Affiliation:
1. Department of Chemistry, Graduate School of Humanities and Sciences, Nara Women’s University , Nara 630-8506, Japan
Abstract
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.