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Register a new userTwo Mott Insulator Theory of Superconductivity in K$_3$X (X: picene, .. p-terphenyl, .. C$_{60}$)
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G. Baskaran
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We look for unifying aspects behind superconductivity in aromatic hydrocarbon and fullerene family K$_3$X (X: picene, .. p-terphenyl, .. C$_{60}$). Aromatic hydrocarbon molecules support RVB states. Consequent stability (aromaticity) makes them reluctant electron acceptors. We argue that X accepts only two (not all three) electrons from K$_3$ and creates charged RVBs in X$^{2-}$, and becomes a (molecular) Cooper pair box. A weak Josephson coupling between X$^{2-}$ molecules creates a Bose Mott insulator, a potential high Tc superconductor. Remaining lone electron in the complex (K$_3)^{2+}$ occupies a suitable metal orbital hybrid. They hybridize weakly through X$^{2-}$ molecular bridges, to form a half filled band of renormalized K atom orbitals, a Fermionic Mott insulator. An interplay of RVB physics and charge transfer (mutual doping) or external doping leads to superconductivity in one or both Mott insulators. In our theory there is room for room temperature superconductivity.
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Far and mid infrared optical pulses have been shown to induce non-equilibrium unconventional orders in complex materials, including photo-induced ferroelectricity in quantum paraelectrics, magnetic polarization in antiferromagnets and transient superconducting correlations in the normal state of cuprates and organic conductors. In the case of non-equilibrium superconductivity, femtosecond drives have generally resulted in electronic properties that disappear immediately after excitation, evidencing a state that lacks intrinsic rigidity. Here, we make use of a new optical device to drive metallic K$_3$C$_{60}$ with mid-infrared pulses of tunable duration, ranging between one picosecond and one nanosecond. The same superconducting-like optical properties observed over short time windows for femtosecond excitation are shown here to become metastable under sustained optical driving, with lifetimes in excess of ten nanoseconds. Direct electrical probing becomes possible at these timescales, yielding a vanishingly small resistance. Such a colossal positive photo-conductivity is highly unusual for a metal and, when taken together with the transient optical conductivities, it is rather suggestive of metastable light-induced superconductivity.
Cs$_3$C$_{60}$ in the A15 structure is an antiferromagnet at ambient pressure in contrast with other superconducting trivalent fullerides. Superconductivity is recovered under pressure and reaches the highest critical temperature of the family. Comparing density-functional calculations with generalized gradient approximation to the hybrid functional HSE, which includes a suitable component of exchange, we establish that the antiferromagnetic state of Cs$_3$C$_{60}$ is not due to a Slater mechanism, and it is stabilized by electron correlation. HSE also reproduces the pressure-driven metalization. Our findings corroborate previous analyses suggesting that the properties of this compound can be understood as the result of the interplay between electron correlations and Jahn-Teller electron-phonon interaction.
Thin films provide a versatile platform to tune electron correlations and explore new physics in strongly correlated materials. Epitaxially grown thin films of the alkali-doped fulleride K$_{3+x}$C$_{60}$, for example, exhibit various intriguing phenomena, including Mott transitions and superconductivity, depending on dimensionality and doping. Surprisingly, in the trilayer case, a strong electron-hole doping asymmetry has been observed in the superconducting phase, which is absent in the three-dimensional bulk limit. Using density-functional theory plus dynamical mean-field theory, we show that this doping asymmetry results from a substantial charge reshuffling from the top layer to the middle layer. While the nominal filling per fullerene is close to $n=3$, the top layer rapidly switches to an $n=2$ insulating state upon hole doping, which explains the doping asymmetry of the superconducting gap. The interlayer charge transfer and layer-selective metal-insulator transition result from the interplay between crystal field splittings, strong Coulomb interactions, and an effectively negative Hund coupling. This peculiar charge reshuffling is absent in the monolayer system, which is an $n=3$ Mott insulator, as expected from the nominal filling.
Superconductivity and ferromagnetism are two antagonistic cooperative phenomena, which makes it difficult for them to coexist. Here we demonstrate experimentally that they do coexist in EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ with $0.2leq xleq0.4$, in which superconductivity is associated with Fe-3$d$ electrons and ferromagnetism comes from the long-range ordering of Eu-4$f$ moments via Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions. The coexistence is featured by large saturated ferromagnetic moments, high and comparable superconducting and magnetic transition temperatures, and broad coexistence ranges in temperature and field. We ascribe this unusual phenomenon to the robustness of superconductivity as well as the multi-orbital characters of iron pnictides.
Recent experiments have reported the emergence of high temperature superconductivity with critical temperature $T_c$ between 43K and 123K in a potassium doped aromatic hydrocarbon para-Terphenyl or p-Terphenyl. This achievement provides the record for the highest Tc in an organic superconductor overcoming the previous record of Tc=38 K in Cs3C60 fulleride. Here we propose that the driving mechanism is the quantum resonance between superconducting gaps near a Lifshitz transition which belongs to the class of Fano resonances called shape resonances. For the case of p-Terphenyl our numerical solutions of the multi gap equation shows that high Tc is driven by tuning the chemical potential by K doping and it appears only in a narrow energy range near a Lifshitz transition. At the maximum critical temperature, Tc=123K, the condensate in the appearing new small Fermi surface pocket is in the BCS-BEC crossover while the Tc drops below 0.3 K where it is in the BEC regime. Finally we predict the experimental results which can support or falsify our proposed mechanism: a) the variation of the isotope coefficient as a function of the critical temperature and b) the variation of the gaps and their ratios 2Delta/Tc as a function of Tc.
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