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arXiv:2312.04034 · Physical Review Materials

Pseudogap formation in organic superconductors

Shusaku Imajo, Takuya Kobayashi, Y. Matsumura, Taiki Maeda, Yasuhiro Nakazawa, Hiromi Taniguchi, Koichi Kindo

Published Dec 26, 2023• 9 citations
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Abstract

The condensation of paired fermions into superfluid states changes progressively depending on the coupling strength. At the midpoint of the crossover between Bardeen-Cooper-Schrieffer (BCS) weak-coupling and Bose-Einstein condensate (BEC) strong-coupling limits, paired fermions condensate most robustly, thereby leading to the emergence of a pseudogap due to enhanced pairing fluctuations. In the case of electrons in solids, excessively strong interactions often induce competing electronic orders instead of strong-coupling superconductivity, and experimental comprehension of the pseudogap remains incomplete. In this study, we provide experimental evidence demonstrating the opening of a pseudogap, marking the incipient stage of the BCS-BEC crossover in the organic system $\ensuremath{\kappa}\text{\ensuremath{-}}(\mathrm{BEDT}\text{\ensuremath{-}}{\mathrm{TTF})}_{2}X$. By controlling electron correlations, we investigate the thermodynamic properties of the BCS-BEC crossover and pseudogap phase. Since the superconductivity of $\ensuremath{\kappa}\text{\ensuremath{-}}{(\text{BEDT}\text{\ensuremath{-}}\mathrm{TTF})}_{2}X$ arises from a simple Fermi liquid that does not exhibit any other electronic orders, our study sheds light on the inherent nature of the BCS-BEC crossover.

DOI
10.1103/physrevmaterials.7.124803

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The condensation of paired fermions into superfluid states changes progressively depending on the coupling strength. At the midpoint of the crossover between Bardeen-Cooper-Schrieffer (BCS) weak-coupling and Bose-Einstein condensate (BEC) strong-coupling limits, paired fermions condensate most robustly, thereby leading to the emergence of a pseudogap due to enhanced pairing fluctuations. In the case of electrons in solids, excessively strong interactions often induce competing electronic orders instead of strong-coupling superconductivity, and experimental comprehension of the pseudogap remains incomplete. In this study, we provide experimental evidence demonstrating the opening of a pseudogap, marking the incipient stage of the BCS-BEC crossover in the organic system \ensuremathκ\ensuremath-(BEDT\ensuremath-TTF)2X\ensuremath{\kappa}\text{\ensuremath{-}}(\mathrm{BEDT}\text{\ensuremath{-}}{\mathrm{TTF})}_{2}X\ensuremathκ\ensuremath-(BEDT\ensuremath-TTF)2​X. By controlling electron correlations, we investigate the thermodynamic properties of the BCS-BEC crossover and pseudogap phase. Since the superconductivity of \ensuremathκ\ensuremath-(BEDT\ensuremath-TTF)2X\ensuremath{\kappa}\text{\ensuremath{-}}{(\text{BEDT}\text{\ensuremath{-}}\mathrm{TTF})}_{2}X\ensuremathκ\ensuremath-(BEDT\ensuremath-TTF)2​X arises from a simple Fermi liquid that does not exhibit any other electronic orders, our study sheds light on the inherent nature of the BCS-BEC crossover.
We theoretically investigate the uniform spin susceptibility $\ensuremath{\chi}$ in the superfluid phase of an ultracold Fermi gas in the region of the Bardeen-Cooper-Schrieffer--Bose-Einstein-condensate (BCS-BEC) crossover. In our previous paper [H. Tajima et al., Phys. Rev. A 89, 033617 (2014)], including pairing fluctuations within an extended TTT-matrix approximation (ETMA), we showed that strong pairing fluctuations cause the so-called spin-gap phenomenon, where $\ensuremath{\chi}$ is anomalously suppressed even in the normal state near the superfluid phase transition temperature Tc{T}_{\mathrm{c}}Tc​. In this paper, we extend this work to the superfluid phase below Tc{T}_{\mathrm{c}}Tc​, to clarify how this many-body phenomenon is affected by the superfluid order. From the comparison of the ETMA $\ensuremath{\chi}$ with the Yosida function describing the spin susceptibility in a weak-coupling BCS superfluid, we identify the region where pairing fluctuations crucially affect this magnetic quantity below Tc{T}_{\mathrm{c}}Tc​ in the phase diagram with respect to the strength of a pairing interaction and the temperature. This spin-gap regime is found to be consistent with the previous pseudogap regime determined from the pseudogapped density of states. We also compare our results with a recent experiment on a 6Li^{6}\mathrm{Li}6Li Fermi gas. Since the spin susceptibility is sensitive to the formation of spin-singlet preformed pairs, our results would be useful for the study of pseudogap physics in an ultracold Fermi gas on the viewpoint of the spin degrees of freedom.
We demonstrate the rise-and-fall of multiple pseudogaps in the Bardeen-Cooper-Schrieffer-Bose-Einstein-condensation (BCS-BEC) crossover in two-band fermionic systems having different pairing strengths in the deep band and in the shallow band. The striking features of this phenomenon are an unusual many-body screening of pseudogap state and the importance of pair-exchange couplings, which induces multiple pseudogap formation in the two bands. The multi-band configuration suppresses pairing fluctuations and the pseudogap opening in the strongly-interacting shallow band at small pair-exchange couplings by screening effects, with possible connection to the pseudogap phenomenology in iron based superconductors. On the other hand, the multiple pseudogap mechanism accompanies with the emergence of binary preformed Cooper pairs originating from interplay between intra-band and pair-exchange couplings.
The pseudogap state of cuprate high-temperature superconductors has been often viewed as either a yet unknown competing order or a precursor state to superconductivity. While awaiting the resolution of the pseudogap problem in cuprates, we demonstrate that local pairing fluctuations, vortex liquid dynamics, and other precursor phenomena can emerge quite generally whenever fermionic excitations remain gapped across the superconducting transition, regardless of the gap origin. Our choice of a tractable model is a lattice band insulator with short-range attractive interactions between fermions in the sss-wave channel. An effective crossover between Bardeen-Cooper-Schrieffer (BCS) and Bose-Einstein condensate (BEC) regimes can be identified in any band insulator above two dimensions, while in two dimensions only the BEC regime exists. The superconducting transition is ``unconventional'' (non-pair-breaking) in the BEC regime, identified by either the bosonic mean field or XY\mathit{XY}XY universality class. The insulator adjacent to the superconductor in the BEC regime is a bosonic Mott insulator of Cooper pairs, which may be susceptible to charge density wave ordering. We construct a function of the many-body excitation spectrum whose nonanalytic changes define a sharp distinction between band and Mott insulators. The corresponding ``second-order transition'' can be observed out of equilibrium by driving a Cooper pair laser in the Mott insulator. We explicitly show that the gap for charged bosonic excitations lies below the threshold for Cooper pair breakup in any BEC regime, despite quantum fluctuations. Our discussion ends with a view of possible consequences for cuprates, where antinodal pair dynamics has certain features in common with our simple sss-wave picture.
Bardeen-Schrieffer-Cooper (BCS) and Bose-Einstein condensation (BEC) occur at opposite limits of a continuum of pairing interaction strength between fermions. A crossover between these limits is readily observed in a cold atomic Fermi gas. Whether it occurs in other systems such as the high temperature superconducting cuprates has remained an open question. We uncover here unambiguous evidence for a BCS-BEC crossover in the cuprates by identifying a universal magic gap ratio 2Δ/k_{B}T_{c}≈6.5 (where Δ is the pairing gap and T_{c} is the transition temperature) at which paired fermion condensates become optimally robust. At this gap ratio, corresponding to the unitary point in a cold atomic Fermi gas, the measured condensate fraction N_{0} and the height of the jump δγ(T_{c}) in the coefficient γ of the fermionic specific heat at T_{c} are strongly peaked. In the cuprates, δγ(T_{c}) is peaked at this gap ratio when Δ corresponds to the antinodal spectroscopic gap, thus reinforcing its interpretation as the pairing gap. We find the peak in δγ(T_{c}) also to coincide with a normal state maximum in γ, which is indicative of a pairing fluctuation pseudogap above T_{c}.
Bardeen-Cooper-Schrieffer (BCS) superfluidity and Bose-Einstein condensation (BEC) are the two extreme limits of the ground state of the paired fermion systems. We report crossover behavior from the BCS limit to the BEC limit realized by varying carrier density in a two-dimensional superconductor, electron-doped zirconium nitride chloride. The phase diagram, established by simultaneous measurements of resistivity and tunneling spectra under ionic gating, demonstrates a pseudogap phase in the low-doping regime. The ratio of the superconducting transition temperature and Fermi temperature in the low-carrier density limit is consistent with the theoretical upper bound expected in the BCS-BEC crossover regime. These results indicate that the gate-doped semiconductor provides an ideal platform for the two-dimensional BCS-BEC crossover without added complexities present in other solid-state systems.
The cold atomic Fermi gas has become the essential paradigm for understanding the crossover between the weak coupling Bardeen-Schrieffer-Cooper (BCS) and strong coupling Bose-Einstein Condensation (BEC) regimes of paired fermion condensates. On tuning the pairing interactions through the crossover, a superfluid becomes optimally robust between the BCS and BEC regimes at what is referred to as the unitary point, giving rise to a maximally peaked phase transition anomaly in the specific heat. We find here, by tracing the jump Δγ\Delta\gammaΔγ in the electronic specific heat coefficient γ\gammaγ at the transition temperature TcT_{\rm c}Tc​ as a function of the gap ratio 2Δ/kBTc2\Delta/k_{\rm B}T_{\rm c}2Δ/kB​Tc​, that a similar thermodynamic signature occurs in the high-TcT_{\rm c}Tc​ superconducting cuprates. On taking Δ\DeltaΔ as the pairing gap in a cold atomic Fermi gas and as the antinodal pseudogap energy in the cuprates, we find Δγ\Delta\gammaΔγ to be asymmetrically peaked at the same value of 2Δ/kBTc≈2\Delta/k_{\rm B}T_{\rm c}\approx2Δ/kB​Tc​≈ 6.5. Its observation in the cuprates and coincidence with a normal state maximum in γ\gammaγ provides a previously overlooked thermodynamic signature of an optimally robust condensate at the BCS-BEC crossover.