No Arabic abstract
We utilize near-infrared pump and mid-infrared probe spectroscopy to investigate the ultrafast electronic response of pressurized VO$_2$. Distinct pump-probe signals and a pumping threshold behavior are observed even in the pressure-induced metallic state showing a noticeable amount of localized electronic states. Our results are consistent with a scenario of a bandwidth-controlled Mott-Hubbard transition.
The insulator-to-metal transition (IMT) of the simple binary compound of vanadium dioxide VO$_2$ at $sim 340$ K has been puzzling since its discovery more than five decades ago. A wide variety of photon and electron probes have been applied in search of a satisfactory microscopic mechanistic explanation. However, many of the conclusions drawn have implicitly assumed a {em homogeneous} material response. Here, we reveal inherently {em inhomogeneous} behavior in the study of the dynamics of individual VO$_2$ micro-crystals using a combination of femtosecond pump-probe microscopy with nano-IR imaging. The time scales of the photoinduced bandgap reorganization in the ultrafast IMT vary from $simeq 40 pm 8$ fs, i.e., shorter than a suggested phonon bottleneck, to $sim 200pm20$ fs, with an average value of $80 pm 25$ fs, similar to results from previous studies on polycrystalline thin films. The variation is uncorrelated with crystal size, orientation, transition temperature, and initial insulating phase. This together with details of the nano-domain behavior during the thermally-induced IMT suggests a significant sensitivity to local variations in, e.g., doping, defects, and strain of the microcrystals. The combination of results points to an electronic mechanism dominating the photoinduced IMT in VO$_2$, but also highlights the difficulty of deducing mechanistic information where the intrinsic response in correlated matter may not yet have been reached.
Strain engineering is a powerful technology which exploits stationary external or internal stress of specific spatial distribution for controlling the fundamental properties of condensed materials and nanostructures. This advanced technique modulates in space the carrier density and mobility, the optical absorption and, in strongly correlated systems, the phase, e.g. insulator/metal or ferromagnetic/paramagnetic. However, while successfully accessing nanometer length scale, strain engineering is yet to be brought down to ultrafast time scales allowing strain-assisted control of state of matter at THz frequencies. In our work we demonstrate a control of an optically-driven insulator-to-metal phase transition by a picosecond strain pulse, which paves a way to ultrafast strain engineering in nanostructures with phase transitions. This is realized by simultaneous excitation of VO$_2$ nanohillocks by a 170-fs laser and picosecond strain pulses finely timed with each other. By monitoring the transient optical reflectivity of the VO$_2$, we show that strain pulses, depending on the sign of the strain at the moment of optical excitation, increase or decrease the fraction of VO$_2$ which undergoes an ultrafast phase transition. Transient strain of moderate amplitude $sim0.1$% applied during ultrafast photo-induced non-thermal transition changes the fraction of VO$_2$ in the laser-induced phase by $sim1$%. By contrast, if applied after the photo-excitation when the phase transformations of the material are governed by thermal processes, transient strain of the same amplitude produces no measurable effect on the phase state.
Phase transitions driven by ultrashort laser pulses have attracted interest both for understanding the fundamental physics of phase transitions and for potential new data storage or device applications. In many cases these transitions involve transient states that are different from those seen in equilibrium. To understand the microscopic properties of these states, it is useful to develop elementally selective probing techniques that operate in the time domain. Here we show fs-time-resolved measurements of V Ledge Resonant Inelastic X-Ray Scattering (RIXS) from the insulating phase of the Mott- Hubbard material V2O3 after ultrafast laser excitation. The probed orbital excitations within the d-shell of the V ion show a sub-ps time response, which evolve at later times to a state that appears electronically indistinguishable from the high-temperature metallic state. Our results demonstrate the potential for RIXS spectroscopy to study the ultrafast orbital dynamics in strongly correlated materials.
On the basis of experimental thermoelectric power results and ab initio calculations, we propose that a metal-insulator transition takes place at high pressure (approximately 6 GPa) in MgV_2O_4.
We have studied the effect of pressure on the pyrochlore iridate Eu$_2$Ir$_2$O$_7$, which at ambient pressure has a thermally driven insulator to metal transition at $T_{MI}sim120$,K. As a function of pressure the insulating gap closes, apparently continuously, near $P sim 6$,GPa. However, rather than $T_{MI}$ going to zero as expected, the insulating ground state crosses over to a metallic state with a negative temperature coefficient of resistivity, calling into question the true nature of both ground states. The high temperature state also crosses over near 6 GPa, from an incoherent to a conventional metal, suggesting a connection between the high and the low temperature states.