Negative to Positive Crossover of Magnetoresistance in Layered WS2 with Ohmic Contact

The discovery of graphene has ignited intensive investigation on two dimensional (2D) materials. Among them, transition metal dichalcogenide (TMDC), a typical representative, attracts much attention due to the excellent performance in field effect transistor (FET) related measurements and applications. Particularly, when TMDC eventually reaches few-layer dimension, a wide range of electronic and optical properties, in striking contrast to bulk samples, are detected. In this Letter, we synthesized single crystalline WS2 nanoflakes by physical vapor deposition (PVD) method and carried out a series of transport measurements of contact resistance and magnetoresistance. Focused ion beam (FIB) technology was applied to deposit Pt electrodes on WS2 flakes. Different from the electron beam lithography (EBL) fabricated electrodes, FIB-deposited leads exhibited ohmic contact, resolving the dilemma of Schottky barrier. Furthermore, a temperature-modulated negative-to-positive transition of magnetoresistance (MR) associated with a crossover of carrier type at similar temperature was demonstrated. Our work offers a pathway to optimize the contact for TMDC and reveals the magnetoresistance characteristics of WS2 flakes, which may stimulate further studies on TMDC and corresponding potential electronic and optoelectronic applications

Ultrafast Optical Control of Order Parameters in Quantum Materials

Developing protocols to realize quantum phases that are not accessible thermally and to manipulate material properties on demand is one of the central problems of modern condensed matter physics. Impulsive electromagnetic stimulus provides an extensive playground not only to exert desired control over the material macroscopic properties but also to optically detect the underlying microscopic mechanisms. Two indispensable components form the cornerstone to realize these goals: a meticulous comprehension of light-induced phenomena and a suitable and versatile platform. Abundant photoinduced phenomena emerge upon light irradiation. A collective oscillation of order parameter can be launched and probed in the weak perturbation regime; further increasing light intensity can transiently modulate the free-energy landscape, inducing a suppression, enhancement, reversal, and switch of order parameters; in the strong non-perturbative excitation regime, the system can be driven nonlinearly with microscopic coupling parameters modified. Understanding these light driven emergent phenomena lays the foundation of optical control and novel functionalities. Quantum materials, embodying a large portfolio of topological and strongly correlated compounds, afford an exceptional venue to realize optical control. Owing to the complex interplay between the charge, spin, orbital, and lattice degrees of freedom, a rich phase diagram can be generated with various phases that are selectively and independently accessible via optical perturbations. They hence offer a wealth of opportunities to not only improve our comprehension of the underlying physics but also develop the next generation of ultrafast technologies. In Chapter I of this thesis, I will first cover a multitude of light-induced emergent phenomena in quantum materials under the framework of time-dependent Landau theory, Keldysh theory, and Floquet theory, and then introduce several canonical microscopic models to quantitatively rationalize the intra- and interactions between different degrees of freedom in quantum materials. As the necessary theoretical background is established, three main experimental techniques that have been extensively utilized in my research: time-resolved reflectivity and Kerr effect, time-resolved second harmonic generation rotational anisotropy, and coherent phonon spectroscopy will be introduced in Chapter II. In Chapter III, I will demonstrate that a light-induced topological phase transition can be engendered concomitant with an inverse-Peierls structural phase transition in elemental Te. In Chapter IV, I will describe signatures of ultrafast reversal of excitonic order in excitonic insulator candidate Ta2NiSe5 and substantiate a manipulation of the reversal as well as the Higgs mode with tailored light pulses. In Chapter V, a light-induced switch of spin-orbit-coupled quadrupolar order in multiband Mott insulator Ca2RuO4 will be introduced. In Chapter VI, a Keldysh tuning of nonlinear carrier excitation and Floquet bandwidth renormalization in strongly driven Ca2RuO4 will be covered.</p

Keldysh space control of charge dynamics in a strongly driven Mott insulator

The fate of a Mott insulator under strong low frequency optical driving conditions is a fundamental problem in quantum many-body dynamics. Using ultrafast broadband optical spectroscopy, we measured the transient electronic structure and charge dynamics of an off-resonantly pumped Mott insulator Ca$_2$RuO$_4$. We observe coherent bandwidth renormalization and nonlinear doublon-holon pair production occurring in rapid succession within a sub-100 femtosecond pump pulse duration. By sweeping the electric field amplitude, we demonstrate continuous bandwidth tuning and a Keldysh cross-over from a multi-photon absorption to quantum tunneling dominated pair production regime. Our results provide a procedure to control coherent and nonlinear heating processes in Mott insulators, facilitating the discovery of novel out-of-equilibrium phenomena in strongly correlated systems.Comment: 6 pages main text, 4 figures, 16 pages supplementary informatio