Theoretical description of phase coexistence in model C60 -: art. no. 021104

被引:25
|
作者
Costa, D
Pellicane, G
Caccamo, C
Schöll-Paschinger, E
Kahl, G
机构
[1] Univ Messina, Ist Nazl Fis Mat, I-98166 Messina, Italy
[2] Univ Messina, Dipartimento Fis, I-98166 Messina, Italy
[3] Vienna Univ Technol, Inst Theoret Phys, A-1040 Vienna, Austria
[4] Vienna Univ Technol, CMS, A-1040 Vienna, Austria
来源
PHYSICAL REVIEW E | 2003年 / 68卷 / 02期
关键词
D O I
10.1103/PhysRevE.68.021104
中图分类号
O35 [流体力学]; O53 [等离子体物理学];
学科分类号
070204 ; 080103 ; 080704 ;
摘要
We have investigated the phase diagram of a pair interaction model of C-60 fullerene [L. A. Girifalco, J. Phys. Chem. 96, 858 (1992)], in the framework provided by two integral equation theories of the liquid state, namely, the modified hypernetted chain (MHNC) implemented under a global thermodynamic consistency constraint, and the self-consistent Ornstein-Zernike approximation (SCOZA), and by a perturbation theory (PT) with various degrees of refinement, for the free energy of the solid phase. We present an extended assessment of such theories as set against a recent Monte Carlo study of the same model [D. Costa, G. Pellicane, C. Caccamo, and M. C. Abramo, J. Chem. Phys. 118, 304 (2003)]. We have compared the theoretical predictions with the corresponding simulation results for several thermodynamic properties such as the free energy, the pressure, and the internal energy. Then we have determined the phase diagram of the model, by using either the SCOZA, the MHNC, or the PT predictions for one of the coexisting phases, and the simulation data for the other phase, in order to separately ascertain the accuracy of each theory. It turns out that the overall appearance of the phase portrait is reproduced fairly well by all theories, with remarkable accuracy as for the melting line and the solid-vapor equilibrium. All theories show a more or less pronounced discrepancy with the simulated fluid-solid coexistence pressure, above the triple point. The MHNC and SCOZA results for the liquid-vapor coexistence, as well as for the corresponding critical points, are quite accurate; the SCOZA tends to underestimate the density corresponding to the freezing line. All results are discussed in terms of the basic assumptions underlying each theory. We have then selected the MHNC for the fluid and the first-order PT for the solid phase, as the most accurate tools to investigate the phase behavior of the model in terms of purely theoretical approaches. It emerges that the use of different procedures to characterize the fluid and the solid phases provides a semiquantitative reproduction of the thermodynamic properties of the C-60 model at issue. The overall results appear as a robust benchmark for further theoretical investigations on higher order C-n>60 fullerenes, as well as on other fullerene-related materials, whose description can be based on a modelization similar to that adopted in this work.
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页数:11
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