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Superheating gold beyond the predicted entropy catastrophe threshold

White, Thomas G. [University of Nevada, Reno, NV (United States)] (ORCID:0000000238654240)·Griffin, Travis D. [University of Nevada, Reno, NV (United States)] (ORCID:0009000794474301)·Haden, Daniel [University of Nevada, Reno, NV (United States)] (ORCID:000000018288664X)·Lee, Hae Ja [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000240355637)·Galtier, Eric [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:000000020396285X)·Cunningham, Eric [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000209764416)·Khaghani, Dimitri [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000251392310)·Descamps, Adrien [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Queen’s University Belfast (United Kingdom)] (ORCID:0000000317086376)·Wollenweber, Lennart [European XFEL GmbH, Schenefeld (Germany)]·Armentrout, Ben [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000319077959)·Convery, Carson [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Columbia University, New York, NY (United States)] (ORCID:0009000068576047)·Appel, Karen [European XFEL GmbH, Schenefeld (Germany)] (ORCID:0000000229022102)·Fletcher, Luke B. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000271207194)·Goede, Sebastian [European XFEL GmbH, Schenefeld (Germany)]·Hastings, J. B. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)]·Iratcabal, Jeremy [University of Nevada, Reno, NV (United States)] (ORCID:0000000196758980)·McBride, Emma E. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Queen’s University Belfast (United Kingdom)] (ORCID:0000000288216126)·Molina, Jacob [University of Nevada, Reno, NV (United States); Princeton University, NJ (United States)] (ORCID:0000000216329375)·Monaco, Giulio [University of Padova (Italy)] (ORCID:0000000324976422)·Morrison, Landon [University of Nevada, Reno, NV (United States); University of Oxford (United Kingdom)] (ORCID:0009000303549082)·Stramel, Hunter [University of Nevada, Reno, NV (United States)]·Yunus, Sameen [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); University of California, Merced, CA (United States)]·Zastrau, Ulf [European XFEL GmbH, Schenefeld (Germany)] (ORCID:0000000235754449)·Glenzer, Siegfried H. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000191120558)·Gregori, Gianluca [University of Oxford (United Kingdom)] (ORCID:0000000241530628)·Gericke, Dirk O. [University of Warwick, Coventry (United Kingdom)] (ORCID:0000000167979004)·Nagler, Bob [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0009000257367842)
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Abstract

In their landmark study, Fecht and Johnson unveiled a phenomenon that they termed the ‘entropy catastrophe’, a critical point where the entropy of superheated crystals equates to that of their liquid counterparts. This point marks the uppermost stability boundary for solids at temperatures typically around three times their melting point. Despite the theoretical prediction of this ultimate stability threshold, its practical exploration has been prevented by numerous intermediate destabilizing events, colloquially known as a hierarchy of catastrophes, which occur at far lower temperatures. Here we experimentally test this limit under ultrafast heating conditions, directly tracking the lattice temperature by using high-resolution inelastic X-ray scattering. Our gold samples are heated to temperatures over 14 times their melting point while retaining their crystalline structure, far surpassing the predicted threshold and suggesting a substantially higher or potentially no limit for superheating. We point to the inability of our samples to expand on these very short timescales as an important difference from previous estimates. These observations provide insights into the dynamics of melting under extreme conditions.

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Laser-produced plasmasMaterials sciencePhase transitions and critical phenomenaStructure of solids and liquidscritical phenomenalaser-produced plasmasmaterials sciencephase transitionsstructure of solids and liquids

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White, Thomas G. [University of Nevada, Reno, NV (United States)] (ORCID:0000000238654240), Griffin, Travis D. [University of Nevada, Reno, NV (United States)] (ORCID:0009000794474301), Haden, Daniel [University of Nevada, Reno, NV (United States)] (ORCID:000000018288664X), Lee, Hae Ja [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000240355637), Galtier, Eric [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:000000020396285X), Cunningham, Eric [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000209764416), Khaghani, Dimitri [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000251392310), Descamps, Adrien [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Queen’s University Belfast (United Kingdom)] (ORCID:0000000317086376), Wollenweber, Lennart [European XFEL GmbH, Schenefeld (Germany)], Armentrout, Ben [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000319077959), Convery, Carson [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Columbia University, New York, NY (United States)] (ORCID:0009000068576047), Appel, Karen [European XFEL GmbH, Schenefeld (Germany)] (ORCID:0000000229022102), Fletcher, Luke B. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000271207194), Goede, Sebastian [European XFEL GmbH, Schenefeld (Germany)], Hastings, J. B. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Iratcabal, Jeremy [University of Nevada, Reno, NV (United States)] (ORCID:0000000196758980), McBride, Emma E. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Queen’s University Belfast (United Kingdom)] (ORCID:0000000288216126), Molina, Jacob [University of Nevada, Reno, NV (United States); Princeton University, NJ (United States)] (ORCID:0000000216329375), Monaco, Giulio [University of Padova (Italy)] (ORCID:0000000324976422), Morrison, Landon [University of Nevada, Reno, NV (United States); University of Oxford (United Kingdom)] (ORCID:0009000303549082), Stramel, Hunter [University of Nevada, Reno, NV (United States)], Yunus, Sameen [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); University of California, Merced, CA (United States)], Zastrau, Ulf [European XFEL GmbH, Schenefeld (Germany)] (ORCID:0000000235754449), Glenzer, Siegfried H. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000191120558), Gregori, Gianluca [University of Oxford (United Kingdom)] (ORCID:0000000241530628), Gericke, Dirk O. [University of Warwick, Coventry (United Kingdom)] (ORCID:0000000167979004), Nagler, Bob [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0009000257367842). 2025-07-23. Superheating gold beyond the predicted entropy catastrophe threshold. https://doi.org/10.1038/s41586-025-09253-y

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