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Current Fluctuations in Nonequilibrium Discontinuous Phase Transitions
Current Fluctuations in Nonequilibrium Discontinuous Phase Transitions
hallmark of discontinuous transitions – in the fluctuations of arbitrary thermodynamic currents, including the
entropy production. In particular, we center our discussion on the conditional statistics, given which phase the
system is in. We highlight the interplay between integration window and metastability lifetime, which is not
manifested in the average current, but strongly influences the fluctuations. We introduce conditional currents
and find, among other predictions, their connection to average and scaled variance through a finite-time version
of Large Deviation Theory and a minimal model. Our results are then further verified in two paradigmatic
models of discontinuous transitions: Schlögl’s model of chemical reactions, and a 12-states Potts model subject
to two baths at different temperatures.
master equation [50] The main feature we introduce in this paper is the notion of
X conditional currents, given which phase i = 0, 1 the system is
X
ṗ x (t) = W xy py − Wyx p x := W xy py , (1) in. Inserting the identity 1 = (1 − It ) + It inside the integral (2)
y y allows us to define the current when the system is in phase 1
as
where W xy ≡ PWy→x denotes the transition rates from y to x
and W xx ≡ − y,x Wyx . The dynamics is taken to be ergodic, Zτ X
and such that W xy > 0 whenever Wyx > 0, ensuring the system Jτ|1 = dt It+ dyz δX(t− ),y δX(t+ ),z . (4)
will relax to a unique steady state p∗x . In general, p∗x will be a 0
y,z
where the tilted operator L(η) depends on both the transition on the interplay between τ and all eigenvalues λi of W. If
matrix W in Eq. (1), and the type of current in question, ac- τ 1/|λi |, for all eigenvalues λi , 0, then the term eλi τ − 1
cording to may be neglected, leading to the widely used expression from
large deviation
L(η) xy = eηdxy W xy , (11)
where, recall, d xx = 0. To evaluate J and Dτ , we only require Dτ = h1|L2 |pi − h1|L1 W+ L1 |pi, (16)
the series expansion of L(η), which we write as L(η) = W +
ηL1 + η2 L2 , for matrices L1(2) given by
where W+ = i,0 λ−1
P
i |xi ihyi | is the Moore-Penrose pseudoin-
verse of W (see Appendix A for more details). Close to the
(L1 ) xy = W xy d xy , (L2 ) xy = W xy d2xy /2. (12)
transition point, there will appear a clear separation of time
scales in the eigenvalues λi . At least one eigenvalue will be
A. Unconditional cumulants very small, of the order λi ∼ −1/τm , while all others will be
much larger (describing the within-phase dynamics). If τ is
large compared to these time scales, but not with respect to
We denote by |pi the column vector whose entries are the τm , then the approximation taking Eq. (15) to (16) will not
steady-state distribution p∗x , and h1| the row vector with all hold true. And since τm scales exponentially with the volume,
entries equal 1. Then, as discussed further in Appendix A, the as we approach the thermodynamic limit, larger and larger
first moment can be written, for arbitrary τ, as values of τ have to be considered. This is a direct illustration
of the non-commutativity of the limits τ → ∞ and V → ∞.
Jτ ≡ J = h1|L1 |pi, (13)
B. Conditional cumulants
which is independent of τ, as expected. Conversely, the diffu-
sion coefficient is written as Eqs. (13) and (14) also apply to the conditional currents (4).
Zτ Zτ 0 One simply has to modify accordingly the tilted operator L(η)
1 0 00 J2τ or, what is equivalent, the matrices L1 and L2 in Eq. (12). For
Dτ = h1|L2 |pi + dτ 0
dτ00 h1|L1 eW(τ −τ ) L1 |pi − .(14)
τ 2 each conditional currentPJτ|i , we define a projection operator
0 0 Πi such that Π1xy = δ x,y z∈S i δy,z ; i.e., which projects onto the
We can also obtain a more explicit expression if we assume states Si associated to phase i = 0, 1. The corresponding tilted
that W is diagonalizable, with eigenvalues λi , right eigenvec- operator will then be defined similarly, but with a current of
tors W|xi i = λi |xi i and left eigenvectors hyi |W = hyi |λi . Since the form dixy = d xy Πiyy , which means one should use instead
the steady-state is unique, one eigenvalue must be zero, say matrices L1 Πi and L2 Πi .
λ0 = 0. The corresponding eigenvectors are then |x0 i = |pi Eq. (13) then yields, taking also into account the factor qi
and hy0 | = h1|. Carrying out the integrals one then finds that in the denominator,
λτ
e i − 1 − λi τ
X
Dτ = h1|L2 |pi + h1|L1 |xi ihyi |L1 |pi , (15) 1
i,0
λ2i τ µi = h1|L1 Πi |pi. (17)
qi
where we used the orthogonality relation h1|xi i = 0, for i , 0.
This expression makes it clear that Dτ will depend sensibly Proceeding similarly with Eq. (14), we find
Zτ Zτ0
h1|L2 Πi |pi 1 0 00 µ2i qi τ
Dτ|i = + dτ 0
dτ00 h1|L1 Πi eW(τ −τ ) L1 Πi |pi − . (18)
qi τqi 2
0 0
And to obtain the covariance in Eq. (9), we simply subtract the combination (1 − q)Dτ|0 + qDτ|1 from Dτ in Eq. (14). Recalling
that Π0 + Π1 = 1, this then yields
Zτ Zτ0 Zτ Zτ0
1 0 00 1 0 00
Cτ = dτ0 dτ00 h1|L1 Π0 eW(τ −τ )
L1 Π1 |pi + dτ0 dτ00 h1|L1 Π1 eW(τ −τ ) L1 Π0 |pi − q(1 − q)µ0 µ1 τ. (19)
τ τ
0 0 0 0
Concerning the timescales of the discontinuous transition, we notice that all diffusion coefficients, Dτ , Dτ|i and Cτ , are sub-
4
1
ject to a similar dependence, which is ultimately associated 1 4
0 (a) ( b)
with the matrix eW(τ−τ ) . Thus, one expects that all quantities
should scale similarly with τ.
q( 1- q)
1 1
q
2 8
by conditioning the dynamics, which we shall henceforth refer C(t − t0 ) = cov(It , It0 ) = q(1 − q)e−(t−t )/τm , (23)
to as γτ|i , will thus fundamentally different from the diffusion
which will thus decay very slowly in time. This means that
coefficients Dτ|i in Eq. (8).
Dτ|i in Eq. (8) will depend very sensibly on the interplay be-
An intuitive argument as to why this is the case goes as tween τ and τm . Conversely, the diffusion coefficients γi , for
follows. The currents (4) are integrated over a certain time the conditional dynamics, will not. And hence, even for mod-
interval τ. Hence, its diffusion coefficient will depend on erately large τ, one expects it to be τ-independent.
correlations between different instants of time, and these are
dramatically affected by the long timescale τm introduced
by the discontinuous transition. In fact, let us define Zt = IV. MINIMAL MODEL
y,z dyz δX(t− ),y δX(t+ ),z , so that Eq. (4) can be written as
P
be non-Markovian, as this would represent a hidden Markov where γ = (1 − q)γ0 + qγ1 is independent of τ and
chain. Instead, a minimal model is one where the dynamics
of It can be assumed to be Markovian, which is justified when f (t) = (e−t − 1 + t)/t. (30)
V is sufficiently large. In this case, instead of the full master
equation (1), we may restrict the dynamics to The interesting part is the last term in Eq. (29). First, it de-
pends on q(1 − q), which is non-negligible only in the vicinity
of the transition point (Fig. 1(b)). Second, it depends on the
d X −a b
qi = Wi j q j , W = . (24) interplay between τ and τm through the function f , which is
dt a −b
j=0,1 shown in Fig. 1(c).
When τ τm we get f (τ/τm ) ' τ/2τm , so that Eq. (29) can
Here a and b represent the rates for the system to jump from be approximated to
phase 0 → 1 and 1 → 0. The steady-state yields q ≡ q1 =
E(It ) = a/(a + b). Moreover, the metastability lifetime in this Dτ ' γ + q(1 − q)(µ1 − µ0 )2 τ/2, τ τm , (31)
case reads τm = 1/(a + b). Finally, from (24) one can compute
the two-time correlation function, which is given in Eq. (23). which is thus linear in τ. Conversely, when τ τm , we get
And since It can take on only two values, once C(t − t0 ) is
known we can reconstruct the full joint distribution Pr(It = Dτ ' γ + q(1 − q)(µ1 − µ0 )2 τm , τ τm , (32)
i, It0 = i0 ), for arbitrary times t, t0 :
which is independent of τ, but linear in τm . Hence, when V
q2 + C(t − t0 ) i = i0 = 1,
is large, this will become exponentially dominant. As a con-
sequence, the large volume diffusion coefficient will actually
Pr(It = i, It0 = i0 ) = (1 − q)2 + C(t − t0 ) i = i0 = 0, (25)
become independent of the γi , and will instead be governed
essentially by the mismatch in conditional averages (µ1 −µ0 )2 ,
q(1 − q) − C(t − t0 ) i , i0 .
in agreement with previous studies on Schlögl’s model [44].
This offers another explicit illustration of the order of limits
The key feature of discontinuous transitions is the fact that
issue, which we depict graphically in Fig. 1(d): For a given τ,
transitions between phases are seldom when V is large. Close
as we increase V the diffusion coefficient will at first increase
to λc , the transition rates a and b will usually behave, up to
exponentially according to Eq. (32). But if τ is fixed, then a
polynomial corrections, as
point will always be reached around which τ ∼ τm . And be-
a ∼ e−V(c0 −ca ∆λ) , b ∼ e−V(c0 +cb ∆λ) , (26) yond this point, the scaling will be given by Eq. (31), which
is at most polynomial in V (due to a potential polynomial vol-
where c0 , ca , cb > 0 are constants and ∆λ = λ − λc . Note ume dependence of µi , γi ).
how the rates are exponentially decreasing with V. Transi- Even though these results were developed for a 2-level
tions hence become rare when V is large. From (26) we also model, they are still expected to hold for a broad class of
get τm ∼ ec0 V , which is the aforementioned exponential de- discontinuous transitions. The reason is that, as discussed in
pendence. Finally, q = (1 + e−cV∆λ )−1 , where c = ca + cb > 0; Ref. [53], the eigenvalues and eigenvectors of the two-level
hence q changes abruptly from 0 to 1 as λ crosses λc , as illus- transition matrix (24) are connected to some of the eigenval-
trated in Fig. 1(a). Since the conditional averages are weakly ues and eigenvectors of the full matrix W in Eq. (1). But, in
dependent on ∆λ, from Eq. (7) we therefore see that J should addition, the full W will also have several other eigenvalues
also change abruptly around λc , interpolating from µ0 to µ1 . associated to the within-phase dynamics. Thus, the step from
Eq. (15) to (29) only assumes that τ is much larger than all
other λi , so that within-phase terms can be neglected.
A. Unconditional diffusion coefficient
allows us to conclude that even the conditional diffusion coef- The bistable region is defined as the interval in the control pa-
ficients will be dominated by jumps between phases, and will rameters for which this equation has three real roots, x0 , x∗ , x1 .
be negligibly affected by the internal fluctuations within each The first and last represent stable states for the most likely
phase. We find this result both relevant and non-trivial. density within each phase, whereas x∗ is unstable and serves
It is also interesting to notice how the sign of the covari- as the phase separator. Hence, we define the phase-indicator
ance (35) depends only on the signs of µ0 and µ1 . A positively in the Schlögl’s model as a random variable It such that It = 1
correlated covariance means that fluctuations above (below) when X(t) > V x∗ and 0 otherwise.]
average in one phase tend to lead to fluctuations above (be- For concreteness, we choose as thermodynamic current the
low) the average in the other; and vice-versa for C < 0. We entropy production Jτ = στ . Whenever there is a transition,
see in Eq. (35) that the covariance will be negative whenever the net current (2) changes by an increment δστ defined ac-
µ0 , µ1 have the same sign. cording to the following rules:
k1
2X + A −−−−→ 3X δστ = µA ,
V. APPLICATIONS
k−1
3X −−−−−→ 2X + A δστ = −µA ,
Next we shall exemplify our main findings in two represen- (41)
k−2
tative systems displaying discontinuous phase transitions: The X −−−−−→ B δστ = µB ,
second Schlögl [54] and a 12-state Potts models connected to
k2
two baths at different temperatures. The former was recently B −−−−→ X δστ = −µB ,
analyzed in Ref. [44]. It represents an ideal laboratory for test-
ing our main prescriptions, since it presents an exact solution. where µA = ln ak1 /k−1 and µB = ln k−2 /bk2 .
The Potts model, on the other hand, is defined in a regular The model was simulated using the Gillespie algorithm.
lattice and exhibits a nonequilibrium phase transition under a We fix ak1 = k−2 = 1, bk2 = 0.2, and take as control pa-
different mechanism. Despite the absence of an exact solu- rameter the chemical potential gradient ∆µ = µB − µA =
tion, all main features about the phase transition and statistics ln [(k−2 ak1 )/(k−1 bk2 )]. For these parameters, the phase co-
about entropy production fluctuations are present. existence point in the thermodynamic limit occurs at ∆µ0 ∼
3.047 [44]. Figs. 2(a) and (b) present a basic characterization
of the steady-state. First, in Fig. 2(a) we show the numerically
A. Schlögl’s model computed metastability timescale τm , as a function of the vol-
ume V, confirming the exponential dependence with V. This
The second Schlögl model [54] describes a system with 3 is obtained by collecting the mean first passage time T xi →x∗
chemical species, A, B and X, supporting two types of chemi- for the system to go from each stable point x0(1) to the unsta-
cal reactions: ble point, x∗ . The rates a and b in Eq. (24) are then given by
k1 k2 a = (2T x0 →x∗ )−1 and b = (2T x1 →x∗ )−1 [56], from which we de-
−*
2X + A −
)−− 3X, −*
)
B−−− X. (36) termine τm = 1/(a + b). Second, Fig. 2(b) characterizes the
k−1 k−2
probability q of finding the system in phase 1, as a function of
Here k±1 , k±2 are kinetic constants that account, respectively, ∆µ − ∆µ0 , for different values of V, where markers are simu-
for catalytic, spontaneous creation and spontaneous annihi- lation data and the curves are a fit of q = (1 + e−cV(∆µ−∆µ0 ) )−1 ;
lation of X. The concentrations of A and B are fixed at a both agree very well for large volumes and/or small ∆µ − ∆µ0 .
and b due to the presence of chemostats. The dynamics of This is expected, since Schlögl’s model is known to have a
pn (t) = P(X(t) = n), for n = 0, 1, 2, . . ., is then described by well defined 2-state limit [53, 55] when V is large.
the master equation [53, 55] Sample stochastic trajectories of the current Jτ [Eq. (2)] as
a function of τ are shown in Fig. 2(c), for fixed ∆µ = 3.35 and
ṗn = fn−1 pn−1 + gn+1 pn+1 − ( fn + gn )pn , (37) V = 10. Red and blue curves represent the situations where
the system start in phases 1 and 0 respectively. For short τ the
where curves tend to remain well separated, so that Jτ behaves as
ak1 n(n − 1) either Jτ|1 or Jτ|0 . The corresponding statistics of Jτ , shown
fn B + bk2 V, (38) in the inset, would thus be a prototypical bimodal distribu-
V
tion. Conversely, when τ τm ∼ 40, transitions between the
k−1 n(n − 1)(n − 2) phases begin to occur, which cause the corresponding distri-
gn B + k−2 n. (39)
V2 bution to change to unimodal.
The conditional mean current and diffusion coefficients are
The concentration x(t) = X(t)/V presents a bistable behavior
shown in Fig. 2(d)-(g). For concreteness, we focus on the
for large V [53], which is determined by the roots of the differ-
special point q = 1/2; i.e., where the two phases are equally
ential equation governing the deterministic behavior of x for
likely. As this depends on V, for each volume we first fix ∆µ
large volumes
as the point where q = 1/2. This reduces the free parameters
dx to V and τ only. The conditional averages µ0(1) as a function
= ak1 x2 + bk2 − k−1 x3 − k−2 x = 0. (40) of the volume are shown in Fig. 2(a). They are both found to
dt
7
104 300
(a) ( b) (c) τ = 15
5000 0.85
250
τ /τ
500
τm
150
q
0.45 V=5 μ1
V = 15 100
100 Jτ
0.25 V = 25
50 50
V = 40 μ0
0.05 0
0 10 20 30 40 50 60 70 - 0.1 0 0.1 1 5 10 50 100 500 1000
V Δμ-Δμ0 τ
12 19.
15 (d ) 549. 17 (e) (f ) 1.3 ( g) τ = 10 1.3
16 10 17.4
τ = 200
15 8 15.9 1.2 1.2
10 366.
ln( Dτ 0)
ln( Dτ 1)
τ = 1000
ln( Dτ)
14
μ0
μ1
r
6 14.4
13 1.1 1.1
5 183. 4 12.8
12
11 2 11.3
1. 1.
0 0. 10 0 9.77 0 10 20 30 40 50 60 70
0 10 20 30 40 50 60 70 0 10 20 30 40 50 60 70 0 10 20 30 40 50 60 70
V V V V
FIG. 2. Conditional currents for Schlögl’s model, computed using the Gillespie algorithm. (a) τm vs.V. (b) q vs. ∆µ − ∆µ0 for different values
of V. Solid lines are a fit of q = (1 + e−cV(∆µ−∆µ0 ) )−1 . (c) Stochastic trajectories of Jτ /τ vs. τ, starting either in phase 1 (red) or phase 0 (blue).
The insets show the corresponding histograms at different times τ. (d)-(g) Mean and diffusion coefficient as a function of V, with τ = 103 and
∆µ fixed by setting q = 1/2. (d) Conditional means µ0(1) [Eq. (6)]. (e) Diffusion coefficient Dτ [Eq. (3)]. (f) Conditional diffusion coefficients
Dτ|i [Eq. (8)]. (g) The ratio r in Eq. (42), as a function of V, for different values of τ. Other parameters: a = k1 = k2 = k−2 = 1 and b = 0.2.
0,9 V=900
V=1600
V=2500 equal area 1e+12 1e+12 (b)
(a) V=3600 0,068 (b) q=1/2 Dτ
0,6 (a)
Dτ|0
φ 1e+09 6
T1V τ=10 1e+08
0,006 6 Dτ|1
1e+06 Pφ τ=5.10
0,066 -Cτ
τm 1e+06 τ=10
7
0,3
10000
10000
0 0 2000 4000 0 2000 4000
0 0,5 1 V=900 V V
0
V 5000 0,064 φ V=1600 3e+09 Dτ|0
0 V=2116
Dτ|1
0,062 0,064 0,066 0,068 0,07 0 0,0005 -1 0,001 1e+09 2e+09
T1 V (c) -Cτ
Dτ
1e+09 (d)
(c) (d)
0,8 0,3 0 0
0 5e+04 1e+05 0 5e+04 1e+05
τ τ=1000
τ
1,1 (f)
J τ=5000 1,01
q (e) τ=10000
0,4 0,2 τ=20000
1 1,1
r|1
r
r|0
0,99 1
1
0,1 1500 3000
0 0,98
0,062 0,064 0,066 0,068 0,07 0,062 0,064 0,066 0,068 0,07 1000 2000 3000 1000 2000 V 3000
T1
V
T1
FIG. 3. Characterization of the Q = 12 Potts model in contact FIG. 4. Unconditional and conditional diffusion coefficients for the
with two thermal baths of temperatures T 1 and T 1 + ∆T (with fixed Q = 12 Potts model. (a) Dτ vs. V for different values of τ. (b) Dτ|i
∆T = 0.9). (a) Order parameter φ vs. T 1 for different volumes and Cτ vs. V with τ = 5 × 106 . (c) Dτ vs.τ for different V. (d)
V. Inset: metastability lifetime τm vs. V. (b) Finite-size analysis Dτ|i and Cτ vs. τ for V = 1600. Continuous lines in (c) and (d) are
of the transition point T 1V vs. V −1 , yielding the asymptotic value the theoretical predictions from Eq. (29). (e) The ratio (42) between
T 01 = 0.0651(1). Inset: distribution of φ at T 1V , for different vol- Dτ and the predictions of the minimal model, Eq. (29), which tends
umes. (c) Phase probability q vs. T 1 , again for different volumes. to unity for large volumes. Curves are for different values of τ. (f)
The continuous lines are fits of q = [1 + Qe−Vc(T1 −T10 ) ]−1 . (d) Average Same, but for r|0 (main plot) and r|1 (inset). In all curves, for each
entropy production rate current J [Eq. (3)], which follows closely the V, we fix T 1 as the value T 1V for which q = 1/2. Other details are as
behavior of q. in Fig. 3.
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