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326 - M. Buzzi , D. Nicoletti , S. Fava 2021
Resonant optical excitation of certain molecular vibrations in $kappa$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br has been shown to induce transient superconducting-like optical properties at temperatures far above equilibrium $T_c$. Here, we report experiments a cross the bandwidth-tuned phase diagram of this class of materials, and study the Mott insulator $kappa$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl and the metallic compound $kappa$-(BEDT-TTF)$_2$Cu(NCS)$_2$. We find non-equilibrium photoinduced superconductivity only in $kappa$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br, indicating that the proximity to the Mott insulating phase and possibly the presence of preexisting superconducting fluctuations are pre-requisites for this effect.
In triangular lattice structures, spatial anisotropy and frustration can lead to rich equilibrium phase diagrams with regions containing complex, highly entangled states of matter. In this work we study the driven two-rung triangular Hubbard model an d evolve these states out of equilibrium, observing how the interplay between the driving and the initial state unexpectedly shuts down the particle-hole excitation pathway. This restriction, which symmetry arguments fail to predict, dictates the transient dynamics of the system, causing the available particle-hole degrees of freedom to manifest uniform long-range order. We discuss implications of our results for a recent experiment on photo-induced superconductivity in ${rm kappa - (BEDT-TTF)_{2}Cu[N(CN)_{2}]Br}$ molecules.
97 - M. Budden , T. Gebert , M. Buzzi 2020
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 super conducting 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.
Superconductivity in organic conductors is often tuned by the application of chemical or external pressure. With this type of tuning, orbital overlaps and electronic bandwidths are manipulated, whilst the properties of the molecular building blocks r emain virtually unperturbed.Here, we show that the excitation of local molecular vibrations in the charge-transfer salt $kappa-(BEDT-TTF)_2Cu[N(CN)_2]Br$ induces a colossal increase in carrier mobility and the opening of a superconducting-like optical gap. Both features track the density of quasi-particles of the equilibrium metal, and can be achieved up to a characteristic coherence temperature $T^* approxeq 50 K$, far higher than the equilibrium transition temperature $T_C = 12.5 K$. Notably, the large optical gap achieved by photo-excitation is not observed in the equilibrium superconductor, pointing to a light induced state that is different from that obtained by cooling. First-principle calculations and model Hamiltonian dynamics predict a transient state with long-range pairing correlations, providing a possible physical scenario for photo-molecular superconductivity.
Optical excitation at terahertz frequencies has emerged as an effective means to manipulate complex solids dynamically. In the molecular solid K3C60, coherent excitation of intramolecular vibrations was shown to transform the high temperature metal i nto a non-equilibrium state with the optical conductivity of a superconductor. Here we tune this effect with hydrostatic pressure, and we find it to disappear around 0.3 GPa. Reduction with pressure underscores the similarity with the equilibrium superconducting phase of K3C60, in which a larger electronic bandwidth is detrimental for pairing. Crucially, our observation excludes alternative interpretations based on a high-mobility metallic phase. The pressure dependence also suggests that transient, incipient superconductivity occurs far above the 150 K hypothesised previously, and rather extends all the way to room temperature.
Using photo-emission electron microscopy with X-ray magnetic circular dichroism as a contrast mechanism, new insights into the all-optical magnetization switching (AOS) phenomenon in GdFe based rare-earth transition metal ferrimagnetic alloys are pro vided. From a sequence of static images taken after single linearly polarized laser pulse excitation, the repeatability of AOS can be measured with a correlation coefficient. It is found that low coercivity enables thermally activated domain wall motion, limiting in turn the repeatability of the switching. Time-resolved measurement of the magnetization dynamics reveal that while AOS occurs below and above the magnetization compensation temperature $T_text{M}$, it is not observed in GdFe samples where $T_text{M}$ is absent. Finally, AOS is experimentally demonstrated against an applied magnetic field of up to 180 mT.
The antiferromagnetic (AFM) to ferromagnetic (FM) first order phase transition of an epitaxial FeRh thin-film has been studied with x-ray magnetic circular dichroism using photoemission electron microscopy. The FM phase is magnetized in-plane due to shape anisotropy, but the magnetocrystalline anisotropy is negligible and there is no preferred in-plane magnetization direction. When heating through the AFM to FM phase transition the nucleation of the FM phase occurs at many independent nucleation sites with random domain orientation. The domains subsequently align to form the final FM domain structure. We observe no pinning of the FM domain structure.
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