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# Peak effect, vortex-lattice melting-line and order–disorder transition in conventional and high-𝑇_𝑐 superconductors

## I Introduction

In type-II superconductors one often observes a peak effect (or fishtail effect) in the critical current density measured as a function of the applied magnetic field $`H`$ at a fixed temperature $`T`$ or as a function of $`T`$ at fixed $`H`$. In conventional low-$`T_c`$ materials this peak effect mainly occurs at magnetic fields $`H`$ near the upper critical field $`H_{c2}(T)`$. In the high-$`T_c`$ $`\mathrm{YBaCuO}`$ crystals, the line of the maximum critical current density, $`H_p(T)`$, frequently lies essentially below the irreversibility line in the $`HT`$ plane, and in sufficiently perfect crystals it exhibits nonmonotonic behavior with temperature. In these perfect crystals the line of maximum current density approaches the flux-line melting line, $`H_m(T)`$, approximately at the so-called upper critical point at which the melting line terminates. When the oxygen deficiency $`\delta `$ in $`\mathrm{YBa}_2\mathrm{Cu}_3\mathrm{O}_{7\delta }`$ increases or the crystal becomes less perfect, the end point tends to the superconducting transition temperature $`T_c`$ at zero magnetic field, while $`H_p(T)`$ becomes a monotonically decreasing function. It is also important to note that at a fixed oxygen concentration the fishtail effect can disappear in pure YBaCuO crystals if the distribution of the oxygen vacancies over the sample becomes uniform.

At present the origin of the peak effect in low-$`T_c`$ and high-$`T_c`$ superconductors is commonly associated with the proliferation of dislocations in the flux-line lattice.  At this first order phase transition induced by quenched disorder in the vortex system, a transformation of a quasiordered Bragg glass  into a disordered amorphous vortex phase occurs. Although different criteria are used for determining the exact position of this transition on the peak-shaped dependence of the critical current density on $`H`$, they all lead to qualitatively similar $`HT`$ phase diagrams, and, for definiteness only, we shall imply below that the phase transition corresponds to the line of the maximum critical current density, $`H_p(T)`$.

A description of this order–disorder phase transition in high-$`T_c`$ superconductors was proposed in Refs.  using the Lindemann criterion. It was implied in these papers that the nature of the order–disorder phase transition is different from the vortex lattice melting transition, but at the critical point both phase transition lines merge. Recently it was refined that the upper critical point does not generally coincide with the point where the order–disorder line reaches the melting curve, and thus the melting line has a portion beyond the intersection point. However, the following should be noted: The results of Refs.  for the disorder–induced transition were obtained in the regime of single vortex pinning when the Larkin pinning length $`L_c`$ is less than $`L_0=ϵa`$ where $`a=(\mathrm{\Phi }_0/H)^{1/2}`$ is the spacing between flux lines, $`\mathrm{\Phi }_0`$ is the flux quantum, and $`ϵ=\lambda _{ab}/\lambda _c1`$ is the anisotropy of the superconductor ($`\lambda _{ab}`$, $`\lambda _c`$ are the London penetration depths in the $`ab`$ plane and along the $`c`$ axis, respectively). When $`T`$ increases, the length $`L_c`$ should exceed $`ϵa`$ at some temperature which lies on the boundary of the single vortex pinning regime. At higher temperatures the disorder was completely neglected in Refs. , and only the melting line of the ideal lattice was derived. Thus, the behavior of the order–disorder line was not actually investigated in the high temperature region, and its connection with the melting line was not established. Besides this, it has remained unclear why the proliferation of dislocations in the vortex lattice of high-$`T_c`$ and low-$`T_c`$ superconductors leads to different phase diagrams.

In the present paper we consider the order–disorder transition line in the high temperature region and obtain the point where the vortex lattice melting and the order–disorder transition lines merge. It turns out that for a given model of the vortex pinning, the resulting $`HT`$ phase diagram is determined only by the Ginzburg number $`Gi`$, which characterizes the thermal fluctuations, and by a parameter $`j_c(0)/j_0(0)`$ that describes the strength of the quenched disorder in the flux-line lattice at $`T=0`$ ($`j_0`$ is the depairing current density and $`j_c`$ is the critical current density in the single vortex pinning regime; both are in the $`ab`$ plane). For different values of these parameters, phase diagrams are obtained which are similar to those observed in experiments for low-$`T_c`$ and high-$`T_c`$ superconductors. Thus, the results of this paper provide a unified approach for analyzing $`HT`$ phase diagrams of various superconductors.

In this paper we consider only magnetic fields exceeding considerably the lower critical field $`H_{c1}`$ and thus disregard the reentrant behavior of the melting transition and do not distinguish between the magnetic field $`H`$ and the magnetic induction $`B`$. Besides this, we deal only with anisotropic three-dimensional superconductors, neglecting completely the decoupling of the superconducting layers. We also assume that $`𝐇`$ is directed along the $`c`$ axis. This assumption simplifies the analysis of the problem, though our final Eqs. (19) to (25) are valid for any direction of the magnetic field.

## II Lindemann criterion

We begin with simple estimates which show that the Lindemann criterion does define the condition for proliferation of dislocations in the flux-line lattice at the order–disorder transition. Consider a dislocation network in the lattice. Let a unit cell of this network have the dimensions $`R_d`$ and $`L_d`$ in the transverse and longitudinal directions to $`𝐇`$, respectively. A comparison of tilt and shear elastic energies yields that $`L_d/R_d[c_{44}(1/R_d,1/L_d)/c_{66}]^{1/2}>1`$ where $`c_{66}`$ and $`c_{44}(k_{},k_{})`$ are the shear and nonlocal tilt moduli of the flux-line lattice. The energy cost for the creation of a dislocation cell is of the order of

$`E_d\epsilon _0L_d`$

where $`\epsilon _0=(\mathrm{\Phi }_0/4\pi \lambda _{ab})^2`$ and $`\lambda _{ab}`$ is the London penetration depth for currents in the $`ab`$ plane. On the other hand, the elastic energy in the volume $`R_d^2L_d`$ is estimated as

$`E_{el}c_{66}L_du^2(R_d,L_d)`$

where $`u^2(R,L)`$ is the correlation function determining the relative displacement of points in the lattice with quenched disorder,

$`u(R,L)[𝐮(R,L)𝐮(0,0)]^2^{1/2}.`$

Here $`𝐮`$ is the transverse displacement of a flux line, $`\mathrm{}`$ means averaging over both thermal and quenched disorder, the first coordinate $`R`$ in $`𝐮(R,L)`$ indicates the position of the flux line in the plane normal to the applied magnetic field, while the second coordinate $`L`$ defines the position of a point on the flux line. Comparing $`E_d`$ and $`E_{el}`$ with account of $`c_{66}\epsilon _0/a^2`$, one arrives at the conclusion that a dislocation network can exist in the lattice if $`u(R_d,L_d)a`$. In other words, $`R_d`$ should be greater than the so called positional correlation length $`R_a`$ within which typical relative vortex displacements are of the order of the lattice spacing $`a`$. However, this is only a necessary but not sufficient condition for the existence of dislocations. Displacements generated by the dislocations facilitate a better adjustment of the vortex lattice to the quenched disorder. The relative deformation of the lattice produced by the dislocations is of the order of $`a/R_d`$. Therefore, the smaller $`R_d`$ is the greater is the gain $`\delta E_{pin}`$ in pinning energy $`E_{pin}`$. Thus, the network first appears at the smallest possible $`R_d`$, and we arrive at the result $`R_dR_a`$ (and $`L_dL_a`$) obtained in Ref. . The relative magnitude of the gain, $`\delta E_{pin}/E_{pin}`$ is determined by the ratio $`a/R_a`$. Hence, for this magnitude to become of the order of unity, $`R_a/a`$ should decrease to a certain constant $`C`$,

$`{\displaystyle \frac{R_a}{a}}=C.`$

This criterion for the appearance of dislocations in the flux-line lattice was obtained in Refs.  (see also Ref. ), and is equivalent to the condition :

$$u^2(a,0)=c_L^2a^2,$$
(1)
where $`c_L`$ is the phenomenological Lindemann constant. This immediately follows from the fact that the ratio of $`u(R_a,0)`$ to $`u(a,0)`$ \[i.e., $`a/u(a,0)`$\] is a function of $`R_a/a`$. Finally, since $`u(a,0)=u(0,L_0)`$ at $`L_0=ϵa`$, one more form of the Lindemann criterion exists:

$$u^2(0,L_0)=c_L^2a^2.$$
(2)
It is just this form that was used in Refs. .

Strictly speaking, the values of the constants $`C`$ and $`c_L`$ may depend on whether the order–disorder transition occurs in the single vortex pinning region or in the region of bundle pinning. However, to understand the essence of the matter, we shall use the simplest approximation: $`c_L`$ will be considered as the same constant for the various regimes of pinning.

## III The order–disorder line. Simplified approach

As well-known, thermal fluctuations of the flux-line lattice lead to a smoothing of the pinning potential and thereby affect the pinning. This thermal depinning is especially important for high-$`T_c`$ superconductors. However, to elucidate possible types of the order–disorder transition line, in this section we completely disregard the thermal fluctuations. The influence of the thermal depinning on the order–disorder line will be analyzed in Sec. IV.

### A Region of single vortex pinning

As has been mentioned above, the order–disorder line $`H_{dis}(T)`$ was studied  inside the single-vortex pinning regime where the Larkin pinning length $`L_c`$ is less than $`L_0=ϵa`$. Since $`L_0>L_c`$, formulas of the random manifold regime for a single vortex are applicable to calculate the displacement correlation $`u(0,L_0)`$,

$$u(0,L_0)\xi (L_0/L_c)^\zeta ,$$
(3)
where $`\xi `$ is the coherence length in the $`ab`$ plane and $`\zeta `$ is the roughness exponent for a flux line. In Ref.  the value $`\zeta 3/5`$ was used, while $`\zeta 5/8`$ in Ref. . Inserting Eq. (3) into Eq. (2), we obtain after simple manipulations:

$$H_{dis}=\frac{\mathrm{\Phi }_0c_L^2}{\xi ^2}\left(\frac{c_LL_c}{ϵ\xi }\right)^\alpha ,$$
(4)
where $`\alpha =2\zeta /(1\zeta )3`$. Eq. (4) coincides with the appropriate formulas of Refs. . For Eq. (4) to be self-consistent, it is necessary to verify that $`L_0>L_c`$ at $`H=H_{dis}`$ or in other words $`H_{dis}<H_{sv}`$ where $`H_{sv}=\mathrm{\Phi }_0ϵ^2/L_c^2`$ is the boundary of the single vortex pinning regime. This condition yields:

$$\frac{ϵ\xi }{L_c}>c_L.$$
(5)
If the inequality (5) is not fulfilled, Eq. (4) is not valid to describe $`H_{dis}`$.

The parameter $`ϵ\xi /L_c`$ generally depends on the temperature $`T`$. For example, according to simple estimates given in Appendix A, Eqs. (A3), (A7), it decreases with $`T`$ and reaches zero at $`T=T_c`$. Moreover, its decrease becomes especially pronounced if the thermal depinning is taken into account. \[In this case the single vortex collective pinning length $`L_c`$ increases sharply when $`T`$ exceeds the characteristic pinning energy $`\stackrel{~}{T}_{dp}^s(T)`$, see Appendix A.\] Thus, even if $`ϵ\xi (0)/c_LL_c(0)>1`$, the order–disorder line $`H_{dis}(T)`$ reaches the boundary of the single vortex pinning regime, $`H_{sv}(T)`$, at some temperature $`T_1`$ defined by the condition

$$\frac{ϵ\xi (T_1)}{L_c(T_1)}=c_L,$$
(6)
and at $`T>T_1`$, Eq. (4) fails.

It is worth noting that the parameter $`ϵ\xi /L_c`$ appearing in Eqs. (4) - (6) and formulas given below characterizes the strength of the disorder in the flux-line lattice and is expressed through the critical current density $`j_c`$ in the single vortex pinning regime,

$$\frac{ϵ\xi }{L_c}=\left(\frac{j_c}{j_0}\right)^{1/2},$$
(7)
where $`j_0`$ is the depairing current density.

### B High temperature region

At $`T>T_1`$ the order–disorder transition line lies above $`H_{sv}(T)`$. In this region of the $`HT`$ plane small-bundle and large-bundle regimes of pinning occur. Hence the transverse collective pinning length $`R_c`$ exceeds $`a`$, and to find $`u(a,0)`$, the results may be used, which were obtained within the framework of the perturbative approach of Larkin and Ovchinnikov. We have:

$$u^2(a,0)\xi ^2(L_0/L_c)^3\left(\frac{1h_{sv}}{1h}\right)^{3/2},$$
(8)
where $`L_0=ϵa`$, $`hH/H_{c2}`$, $`h_{sv}H_{sv}/H_{c2}`$, the upper critical field $`H_{c2}=\mathrm{\Phi }_0/2\pi \xi ^2`$, and $`L_c`$ is the single vortex collective pinning length. Note that Eq. (8) differs from formula (4.17) of Ref.  by the last factor containing $`h`$ and $`h_{sv}`$. This factor takes into account the possibility that $`1h`$ is small; in Ref.  the correlation function $`u^2(R,L)`$ is given without taking account of this possibility. The origin of this factor is the following. The quantity $`u^2`$ is proportional to $`nf_{pin}^2\lambda _{ab}/Hc_{66}^{3/2}`$. When $`h1`$, one has $`\lambda _{ab}(1h)^{\frac{1}{2}}`$, $`c_{66}(1h)^2`$ (see Ref. ), while $`f_{pin}^2\epsilon _0^2(1h)^2`$ (see Ref.  and also Appendix A). The combination of these factors gives Eq. (8), in which the additional constant factor $`(1h_{sv})^{3/2}`$ has been introduced to provide a smooth crossover of this expression to the appropriate formula for the single vortex pinning regime at $`h=h_{sv}`$.

Inserting formula (8) into Eq. (1), we obtain an equation for $`h_{dis}=H_{dis}/H_{c2}`$,

$$h_{dis}(1h_{dis})^3=2\pi c_L^2\left(\frac{ϵ\xi }{c_LL_c}\right)^6(1h_{sv})^3,$$
(9)
where $`h_{sv}=H_{sv}/H_{c2}=2\pi (ϵ\xi /L_c)^2`$ and the right hand side depends only on the temperature. Note that at $`T=T_1`$, when $`ϵ\xi /L_c=c_L`$, one has $`h_{dis}(T_1)=2\pi c_L^2=h_{sv}(T_1)`$, in agreement with Eq. (4). A simple analysis shows that $`2\pi c_L^2`$ should be greater than $`0.25`$ but less than $`1`$ (i.e., $`0.2c_L0.4`$) for Eq. (9) to have a solution at $`TT_1`$. If $`c_L<0.2`$, the order–disorder line terminates at $`T=T_1`$, which is impossible. On the other hand, if $`c_L>0.4`$, one finds from Eq. (9) that $`h_{dis}>1h_{sv}`$, i.e., the root of the equation lies in the upper region of single vortex pinning where Eq. (9) is not valid. For this reason, in the following we assume the conditions $`0.2c_L0.4`$ to be fulfilled and, for definiteness, take $`c_L=0.25`$ in the subsequent calculations.

### C Types of phase diagrams

We begin the analysis of phase diagrams with the case

$`D>c_L`$

where $`Dϵ\xi (0)/L_c(0)`$ is the value of the parameter $`ϵ\xi /L_c`$ at $`T=0`$. Figure 1 shows the line $`H_{dis}(T)`$ calculated by solving Eq. (9) (for $`H_{dis}>H_{sv}`$) and Eq. (4) (for $`H_{dis}<H_{sv}`$). In the construction of this figure, as well as in all examples below, we use $`H_{c2}(T)=H_{c2}(0)[1(T/T_c)^2]`$ and $`\alpha =3`$ (i.e., $`\zeta =3/5`$). Besides this, taking into account the formula (A13) of Appendix A, we employ the following simple approximation for the parameter $`ϵ\xi /L_c`$:

$$\frac{ϵ\xi (T)}{L_c(T)}Dg_0(t)$$
(10)
with

$$g_0(t)=(1t^2)^{1/2},$$
(11)
where $`tT/T_c`$. The increase of $`H_{dis}`$ and its subsequent maximum are seen in the vicinity of $`T_1`$. As to $`h_{dis}`$, this normalized quantity increases monotonically above $`T_1`$. When $`1h_{dis}1`$, an approximate solution of Eq. (9) is:

$$\frac{H_{dis}(T)}{H_{c2}(T)}1\left(\frac{2\pi }{c_L^4}\right)^{1/3}\left(\frac{ϵ\xi }{L_c}\right)^2.$$
(12)
This formula shows that and how $`H_{dis}(T)`$ approaches $`H_{c2}(T)`$, which is also seen in Fig. 1. Interestingly, according to this formula, the order–disorder transition occurs outside the upper region of single vortex pinning, but its position correlates with the boundary of this region: $`[1h_{dis}(t)]/[1h_{sv}(t)]=(2\pi c_L^2)^{2/3}>1`$. It should be also noted that in the case under study (i.e. when the thermal fluctuations are negligible) the mean-field $`H_{c2}(T)`$ practically coincides with the melting line $`H_m(T)`$. Thus, we obtain for $`D>c_L`$ that in the high temperature region a peak effect occurs near the melting line, while with decreasing $`T`$ the position of the peak in $`j_c(H)`$ shifts downwards from this line. This situation is reminiscent of that of perfect high-$`T_c`$ superconductors.

In this context it is also useful to note the following: The density of the dislocations in the vortex liquid is essentially higher than in the disordered vortex solid phase near the order–disorder transition. However, if in the $`HT`$ plane the order–disorder transition occurs sufficiently below the melting line of the clean superconductor, then in the disordered solid phase, at the field corresponding to the melting transition, the density of the dislocations generated by the quenched disorder may become of the order of the density characteristic for the liquid phase. In this case the melting transition disappears. In other words, the melting line $`H_m(T)`$ terminates when $`H_{dis}(t)`$ deviates from it appreciably.

If the strength of the disorder is sufficiently small,

$`D{\displaystyle \frac{ϵ\xi (0)}{L_c(0)}}<c_L,`$

the order–disorder line lies entirely outside the region of single vortex pinning, Fig. 2, and is described by Eq. (9) at any $`T<T_c`$, while Eq. (4) is not valid at all. In the special situation when $`D`$ is markedly less than $`c_L`$, a peak effect occurs near $`H_{c2}(T)`$ and its position in the $`HT`$ plane is approximately given by Eq. (12). In this case the resulting phase diagram looks like that of low-$`T_c`$ superconductors. The transition from one type of phase diagram to the other occurs when $`D=c_L`$.

It has been assumed in this section that the parameter $`ϵ\xi /L_c`$ decreases with increasing $`T`$. However, the $`\delta T_c`$ pinning (due to spatial variations of $`T_c`$) leads to an increasing function $`g_0(t)`$, see Eq. (A14) in Appendix A. In this case, if $`D>c_L`$, the formula (4) remains valid up to $`T_c`$. But if $`D<c_L`$, a temperature $`T_0`$ exists, determined by the condition

$`{\displaystyle \frac{ϵ\xi (T_0)}{L_c(T_0)}}=c_L,`$

and at $`T<T_0`$ equation (9) should be used, while at $`T>T_0`$ formula (4) holds. In other words, we have a situation which is opposite to that described above. In Fig. 3 the order–disorder line is shown for the case when $`g_0(t)`$ is given by Eq. (A14). Note that in this case, according to formula (4), one has $`H_{dis}(1t^2)^{3/2}`$ in the high temperature region of the phase diagram. This result qualitatively agrees with the measurements on $`\mathrm{YBa}_2\mathrm{Cu}_3\mathrm{O}_{7\delta }`$ crystals when $`\delta `$ is not small, or when the crystals are not too perfect.

## IV The order–disorder line with account of thermal fluctuations

It is well-known that thermal fluctuations of the flux-line lattice play an important role in high-$`T_c`$ superconductors. In particular, for this reason the flux-line lattice melts essentially below the mean-field $`H_{c2}`$ line. In this section we study the influence of thermal fluctuations on the order–disorder line.

Thermal fluctuations lead to a smoothing of the pinning potential and thus increase the Larkin length $`L_c`$. The length $`L_c`$ specifies the boundary of the single vortex pinning region and it enters the key parameter of the collective pinning theory, $`ϵ\xi /L_c`$. Here we reserve the notation $`L_c`$ for the true length renormalized by the fluctuations, while the Larkin length defined without account of the fluctuations will be denoted below as $`L_c^0`$. Note that just $`L_c^0`$ has been used in Sec. III, and just this quantity is described by Eq. (10). Apart from increasing $`L_c`$, the thermal fluctuations of the flux-line lattice also modify the correlation function (3) as follows:

$$u^2(0,L_0)r_p^2(L_0/L_c)^{2\zeta },$$
(13)
where $`r_p^2=\xi ^2+u_T^2`$, and $`u_T`$ is the magnitude of these fluctuations, which depends on the temperature and on the magnetic field. It is implied in Eq. (13) that $`L_0=ϵa>L_c`$. As to the correlation function (8), the collective pinning theory gives

$$u^2(a,0)\xi ^2(L_0/L_c^0)^3\left(\frac{1h_{sv}}{1h}\right)^{3/2}\left(\frac{\xi }{r_p}\right)^4$$
(14)
for $`L_0<L_c`$, i.e. at $`h>h_{sv}=2\pi (ϵ\xi /L_c)^2`$.

Since $`u(a,0)=u(0,L_0)`$, the correlation functions (13) and (14) must coincide at $`L_0=L_c`$ (or equivalently at $`h=h_{sv}`$). This condition yields

$$L_c(t)=L_c^0(t)\frac{r_p^2(t,H_{sv}(t))}{\xi ^2(t)}.$$
(15)
In fact, formula (15) is an equation for $`L_c`$ since we have the relationship $`H_{sv}=\mathrm{\Phi }_0ϵ^2/L_c^2`$. This equation enables us to find $`L_c(t)`$, and thus $`H_{sv}(t)`$, self-consistently.

To proceed, we have to estimate the magnitude of thermal displacements of the lattice, $`u_T`$, relative to its equilibrium position. In the case of the ideal vortex lattice, $`u_T`$ was calculated in many papers; see, e.g., Refs. . This magnitude, as well as the correlation functions (8) and (14), depends on the elastic moduli of the lattice. However, in deriving Eqs. (8), (14) the contribution associated with the compression modulus $`c_{11}`$ was neglected. Hence, it is consistent to use the same approximation in the calculation of $`u_T^2`$. This simplifies the appropriate formula for $`u_T^2`$, and we obtain

$$u_T^2\xi ^2t\left(\frac{Gi}{1t^2}\right)^{1/2}h^{1/2}f(h),$$
(16)
where $`h=H/H_{c2}(t)`$, $`t=T/T_c`$, $`H_{c2}(t)=H_{c2}(0)(1t^2)`$, $`Gi`$ is the Ginzburg number,

$`Gi={\displaystyle \frac{1}{2}}\left({\displaystyle \frac{T_c}{H_c^2(0)ϵ\xi ^3(0)}}\right)^2,`$

which characterizes the strength of the thermal fluctuations, and $`H_c`$ is the thermodynamic magnetic field of the superconductor. The function $`f(h)`$ has the form:

$$f(h)=\frac{2\beta _A}{1h}\frac{[1+(1+\stackrel{~}{c})^2]^{1/2}1}{\stackrel{~}{c}(1+\stackrel{~}{c})},$$
(17)
with $`\stackrel{~}{c}=0.5[\beta _A(1h)]^{1/2}`$, and $`\beta _A=1.16`$.

The quenched disorder changes $`u_T^2`$. However, when the transverse collective pinning length $`R_c`$ is considerably greater than $`a`$, the above result for the ideal lattice is a good approximation. This is due to the fact that the main contribution to $`u_T`$ results from the thermal fluctuations with short wavelengths ($`k_{}1/a`$), while the quenched disorder essentially distorts the lattice only on the scale $`R_c`$. Thus, we may use Eq. (16) in the case of the nonideal lattice if bundle pinning occurs. But in the single vortex pinning regime the influence of the disorder is essential, and one has $`u_T^2L_c`$. To account for this result, we introduce an additional factor $`L_c/ϵa`$ in the formula (16) and thus obtain

$$u_T^2\xi ^2t\left(\frac{Gi}{1t^2}\right)^{1/2}h_{sv}^{1/2}f(h)$$
(18)
in the single vortex pinning region at $`h<h_{sv}`$.

Inserting expression (16) into formula (15) and using definition (10) for $`ϵ\xi /L_c^0`$, we obtain the following equation for $`h_{sv}=H_{sv}/H_{c2}`$:

$$h_{sv}^{1/2}(t)=(2\pi )^{1/2}Dg_0(t)t\left(\frac{Gi}{1t^2}\right)^{1/2}f(h_{sv}(t)).$$
(19)
With increasing $`t`$ the function $`h_{sv}(t)`$ reaches zero at some $`t_{dp}^s<1`$, and Eq. (19) is valid at $`tt_{dp}^s`$. In the region $`t>t_{dp}^s`$ the length $`L_c`$ is infinite in size, and the single vortex pinning regime is absent, i.e., $`h_{sv}(t)=0`$ at $`t>t_{dp}^s`$. The value of $`t_{dp}^s`$ is found by equating $`h_{sv}`$ to zero in formula (19):

$$t_{dp}^s=\frac{(2\pi )^{1/2}D}{Gi^{1/2}f(0)}g_0(t_{dp}^s)[1(t_{dp}^s)^2]^{1/2}.$$
(20)
It may be verified that the right hand side of Eq. (20) coincides (up to a numerical factor of the order of unity) with the dimensionless characteristic pinning energy $`\stackrel{~}{T}_{dp}^s/T_c`$, see Appendix A. Thus, in agreement with physical considerations, we obtain that the essential renormalization of $`L_c`$ occurs at such temperatures $`T`$ that $`T\stackrel{~}{T}_{dp}^s(T)`$.

It should be noted that our result for $`L_c`$ ($`L_c\mathrm{}`$ at $`tt_{dp}^s`$) differs in some respects from that presented in Ref.  where $`L_c`$ increases exponentially at $`tt_{dp}^s`$. However, in the framework of our approximation, $`H_{c1}=0`$, we may consider $`L_c`$ as infinite if it becomes of the order of $`\lambda `$. Hence, the difference between the results is, in fact, small. But our approach provides the continuity of the correlation functions (13), (14) at $`h=h_{sv}`$.

Equation (19) specifies the single vortex pinning (SVP) region existing at relatively low magnetic fields \[$`0<h<h_{sv}(t)`$\]. However, formulas (14), (16) enable one to find also the upper region in which the vortex system returns to this type of pinning again. The appropriate equation results from the condition $`u(a,0)=r_p`$, and has the following form:

$`(1h)\left[h^{1/2}+t\left({\displaystyle \frac{Gi}{1t^2}}\right)^{1/2}f(h)\right]^2=`$ (21)
$`2\pi \left(Dg_0(t)\right)^2[1h_{sv}(t)],`$ (22)
As might be expected, at $`h=h_{sv}`$ this equation goes over into Eq. (19). However, in a certain temperature interval it has two additional real roots which form the boundary of the upper SVP region, $`h_{sv}^{up}`$ (see Fig. 5 below). Here we do not consider this issue in detail, but qualitatively describe the effect of thermal fluctuations on the shape of the upper SVP region specified above without their account. Although the softening of the vortex lattice near $`H_{c2}`$ is favorable for single vortex pinning, this softness also leads to an increase of the thermal fluctuations $`u_T`$, which reduces the strength of pinning. As a result, the upper region does not touch $`H_{c2}(t)`$ except for the point $`t=0`$ (at $`t>0`$ and $`H=H_{c2}`$ we have $`u_T=\mathrm{}`$). Besides this, since $`u_T`$ increases with $`t`$, the upper region does not extend to $`T_c`$. Of course, one should realize that the part of the boundary of this SVP region lying above the vortex lattice melting curve has only formal meaning, since it does not account for the vanishing shear modulus at the melting. On the other hand, it is quite possible that the sharp melting transition disappears when the melting line enters the upper SVP region (or even before it; see Sec. V).

Inserting expressions (13) and (18) in formula (2), we arrive at an equation for $`h_{dis}=H_{dis}/H_{c2}`$ which generalizes formula (4):

$`h_{dis}\left[1+t\left({\displaystyle \frac{Gi}{1t^2}}\right)^{1/2}{\displaystyle \frac{f(h_{dis})}{(h_{sv}(t))^{1/2}}}\right]^{1/(1\zeta )}=`$ (23)
$`2\pi c_L^2\left({\displaystyle \frac{2\pi c_L^2}{h_{sv}(t)}}\right)^{\alpha /2}.`$ (24)
This equation is valid in the single vortex pinning regime when $`h_{dis}h_{sv}`$. For example, if $`g_0(t)`$ is a decreasing function of $`t`$, the order–disorder line lies in the single vortex pinning region and is described by Eq. (22) at $`t<t_1`$. In the case $`D>c_L`$ the temperature $`t_1`$ is found from the equation:

$$h_{sv}(t_1)=2\pi c_L^2\left[1+t\left(\frac{Gi}{1t^2}\right)^{1/2}\frac{f(h_{sv}(t))}{(h_{sv}(t))^{1/2}}\right]_{t=t_1}^1,$$
(25)
which generalizes condition (6). At $`D<c_L`$ the line is entirely outside this region, and thus one has $`t_1=0`$. If $`g_0(t)`$ is an increasing function of temperature, more complicated situations can occur.

Inserting formulas (14) and (16) into relation (1), we obtain the equation for $`h_{dis}(t)`$:

$`h_{dis}(1h_{dis})^3\left[1+t\left({\displaystyle \frac{Gi}{1t^2}}\right)^{1/2}{\displaystyle \frac{f(h_{dis})}{(h_{dis})^{1/2}}}\right]^4=`$ (26)
$`2\pi c_L^2\left({\displaystyle \frac{Dg_0(t)}{c_L}}\right)^6[1h_{sv}(t)]^3,`$ (27)
which generalizes Eq. (9). This equation is valid in the bundle pinning region.

Let us now present formulas for the melting line which is determined by the Lindemann criterion, $`u_T^2=c_L^2a^2`$, different from Eqs. (1), (2). This well-known empirical criterion based on the magnitude of the thermal fluctuations, was justified in Ref.  for the case of the ideal vortex lattice. According to this paper, different physical mechanisms lead to the proliferation of dislocations at the vortex lattice melting and at the order–disorder transition. While the disorder–induced transition is driven by an adjustment of the flux-line lattice to the disorder, the thermal melting is governed by the entropy gain associated with the creation of dislocations. Hence, the Lindemann constant $`c_L`$ for the melting may, in principle, differ from that used in Eqs. (22)-(24). However, for the sake of simplicity we take these constants $`c_L`$ as equal in the following analysis. Thus, if the melting line $`h_m(t)=H_m/H_{c2}`$ does not intersect $`h_{sv}(t)`$, it is described by the equation:

$$t\left(\frac{Gi}{1t^2}\right)^{1/2}h_m^{1/2}f(h_m)=2\pi c_L^2.$$
(28)
But if the melting line lies below $`h_{sv}(t)`$, an additional factor $`(h_m/h_{sv})^{1/2}`$ should be inserted on the left hand side of Eq. (25), cf. Eqs. (16) and (18). Finally, we note that in expression (25), as well as in Eqs. (16), (18)-(24), the factor $`1t^2`$ represents the temperature dependence of the upper critical field, $`1t^2=H_{c2}(t)/H_{c2}(0)`$. Thus, if another form of this dependence is implied, the appropriate modification of all these equations is straightforward.

Summing up, we may state the following: For given $`g_0(t)`$, equations (19)-(25) enable us to calculate the order–disorder line $`h_{dis}(t)`$, the melting line $`h_m(t)`$ and the boundaries of the single vortex pinning regime $`h_{sv}(t)`$, $`h_{sv}^{up}(t)`$ with account of the thermal fluctuations. The function $`g_0(t)`$ in Eq. (10) is determined by the pinning mechanism and by the temperature dependences of $`\xi `$ and $`\lambda `$, see Appendix A.

## V Analysis of phase diagrams

It is important to emphasize that for given $`g_0(t)`$ Eqs. (19)-(25) depend only on two parameters: the strength of quenched disorder, $`D=ϵ\xi (0)/L_c(0)`$, and the strength of the thermal fluctuations, $`Gi`$. In this sense, the equations and figures of Sec. III correspond to the limiting case $`Gi0`$. We consider now new features of the phase diagram which appear in the real situation of finite $`Gi`$.

### A Numerical results

An example of the phase diagram in the case $`D>c_L`$ is shown in Fig. 4. Note that the order–disorder line terminates at some temperature $`t_e<1`$. This termination is associated with an increase of the thermal fluctuations and thus with an enhanced smoothing of the pinning potential when the order–disorder line approaches $`H_{c2}`$. Interestingly, the end point lies near the so-called depinning line where $`u_T^2=\xi ^2`$. Another new feature of the phase diagram is the intersection of the melting and the order–disorder lines. Thus, we obtain the point where both lines merge. It is seen from Fig. 4 that at this point the position of the critical current peak begins to shift sharply downward from the melting curve, in agreement with the experimental data. Hence, as was mentioned in Sec. III C, the upper critical point for the melting is likely to occur somewhere nearby. The portion of the order–disorder line lying above the melting curve has no physical meaning since the density of dislocations in the liquid phase is already higher than in the disordered solid phase. Note also that the rise of $`H_{dis}(t)`$ at $`T>T_1`$ becomes considerably steeper than in the case $`Gi=0`$.

The intersection of the order–disorder line with the melting curve occurs also for $`D<c_L`$. In this case, when $`Gi`$ increases, the decrease of $`H_{dis}`$ with $`T`$ diminishes, and eventually $`H_{dis}`$ becomes an increasing function of $`t`$, see Fig. 5. Therefore, if $`Gi10^2`$ (this value is typical for $`\mathrm{YBaCuO}`$ crystals), the temperature behavior of the order–disorder line is similar to that obtained for $`D>c_L`$, and the phase diagrams in both these cases are of the same type.

In Fig. 5 we also show the upper region of single vortex pinning. It is important to note that the intersection point of the order–disorder line and the melting line occurs clearly before the melting curve enters this region, and so at the intersection point the transverse collective pinning length $`R_c`$ and the positional correlation length $`R_a`$ (the dislocation spacing) both considerably exceed the flux-line spacing $`a`$. This fact justifies the assumed weak influence of quenched disorder on the vortex lattice melting and the application of Eq. (24) up to the intersection point.

If the parameter $`D`$ increases, e.g., as a result of irradiation or of reduction of the oxygen content in $`\mathrm{YBa}_2\mathrm{Cu}_3\mathrm{O}_{7\delta }`$ crystals (see Appendix A), then the order–disorder line shifts down, while the temperature of the intersection point (and thus the temperature of the upper critical point for the melting line) increases, Fig. 6. These results are in agreement with the experimental findings for $`\mathrm{YBa}_2\mathrm{Cu}_3\mathrm{O}_{7\delta }`$ crystals. However, although the obtained results qualitatively describe the phase diagram of these crystals and its evolution with varying $`D`$, it should be emphasized that the intersection point does not reach $`T_c`$ at reasonable values of the disorder parameter $`D`$.

Consider now the case when $`g_0(t)`$ increases with $`t`$. This situation occurs in the model of $`\delta T_c`$ pinning, see Appendix A. The appropriate phase diagrams are presented in Figs. 7-9. It is important to note the following: At sufficiently strong disorder, the line $`H_{dis}(t)`$ monotonically decreases with temperature and practically reaches $`T_c`$. When the strength of the disorder decreases, the order–disorder line exhibits nonmonotonic behavior with $`t`$, and the temperature of the intersection point, $`t_i`$, goes down. Thus, in contrast to the case of a decreasing function $`g_0(t)`$, the model of $`\delta T_c`$ pinning correctly reproduces all the features of the experimental data for $`\mathrm{YBa}_2\mathrm{Cu}_3\mathrm{O}_{7\delta }`$ crystals. In particular, the results presented in Fig. 8 closely resemble the development of the order–disorder line with variations of the oxygen deficiency $`\delta `$, see, e.g., Fig. 9 in Ref. .

The results of this section may also provide an explanation of the findings obtained in Ref. . It was shown in this paper that the flux-line pinning in pure $`\mathrm{YBa}_2\mathrm{Cu}_3\mathrm{O}_{7\delta }`$ crystals is mainly due to a nonuniform distribution of oxygen vacancies over the sample. Changing the conditions of annealing of the sample, Erb et al. changed this distribution at a fixed $`\delta `$. When the distribution became more homogeneous, the fishtail effect disappeared. Since the spatial fluctuations in the density of oxygen vacancies strengthen the $`\delta T_c`$ pinning, we get an additional confirmation of the hypothesis that this type of pinning plays the main role in not too perfect $`\mathrm{YBaCuO}`$ crystals, and so the fishtail effect exists up to high temperatures, as shown in Figs. 7, 8 for large $`D`$. When, after annealing, the crystal becomes more perfect, and the above-mentioned spatial fluctuations are reduced, the value of the parameter $`D`$ appears to decrease considerably. (Moreover, it is conceivable that some other type of pinning begins to dominate.) Thus, we arrive at the situation when a fishtail effect is absent, at least in the region of not too high magnetic fields, as it follows from the data shown in Figs. 6 and 8 for small $`D`$.

Finally, we briefly describe the case of small Ginzburg numbers which occurs for conventional superconductors. In this case the temperatures $`t_{dp}^s`$ and $`t_i`$ are practically equal to unity, the melting line almost coincides with $`H_{c2}(t)`$, and the phase diagrams tend to those shown in Figs. 1-3. Thus, the results of the simplified approach of Sec. III can be well applied to such superconductors.

### B Approximate formulas. Discussion

We now present analytical results which give some insight into the origin of the above-mentioned features of the phase diagrams. Let us start with the melting line. If $`[Gi/(1t^2)]^{1/2}2\pi c_L^2`$, the normalized field $`h_m=H_m/H_{c2}`$ is close to unity, and we obtain from Eq. (25)

$$1h_m\left(\frac{f_1(1)}{2\pi c_L^2}\right)^{2/3}t^{2/3}\left(\frac{Gi}{1t^2}\right)^{1/3},$$
(29)
where

$`f_1(h)(1h)^{3/2}f(h)`$

is defined through the function $`f(h)`$ given by Eq. (17), with $`f_1(1)1.78`$. Equation (26) agrees with the strict result derived for clean superconductors without using the Lindemann criterion. Formula (26) expressed in usual units ($`H_m=h_mH_{c2}`$) means that

$`H_{c2}(t)H_m(t)Gi^{1/3}(1t^2)^{2/3}.`$

The right hand side of this expression is the width of the fluctuation region in not too small magnetic fields, $`hGi`$. In the opposite limiting case when $`f_1(0)[Gi/(1t^2)]^{1/2}2\pi c_L^2`$ \[but the temperature is outside the critical region for zero magnetic field, $`Gi<(1t^2)`$\], the field $`h_m`$ is small, and Eq. (25) yields:

$$h_m=\left(\frac{2\pi c_L^2}{f_1(0)t}\right)^2\frac{1t^2}{Gi},$$
(30)
where $`f_1(0)2.34`$. In fact, this is the well-known result for clean superconductors,

$`H_m(1t)^2.`$

Note that for Eq. (27) to hold in a sufficiently wide temperature region, the Ginzburg number should not be too small. Finally, we point out an interesting feature of Eq. (25) that follows from our numerical analysis. The formula

$$H_m=A(1t^2)^\gamma ,$$
(31)
with some constants $`A`$ and $`\gamma `$ turns out to give a very good fit to $`H_m(t)`$ determined by Eq. (25) in the wide temperature interval $`0.5<t<0.98`$, see Fig. 10. The values of the parameters $`A`$ and $`\gamma `$ depend on $`Gi`$, and the exponent $`\gamma `$ increases with increasing $`Gi`$. In particular, we find $`1.24<\gamma <1.59`$ when $`0.001<Gi<0.01`$. In this connection it is worth noting that formulas of the type of Eq. (28) are widely used to approximate experimental data, and frequently an exponent $`\gamma 4/3`$ is found, which is characteristic for the fluctuation region of a 3D $`XY`$-type phase transition. We emphasize here that a good fit by such formulas does not necessarily mean the existence of a large fluctuation region in zero magnetic field, but may result from the specific form of the expression \[Eq. (25)\] describing the melting line.

In the case of $`\delta T_c`$ pinning the melting line may lie inside the region of single vortex pinning, i.e. the inequality $`h_{sv}>h_m`$ may hold. This occurs if the parameter $`\nu `$ (see Ref. , p. 1218),

$$\nu \frac{(2\pi )^{3/2}D^3}{Gi^{1/2}},$$
(32)
is sufficiently large, $`\nu ^{1/3}1`$. Although in this case the shape of the melting line requires a special investigation and is not discussed in detail here, it should be realized that the sharp melting transition may disappear in this region.

Let us now analyze Eq. (24) which describes the line $`h_{dis}(t)`$ in the region $`h>h_{sv}`$. To understand the behavior of this line, we note the following: The function $`f_1(h)=(1h)^{3/2}f(h)`$ decreases monotonically with increasing $`h`$; its variation in the interval $`0<h<1`$ is not large, $`f_1(1)/f_1(0)0.76`$, and so if one considers $`f_1(h)`$ as constant, $`f_1(h)=f_1(0)f_12.34`$, this leads to a sufficiently accurate approximation in solving Eq. (24). In this approximation Eq. (24) becomes a quadratic equation in the variable $`h_{dis}^{1/2}(1h_{dis})^{3/2}`$, and its solution has the form:

$`h_{dis}^{1/2}(1h_{dis})^{3/2}=`$ (33)
$`F_DF_T+[(F_DF_T)^2(F_T)^2]^{1/2}`$ (34)
where $`F_D`$ and $`F_T`$ are the following functions of temperature:

$`F_D(t)={\displaystyle \frac{(2\pi )^{1/2}[Dg_0(t)]^3}{2c_L^2}}[1h_{sv}(t)]^{3/2},`$ (35)
$`F_T(t)=f_1t\left({\displaystyle \frac{Gi}{1t^2}}\right)^{1/2}.`$ (36)
At $`t=0`$ we have $`F_T(0)=0`$, and equation (30) goes over into Eq.(9). Thus, the effect of thermal fluctuations is reduced to a renormalization of the right hand side of Eq. (9) \[including the change of the function $`h_{sv}(t)`$ according to Eq. (19)\]. Note that the magnitude of this renormalization (i.e., the ratio $`F_T/F_D`$) is mainly determined by the parameter $`\nu ^1`$, see Eq. (29). Interestingly, in contrast to the case of the $`\delta T_c`$ pinning where $`\nu `$ appears as a result of the specific temperature dependence of $`g_0`$, Eq. (A14), we now conclude that the parameter $`\nu `$ characterizes the relative strength of pinning of any type.

It should be emphasized that the right hand side of Eq. (30) is real only if $`F_D2F_T`$. Thus, we find that the order–disorder line terminates at a temperature $`t_e`$ which satisfies the equation

$$F_D(t_e)=2F_T(t_e).$$
(37)
Taking into account Eqs. (16) and (31), it is easy to determine the ratio $`u_T^2/\xi ^2`$ at the end point of the order–disorder line, $`t=t_e`$, $`h=h_{dis}(t_e)`$:

$`{\displaystyle \frac{u_T^2}{\xi ^2}}=F_T(t_e)h^{1/2}(1h)^{3/2}={\displaystyle \frac{F_T(t_e)}{F_T(t_e)}}=1.`$

Hence, this end point lies on the so-called depinning line defined by the condition $`u_T^2=\xi ^2`$, see Figs. 4, 5. It can be also verified that $`t_e`$ is always less than the temperature $`t_{dp}^s`$ determined by Eq. (20).

As has already been mentioned above, only the intersection point of the melting and the order–disorder lines has a physical meaning rather than the end point of $`H_{dis}(t)`$. The temperature of this intersection point, $`t_i`$, can be simply estimated using formulas (26) and (30). Then we arrive at the following equation for $`t_i`$:

$`4\pi c_L^2F_D(t_i)=(1+2\pi c_L^2)^2F_T(t_i),`$

or explicitly,

$$t_i=\nu \frac{[g_0(t_i)]^3(1t_i^2)^{1/2}[1h_{sv}(t_i)]^{3/2}}{f_1(1+2\pi c_L^2)^2}.$$
(38)
This equation suggests that the temperature of the intersection point, $`t_i`$, depends on the parameters $`Gi`$ and $`D`$ mainly through their combination $`\nu `$, Eq. (29). The data of Fig. 11 support this hypothesis, viz., at given $`g_0(t)`$ the temperatures $`t_i`$ calculated for various $`Gi`$ fall on the same curve. Of course, this prediction, as well as any quantitative conclusion based on Eqs. (19)-(25), requires an experimental verification since a number of simplifying assumptions were made above. In particular, $`c_L`$ was assumed to be the same constant for the melting and for the order–disorder transition in all the pinning regimes. On the other hand, according to Eq. (32), the dependence of $`t_i`$ on $`c_L`$ is relatively weak.

Since $`t_i`$ specifies the width of the temperature region where the order–disorder transition exists, the data of Fig. 11 mean that this width is characterized by the parameter $`\nu `$. These data also shed light on the different behavior of $`H_{dis}(t)`$ in Figs. 6 and 8 at large values of $`D`$. To elucidate the results of Fig. 11 and the conclusions made on their basis, let us analyze Eq. (32) in two limiting cases. If $`\nu 1`$, one obtains the following estimate from this equation:

$`t_i0.42(1+2\pi c_L^2)^2\nu .`$

In other words, we have a situation qualitatively similar to that shown in Fig. 6 or in Fig. 8 for the smallest $`D`$. In this case the order–disorder transition occurs only at very low temperatures $`t<t_i`$, while the portion of the melting line at $`t>t_i`$ has a large extension. Note that, according to the estimates of $`Gi`$ and $`D`$ presented in Ref. , such a situation must take place in pure crystals of 2H-NbSe<sub>2</sub>, which were investigated in numerous papers. This conclusion does not contradict the observation of a peak effect in these crystals, since a peak effect can signalize not only the order–disorder transition, as it has been implied so far, but also the vortex lattice melting. Of course, the features of the peak effect may differ in these two cases.

In the opposite limit, $`\nu 1`$, the order–disorder transition reaches $`T_c`$, while the region of “pure” melting ($`t_i<t<1`$) is contracted. This limit just corresponds to conventional superconductors for which $`Gi1`$, see Figs. 1-3. However, in the process of approaching this limit, the evolution of the phase diagram is different for the different models of pinning, i.e., in the cases of Eqs. (A13) and (A14). That is why Figs. 6 and 8 differ from each other at large values of $`D`$. If Eq. (A13) is valid, one finds from Eq. (32) that

$`1t_i^21.5(1+2\pi c_L^2)\nu ^{1/2}.`$

Thus, a large $`\nu `$ is required for the temperature $`t_i`$ to reach unity, see Fig. 6. In the case of Eq. (A14) the right hand side of Eq. (32) already exceeds unity at a finite value $`\nu `$ ($`\nu 1`$), and at such $`\nu `$ the line $`H_{dis}(t)`$ practically reaches the point $`T=T_c`$, $`H=0`$, see Fig. 8 for the largest $`D`$.

### C Upper critical point.

Let us now discuss the upper critical point on the vortex lattice melting curve. In principle, two scenarios are possible. In the first one the upper critical point does not coincide with the intersection point of the melting and the order–disorder lines and is located at a higher magnetic field than this intersection point. In fact, in this case the intersection of the two different phase transition lines occurs, and one of them (the order–disorder line) terminates at the intersection while the other one continues for some distance which seems to depend on the detailed position of the lines in the $`HT`$ plane. This scenario is based on the difference in the density of dislocations, $`\rho `$, generated at the melting and the order–disorder transition: at the melting one has $`\rho a^2`$, while at the order–disorder transition $`\rho R_a^2a^2`$. The position of the upper critical point on the melting line is determined by the condition that the density of dislocations in the disordered vortex solid phase reaches a value typical for the liquid (i.e., the dislocation spacing $`R_a`$ calculated on the melting curve reduces to the vortex spacing $`a`$). It is this scenario that is assumed in our paper.

In the second scenario the upper critical point coincides with the intersection point. In this case the above-mentioned point is ordinary rather than singular for the free energy of the vortex system, since a continuous phase transition separating the disordered vortex solid phase from the vortex liquid does not seem to exist. Thus, there is only one phase transition line which describes both the melting and the order–disorder transitions. This unified line originates from the melting curve of clean superconductors, gradually evolving from it as the strength of the quenched disorder increases. The “upper critical point” is then simply the point where on the melting line $`R_a`$ reduces to $`a`$ and the line experiences a bend. However, for this scenario to occur, the calculated intersection point must lie in the single vortex pinning region. Otherwise, one obtains $`R_a>R_ca`$ at this point and returns to the first scenario.

Our results argue in favor of the first scenario since in the framework of the used approximations the intersection points never reach the upper region of single vortex pinning (see, e.g., Fig. 5). Note that this scenario is also supported by recent numerical simulations.

## VI Conclusions

In this paper, using the Lindemann criterion and results of the collective pinning theory, we have derived equations (19)-(25) which enable one to calculate the order–disorder transition line $`H_{dis}(t)`$ with account of both pinning-caused and thermal fluctuations in the whole temperature interval of its existence. The boundaries of the single vortex pinning region, $`H_{sv}(t)`$, $`H_{sv}^{up}(t)`$, and the melting line $`H_m(t)`$ are also found from these equations. The equations turn out to depend only on the Ginzburg number $`Gi`$ which characterizes thermal fluctuations, on the strength of the quenched disorder, $`D`$,

$`D={\displaystyle \frac{ϵ\xi (0)}{L_c(0)}}=\left({\displaystyle \frac{j_c(0)}{j_0(0)}}\right)^{1/2},`$

and on the function $`g_0(t)`$ defined by the pinning mechanism and by the temperature dependences of $`\xi `$ and $`\lambda `$, Appendix A. For example, the pinning mechanism considered in Ref.  leads to a $`g_0(t)`$ described by Eq. (A13), while the $`\delta T_c`$ pinning results in Eq. (A14). Using our equations one can analyze the phase diagrams of various superconductors. Moreover, our analysis in principle allows to obtain information on the true form of the function $`g_0(t)`$, i.e., on the mechanism of pinning in a superconductor.

At small $`Gi`$ we obtain phase diagrams typical for low-$`T_c`$ superconductors. In this case the obtained results practically coincide with the results of the simplified approach presented in Sec. III. We also analyze phase diagrams with $`Gi10^2`$ since such values of $`Gi`$ are characteristic for the $`\mathrm{YBa}_2\mathrm{Cu}_3\mathrm{O}_{7\delta }`$ superconductors. We consider both a typical case where $`g_0(t)`$ decreases with $`t`$ \[Eq. (A13)\] and a case where $`g_0(t)`$ increases with $`t`$ \[Eq. (A14)\]. In both these cases the obtained results qualitatively describe the phase diagram of $`\mathrm{YBaCuO}`$ crystals and its evolution with varying $`D`$, which can be caused by irradiation or by reduction of the oxygen content in these crystals. However, we find that the model of $`\delta T_c`$ pinning \[Eq. (A14)\] more correctly reproduces all the features of the experimental data for $`\mathrm{YBa}_2\mathrm{Cu}_3\mathrm{O}_{7\delta }`$ crystals.

Our results support the idea that the upper critical point on the melting curve of high-$`T_c`$ superconductors does not generally coincide with the intersection point of the melting and the order–disorder lines (although the distance between them is possibly small). We predict the position of this intersection point in the $`HT`$ plane. We suppose that the temperature corresponding to this point is determined mainly by the parameter $`\nu `$, Eq. (29), i.e., by a combination of the parameters $`D`$ and $`Gi`$.

###### Acknowledgements.

G.P.M. acknowledges the hospitality of the Max-Planck-Institut für Metallforschung, Stuttgart. E.H.B. wishes to acknowledge the hospitality of the Institute for Superconducting and Electronic Materials, University of Wollongong, Australia, where part of this work was performed, and financial support from the Australian Research Council, IREX Program.

## A Estimates of the parameters

The results of this paper are based on the collective pinning theory. It is assumed in this theory that the disorder in the flux-line lattice is generated by point defects of size not exceeding the coherence length $`\xi (0)`$. Here, in the framework of three widely used models of pinning, we express the quantities $`ϵ\xi /L_c`$ and $`\stackrel{~}{T}_{dp}^s`$ through the characteristics of the point defects, viz., their concentration $`n`$ and mean radius $`r_0`$. These expressions enable us to get some idea of the temperature dependences of these quantities and to understand the changes of the phase diagram when $`n`$ and $`r_0`$ are varied.

In the first model, pinning is due to the gain in the condensation energy when a vortex core is located at a defect. This gain $`ϵ_{pin}`$ is of the order $`(H_c^2/8\pi )4\pi r_0^3/3`$, where $`H_c`$ is the thermodynamic magnetic field and $`r_0`$ the radius of the defect. Then one obtains the following estimates for the mean elementary pinning force exerted by one point defect $`f_{pin}ϵ_{pin}/\xi `$:

$$f_{pin}\epsilon _0\left(\frac{r_0}{\xi }\right)^3,$$
(A1)
and for the single vortex collective pinning length $`L_c=n^{1/3}(ϵ^2\epsilon _0/f_{pin})^{2/3}`$ \[with $`ϵ=\lambda _{ab}/\lambda _c`$, $`\epsilon _0=(\mathrm{\Phi }_0/4\pi \lambda _{ab})^2`$\]:

$$L_c\frac{ϵ^{4/3}}{n^{1/3}}\left(\frac{\xi }{r_0}\right)^2.$$
(A2)
Using these estimates, we find the key parameter (7),

$$\frac{ϵ\xi }{L_c}\left(\frac{nr_0^3}{ϵ}\right)^{1/3}\frac{r_0}{\xi },$$
(A3)
and the characteristic pinning energy $`\stackrel{~}{T}_{dp}^s`$ described by the expression $`\xi (f_{pin}^2nL_c\xi ^2)^{1/2}`$,

$$\stackrel{~}{T}_{dp}^sϵ^{2/3}\epsilon _0(nr_0^3)^{1/3}r_0.$$
(A4)
A different mechanism of pinning is due to the scattering of quasiparticles by the defect as calculated in Ref. . A scattering center facilitates deformations of the order parameter up to distances of the order of the zero-temperature coherence length $`\xi (0)`$. Hence, it is energetically advantageous for a vortex core to sit at a scattering center. This mechanism leads to the pinning force $`f_{pin}(H_c^2/8\pi )r_0^2\xi (0)/\xi `$, and we obtain

$`f_{pin}`$ $``$ $`\epsilon _0\left({\displaystyle \frac{r_0}{\xi }}\right)^2{\displaystyle \frac{\xi (0)}{\xi }},`$ (A5)
$`L_c`$ $``$ $`{\displaystyle \frac{ϵ^{4/3}}{n^{1/3}}}\left({\displaystyle \frac{\xi }{r_0}}\right)^{4/3}\left({\displaystyle \frac{\xi }{\xi (0)}}\right)^{2/3},`$ (A6)
$`{\displaystyle \frac{ϵ\xi }{L_c}}`$ $``$ $`\left({\displaystyle \frac{nr_0^3}{ϵ}}\right)^{1/3}\left({\displaystyle \frac{r_0\xi ^2(0)}{\xi ^3}}\right)^{1/3},`$ (A7)
$`\stackrel{~}{T}_{dp}^s`$ $``$ $`ϵ^{2/3}\epsilon _0(nr_0^3)^{1/3}(r_0\xi ^2(0))^{1/3}.`$ (A8)
Strictly speaking, formulas (A5)-(A8) are valid if $`\pi r_0^2\xi (0)n<1`$. This type of pinning is sometimes called $`\delta l`$ pinning. Note that equations (A5)-(A8) and (A1)-(A4) have the same dependences on $`n`$, $`ϵ`$ and temperature. They thus describe two different contributions to one pinning mechanism, with the contribution of Eqs. (A5)-(A8) always dominating when $`r_0<\xi (0)`$.

If the pinning centers in $`\mathrm{YBa}_2\mathrm{Cu}_3\mathrm{O}_{7\delta }`$ are clusters of oxygen vacancies, it is useful to keep in mind that

$$\frac{4\pi }{3}r_0^3n=c\delta ,$$
(A9)
where the constant $`c`$ equals $`2`$ if these clusters are formed by $`\mathrm{YBa}_2\mathrm{Cu}_3\mathrm{O}_{6.5}`$ phase. Thus, when $`r_0`$ decreases at a fixed $`\delta `$, the parameters $`ϵ\xi /L_c`$ and $`T_{dp}^s`$ also decrease.

In high-$`T_c`$ superconductors the pinning can be due to spatial fluctuations in the density of the oxygen vacancies, which results in variations of $`T_c`$ over the sample. One has the following estimates for this $`\delta T_c`$ pinning:

$`{\displaystyle \frac{ϵ\xi }{L_c}}`$ $``$ $`\left({\displaystyle \frac{n\xi }{ϵ}}\right)^{1/3},`$ (A10)
$`\stackrel{~}{T}_{dp}^s`$ $``$ $`ϵ^{2/3}\epsilon _0(n\xi ^4)^{1/3},`$ (A11)
where $`n`$ is the density of oxygen vacancies. This pinning can occur when $`nϵ\xi (0)^3>1`$.

The above equations enable us to estimate the temperature dependence of the quantities $`ϵ\xi /L_c`$ and $`\stackrel{~}{T}_{dp}^s`$. For this purpose, we insert the expressions

$$\frac{\xi (T)}{\xi (0)}=\frac{\lambda (T)}{\lambda (0)}=\left(1\frac{T^2}{T_c^2}\right)^{1/2}$$
(A12)
in the appropriate formulas. In particular, it follows from Eqs. (10), (A3), (A7) that for $`\delta l`$ pinning

$$g_0(t)\frac{1}{D}\left(\frac{ϵ\xi (T)}{L_c(T)}\right)=(1t^2)^{1/2},$$
(A13)
where $`tT/T_c`$, $`Dϵ\xi (0)/L_c(0)`$, while according to Eq. (A10), one finds for $`\delta T_c`$ pinning

$$g_0(t)=(1t^2)^{1/6}.$$
(A14)


text:
# Competitive random sequential adsorption of point and fixed-sized particles: analytical results

## Abstract

We study the kinetics of competitive random sequential adsorption (RSA) of particles of binary mixture of points and fixed-sized particles within the mean-field approach. The present work is a generalization of the random car parking problem in the sense that it considers the case when either a car of fixed size is parked with probability $`q`$ or the parking space is partitioned into two smaller spaces with probability $`(1q)`$ at each time event. This allows an interesting interplay between the classical RSA problem at one extreme ($`q=1`$), and the kinetics of fragmentation processes at the other extreme ($`q=0`$). We present exact analytical results for coverage for a whole range of $`q`$ values, and physical explanations are given for different aspects of the problem. In addition, a comprehensive account of the scaling theory, emphasizing on dimensional analysis, is presented, and the exact expression for the scaling function and exponents are obtained.

PACS number(s): 05.20.Dd,02.50.-r,05.40-y

The kinetics of adsorption or deposition of particles on a substrate is one of the most common phenomena that occurs in many branches of science and technology including physics, chemistry, biophysics and medicine. Examples include adsorption of macromolecules and microscopic particles such as polymers, colloid, bacteria, protein or latex particles  on solid surfaces. Due to its importance, it has been studied extensively through all avenues of research comprising experimental, numerical and analytical means. Owing to the complex nature of the process, one can hardly make any progress analytically in more than one dimension and therefore most of the analytical work remains confined within one dimension only, where it is exactly solvable. The $`1d`$ problem is not at all a pedagogical matter, instead it has been very useful to provide a deep understanding of the underlying mechanism and it has offered an insight into more realistic models in higher dimensions. It has also been used as a test model to verify the results obtained from numerical simulations and data achieved through real life experiments (for extensive review see ).

The simplest model one can think of that can capture the generic feature of the process is the kinetics of random sequential adsorption (RSA) of particles of a fixed size on a clean substrate . This is popularly known as the random car parking problem. This has both an instructional value as well as a long historical significance. The basic rules of the processes are (i) at each time event one particle is adsorbed, (ii) the sites for deposition of adsorbing particles are chosen randomly and (iii), once the site is chosen, the event is successful if the site is empty; otherwise, the particle goes back to the particle reservoir and competes again for further pick up on an equal footing with the rest of the particles in the reservoir. Within this model, no two particles or any of their parts can occupy the same spatial position in the substrate. This means that particle overlapping is forbidden and hence the resulting model describes the kinetics and structure formation of a monolayer. Moreover, once deposited, particles are clamped permanently, making them immobile; therefore, the state of the site at each time step is changed irreversibly from an empty to a filled state. The irreversible nature of the process causes the lack of a detailed balance and drives the system out of equilibrium. Therefore, one can no longer use the well developed standard statistical mechanics approach fit for its equilibrium counterpart. A unique yet fascinating feature of the RSA processes is the existence of a jamming limit in the arbitrary dimension. This is the state when it is impossible to deposit even one single further particle on the substrate, despite the presence of gaps (voids), which are in fact not large enough to allow any further deposition.

To bring the RSA problem closer to real life experiment, there exist many interesting variants of this model. Examples include cooperative sequential adsorption (CSA) , the accelerated random sequential adsorption (ARSA) model , the ballistic deposition (BD)  model, the RSA on disordered substrates , the RSA of growing objects  and many attempts to include transport of depositing particles by diffusion . Recently, there has been an increasing interest in the study of the RSA of mixture of particles of different degree, comprising binary mixture of greatly differing diameters , and continuous mixture of sizes obeying a power-law size distribution . It is important to note that in the former two cases, the ultimate structure in the long time limit is described by the jamming coverage, whereas in the latter case, the resulting monolayer is uniquely characterised by an exponent called fractal dimension, since the arising pattern is a fractal . The motivation of our present work comes from Bertelt and Privman , who studied the binary mixture of monomers and k-mers on 1-d lattice as well as Talbot and Schaaf , who studied the RSA of binary mixture of greately differing sizes. Bertelt and Privman obtained an approximate expression for the coverage for continuum model by taking $`k\mathrm{}`$.

In the present work, we concentrate on the binary mixture of fixed size and point particles, instead of pointlike particles, in a $`1d`$ substrate. We give an exact solution for the gap size distribution function and a continuous spectrum of jamming coverage depending on the probability at which cars are parked. It is note worthy to mention that within the RSA model only one particle can be adsorbed at each time step. This is the basic principle of the RSA process and it is indispensable if we want to call it sequential adsorption. In our investigation we consider the case when either a car is parked with probability $`q`$ or the parking space is partitioned with probability $`(1q)`$. That is, points and fixed sized particles compete for deposition, and at each time step only one of the two events is successful, and hence we call it competitive sequential adsorption. Indeed, we find that both the resulting dynamics and the final coverage differ significantly from previous studies. We find that the RSA of mixture of point-like and fixed size particles, points and fixed size particles and binary mixture of significantly differing size behave in a completely different way. This means that one has to be very careful in making any approximation, since the final results are very prone to the exact ratio of the particle sizes. The beauty of the present work is that the results are exact and obtained analytically.

In addition, we present an explicit scaling description with special emphasis on the dimensional analysis. It is worth to mention that, despite the long history of the RSA problem, a proper description of the scaling theory has remained untouched, although it has been a potential candidate for this. Dimensional analysis provides an insight into the problem and of course one cannot get things wrong if one remains faithful to the dimensional consistency.

We first give the general rate equation that describes the sequential deposition of particles, whose sizes and positions are determined by the specific choice of the model. Let us denote $`P(x,t)`$ as the gap size distribution function of size $`x`$ at time $`t`$, consequently $`P(x,t)`$ obeys the following integro-differential equation

$$\frac{P(x,t)}{t}=P(x,t)_0^x𝑑zp(z)_0^{xz}𝑑yF(xyz,y|z)+2_x^{\mathrm{}}𝑑yP(y,t)_0^{yx}𝑑zp(z)F(x,yxz|z).$$
(1)
Here $`p(z)`$ is called the parking distribution function, that determines the size of the depositing particle and $`F(xyz,y|z)`$ is the deposition kernel, that determines the rate $`a(x,z)=_0^x𝑑zp(z)_0^{xz}𝑑yF(xyz,y|z)`$ at which an interval of size $`x`$ is destroyed by the deposition of a particle of size $`z`$, thus creating two new intervals of size $`xyz`$ and $`y`$. The first term on the right hand side of the Eq. $`(1)`$ describes the destruction of the interval of size $`x`$ and the second term their creation from the interval $`y`$ ($`y>x`$). Note that if one chooses $`F(x,y|z)=1`$ and $`p(x)=\delta (x\sigma )`$ ($`\sigma `$ is the size of the depositing particle) then the Eq. ($`1`$) simply describes the classical car parking problem . It is further interesting to note that if one chooses $`p(z)=\delta (z)`$ then the resulting equation describes the random sequential deposition of points, which is equivalent to the standard binary fragmentation of particles . In fact, the car parking problem can be interpreted as placing cuts with finite thickness and fragmenting particles into two pieces at each time step. The connection between the RSA and the binary fragmentation process was first noted by Ziff .

In order to gain a detailed insight into the process, we first study the RSA of point-sized particles alone, which in fact describes the kinetics of the binary fragmentation process. Let us consider the simplest case when $`F(x,y)=1`$, which is known as the random scission model ; the resulting equation is

$$\frac{P(x,t)}{t}=xP(x,t)+2_x^{\mathrm{}}P(y,t)𝑑y.$$
(2)
First, note that $`a(x)=x`$ is the quantity that describes the rate and therefore it must bear the dimension inverse of time $`t`$. This means that $`x`$ and $`t`$ are interlocked and any one of these two variables can be expressed in terms of the other one. On the other hand, since $`x`$ and $`t`$ are the only two governing parameters, the quantity $`P(x,t)`$ can also be expressed in terms of one parameter alone. Therefore, assuming $`t`$ to be the independent parameter, we can write the following scaling ansatz

$$P(x,t)P_0(t)\varphi (x/s(t))$$
(3)
where $`\varphi (\xi )`$ is known as the scaling function. The Eq. ($`2`$) will admit scaling if we can choose a time dependent scale $`s(t)`$ for the spatial variable, and $`P_0(t)`$ for the particle size distribution function so that all plots of $`P(x,t)/P_0(t)`$ against $`x/s(t)`$ for any initial distribution collapse onto one single curve. This can only be true if both $`P_0(t)`$ and $`s(t)`$ show a powerlaw behaviour. This is due to the fact that $`P_0(t)`$ and $`s(t)`$ must bear the dimensions of $`P(x,t)`$ and $`x`$ respectively. On the other hand, the dimension of any physical quantity must be of power-monomial nature, i.e. we can write

$$P_0(t)t^\alpha \mathrm{and}s(t)t^z.$$
(4)
Simple dimensional analysis of Eq. ($`1`$) immediately reveals $`z=1`$ and since it describes the conservation of mass, i.e $`_0^{\mathrm{}}xP(x,t)𝑑x`$, it is independent of time and yields $`\alpha =2`$. The solution of the Eq. (1) is now well known and reads as

$$P(x,t)t^2e^{xt}$$
(5)
which gives $`\varphi (\xi )=e^\xi `$. Therefore, both the exact solution and the dimensional analysis confirm that $`t^2`$ bears the dimension of $`P(x,t)`$ and $`x`$ bears the dimension inverse of time. We shall use this result later.

We now study the random sequential deposition of a mixture of points and of particles of size $`\sigma `$. Considering the rate equation for the classical car parking problem and the binary fragmentation model, we can write the following equation

$$\frac{P(x,t)}{t}=(xq\sigma )P(x,t)+2q_{x+\sigma }^{\mathrm{}}𝑑yP(y,t)+2(1q)_x^{\mathrm{}}P(y,t)𝑑y\mathrm{for}x\sigma $$
(6)
and

$$\frac{P(x,t)}{t}=2q_{x+\sigma }^{\mathrm{}}𝑑yP(y,t)+(1q)\left(xP(x,t)+2_x^{\mathrm{}}P(y,t)𝑑y\right)\mathrm{for}x<\sigma .$$
(7)
This is an obvious generalization of the RSA problem, in which at each time event a particle of size $`\sigma `$ is deposited with probability $`q`$ or a point is deposited with probability $`(1q)`$. Another way of interpreting the present model is that at each time event a car is parked with probability $`q`$ on the one dimensional parking space or the parking space is divided into smaller spaces with probability $`(1q)`$. Knowing the solution of Eq. ($`2`$) and the solution for the car parking problem alone, we write the following ansatz

$$P(x,t)=A(t)e^{(xq\sigma )B(t)}$$
(8)
where $`A(t)`$ and $`B(t)`$ are yet to be determined. The simplest way of finding $`B(t)`$ is by appreciating that the argument of an exponential function must be a dimensionless quantity. On the other hand Eq. ($`6`$) implies that $`(xq\sigma )`$ is the rate at which gaps of size $`x`$ are destroyed, and hence it must bear the dimension inverse of time. Therefore, only $`B(t)t`$ can make the solution physically acceptable. In order to obtain the solutions for $`A(t)`$ and $`B(t)`$ one can also substitute the ansatz into the Eq. (6). This gives two differential equations, (i) the differential for $`B(t)`$, $`\frac{dB(t)}{dt}=1`$ and (ii) the differential equation for $`A(t)`$

$$\frac{d\mathrm{ln}A(t)}{dt}=2q\frac{e^{\sigma t}}{t}+2(1q)/t.$$
(9)
Both the equations should be solved subject to the initial condition that we start the process with an empty substrate i.e. $`P(x,0)=0`$. Therefore, the solution for $`B(t)`$ is trivial, which only confirms the solution we obtained through the dimensional analysis. Note that the solution of the equation for $`A(t)`$ must be of the form $`A(t)t^2`$, since $`P(x,t)`$ must bear the dimension of $`t^2`$. It is then quite straightforward to obtain the solution of Eq. (9) which is

$$A(t)=t^2F_q(\sigma t)$$
(10)
where $`F_q(\sigma t)=e^{2q_0^{\sigma t}\frac{(1e^u)}{u}𝑑u}`$. Therefore, the solutions of Eqs. (6) and (7) are

$$P(x,t)=t^2F_q(\sigma t)e^{(xq\sigma )t}\mathrm{for}x\sigma $$
(11)
and

$$P(x,t)=_0^t𝑑\tau \tau F_q(\sigma \tau )e^{(xq\sigma )\tau }\left[2qe^{\sigma \tau }+(2\tau )(1q)\right]\mathrm{for}x<\sigma .$$
(12)
The above solutions imply that we can still recover the solution of the binary fragmentation process by taking $`\sigma =0`$. It is important to mention that the solution of Eq. (6) alone is enough to provide us with all the interesting information we need. In fact, we never use the solution for $`P(x,t)`$ when $`x<\sigma `$, which is also true in the case of the classical car parking problem.

To give a scaling analysis and for better clarity we define $`P(x,t)P((xq\sigma ),t)`$ for $`x\sigma `$, then we find that the solution of Eq. (6) satisfies the following identity

$$P((xq\sigma )\lambda ,t/\lambda )=\lambda ^2P((xq\sigma ),t).$$
(13)
This relation is the hallmark for the existence of scale invariance and it is equivalent to a data-collapse formalism , as we shall show below. It means that if the deposition rate $`(xq\sigma )`$ is increased by a factor $`\lambda `$, and the observation time is decreased by the same factor, then the resulting structure would look the same except for a numerical prefactor. In other words, increasing $`(xq\sigma )`$ by a factor of $`\lambda `$ and decreasing $`t`$ by the same factor means that the numerical value of the gap size distribution function is reduced by a factor of $`\lambda ^2`$. Since the Eq. (13) is true for all positive values of $`\lambda `$, we can choose $`\lambda =t`$ in Eq. (13) then

$$P_{scale}=P(\xi ,1)=\varphi (\xi ,\eta )$$
(14)
where

$$P_{scale}=\frac{P}{t^2};\eta =\sigma t\mathrm{and}\xi =(xq\sigma )t$$
(15)
and $`\varphi (\xi ,\eta )`$ is the scaling function. Comparing with the explicit result we get

$$\varphi (\xi ,\eta )=F_q(\eta )e^\xi $$
(16)
and hence $`\varphi `$ is indeed a dimensionless quantity. Therefore, if $`P_{scale}`$ is plotted against the scaled size $`\xi `$, then the entire family of curves collapses into one single curve described by the function $`\varphi (\xi ,\eta )`$. This is possible due to the fact that the scaling function depends only on a dimensionless quantity, the numerical value of which must be independent of the choice of units. The method of data collapse is a very powerful technique for establishing scaling and it is especially useful to analyze and extract exponents from data obtained from numerical simulations or from real life experiments.

The most important quantity of interest in the RSA process is the coverage or jamming limit which is defined as

$$\theta (t)=1_0^{\mathrm{}}xP(x,t)𝑑x.$$
(17)
It tells us the fraction of the substrate covered by the depositing particles. In the case of classical random car parking problem only 74.759 percent of the total substrate is covered by the depositing particles. It is now interesting to see, how the deposition of points or the division of parking spaces changes the jamming limit. In the present case, of course, there is always space for adsorption of points as the points do not have any width due to their inherent definition. Hence, they do not contribute to the coverage or the jamming limit. Therefore, in this model the jamming limit is the state when there are no more gaps available for the adsorption of particles of size $`\sigma `$. Once this state is achieved, it is no longer necessary to continue the process as far as the jamming limit is concerned. So, it would be interesting to see in what way the coverage changes, if at all.

To find this out, it is more convenient to deal with the rate equation for the coverage than the coverage itself. Combining Eq. (6-7) and Eq. (17) we get

$$\frac{d\theta }{dt}=q\sigma _\sigma ^{\mathrm{}}𝑑x(x\sigma )P(x,t).$$
(18)
Clearly it states that only fixed size particles contribute to the coverage. Notice that the right hand side of Eq. (18) bears the dimension inverse of time, as it should be. Substituting the solution of Eq. (6) into this and integrating it, we find the final expression for the jamming limit

$$\theta (\mathrm{})=q_0^{\mathrm{}}𝑑sF_q(s)e^{(1q)s}.$$
(19)
This is a dimensionless quantity and hence, upon transition from one unit of measurement to another within a given class, its numerical value must remain unchanged. Therefore, the final coverage or the jamming limit $`\theta (\mathrm{})`$ is independent of the size of the depositing particle $`\sigma `$, which is indeed a non-trivial and interesting result. This also reflects the fact that the gap size distribution function $`P((xq\sigma ),t)`$ satisfies the exact identity (Eq. (13)) and the function $`F_q(\sigma t)`$ is a dimensionless quantity. In fact, all properties of interest are independent of the size of the depositing particle, and the rate at which they are adsorbed is due to the existence of the scaling property. Clearly, if $`\sigma `$ is increased by a factor $`\lambda `$, then the time to reach the jamming configuration is reduced by a factor $`\lambda `$. However, this is true only if the substrate is sufficiently large in comparison to the depositing particle. One can now obtain a whole range of values for the jamming limit by just tuning the $`q`$ value. Fig. 1. shows that the jamming limit starts from zero at $`q=0`$, since there the problem reduces itself to the random sequential adsorption of points. Note the inherent definition of point that does not occupy space. Therefore, one might apprehend that it does not play any role in achieving the jamming limit if it is adsorbed sequentially with a fixed size particle. However, note that once a point is deposited, it excludes fixed-sized particles from landing within around $`\sigma /2`$, which is the distance between the point where it is chosen to land and the centre of the fixed sized particle. This exclusion will certainly have effect on the resulting dynamics of the process.

In other words, a point divides the substrate, and hence each successful deposition of points creates two new ends belonging to two different gaps. No particle can be adsorbed on a space which belongs to two different gaps i.e. overlapping of points is forbidden. We find that for $`q>0`$, the jamming limit changes nontrivially. Fig. (1) exhibits a $`3`$ dimensional view of the jamming limit against time and the probability $`q`$ with which fixed-size particles are adsorbed. Fig. (2) is the cross-section of the coverage-time plane at $`q=1`$ and $`q=1/2`$ of fig. (1). It is generally believed that if a mixture contains a small number of particles of different sizes, then the kinetics and jamming limit are primarily determined by the smallest size which in the present case is a point particle. However, in our study we find that the jamming limit is primarily determined by the larger particle; yet its dynamics and other aspects are influenced by the size of the smaller particle. For $`q>0`$, the jamming limit is always smaller than its corresponding classical counterpart. Fig. (2) is plotted to demonstrate the slower approach to the jamming limit as $`q`$ value decreases. This is due to the fact that the adsorption of points leads to the crowding of more partition in the parking space than to the adsorption of fixed sized particles. Fig. (3) in fact is the cross-section of coverage-$`q`$ plane of Fig. (1) at the state when the system has achieved the jamming limit. It shows that the jamming limmit increases monotonously as fixed-size particles wins more in the competition with the point particles for adsorption. However, it does not increase linearly with $`q`$, instead one can subdivide the whole curve into a number of regimes of width $`0.2`$ in $`q`$ values, so that in each regime they can be well approximated to a straight line. However, notice that, between $`q=0.95`$ and $`q=1`$, the coverage increases much stronger than in any previous regime. The appearance of a non-linear rise becomes more pronounced if it is plotted in the larger scale.

In conclusion, the present model, though simple, can yet capture some generic features of the RSA of mixture of particles such as coverage and the scaling behaviour. We find that the coverage of mixture of points with fixed-sized particles stays always lower than its classical counterpart. It would be interesting to see how the results change when both the contents of the binary mixture are of a finite size but differ in length which we intend to present in a forthcoming paper . In addition, we give an extensive scaling description of the RSA problem which has not been addressed so far. One potential application of the present work could be the simple cyclization reaction process where adjacent pendant groups link randomly along the polymer, or the polymer itself undergoes a possible degradation. This is in fact a natural generalization of the original work by Folry . We believe the present work will shed a new insight into the underlying mechanism of the problem and will help guiding numerical and experimental works dealing with more realistic situations addressing the adsorption of mixture.

We are grateful to P. L. Krapivsky and G. J. Rodgers for useful correspondence during the work. MKH is grateful to the Alexander von Humboldt Foundation for awarding the fellowship.