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Droplet coalescence is ubiquitous in nature, and its regulation is significant in industrial processes and biomedical applications. While bare droplets suddenly coalesce in contact, the droplets covered with liquid-repellent particles to form “liquid marbles (LMs)” are not. Previously, the external stimuli-responsive breakage of the particle layer enabled the regulation of the coalescence timing. However, preprogramming the coalescence timing of droplets without stimuli is challenging. In this work, we report LMs that break the particle layer in preprogrammed time. The particles have a core wettable site and are tethered with a low-wettability flexible molecular chain, which gradually increases wettability with time. The time-dependent wettability variation is owing to the adaptation of the molecular chain; thus, it is repeatedly available, and its speed is controllable by chain length. The formed LMs expose bare droplet surfaces in preprogrammed timing, which enables the modulation of coalescence timing from 2 to 40 minutes without relying on external stimuli. Moreover, the additivity of the particles enabled the fine-tuning of the coalescence time with 1-minute resolutions. Further, the contact of several LMs with different adaptation times enabled cascade droplet coalescence, opening a new route for droplet manipulation.

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  This is the peer reviewed version of the following article: C. Mishra, D. Sarkar, N. Barman, S. Kumar, M. Tenjimbayashi, U. Manna, Modulating Coalescence Timing of Liquid Marbles via Wettability Adaptation. Adv. Mater. 2025, 37, 2420342, which has been published in final form at https://doi.org/10.1002/adma.202420342. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.

Keyword: Liquid marble, Adaptive wetting

Date published: 2025-04-08

Publisher: Wiley

Journal:

• Advanced Materials (ISSN: 09359648) vol. 37 issue. 24

Funding:

• Science and Engineering Research Board CRG/2022/000710
• Science and Engineering Research Board DBT BT/PR45283/NER/95/1919/2022
• Ministry of Electronics and Information technology 5(1)/2022‐NANO

Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.5557

First published URL: https://doi.org/10.1002/adma.202420342

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Updated at: 2025-07-02 16:54:30 +0900

Published on MDR: 2026-04-08 08:23:33 +0900