We report on systematic investigation of hot carrier dynamics in Ti4O7 by ultrafast time-resolved optical reflectivity. We find the transient indication for its two-step insulator-metal (I-M) transition, in which two phase transitions occur from long-range order bipolaron low-temperature insulating (LI) phase to disordered bipolaron high-temperature insulating (HI) phase at Tc1 and to free carrier metallic (M) phase at Tc2. Our results reveal that photoexcitation can effectively lower down both Tc1 and Tc2 with pump fluence increasing, allowing a light-control of I-M transition. We address a phase diagram that provides a framework for the photoinduced I-M transition and helps the potential use of Ti4O7 for photoelectric and thermoelectric devices.
We investigate the hot carrier dynamics of ZrTe$_5$ by ultrafast time-resolved optical reflectivity. Our results reveal a phonon-mediated across-gap recombination, consistent with its temperature-dependent gap nature as observed previously by photoemission. In addition, two distinct relaxations with a kink feature right after initial photoexcitation are well resolved, suggesting the complexity of electron thermalization process. Our findings indicate that correlated many-body effects play important role for the transient dynamics of ZrTe$_5$.
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.
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.
We investigate ultrafast dynamics from photoinduced reflectivity of Sr2RhO4 by using femtosecond near-infrared pulses. We observe a clear temperature-dependent anomaly in its electronic dynamics which slows down below 160 K. In addition, coherent oscillations of the A1g symmetric 5.3-THz phonon exhibit a 90-degree shift in its initial phase across TS, indicating a structural change in octahedral rotation distortions. We propose that octahedral structure in Sr2RhO4 evolves at around TS, and it can influence on the non-equilibrium dynamics of photoinduced carriers as well as real-time phonon responses.
The control of materials properties with light is a promising approach towards the realization of faster and smaller electronic devices. With phases that can be controlled via strain, pressure, chemical composition or dimensionality, nickelates are good candidates for the development of a new generation of high performance and low consumption devices. Here we analyze the photoinduced dynamics in a single crystalline NdNiO$_3$ film upon excitation across the electronic gap. Using time-resolved reflectivity and resonant x-ray diffraction, we show that the pump pulse induces an insulator-to-metal transition, accompanied by the melting of the charge order. Finally we compare our results to similar studies in manganites and show that the same model can be used to describe the dynamics in nickelates, hinting towards a unified description of these photoinduced phase transitions.
X. C. Nie
,Hai-Ying Song
,Xiu Zhang
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(2018)
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"Photoinduced two-step insulator-metal transition in Ti4O7 by ultrafast time-resolved optical reflectivity"
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Xuchen Nie
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