Failure of Ornstein–Zernike asymptotics for the pair correlation function at high temperature and small density
Abstract
We report on recent results that show that the pair correlation function of systems with exponentially decaying interactions can fail to exhibit Ornstein–Zernike asymptotics at all sufficiently high temperatures and all sufficiently small densities. This turns out to be related to a lack of analyticity of the correlation length as a function of temperature and/or density and even occurs for one-dimensional systems.
In 1914, Ornstein and Zernike [1] introduced their celebrated equation for the density-density pair correlation function :
(1) |
where denotes the direct correlation function and the density. Using (1), Zernike [2] determined the asymptotic behavior of the pair correlation function of systems with short-range interactions (meaning here interactions decaying faster than some exponentially decreasing function of the distance):
(2) |
as the Euclidean norm tends to infinity. His derivation relied on a certain mass gap assumption: , which was believed to hold in wide generality for short-range models at low density [3].
It is usually expected that OZ behavior as displayed in (2) should hold for general simple fluids with short-range interactions at sufficiently high temperature and/or sufficiently small density. In this letter, we report on recent results that show that such is not necessarily the case. As will be explained below, this failure can be seen as resulting from a violation of the mass gap assumption.
For the sake of simplicity of exposition, we restrict our presentation to ferromagnetic Ising models on , but our results should hold in wide generality and have been established for other models in [4] (including the self-avoiding walk, Potts models, Bernoulli percolation, the massive Gaussian Free Field and the XY model). We start by discussing a simplified setting and then turn to a more general framework, in which some interesting new aspects emerge. A heuristic explanation of the underlying mechanism, relating the latter to a suitable condensation phenomenon, is also provided.
I Overview in a simplified setting
An anisotropic version of the OZ asymptotics (2) has been rigorously derived for finite-range ferromagnetic Ising models on , both above the critical temperature [5, 6] and when the magnetic field is non-zero [7]: in both cases, as tends to infinity,
(3) |
where both and the inverse correlation length are positive, analytic functions of the direction . The same behavior still holds as long as the interaction decays super-exponentially [8]. Of course, this cannot be true for interactions decaying sub-exponentially, since the pair correlation function cannot decay slower than the interaction, as seems to have been first noted by Widom [9].
Let us thus restrict our attention to coupling constants of the form
(4) |
for some and . (More general forms will be considered below.) Let us also assume for simplicity that there is no magnetic field (and omit it from the notation). We emphasize, however, that the analysis below can also be done by fixing some arbitrary and looking at the behavior of .
Let be a unit vector in and denote the inverse correlation length in direction by
where is a vertex of which is closest to . It is known [10] that for all , where denotes the inverse critical temperature. In addition, it is easy to prove that is decreasing in and satisfies
(5) |
Moreover, [11]. The behavior in (5) is in sharp contrast with what happens when the interaction decays super-exponentially (in which case ) and opens up the possibility that saturates at a finite temperature: for all , for some .
Observe that, if the latter were to occur, then there would be several remarkable consequences:
-
•
The inverse correlation length would not depend analytically on the temperature in the whole high-temperature regime .
-
•
One of the basic assumptions of OZ theory, namely that the rate of decay of the pair correlation function is strictly slower than the rate of decay of the interaction (in the present case, ) would be violated.
It turns out that such a saturation phenomenon can occur, in any dimension. Whether or not it does so depends on the value of the exponent . Namely, saturation occurs (that is, ) if and only if
(6) |
In particular, even when , the inverse correlation length is a non-analytic function of whenever , which contrasts with the well-known analyticity of all thermodynamic quantities [12, 13].
II General setting
Let us now consider coupling constants of the form
(7) |
where is an arbitrary norm on and the prefactor is positive and sub-exponential, in the sense that . We also assume that it behaves in an approximately isotropic manner: there exists and a function such that for all .
In order to ease the formulation of the extension of (6) to this more general framework, we need to make an additional genericity assumption on the direction . Let be the unit-ball associated to the norm . Given a direction , consider the corresponding point . By convexity, every close enough to can be written as
(8) |
where is some small real number, is unit vector in the tangent plane to at , is a unit vector normal to the tangent plane and is some non-negative convex function defined on the tangent plane such that (see Figure 1).

Our assumption on the direction is that the qualitative behavior of is the same in all directions : there exist and a non-decreasing convex function such that, for any unit vector in the tangent plane and small enough, we have
(9) |
When this holds, we will say that is quasi-isotropic in direction . Examples when quasi-isotropy is satisfied in every direction include -norms with .
Our main result on whether is the following:
Theorem 1
Fix a direction in which is quasi-isotropic. Then, saturation occurs in direction (that is, ) if and only if
(10) |
(In (10), we make the convention when .)
III An example
In this section, we illustrate on a specific example the direction-dependence of the saturation phenomenon.
Let us consider the model on with interaction
where is the -norm and we assume that .
Let be a unit vector in and let us write . When both and are nonzero, the local parametrization (8) of at applies with
so that one can choose . Condition (10) then implies that there is saturation in direction if and only if , as in (6) (which should not be surprising, since has the same qualitative behavior in both cases).
In the remaining cases ( or ), the local parametrization (8) of at applies with
so that one can choose . Therefore, in this case, there is saturation in direction if and only if
This clearly shows that the occurrence of saturation depends on both the temperature and the direction. In particular, when , when but is positive for all other directions.
IV An underlying condensation phenomenon
When , the 2-point function of the Ising model admits a graphical representation as a sum over paths:
(11) |
where the sum is over edge-self-avoiding paths connecting to and is a suitable non-negative weight [14]. Suppose that . It turns out that the saturation phenomenon occurring at corresponds to a change of behavior of the typical paths contributing to the sum in (11). When , typical paths have a length of order and behave diffusively, whereas when , typical paths contain steps: there is a giant step connecting a vertex close to to a vertex close to , see Fig. 2. This change of behavior is reminiscent of condensation phenomena for sums of random variables; we refer to [15] for a review.


V Proof in dimension 1
We consider the Ising model on with interactions as in (7); for simplicity, we assume that for all and that is monotone in . Introduce the generating functions (Laplace transforms)
Note that has radius of convergence , while has radius of convergence . Moreover, since we are assuming that , condition (10) is equivalent to and to .
Our analysis below will be based on the following inequalities satisfied by the weights in (11) (see [14]): there exists such that, if ,
(12) |
Note that the lower bound immediately implies that (simply consider the path composed of a single step from to in (11)).
V.1 Proof that (10) implies
V.2 A comment on OZ equation at low density
Let us pause a moment to make a comment about the previous argument. Consider the OZ equation (1). Taking and the Laplace transforms of and , one obtains the relation . For , (ferromagnetic assumption), and supposing that the asymptotic decay of coincides with the one of (which is for example the case in the Percus–Yevick approximation), the radii of convergence of are and respectively. Moreover, the same argument as previously implies that when and is small enough, and therefore that (failure of mass gap). In higher dimensions, the same argument (with more involved considerations about the link between the convergence domains of and ) is at the heart of the general condition (10).
V.3 Proof that implies
Since is non-summable, there exists such that
Let and . We have
where we used in the second line; the fact that is sub-exponential in the third line; the choice of in the fourth line. This immediately implies that . Since was arbitrary, we conclude that .
VI Failure of Ornstein-Zernike asymptotics
In this section, we illustrate, in a simple example, the mechanism leading to a violation of OZ asymptotics when saturation occurs. Let us thus consider the Ising model on with coupling constants of the form
(Again, we refer to [4] for a treatment of the general case in any dimension.)
In the previous section, it was shown that saturation occurs when
(13) |
We are going to show that there exists such that
(14) |
The lower bound follows directly from (11) by considering the path composed of a single step from to . For the upper bound, note first that (12) implies
(15) |
where in the last line, we assumed that is the vector with maximal -norm and used that . Observe now that, for any two real numbers with , we have
since is negative (by (13)). Using this observation times, it follows that
(16) |
where we used for the first inequality and and for the second one.
VII Conclusion
We have considered an Ising model with exponentially decaying interactions and have explained how the latter can, in suitable circumstances, undergo a saturation “transition”, in which the rate of exponential decay of the pair correlation function coincides with the rate of exponential decay of the interaction over a non-empty interval of temperatures (where is in general direction-dependent). Since the inverse correlation length becomes independent of the temperature below , it is not an analytic function of on . When this occurs, the pair correlation function fails to exhibit Ornstein–Zernike asymptotics for all .
A number of issues remain open. We have limited our analysis, for technical reasons, to ferromagnetic systems. It is unclear to us whether the general phenomenology changes when this assumption is dropped. In addition, the behavior of the system at is not understood, although it can be shown that in one-dimensional ferromagnetic systems, saturation does not occur at [8].
Acknowledgements.
YA thanks Hugo Duminil-Copin for financial support. YV was partially supported by the Swiss National Science Foundation through the NCCR SwissMAP.References
- Ornstein and Zernike [1914] L. S. Ornstein and F. Zernike, Accidental deviations of density and opalescence at the critical point of a single substance, KNAW, Proceedings, 17 II, 793 (1914).
- Zernike [1916] F. Zernike, The clustering-tendency of the molecules in the critical state and the extinction of light caused thereby, KNAW, Proceedings, 18 II, 1520 (1916).
- Fisher [1964] M. E. Fisher, Correlation functions and the critical region of simple fluids, J. Math. Phys. 5, 944 (1964).
- Aoun et al. [2021] Y. Aoun, D. Ioffe, S. Ott, and Y. Velenik, Non-analyticity of the correlation length in systems with exponentially decaying interactions, Commun. Math. Phys. 10.1007/s00220-021-04038-6 (2021).
- Campanino et al. [2003a] M. Campanino, D. Ioffe, and Y. Velenik, Ornstein-Zernike theory for finite range Ising models above , Probab. Theory Related Fields 125, 305 (2003a).
- Campanino et al. [2003b] M. Campanino, D. Ioffe, and Y. Velenik, Rigorous non-perturbative Ornstein-Zernike theory for Ising ferromagnets, Europhys. Letters 62, 182 (2003b).
- Ott [2020] S. Ott, Sharp asymptotics for the truncated two-point function of the Ising model with a positive field, Commun. Math. Phys. 374, 1361 (2020).
- [8] Y. Aoun, S. Ott, and Y. Velenik, work in progress.
- Widom [1964] B. Widom, On the radial distribution function in fluids, J. Chem. Phys. 41, 74 (1964).
- Aizenman et al. [1987] M. Aizenman, D. J. Barsky, and R. Fernández, The phase transition in a general class of Ising-type models is sharp, J. Stat. Phys. 47, 343 (1987).
- McBryan and Rosen [1976] O. A. McBryan and J. Rosen, Existence of the critical point in field theory, Commun. Math. Phys. 51, 97 (1976).
- Ruelle [1975] D. Ruelle, Equilibrium statistical mechanics of one-dimensional classical lattice systems, Lecture Notes in Physics 39, 449 (1975).
- Dobrušin [1974] R. L. Dobrušin, Analyticity of correlation functions in one-dimensional classical systems with polynomially decreasing potential, Mat. Sb. (N.S.) 94(136), 16 (1974).
- Pfister and Velenik [1999] C.-E. Pfister and Y. Velenik, Interface, surface tension and reentrant pinning transition in the D Ising model, Commun. Math. Phys. 204, 269 (1999).
- Godrèche [2019] C. Godrèche, Condensation for random variables conditioned by the value of their sum, J. Stat. Mech. , 063207 (2019).