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New polymorphs β and γ of bis‐3‐nitrophenyl disulphide, crystallized above 0.3 GPa, are less dense than the ambient‐pressure polymorph α. This counterintuitive density relation results from the high‐entropy nucleation and subsequent kinetic crystallization. The work performed by pressure compensates the high entropy and temperature product, substantiated in varied conformers and increased chemical potential. Pressure‐increased viscosity promotes the kinetic polymorphs, in accordance with empirical Ostwald's rule of stages. It contrasts to mechanochemical techniques, favouring high‐density polymorphs. [ABSTRACT FROM AUTHOR]

Crystal growth, high-pressure chemistry, kinetic crystallization, nucleation, polymorphism Front Cover: High-pressure Nucleation of Low-Density Polymorphs (Chem. Eur. J. 24/2021) Keywords: crystal growth; high-pressure chemistry; kinetic crystallization; nucleation; polymorphism EN crystal growth high-pressure chemistry kinetic crystallization nucleation polymorphism 6995 6995 1 04/30/21 20210426 NES 210426 B Low-density polymorphs b obtained in a high-pressure environment are reported in this work. [Extracted from the article]