 23 https://doi.org/10.1021/ma401872u	journal	November 2013
Ultrastable nanostructured polymer glasses Guo, Yunlong; Morozov, Anatoli; Schneider, Dirk Nature Materials, Vol. 11, Issue 4 https://doi.org/10.1038/nmat3234	journal	February 2012
Ultrastable glasses from in silico vapour deposition Singh, Sadanand; Ediger, M. D.; de Pablo, Juan J. Nature Materials, Vol. 12, Issue 2 https://doi.org/10.1038/nmat3521	journal	January 2013
Ultrastable metallic glasses formed on cold substrates Luo, P.; Cao, C. R.; Zhu, F. Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-03656-4	journal	April 2018
Ultrastable monodisperse polymer glass formed by physical vapour deposition Raegen, Adam N.; Yin, Junjie; Zhou, Qi Nature Materials, Vol. 19, Issue 10 https://doi.org/10.1038/s41563-020-0723-7	journal	July 2020
Spontaneous formation of metastable orientation with well-organized permanent dipole moment in organic glassy films Tanaka, Masaki; Auffray, Morgan; Nakanotani, Hajime Nature Materials, Vol. 21, Issue 7 https://doi.org/10.1038/s41563-022-01265-7	journal	May 2022
Mobility gradients yield rubbery surfaces on top of polymer glasses Hao, Zhiwei; Ghanekarade, Asieh; Zhu, Ningtao Nature, Vol. 596, Issue 7872 https://doi.org/10.1038/s41586-021-03733-7	journal	August 2021
Density and birefringence of a highly stable α,α,β-trisnaphthylbenzene glass Dalal, Shakeel S.; Sepúlveda, A.; Pribil, Greg K. The Journal of Chemical Physics, Vol. 136, Issue 20 https://doi.org/10.1063/1.4719532	journal	May 2012
Elastically cooperative activated barrier hopping theory of relaxation in viscous fluids. I. General formulation and application to hard sphere fluids Mirigian, Stephen; Schweizer, Kenneth S. The Journal of Chemical Physics, Vol. 140, Issue 19 https://doi.org/10.1063/1.4874842	journal	May 2014
How much time is needed to form a kinetically stable glass? AC calorimetric study of vapor-deposited glasses of ethylcyclohexane Chua, Y. Z.; Ahrenberg, M.; Tylinski, M. The Journal of Chemical Physics, Vol. 142, Issue 5 https://doi.org/10.1063/1.4906806	journal	February 2015
Thermal stability of vapor-deposited stable glasses of an organic semiconductor Walters, Diane M.; Richert, Ranko; Ediger, M. D. The Journal of Chemical Physics, Vol. 142, Issue 13 https://doi.org/10.1063/1.4916649	journal	April 2015
Orientational anisotropy in simulated vapor-deposited molecular glasses Lyubimov, Ivan; Antony, Lucas; Walters, Diane M. The Journal of Chemical Physics, Vol. 143, Issue 9 https://doi.org/10.1063/1.4928523	journal	September 2015
Long-range correlated dynamics in ultra-thin molecular glass films Zhang, Yue; Glor, Ethan C.; Li, Mu The Journal of Chemical Physics, Vol. 145, Issue 11 https://doi.org/10.1063/1.4962734	journal	September 2016
Local glass transition temperature T g ( z ) of polystyrene next to different polymers: Hard vs. soft confinement Baglay, Roman R.; Roth, Connie B. The Journal of Chemical Physics, Vol. 146, Issue 20 https://doi.org/10.1063/1.4975168	journal	May 2017
Using deposition rate to increase the thermal and kinetic stability of vapor-deposited hole transport layer glasses via a simple sublimation apparatus Kearns, Kenneth L.; Krzyskowski, Paige; Devereaux, Zachary The Journal of Chemical Physics, Vol. 146, Issue 20 https://doi.org/10.1063/1.4979814	journal	May 2017
Comparing refractive index and density changes with decreasing film thickness in thin supported films across different polymers Han, Yixuan; Huang, Xinru; Rohrbach, Alan C. W. The Journal of Chemical Physics, Vol. 153, Issue 4 https://doi.org/10.1063/5.0012423	journal	July 2020
Physical vapor deposition as a route to hidden amorphous states Dawson, K. J.; Kearns, K. L.; Yu, L. Proceedings of the National Academy of Sciences, Vol. 106, Issue 36 https://doi.org/10.1073/pnas.0901469106	journal	July 2009
Suppression of tunneling two-level systems in ultrastable glasses of indomethacin Perez-Castaneda, T.; Rodriguez-Tinoco, C.; Rodriguez-Viejo, J. Proceedings of the National Academy of Sciences, Vol. 111, Issue 31 https://doi.org/10.1073/pnas.1405545111	journal	July 2014
Tunable molecular orientation and elevated thermal stability of vapor-deposited organic semiconductors Dalal, Shakeel S.; Walters, Diane M.; Lyubimov, Ivan Proceedings of the National Academy of Sciences, Vol. 112, Issue 14 https://doi.org/10.1073/pnas.1421042112	journal	March 2015
Decoupling of surface diffusion and relaxation dynamics of molecular glasses Zhang, Yue; Fakhraai, Zahra Proceedings of the National Academy of Sciences, Vol. 114, Issue 19 https://doi.org/10.1073/pnas.1701400114	journal	April 2017
Effects of microstructure formation on the stability of vapor-deposited glasses Moore, Alex R.; Huang, Georgia; Wolf, Sarah Proceedings of the National Academy of Sciences, Vol. 116, Issue 13 https://doi.org/10.1073/pnas.1821761116	journal	March 2019
Glasses denser than the supercooled liquid Jin, Yi; Zhang, Aixi; Wolf, Sarah E. Proceedings of the National Academy of Sciences, Vol. 118, Issue 31 https://doi.org/10.1073/pnas.2100738118	journal	July 2021
Surface equilibration mechanism controls the molecular packing of glassy molecular semiconductors at organic interfaces Fiori, Marie E.; Bagchi, Kushal; Toney, Michael F. Proceedings of the National Academy of Sciences, Vol. 118, Issue 42 https://doi.org/10.1073/pnas.2111988118	journal	October 2021
Mechanical characterization of bulk Sylgard 184 for microfluidics and microengineering Johnston, I. D.; McCluskey, D. K.; Tan, C. K. L. Journal of Micromechanics and Microengineering, Vol. 24, Issue 3 https://doi.org/10.1088/0960-1317/24/3/035017	journal	February 2014
The mechanical properties of the rubber elastic polymer polydimethylsiloxane for sensor applications Lötters, J. C.; Olthuis, W.; Veltink, P. H. Journal of Micromechanics and Microengineering, Vol. 7, Issue 3 https://doi.org/10.1088/0960-1317/7/3/017	journal	September 1997
Polynomial fitting techniques applied to opto-mechanical properties of PDMS Sylgard 184 for given curing parameters Santiago-Alvarado, A.; Cruz-Félix, A. S.; González-García, J. Materials Research Express, Vol. 7, Issue 4 https://doi.org/10.1088/2053-1591/ab8339	journal	April 2020
Substrate and Chain Size Dependence of Near Surface Dynamics of Glassy Polymers Qi, D.; Fakhraai, Z.; Forrest, J. A. Physical Review Letters, Vol. 101, Issue 9 https://doi.org/10.1103/PhysRevLett.101.096101	journal	August 2008
Surface Self-Diffusion of an Organic Glass Zhu, L.; Brian, C. W.; Swallen, S. F. Physical Review Letters, Vol. 106, Issue 25 https://doi.org/10.1103/PhysRevLett.106.256103	journal	June 2011
High-performance organic light-emitting diodes comprising ultrastable glass layers Ràfols-Ribé, Joan; Will, Paul-Anton; Hänisch, Christian Science Advances, Vol. 4, Issue 5 https://doi.org/10.1126/sciadv.aar8332	journal	May 2018
Organic Glasses with Exceptional Thermodynamic and Kinetic Stability Swallen, S. F.; Kearns, K. L.; Mapes, M. K. Science, Vol. 315, Issue 5810 https://doi.org/10.1126/science.1135795	journal	January 2007
Measuring the Surface Dynamics of Glassy Polymers Fakhraai, Z.; Forrest, J. A. Science, Vol. 319, Issue 5863 https://doi.org/10.1126/science.1151205	journal	February 2008
Glass Transition Dynamics and Surface Layer Mobility in Unentangled Polystyrene Films Yang, Z.; Fujii, Y.; Lee, F. K. Science, Vol. 328, Issue 5986 https://doi.org/10.1126/science.1184394	journal	June 2010
A Direct Quantitative Measure of Surface Mobility in a Glassy Polymer Chai, Y.; Salez, T.; McGraw, J. D. Science, Vol. 343, Issue 6174 https://doi.org/10.1126/science.1244845	journal	February 2014
Structure-property relationships from universal signatures of plasticity in disordered solids Cubuk, E. D.; Ivancic, R. J. S.; Schoenholz, S. S. Science, Vol. 358, Issue 6366 https://doi.org/10.1126/science.aai8830	journal	November 2017
Surface-Mediated Formation of Stable Glasses Luo, Peng; Fakhraai, Zahra Annual Review of Physical Chemistry, Vol. 74, Issue 1 https://doi.org/10.1146/annurev-physchem-042018-052708	journal	April 2023
Thin-coating contact mechanics with adhesion Reedy, E. D. Journal of Materials Research, Vol. 21, Issue 10 https://doi.org/10.1557/jmr.2006.0327	journal	October 2006
High-density stable glasses formed on soft substrates Luo, Peng; Wolf, Sarah E.; Govind, Shivajee figshare https://doi.org/10.6084/m9.figshare.25000454.v1	dataset	January 2024

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