We show that two liquid states can exist in distinguishable helium-4 (4He) obeying Boltzmann statistics by path integral centroid molecular dynamics (CMD) simulations. This is an indication of quantum liquid polyamorphism induced by the nuclear quantum effect. For 0.08-3.3 K and 1-500 bar, we extensively conducted the isothermal-isobaric CMD simulations to explore not only possible states and state diagram but also the state characteristics. The distinguishable 4He below 25 bar does not freeze down to 0.1 K even though it includes no Bosonic exchange effect and, therefore, no Bose condensation. One liquid state, low quantum-dispersion liquid (LQDL), is nearly identical to normal liquid He-I of real 4He. The other is high quantum-dispersion liquid (HQDL) consisting of atoms with longer quantum wavelength. This is another non-superfluid existing below 0.5 K or the temperatures of LQDL. The HQDL is also a low-entropy and fragile liquid to exhibit, unlike conventional liquids, rather gas-like relaxation of velocity autocorrelation function, while there the atoms diffuse without noticeable contribution from quantum tunneling. The LQDL-HQDL transition is not a thermodynamic phase transition but a continuous crossover accompanied by the change in the expansion factor of quantum wavelength. Freezing of HQDL into the low quantum-dispersion amorphous solid occurs by heating from 0.2 to 0.3 K at 40-50 bar, while this P-T condition coincides with the Kim-Chan normal-supersolid phase boundary of real 4He. The obtained state diagram was compared to that of the confined subnano-scale 4He systems, where Bosonic correlation is considerably suppressed.
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Nanotechnology
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Institute of Nonlinear Optics, College of Science, JiuJiang University, Jiangxi 334000, People's Republic of China.
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College of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, China.
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Research Center for Energy and Environmental Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
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View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Centre for Robotics and Automation, Department of Biomedical Engineering, City University of Hong Kong, Hong Kong 999077, China.
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