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Register a new userElectronic correlations stabilize the antiferromagnetic Mott state in Cs$_3$C$_{60}$
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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.
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Former extensive studies of superconductivity in the textit{A}$_{3}$C$_{60}$ compounds, where textit{A} is an alkali, have led to consider that Bardeen Cooper Schrieffer (BCS) electron-phonon pairing prevails in those compounds, though the incidence of electronic Coulomb repulsion has been highly debated. The discovery of two isomeric fulleride compounds Cs$_{3}$C$_{60}$ which exhibit a transition with pressure from a Mott insulator (MI) to a superconducting (SC) state clearly re-opens that question. Using pressure ($p$) as a single control parameter of the C$_{60}$ balls lattice spacing, one can now study the progressive evolution of the SC properties when the electronic correlations are increased towards the critical pressure $p_{c}$ of the Mott transition. We have used $^{13}$C and $^{133}$Cs NMR measurements on the cubic phase A15-Cs$_{3}$C$_{60}$ just above $p_{c}=5.0(3)$ kbar, where the SC transition temperature $T_{c}$ displays a dome shape with decreasing cell volume. From the $T$ dependence below $T_{c}$ of the nuclear spin lattice relaxation rate $(T_{1})^{-1}$ we determine the electronic excitations in the SC state, that is $2Delta$, the SC gap value. We find that $2Delta $ increases with decreasing $p$ towards $p_{c}$, where $T_{c}$ decreases on the SC dome, so that $2Delta /k_{B}T_{c}$ increases regularly upon approaching the Mott transition. These results bring clear evidence that the increasing correlations near the Mott transition are not significantly detrimental to SC. They rather suggest that repulsive electron interactions might even reinforce elecron-phonon SC, being then partly responsible for the large $T_{c}$ values, as proposed by theoretical models taking the electronic correlations as a key ingredient.
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.
We report $^{133}$Cs NMR and $^{75}$As Nuclear Quadrupole Resonance (NQR) measurements on the normal metallic state above $T_c$ of a quasi-one-dimensional superconductor Cs$_2$Cr$_3$As$_3$ ($T_c < 1.6$~K). From the $^{133}$Cs NMR Knight shift $^{133}K$ measured at the Cs1 site, we show that the uniform spin susceptibility $chi_{spin}$ increases from 295~K to $sim$ 60~K, followed by a mild suppression; $chi_{spin}$ then levels off below $sim$10~K. In contrast, a vanishingly small magnitude of $^{133}K$ indicates that Cs2 sites contribute very little to electrical conduction and the exchange interactions between 3d electrons at Cr sites. Low frequency Cr spin dynamics, reflected on $^{75}$As $1/T_1T$ (the nuclear spin-lattice relaxation rate $1/T_1$ divided by temperature $T$), shows an analogous trend as $chi_{spin}$. Comparison with the results of $1/T_1T$ near $T_c$ with Rb$_2$Cr$_3$As$_3$ ($T_c=6.1$~K) and Rb$_2$Cr$_3$As$_3$ ($T_c=4.8$~K) establishes a systematic trend that substitution of K$^{+}$ ions with larger alkali ions progressively suppresses Cr spin fluctuations together with $T_c$.
We report on a contrasting behavior of the in-plane and out-of-plane magnetoresistance (MR) in heavily underdoped antiferromagnetic (AF) YBa_2Cu_3O_{6+x} (x<0.37). The out-of-plane MR (I//c) is positive over most of the temperature range and shows a sharp increase, by about two orders of magnitude, upon cooling through the Neel temperature T_N. A contribution associated with the AF correlations is found to dominate the out-of-plane MR behavior for H//c from far above T_N, pointing to the key role of spin fluctuations in the out-of-plane transport. In contrast, the transverse in-plane MR (I//a(b);H//c) appears to be small and smooth through T_N, implying that the development of the AF order has little effect on the in-plane resistivity.
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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