An Explanation of the Temperature-Dependent Upper Critical Field Data of H3S on the Basis of the Thermodynamics of a Superconductor in a Magnetic Field

Abstract

Excellent fits to a couple of the data-sets on the temperature (T)-dependent upper critical field (Hc2) of H3S (critical temperature, Tc ≈ 200 K at pressure ≈ 150 GPa) reported by Mozaffari, et al. (2019) were obtained by Talantsev (2019) in an approach based on an ingenious mix of the Ginzberg-Landau (GL), the Werthamer, Helfand and Hohenberg (WHH), and the Gor’kov, etc., theories which have individually been employed for the same purpose for a long time. Up to the lowest temperature (TL) in each of these data-sets, similarly accurate fits have also been obtained by Malik and Varma (2023) in a radically different approach based on the Bethe-Salpeter equation (BSE) supplemented by the Matsubara and the Landau quantization prescriptions. For T < TL, however, while the (GL, WHH, etc.)-based approach leads to Hc2(0) ≈ 100 T, the BSE-based approach leads to about twice this value even at 1 K. In this paper, a fit to one of the said data-sets is obtained for the first time via a thermodynamic approach which, up to TL, is as good as those obtained via the earlier approaches. While this is interesting per se, another significant result of this paper is that for T < TL it corroborates the result of the BSE-based approach.

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Malik, G. (2024) An Explanation of the Temperature-Dependent Upper Critical Field Data of H3S on the Basis of the Thermodynamics of a Superconductor in a Magnetic Field. World Journal of Condensed Matter Physics, 14, 45-50. doi: 10.4236/wjcmp.2024.143005.

1. Introduction

The temperature (T)-dependent values of the upper critical field Hc2 of two samples of H3S reported by Mozaffari, et al. [1] were explained by the authors on the basis of both the Ginzberg-Landau (GL) theory and the Werthamer, Helfand and Hohenberg (WHH) theory [2]. Based on a mix of these and other well-known theories, e.g., Gor’kov theory [3], accurate fits to the same data-sets were obtained by Talantsev [4] via four alternative equations. Each of these equations invoked two or more parameters from the following sample-specific set of the properties of the superconductor (SC): Σ1 = {Critical temperature (Tc), gap, coherence length and penetration depth at T = 0, jump in sp. ht.}. In the following, we refer to this phenomenological approach as Approach I.

Fits as good as those obtained via Approach I for the above data-sets have also been obtained in [5] and [6] via a T-, chemical potential (μ)- and applied field (H)-incorporated equation for pairing [7]. This equation—derived in [8] and subjected to a correction in [7]—is obtained via a 4-d Bethe-Salpeter equation (BSE) which is temperature-generalized via the Matsubara prescription at the expense of the 4th dimension. The resulting 3-d equation is subjected to the Landau quantization scheme which causes the transverse components of momentum to be quantized into Landau levels. The 1-d equation thus obtained depends on the set Σ2 = {μ, T, H, the Debye temperature of the SC, the magnetic interaction parameter, the effective mass of the electron, and the Landau index}, which is radically different from Σ1. Hereafter we shall refer to the BSE-based approach as Approach II.

The purpose of this note is:

a) To present an approach which is neither dependent on the theories employed in Approach I nor on the rather specialized methodology of Approach II, but is based for the first time on the thermodynamics of an SC in a magnetic field via an adaptation of the Clausius-Clapeyron equation (CCE).

b) To shed light on the contrasting results that Approaches I and II yield for the values of Hc2(T) for T close to 0 K. To elaborate, the lowest temperature (TL) for which the empirical values of Hc2(T) were reported in [1] are: Sample 1, Tc = 173.7 K: TL1 = 55.09 K; Sample 2, Tc = 191 K: TL2 = 105.1 K. While both the approaches lead to almost equally good fits to the empirical data up to TL1 and TL2, the values of Hc2(T) that they lead to for T < TL1 or TL2 are significantly different. In Approach I, for values of T from about 10 to 0 K, the Hc2(T) vs. T plot is almost parallel to the T-axis; the value of Hc2(0) for each of the two samples is ≈ 100 × 104 G (100 Tesla). In Approach II, on the other hand, for the same range of T, there is an upward swing of the Hc2(T) vs. T plot, leading to values of Hc2 even at T = 1 K that are about twice the corresponding values in Approach I.

Since the most familiar form of the CCE is one that relates the change in the pressure of a system with T when it is undergoing a liquid ↔ gas or solid ↔ liquid phase transition, see, e.g., [9], we need to adapt this equation to the situation when pressure is kept constant and the solid ↔ liquid phase transition is brought about by H—as is the case for H3S. This is done in the next section. Application of the thus obtained equation to Sample 1—which has been stated to be prepared from condensed liquid H2S [1]—is taken up in Section 3. The final section sums up our findings.

2. The CCE in a Magnetic Field

When pressure is maintained at a constant value and the change from a normal (N)-state to the superconducting (S)-state, and vice-versa, takes place due to an applied field H, the differential of the Gibbs function for the two states are:

S-State: dG| S = S s dTV M S dH (1)

N-state: dG| N = S N dT, (since MN = 0) (2)

where S denotes entropy and V the volume of the sample, and M is the magnetic moment per unit volume.

It follows from the equality of dG| S and dG| N dictated by the coexistence of the two phases on the locus of the point of phase transition that

( S S S N )dT=V M s dH. (3)

As usual, in this equation ( S S S N )= L m J/T , where Lm is the latent heat that brings about the change of phase and J is the mechanical equivalent of heat (4.19 × 107 ergs/cal) employed to convert calories into ergs. There now remains MS to be specified which satisfies the equation B S =H+4π M S . If the SC we are dealing with were a type I SC which is a perfect diamagnet, we would have had the magnetic induction parameter BS = 0 and therefore MS = −H/4π. Since H3S is known to be a type II SC, BS ≠ 0 and hence we need to parametrize BS in terms of H and t in order to have a tractable problem. To this end, we assume that

B S = αtH/ ( 1+αt ) , (4)

where α is a constant and t = T/Tc. Thus, M S = H/ [ 4π( 1+αt ) ] and we now have (3) as

( 1+αt ) dt t = VH 4π L m J dH,

or,

texp( αt )=Cexp( V H 2 8π L m J ),

where C, a dimensionless constant since α, t and ( V H 2 / L m J ) are dimensionless, can be fixed by putting H = 0 corresponding to t = 1. Thus,

Eq1( t,H,α, L m )texp[ α( 1t ) ]exp( V H 2 8π L m J )=0. (5)

3. Application of the CCE in a Magnetic Field to a Sample of H3S

Gleaned from (1), the specifications of the sample subjected to pressure of 160 GPa and the empirical values of its Hc2(T) employed by us are as follows:

Diameter of the sample, d = 40 × 104 cm; thickness of the sample, th = 4 × 104 cm;

Volume of the sample (π d th) = 5.0265 × 106 cm3;

Tc = 173.7 K;

Values of Hc2(T) at 24 points—shown in Figure 1—for 55.09 K ≤ T ≤ 173.7 K:

62.45 × 104 G ≥ Hc2(T) ≥ 0 G.

In particular,

For T1 = 69.99 K, Hc2(T1) = 54.31 × 104 G (6)

For T2 = 141.6 K, Hc2(T2) = 12.62 × 104 G (7)

To find the unknowns α and Lm in (5), we simultaneously solve

Eq1( t 1 = T 1 / T c , H c2 ( T 1 ),α, L m ) and Eq1( t 2 = T 2 / T c , H c2 ( T 2 ),α, L m ),

where T1, T2 and the corresponding values of Hc2 are as given in (6) and (7), respectively. Thus,

α=1.01757,  L m =4.6709× 10 3  cal (8)

We can now solve (5) to obtain the value of Hc2 for any value of t. The results of this exercise carried out for 20 values of T between 1 and 173.7 K are given in Figure 1 which also includes the empirical values of Hc2 in the range of T noted above (6).

Figure 1. The continuous curve is the fit obtained via (5) to the empirical values of Hc2(T)—denoted by filled circles—as reported in [1] for 55.09 K ≤ T ≤ 173.7 K.

4. Discussion and Conclusion

The fit to the empirical data shown in Figure 1 can be seen as providing a posteriori justification for the expression of BS in terms of t and H noted in (4). We believe that this relation can also be validated empirically via a set-up similar to the one recently employed by Minkov et al. [10] to determine the trapped magnetic fluxes in H3S and LaH10 in order to obtain the lower critical field Hc1 of these SCs. It is interesting to note that the results plotted in Figure 1 and obtained by assuming Bs to vary as in (4) and Lm to have a constant value can also be formally obtained by assuming MS to have the value −H/4π (i.e., by assuming H3S to be a type I SC) and paying the price of making Lmt-dependent via Lm = Lm0(1 + αt), where α = −1.01757 and Lm0 = 4.6709 × 103 cal - vide (8).

We would like to note that the value of Lm given in (8) is not per gram, but for the whole of the tiny sample whose mass is not given.

Now a matter of detail. It is pertinent to ask: how does the plot given in Figure 1 change if α and Lm are determined not via the choice of (T1, Hc2(T1)) and (T2, Hc2(T2)) noted in (6) and (7), respectively, but by the choice of two different points in the neighborhood of these points? The answer to this question is: indeed, the plot changes, but does so marginally. However, the feature of its upswing as T → 0 K persists unmistakably. The slight shifting of the plot when points other than those specified in (6) and (7) are employed to fix α and Lm is not surprising in view of the uncertainties in the reported values of (T, Hc2(T)), which is evidenced by the values of Hc2(T) given in the data as 21.02 and 23.88 T for the same value of T, viz., 130.1 K.

The Hc2(T) data of H3S addressed here via a thermodynamic approach have been dealt with earlier via approaches as different as the GL or the WHH, etc., theories, or via the field-theoretic approach provided by the BSE. These different approaches should be seen as complementing each other because they shed light on different features of the same phenomenon. Based on the simple framework of the thermodynamics of an SC in a magnetic field, a virtue of the present approach is that it does not require familiarity with the rather formidable theoretical apparatus employed by each of the earlier approaches.

To conclude, we have for the first time obtained in this paper via a thermodynamic approach a fit to the Hc2(T) data of a sample of H3S which, up to TL, is nearly as good as those obtained earlier via several radically different approaches. For T < TL, however, our findings are in accord with those of Approach II.

Acknowledgements

The author thanks Dr. Usha Malik for a critical reading of the manuscript.

Conflicts of Interest

The author declares no conflicts of interest regarding the publication of this paper.

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