Cooling quasiparticles in A${}_3$C${}_{60}$ fullerides by excitonic mid-infrared absorption

Abstract

Long after its discovery superconductivity in alkali fullerides A${}_3$C${}_{60}$ still challenges conventional wisdom. The freshest inroad in such ever-surprising physics is the behaviour under intense infrared (IR) excitation. Signatures attributable to a transient superconducting state extending up to temperatures ten times higher than the equilibrium $T_c\sim$ 20 K have been discovered in K${}_3$C${}_{60}$ after ultra-short pulsed IR irradiation -- an effect which still appears as remarkable as mysterious. Motivated by the observation that the phenomenon is observed in a broad pumping frequency range that coincides with the mid-infrared electronic absorption peak still of unclear origin, rather than to TO phonons as has been proposed, we advance here a radically new mechanism. First, we argue that this broad absorption peak represents a "super-exciton" involving the promotion of one electron from the $t_{1u}$ half-filled state to a higher-energy empty $t_{1g}$ state, dramatically lowered in energy by the large dipole-dipole interaction acting in conjunction with Jahn Teller effect within the enormously degenerate manifold of $\left(t_{1u}{)}^2\right(t_{1g}{)}^1$ states. Both long-lived and entropy-rich because they are triplets, the IR-induced excitons act as a sort of cooling mechanism that permits transient superconductive signals to persist up to much larger temperatures.

16 pages article and 19 pages supplementary notes

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