Dispersion of plasmons in three-dimensional superconductors
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Dispersion of plasmons in three-dimensional superconductors T. Repplinger, M. Gélédan and H. Kurkjian Laboratoire de Physique Théorique, Université de Toulouse, CNRS, UPS, 31400, Toulouse, France S. Klimin and J. Tempere TQC, Universiteit Antwerpen, Universiteitsplein 1, B-2610 Anvers, Belgique We study the plasma branch of an homogeneous three-dimensional electron gas in an s-wave superconducting state. We focus on the regime where the plasma frequency ωp is comparable to the gap ∆, which is experimentally realized in cuprates. Although a sum rule guarantees that the arXiv:2201.11421v1 [cond-mat.supr-con] 27 Jan 2022 departure of the plasma branch always coincides with the plasma frequency, the dispersion and lifetime of the plasmons is strongly affected by the presence of the pair condensate, especially at energies close to the pair-breaking threshold 2∆. When ωp is above 1.7∆, the level repulsion is strong enough to give the plasma branch an anomalous, negative dispersion with a minimum at finite wavelength. At non-zero temperature and at ωp > 2∆, we treat in a non-perturbative way the coupling of plasmons to the fermionic excitations, and show that a broadened plasma resonance inside the pair-breaking continuum coexists with an undamped solution in the band gap. This resonance splitting is associated with the presence of multiple poles in the analytic continuation of the propagator of the Cooper pairs. Introduction: Despite being a very mature experimen- damental understanding of superconductivity and long- tal platform, supporting numerous technical applications, range interactions in many-body physics, those modes superconductors still hold some of the most fundamental can also be used in plasmonics, or to probe and ma- open questions of many-body physics. The impressively nipulate superconducting materials [18]. Experimental high critical temperature (Tc ) and the unconventional research on Josephson plasmons, which describe trans- Cooper pairing in cuprates and iron-based superconduc- verse plasmonic excitations is superconducting layers is tors are the most famous of those fascinating questions. still very active today [19]. However, even some properties of conventional Bardeen- At low energy-momentum, plasmons can be described Cooper-Schrieffer (BCS) superconductors are still inten- by phenomenological approaches based on London elec- sively discussed, such as the existence of an amplitude trodynamics [20], but a microscopic theory is needed collective mode [1–3], reminiscent of the Higgs mode in when the eigenfrequency of plasmons approaches the high-energy physics. pair-breaking threshold. In this regime, the theoreti- In fact, even for such usual behavior as plasma oscil- cal literature is still hesitant, in particular in the cases lations (the collective modes of the electronic density), where a complex plasma mode describing a damped res- superconductors are still not fully understood. In a pio- onance is expected. Here, we reveal that remarkable neering work, Anderson [4] has shown that the phononic phenomena affecting the plasma dispersion in presence (Goldstone) branch that exists in a neutral fermionic con- of superconducting order have been overlooked. Like densate acquires a gap corresponding to the plasma fre- Anderson, we consider the reference situation of an quency ωp in presence of long-range Coulomb interaction. isotropic three-dimensional (3D) s-wave superconductor This mechanism later became famous due to its analogy but our study can be readily extended to layered ge- with the phenomenon of mass acquisition in high-energy ometries or anisotropic pairing. Due to the repulsion of physics. The work of Anderson has then been revisited in the pair-breaking threshold, the plasma branch acquires the context of high-Tc superconductivity [5–9], and nu- a negative curvature and thus a minimum at non-zero clear/neutronic matter [10]. While Anderson focused on wavenumber when ωp is between 1.696∆ and 2∆ at zero the regime of large ωp , the frequency of transverse plas- temperature. At larger wavenumber, nonzero tempera- mons in layered superconductors such as cuprates often ture or when ωp > 2∆, the plasma branch enters the pair- lies below the pair-breaking threshold 2∆ [11–13], such breaking continuum but remains observable with a finite that an undamped plasma branch can be expected. The lifetime that we calculate using recently develop technics departure of the plasma branch was shown to always co- [21–23] to treat the coupling to the fermionic continuum. incide with ωp [9], and as temperature or excitation mo- We find a rich resonance structure in the density-density menta were varied, a duplication of the plasma resonance response function, with several peaks both above and be- was observed, with a low-energy branch at energies below low the pair-breaking threshold, which we relate to the 2∆ and a high-energy one above [14–16]. existence of multiple poles in the analytic continuation The existence of such low-energy plasmons was cited as [21, 23, 24] of the propagator the density-phase fluctua- a possible explanation of the critical temperature increase tions. In the quasiphononic regime ωp 2∆ correspond- in cuprates [17]. Besides their importance for the fun- ing to the experimental situation in cuprates [13, 15], the
2 q plasma eigenfrequency behaves as ωp2 + ωq,n 2 where ω q,n We give here its generic expression is the phononic dispersion of the neutral fermion conden- + − sate [14]. Finally, we show that when temperature in- X πij (1 − f+ − f− ) πij (f+ − f− ) Πij (z, q) = − creases towards Tc , the plasmons gradually recover their 2 z − (+ + − ) 2 z − (+ − − )2 2 k normal (undamped) dispersion [25], except in a region of (4) size ∆2 /T around the pair-breaking threshold. All these in terms of the Fermi-Dirac occupation numbers f± = unusal behaviors should have important consequences on 1/(1 + exp(± /T )), free-fermion ξ± = ξq/2±k and BCS the electromagnetic and transport properties of super- energies ± = q/2±k with ξk = k 2 /2m − µ and k = conductors. p ± ξk2 + ∆2 . The coefficients πij can be deduced from Linear response within RPA: We study an homoge- Eq. (36) in [28]. The first term in Eq. (4) gives rise to neous electron gas evolving in a cubic volume V with the pair-breaking continuum {q/2+k + q/2−k }k , gapped a average density ρ, defining the Fermi wavenumber at low q by the pair-breaking threshold 2∆. The second ρ = kF3 /3π 2 . Electrons interact through both the long- term exists only at T 6= 0 and gives rise to the gapless range Coulomb potential VC (r) ∝ 1/r and a short-range quasiparticle-quasihole continuum {q/2+k − q/2−k }k part, responsible for s-wave Cooper pairing, and mod- The spectrum of the collective modes is found as the elled by a contact potential of coupling constant g: poles of χ, hence as the zeros of M : V (r1 , r2 ) = gδ(r1 − r2 ) + VC (r1 − r2 ) (1) detM↓ (zq , q) = 0 (5) We note that a momentum cutoff at the Debye frequency should be used to regularize the divergence caused by The ↓ sign recalls that when the collective mode is cou- the contact potential, although in the following discus- pled to the pair-breaking [21] or quasiparticle-hole con- sion this cutoff can safely be send to infinity. In terms tinuum [23, 31], it is complex energy is found only after of the electron mass m and wavenumber q, the Fourier an analytic continuation of M from upper to lower half- transform of the Coulomb potential is VC (q) = mωp2 /ρq 2 complex plane. (we use ~ = kB = 1 throughout the article). The present analysis of the plasmon dispersion focuses We imagine that the system is driven at fixed frequency on the typical weak-coupling regime of superconductors, ω and wavenumber q by an external field (for example with ∆ much smaller than the Fermi energy F , and the an electromagnetic field) and we study the collective re- excitation wavelength comparable to the Cooper pair size sponse within linear response theory. The response func- ξ = kF /2m∆. In this regime, the fluctuation of the mod- tion can be computed either using a path integral formal- ulus of the order parameter are decoupled from the phase- ism [26] with both a pair and density auxiliary fields, or density fluctuations: in the Random Phase Approximation (RPA), neglecting as in [4] the exchange-scattering diagrams (the effect of detM↓ = 0 ⇐⇒ M11,↓ M33,↓ − M13,↓ 2 = 0 or M22,↓ = 0 those diagrams is discussed in Ref. [27]). In a supercon- (6) ductor, since the density response δρ is coupled to the The second condition gives rise the “pair-breaking” or fluctuations of the order parameter, in phase δθ and a “Higgs” modulus mode which in the weak-coupling regime priori in modulus δ|∆|, the linear response function χ is is insensitive to Coulomb interactions [22, 32]. Here, we a 3 × 3 matrix: study the density-phase modes, fulfilling the first condi- tion. 2i∆δθ(q, ω) uθ (q) Anomalous dispersion of long wavelength plasmons: 2δ|∆(q, ω)| = χ(ω, q) u|∆| (q) , (2) We first study analytically the plasmon dispersion in the gδρ(q, ω) uρ (q) limit q 1/ξ, where, by analogy with the normal case [25], one can expect the quadratic law [7]: where uθ , u|∆| and uρ are respectively the phase, modulus and density driving fields [28]. The response matrix χ is expressed in terms of the bare propagator Π as χ = q2 zq = ω0 + α + O(q 4 ) (7) −M −1 Π with 2m The expansion in powers of q is more easily performed V /g 0 0 M = Π − D and D ≡ 0 V /g 0 (3) using the recombined matrix: 0 0 V /2VC (q) M11 zM13 + 2∆M11 M f= Remark that due to the Coulomb potential M and Π zM13 + 2∆M11 z 2 M33 + 4∆zM13 + 4∆2 M11 do not commute, such that χ is not a symmetric matrix. (8) The matrix Π was computed for instance in Refs. [28–30]. In particular the origin ω0 of the plasma branch is found
3 simply by solving M f33 = 0 to lowest order in q. We have 0 1.696 10 2 2 z2 8 1.5 ρV q ∆Im α/F M33 = f 1− 2 1 2m ωp 6 ∆Re α/F + 0.5 Xm e 33 (1 − f+ − f− ) me − (f+ − f− ) 4 + 2 2 − 2 33 (9) 0 z − (+ + − ) z − (+ − − )2 2 2 3 4 5 6 k ωp /∆ 0 where we have used a sum rule1 to sim- −2 T =0 T /∆ = 10 plify the first line, and we set m e± 33 = T → Tc [ξ+ − ξ− ] [+ ± − ] + − ∓ ξ+ ξ− ∓ ∆ /2+ − . 2 2 The −4 0 0.5 1 1.5 2 2.5 3 3.5 4 4.5 summation on the second line is of order q 4 and will ωp /∆ only affect the expression of the dispersion parameter α. Thus, the origin ω0 of the plasma branch always FIG. 1: Dispersion parameter Re α (multiplied by ∆/F to coincides with the plasma frequency [9] have a finite weak-coupling limit), in function of the plasma frequency at zero (black curve) and high temperature (red ω0 = ωp (10) curve). The normal dispersion 6F /5ωp is shown by the red dotted curve. The value where α changes sign at T = 0 is indi- This expected results shows that superconductivity does cated by the black dotted line. Inset: the damping parameter Im α, which becomes nonzero inside the pair-breaking contin- not affect the departure of the plasma branch. As we uum [2∆, +∞[ (red area). now explain, the situation is quite different for the low-q dispersion and lifetime. To extract the curvature α of the plasma branch, we ωp 2∆, the second term in (12) becomes negligi- expand M f33 to subleading order in q, and consider the 2 ble, such that we recover the normal plasmon dispersion other matrix elements α → 6F /5ωp [25]. In the opposite « quasiphononic » X m+ (1 − f+ − f− ) limit ωp 2∆, which corresponds to the experimental m− 11 (f+ − f− ) V M11 = 11 2 2 − 2 2 − situation of Refs. [13, 15], rather than expanding for fixed z − (+ + − ) z − (+ − − ) g z as prescribed by (7), one should expand for q → 0 while k + e 13 (1 − f+ − f− ) − e (f+ − f− ) keeping z/vF comparable to q [14]. This yields2 X m m M f13 = 2 2 − 2 13 (11) z − (+ + − ) z − (+ − − )2 q k zq −→ ωp2 + c2 q 2 (13) q→0 with m±11 = (+ ± − )(+ − ± ξ+ ξ− ± ∆ )/2+ − and 2 cq/ωp fixed ± e 13 = ±(+ ± − )(2ξ+ ξ− + 2∆ − + − − )∆/2+ − . At m 2 2 2 √ zero temperature, this yields the fully analytic expression where c = vF / 3 is the speed-of-sound of the weakly- of α: interacting condensate of neutral fermions. At nonzero temperature, α depends on the dimen- 6F 32F ∆2 Arcsin (ωp /2∆) sionless temperature T̄ = T /∆ and plasma frequency α= − (12) ω̄p = ωp /∆. We find q 5ωp 15ωp ω 4∆2 − ω 2 p p F 6ω̄p 8 which is shown as a black curve on Fig. 1. This expression α= (I3 + J0 − J2 ) − I1 (14) ∆ 5 3ω̄p remains valid when ωp > 2∆ and the plasma branch is embedded in the pair-breaking continuum. In this case, in terms of the dimensionless integrals In = one should use ωp → ωp + i0+ and Im α < 0 describes R +∞ th(/2T̄ ) R +∞ dξ n (ω̄2 −42 ) and Jn = 2T̄ ω̄2 0 1 dξ with 0 n ch2 (/2T̄ ) the nonzero damping rate of plasmons. We note that p p ξ + 1. The red curve in Fig. 1 shows α in p = 2 the repulsion of the pair-breaking threshold leads to a squareroot divergence of Re α and Im α when approach- the vicinity of the critical temperature T /Tc = 0.9989 ing the pair-breaking threshold respectively from below (T /∆ = 10). We observe that α tends to its normal and above. This opens an interval ωp ∈ [1.696∆, 2∆[ limit 6F /5ωp uniformly except in a neighborhood of size where plasmons have an anomalous negative dispersion ≈ ∆2 /T around the pair-breaking threshold 2∆. There, at the origin (Reα < 0). In the conventional limit the divergence of the real and imaginary part is preserved whenever T < Tc , showing that a regime of anomalous 1 P Explicitely, we have used k [(1 − f+ − f− ) (+ + − ) + − − ξ+ ξ− − ∆ −(f+ − f− ) (+ − − ) + − + ξ+ ξ− + ∆2 ] 2 2 Note that this is consistent with the behavior of α in the limit /2+ − = ρV q 2 /2m. ωp /∆ → 0.
4 plasmon dispersion subsists until the transition to the 2.2 2.5 normal phase. In usual situations, ωp is fixed in units 2.1 of the Fermi energy F , but the ratio ωp /∆(T ) can still 2 be adjusted by varying the temperature. The negative 2 plasma dispersion will thus eventually occur when in- 1.5 ωqmin /∆ qmin ξ creasing the temperature provided ωp < 2∆(T = 0). 1.9 1 Near Tc , we note that the plasma branch may also in- 1.8 teract with the phononic Carlson-Goldman excitations 0.5 [7, 29, 33] describing the motion of the superconduct- 1.7 ing electrons embedded in a majority of normal carri- 1.6 0 ers. A convincing description of this phenomenon re- 1.6 1.70 1.8 2 2.2 2.4 2.6 2.8 quires going beyond the collisionless regime of undamped ωp /∆ fermionic quasiparticles [34], which is beyond the scope of this work. FIG. 2: The dispersion minimum ωqmin and the wavenumber One could be surprised than plasmons remain un- qmin at which it is reached in function of the plasma frequency. damped (Im α = 0) for ωp < 2∆ despite the nonzero For ωp < 1.696, qmin is identically 0 and ωqmin coincides with temperature, which provides a decay channel through ωp (oblique dotted line). In the limit ωp → +∞, qmin diverges linearly and ωqmin tends to 2∆. quasiparticle-quasihole excitations. In fact, to absorb a plasmon (i.e. to satisfy the resonance condition ωp = q+k/2 − q−k/2 ) quasiparticles need to have a wavenum- the analytically continued matrix M . At T = 0, the pair- ber k > 2mωp /q. The plasmon lifetime thus follows an 2 2 breaking threshold 2∆ and the second branching point activation law Imzq ∝ e−2mωp /q T which is exponentially [14] suppressed in the limit ∆/F , T /F → 0 with ωp , q of order ∆, 1/ξ. Intrinsic plasmon damping at ωp < 2∆ is r q2 thus essentially a strong-coupling effect. ω2 = 4∆2 + F (16) 2m We conclude this section by computing the matrix residue Zq = limz→zq (z − zq )χ(z, q), which quantifies divide the real axis in three analyticity windows (I, II and the spectral weight of the plasma resonance. Writ- III, see the inset of Fig. 3), each supporting a separate z→ωp ing χ = −1 − M −1 D and using d(detM )/dz → complex root (ωqI , zqII , zqIII respectively) of Eq. (5). This q→0 suggests a splitting of the plasma resonance into 3 peaks. M11 M22 dMf33 /z 2 dz together with M11 = z 2 M33 /4∆2 = While the quadratic Eq. (7) give the low-q dispersion of −zM13 /2∆ to leading order in q, we obtain, in the phase- ωqI and zqIII (respectively for ωp < 2∆ and ωp > 2∆), the density sector: pole of window II starts from 2∆ and departs following ωp 4m∆ 1 ! a non-integer power-law: ρg q 2 Zq = ∆ ωp2 2m + O(q 2 ) (15) ω /2∆ s 3/2 i±1 4∆2 ρg q 2 p 8 kF q II 7/4 zq = 2∆ − √ 1 − + O q Note that the phase and density excitation channels (re- ∆ 3π 2 ωp2 2m spectively first and second line of Zq ) dominate respec- (17) tively in the limits ωp → 0 and ωp → +∞. where the sign of the real part of zqII − 2∆ is negative Dispersion minimum and resonance splitting at non- if ωp < 2∆ and positive otherwise (in either case zqII re- vanishing wavenumber: Outside the limit qξ 1, we mains outside the natural interval [2∆, ω2 ] of window II). study the dispersion of plasmons by numerically evaluat- Remarkably, when ωp = 2∆ the quadratic law reemerges q2 ing the M matrix. We first characterize on Fig. 2 the dis- zqII = 2∆ − (0.0184 + 0.9953i) ∆F 2m + O(q 4 ). Those re- persion minimum of the plasma branch. For ωp > 1.696, sults are obtained by expanding at low q as prescribed it is reached at a nonzero wavenumber qmin (blue curve by Eq. (10) in [21]. in Fig. 2), such that the band gap of the plasma branch On Fig. 3, we show the dispersion relation of these (black curve) is strictly lower than ωp . As visible on solutions for ωp = 1.9∆. In this case ωqI supports the Fig. 2, this undamped plasma branch at ωq < 2∆ persists main plasma branch departing in ωp (while for ωp > 2∆ even when ωp > 2∆. This is a first sign of the splitting the main branch would be supported by zqIII ), zqII belongs of the plasma resonance. However, in the normal limit to an indirect region of the analytic continuation (specifi- ωp /∆ → +∞ the undamped branch tends uniformly to cally RezqII < 2∆) and zqIII follows rather closely the angu- 2∆ with a vanishingly small spectral weight. lar point ω2 . This subtle analytic structure is reflected in Since we expect the plasma branch to eventually enter frequency behavior of the density-density response func- the pair-breaking continuum, the characterization of the tion shown on Fig. 4. Besides the Dirac peak below 2∆, resonance at finite q requires a numerical exploration of one (black curve) then two (grey curves) broadened peaks
5 3.5 Sec I 5 Sec II qξ = 0.2 3 Sec II, modulus mode qξ = 0.5 Sec III 4 qξ = 1.0 2∆ 2.5 χρρ (ω + i0+ ) ω2 Reωq /∆ 3 2 • Imz 1.5 (I) 2 ωq 2∆ ω2 Rez × × × 0 1 I II III 1 × (II) ×zq(III) zq 0.5 0 0 0.5 1 1.5 2 2.5 3 3.5 1.8 2 2.2 2.4 2.6 2.8 3 qξ ω/∆ FIG. 3: The eigenfrequency Rezq of the plasma branch in FIG. 4: Density-density response of the superconductor in function of the wave vector q (in unit of the inverse pair radius function of the excitation frequency ω at fixed plasma fre- ξ = kF /2m∆), with ωp = 1.9∆. The angular points 2∆ and quency ωp = 1.9∆ and excitation wave number q = 0.2/ξ, ω2 (Eq. (16)) are shown as dotted lines. The analytic windows 0.5ξ and 1.0ξ (corresponding to the vertical dotted lines in are shown in colors: white for ω < ω1 (window I), blue for Fig. 3). The angular points 2∆ and ω2 (q) are marked by verti- ω1 < ω < ω2 (window II) and red for ω > ω2 (window III). cal dotted lines. Besides the Dirac peaks below 2∆, broadened The solution of Eq. (6) in each window in shown as a solid line peaks are visible inside the pair-breaking continuum. Thin in the corresponding color. The inset shows their schematic dashed lines show the modulus response ρg/F M22 (ω + i0+ ). trajectories in the complex plane after analytic continuation. In window II, the pair-breaking mode (solution of M22,↓ = 0) is shown as a dashed line. The dispersion minimum of the undamped solution below 2∆ is shown by the black dot. [2] Romain Grasset, Yann Gallais, Alain Sacuto, Maximi- lien Cazayous, Samuel Mañas Valero, Eugenio Coronado, and Marie-Aude Méasson. Pressure-Induced Collapse of the Charge Density Wave and Higgs Mode Visibility in appear inside the pair-breaking continuum [5] as q is in- 2H-TaS2 . Phys. Rev. Lett., 122:127001, Mar 2019. creased. In the time domain, this remarkable frequency [3] Ryusuke Matsunaga, Yuki I. Hamada, Kazumasa Makise, behavior corresponds to an evolution (after e.g. an elec- Yoshinori Uzawa, Hirotaka Terai, Zhen Wang, and Ryo tromagnetic quench of the electronic density) where the Shimano. Higgs Amplitude Mode in the BCS Supercon- system oscillated at several frequencies: an exponentially ductors Nb1−x Tix N Induced by Terahertz Pulse Excita- decaying high-frequency component and a long-lived low- tion. Phys. Rev. Lett., 111:057002, July 2013. [4] P. W. Anderson. Random-Phase Approximation in the frequency component. Theory of Superconductivity. Phys. Rev., 112:1900–1916, Conclusion: We have described the low-q quadratic December 1958. dispersion of superconducting plasmons in 3D, and the [5] H. A. Fertig and S. Das Sarma. Collective excitations and resonance splitting which occurs when the eigenenergy mode coupling in layered superconductors. Phys. Rev. B, nears the pair-breaking threshold. For a more realistic 44:4480–4494, Sep 1991. description of plasmons in cuprates, our study should [6] R. Côté and A. Griffin. Cooper-pair-condensate fluctu- ations and plasmons in layered superconductors. Phys. be extended to 2D superconductors [35], with possibly Rev. B, 48:10404–10425, Oct 1993. Josephson interlayer couplings [16, 36]. Our work may [7] S.N. Artemenko and A.G. Kobel’kov. Collective modes in also be applied to superfluids of ultracold fermions [37] layered superconductors. Physica C: Superconductivity, where different kind of long-range interactions can be en- 253(3):373–382, 1995. gineered with dipolar atoms [38]. [8] D. van der Marel. Collective modes of spin, density, We acknowledge financial support from the Research phase, and amplitude in exotic superconductors. Phys. Foundation-Flanders (FWO- Vlaanderen) Grant No. Rev. B, 51:1147–1160, January 1995. [9] Yoji Ohashi and Satoshi Takada. On the plasma oscilla- G.0618.20.N, and from the research council of the Uni- tion in superconductivity. Journal of the Physical Society versity of Antwerp. of Japan, 67(2):551–559, 1998. [10] M. Baldo and C. Ducoin. Plasmons in strong supercon- ductors. Physics of Atomic Nuclei, 74(10):1508, 2011. [11] K. Tamasaku, Y. Nakamura, and S. Uchida. Charge dy- namics across the CuO2 planes in La2−x Srx CuO4 . Phys. [1] M.-A. Méasson, Y. Gallais, M. Cazayous, B. Clair, Rev. Lett., 69:1455–1458, Aug 1992. P. Rodière, L. Cario, and A. Sacuto. Amplitude Higgs [12] O. Buisson, P. Xavier, and J. Richard. Observation of mode in the 2H − NbSe2 superconductor. Phys. Rev. B, Propagating Plasma Modes in a Thin Superconducting 89:060503(R), February 2014. Film. Phys. Rev. Lett., 73:3153–3156, December 1994.
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