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Akira Yoshida

Publications and source records attributed to Akira Yoshida.

5 recordsLinked to original sources

Gibbs Factorials Become Kinetic in History-Dependent Reactions

Gibbs factorials are usually regarded as equilibrium counting factors. We show that they can also appear directly in a measurable kinetic observable when products formed at different stages are statistically distinguished in the history ensemble. In a model designed to isolate the essential ingredients, transient AB$_2$ complexes are stabilized as C molecules either in a single operation or through a two-stage procedure. The mean-waiting-time ratio is governed by a kinetic advantage factor $\mathcal{A}_C$ defined from equilibrium probabilities. A fluctuation-theorem argument identifies the dominant contribution $n_{\mathrm C}!/[n_{\mathrm m}!(n_{\mathrm C}-n_{\mathrm m})!]$, where $n_{\mathrm m}$ is the intermediate product number and $n_{\mathrm C}$ is the final target. This Gibbs factorial arises because products formed before and after the intermediate operation are statistically distinguished in the history ensemble, although the final molecules are macroscopically identical. Molecular dynamics simulations confirm the predicted combinatorial scaling of the mean-waiting-time ratio.

cond-mat.stat-mech

Global thermodynamics for isothermal fluids under gravity

We develop a formulation of global thermodynamics for equilibrium systems under the influence of gravity. The free energy for simple fluids is extended to include a dependence on $(T, V, N, mgL)$, where $L$ represents the vertical system length in the direction of gravity. A central idea in this formulation is to uniquely fix the reference point of the gravitational potential, ensuring a consistent thermodynamic framework. Using this framework, we derive the probability density of thermodynamic quantities, which allows us to define a variational function for determining equilibrium liquid-gas coexistence under gravity. The resulting free energy landscape, derived from the variational function, reveals the local stability of liquid-gas configurations. Specifically, the liquid phase resides at the lower portion of the system due to gravity, while the inverted configuration (with liquid on top) is also locally stable in this landscape. Furthermore, we characterize the transition between these liquid-gas configurations as a first-order phase transition using the thermodynamic free energy of $(T,V,N,mgL)$. Finally, we validate the predictions of global thermodynamics through molecular dynamics simulations, demonstrating the applicability and accuracy of the proposed framework.

cond-mat.stat-mech

Heat-induced liquid hovering in liquid-gas coexistence under gravity

We study a liquid-gas coexistence system in a container under gravity with heat flow in the direction opposite to gravity. By molecular dynamics simulation, we find that the liquid buoys up and continues to float steadily. The height at which the liquid floats is determined by a dimensionless parameter related to the ratio of the temperature gradient to gravity. We confirm that supercooled gas remains stable above the liquid. We provide a phenomenological argument for explaining the phenomenon from a simple thermodynamic assumption.

cond-mat.stat-mech

Quasi-static decomposition and the Gibbs factorial in small thermodynamic system

For small thermodynamic systems in contact with a heat bath, we determine the free energy by imposing the following two conditions. First, the quasi-static work in any configuration change is equal to the free energy difference. Second, the temperature dependence of the free energy satisfies the Gibbs-Helmholtz relation. We find that these prerequisites uniquely lead to the free energy of a classical system consisting of $N$-interacting identical particles, up to an additive constant proportional to $N$. The free energy thus determined contains the Gibbs factorial $N!$ in addition to the phase space integration of the Gibbs-Boltzmann factor. The key step in the derivation is to construct a quasi-static decomposition of small thermodynamic systems.

cond-mat.stat-mech

Work relation for determining the mixing free energy of small-scale mixtures

In thermodynamically characterizing a mixture comprising a finite number of molecules, we consider two kinds of protocol for producing a mixture from a pure substance. The first is a single alchemical operation, whereas the second is a series of processes with feedback control in information thermodynamics and conventional mixing with semipermeable membranes. A comparison of the two numerically determined free-energy changes provides a combinatorial factor that indicates the indistinguishability of the molecules and an alternative Jarzynski equality. The comparison also uncovers a work relation for determining the mixing free energy without using semipermeable membranes. We demonstrate a numerical calculation of applying the work relation to a mixture of argon and krypton. The mixing free energy clearly shows the characteristics of liquid--vapor transition.

cond-mat.stat-mech