Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userFirst-order kinetics bottleneck during photoinduced ultrafast insulator-metal transition in 3D orbitally-driven Peierls insulator CuIr$_{2}$S$_{4}$
95
0
0.0
(
0
)
Authors
M. Naseska
Ask ChatGPT about the research
No Arabic abstract
The spinel-structure CuIr$_{2}$S$_{4}$ compound displays a rather unusual orbitally-driven three-dimensional Peierls-like insulator-metal transition. The low-T symmetry-broken insulating state is especially interesting due to the existence of a metastable irradiation-induced disordered weakly conducting state. Here we study intense femtosecond optical pulse irradiation effects by means of the all-optical ultrafast multi-pulse time-resolved spectroscopy. We show that the structural coherence of the low-T broken symmetry state is strongly suppressed on a sub-picosecond timescale above a threshold excitation fluence resulting in a structurally inhomogeneous transient state which persists for several-tens of picoseconds before reverting to the low-T disordered weakly conducting state. The electronic order shows a transient gap filling at a significantly lower fluence threshold. The data suggest that the photoinduced-transition dynamics to the high-T metallic phase is governed by first-order-transition nucleation kinetics that prevents the complete ultrafast structural transition even when the absorbed energy significantly exceeds the equilibrium enthalpy difference to the high-T metallic phase. In contrast, the dynamically-decoupled electronic order is transiently suppressed on a sub-picosecond timescale rather independently due to a photoinduced Mott transition.
rate research
Read More
Ultrafast dynamics across the photoinduced three-dimensional Peierls-like insulator-metal (IM) transition in CuIr$_{2}$S$_{4}$ was investigated by means of the all-optical ultrafast multi-pulse time-resolved spectroscopy. The structural coherence of the low-$T$ broken symmetry state is strongly suppressed on a sub-picosecond timescale above a threshold excitation fluence of $F_{mathrm{c}}approx3$ mJ/cm$^{2}$ (at 1.55-eV photon energy) resulting in a structurally inhomogeneous transient state which persists for several-tens of picoseconds before reverting to the original low-$T$ state. The electronic order shows a transient gap filling at a significantly lower fluence threshold of $sim0.6$~mJ/cm$^{2}$. The data suggest that the photoinduced-transition structural dynamics to the high-$T$ metallic phase is governed by first-order-transition nucleation kinetics that prevents the complete structural transition into the high-$T$ phase even at excitation fluences significantly larger than $F_{mathrm{c}}$. In contrast, the dynamically-decoupled electronic order is suppressed rather independently due to a photoinduced Mott transition.
Ultrafast transient reflectivity across the unusual three-dimensional Peierls-like insulator-metal (IM) transition in CuIr_{2}S_{4} was measured as a function of temperature. The low-temperature insulating-phase transient response is dominated by broken-symmetry-induced coherent lattice oscillations that abruptly vanish at the IM transition. The coherent mode spectra are consistent with Raman spectra reported in literature. The origin of the broken-symmetry-induced is also briefly discussed.
We present measurements of the optical spectra on single crystals of spinel-type compound cis. This material undergoes a sharp metal-insulator transition at 230 K. Upon entering the insulating state, the optical conductivity shows an abrupt spectral weight transfer and an optical excitation gap opens. In the metallic phase, Drude components in low frequencies and an interband transition peak at $sim 2 eV$ are observed. In the insulating phase, a new peak emerges around $0.5 eV$. This peak is attributed to the transition of electrons from the occupied Ir$^{3+}$ $t_{2g}$ state to upper Ir$^{4+}$ $t_{2g}$ subband resulting from the dimerization of Ir$^{4+}$ ions in association with the simultaneous formations of Ir$^{3+}$ and Ir$^{4+}$ octamers as recently revealed by the x-ray diffraction experiment. Our experiments indicate that the band structure is reconstructed in the insulating phase due to the sudden structural transition.
The metal-insulator transition (MIT) is one of the most dramatic manifestations of electron correlations in materials. Various mechanisms producing MITs have been extensively considered, including the Mott (electron localization via Coulomb repulsion), Anderson (localization via disorder) and Peierls (localization via distortion of a periodic 1D lattice). One additional route to a MIT proposed by Slater, in which long-range magnetic order in a three dimensional system drives the MIT, has received relatively little attention. Using neutron and X-ray scattering we show that the MIT in NaOsO3 is coincident with the onset of long-range commensurate three dimensional magnetic order. Whilst candidate materials have been suggested, our experimental methodology allows the first definitive demonstration of the long predicted Slater MIT. We discuss our results in the light of recent reports of a Mott spin-orbit insulating state in other 5d oxides.
Crystal structure of spinel compound CuIr$_{2}$S$_{4}$ was examined by powder X-ray diffraction for the insulating phase below the metal-insulator transition at $T_{MI}$ = 230 K. The superstructure spots are reproduced by considering the displacement of Ir atoms. A model for the ionic ordering of Ir$^{4+}$ and Ir$^{3+}$ with the same number is proposed for the insulating phase on the basis of the structural analysis. The model suggests that the structural change at $T_{MI}$ is driven by the formation Ir$^{4+}$ dimers. In addition, we found that the superstructure spots becomes significantly weak below 60 K, without any significant effects on electric and magnetic properties. Possible mechanism for the transition is discussed.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
