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.
}, address = {1200 East California Boulevard, Pasadena, California 91125}, advisor = {Hsieh, David}, } @phdthesis{10.7907/0shs-fa90, author = {Shan, Junyi}, title = {Non-Thermal Optical Engineering of Strongly-Correlated Quantum Materials}, school = {California Institute of Technology}, year = {2022}, doi = {10.7907/0shs-fa90}, url = {https://resolver.caltech.edu/CaltechTHESIS:05112022-213102696}, abstract = {This thesis develops multiple optical engineering mechanisms to modulate the electronic, magnetic, and optical properties of strongly-correlated quantum materials, including polar metals, transition metal trichalcogenides, and copper oxides. We established the mechanisms of Floquet engineering and magnon bath engineering, and used optical probes, especially optical nonlinearity, to study the dynamics of these quantum systems.
Strongly-correlated quantum materials host complex interactions between different degrees of freedom, offering a rich phase diagram to explore both in and out of equilibrium. While static tuning methods of the phases have witnessed great success, the emerging optical engineering methods have provided a more versatile platform. For optical engineering, the key to success lies in achieving the desired tuning while suppressing other unwanted effects, such as laser heating.
We used sub-gap optical driving in order to avoid electronic excitation. Therefore, we managed to directly couple to low-energy excitation, or to induce coherent light-matter interactions. In order to elucidate the exact microscopic mechanisms of the optical engineering effects, we performed photon energy-dependent measurements and thorough theoretical analysis. To experimentally access the engineered quantum states, we leveraged various probe techniques, including the symmetry-sensitive optical second harmonic generation (SHG), and performed pump-probe type experiments to study the dynamics of quantum materials.
I will first introduce the background and the motivation of this thesis, with an emphasis on the principles of optical engineering within the big picture of achieving quantum material properties on demand (Chapter I). I will then continue to introduce the main probe technique used in this thesis: SHG. I will also introduce the experimental setups which we developed and where we conducted the works contained in this thesis (Chapter II). In Chapter III, I will introduce an often overlooked aspect of SHG studies – using SHG to study short-range structural correlations. Chapter IV will contain the theoretical analysis and experimental realizations of using sub-gap and resonant optical driving to tune electronic and optical properties of MnPS₃. The main tuning mechanism used in this chapter is Floquet engineering, where light modulates material properties without being absorbed. In Chapter V, I will turn to another useful material property: magnetism. First I will describe the extension of the Floquet mechanism to the renormalization of spin exchange interaction. Then I will switch gears and describe the demagnetization in Sr₂Cu₃O₄Cl₂ by resonant coupling between photons and magnons. I will end the thesis with a brief closing remark (Chapter VI).
}, address = {1200 East California Boulevard, Pasadena, California 91125}, advisor = {Hsieh, David}, } @phdthesis{10.7907/tt7b-fm83, author = {Deshpande, Tejas Makarand}, title = {Development of Tools for Probing Order in Single Crystals Using Electron and Photon Spectroscopy}, school = {California Institute of Technology}, year = {2020}, doi = {10.7907/tt7b-fm83}, url = {https://resolver.caltech.edu/CaltechTHESIS:06022020-110730808}, abstract = {Discovering novel quantum phases of matter–from emergent behavior of strongly-correlated electrons in solid-state systems to superfluidity in quantum degenerate liquids–has been a cornerstone of condensed matter physics for many decades. In the most recent decades, however, the discovery of topological phases has emphasized the importance of symmetry, in addition to the conventional paradigm of symmetry breaking, in the definition of the order parameter, Ψ, and hence the quantum phase it represents. Naturally, novel experimental tools, capable of coupling to said order parameter, directly or indirectly, are required to discover conventionally elusive quantum phases. In this thesis, I will discuss experimental techniques, using both photon and electron spectroscopy, to study exotic electronic phases in single crystals. The thesis will be divided into two unequal parts: (a) the development of a high-energy-resolution sub-Kelvin angle-resolved photoemission spectroscopy apparatus to study 3D time-reversal invariant topological superconductors, and (b) the experiments exploiting the non-linear and time-resolved aspects of femtosecond lasers to study a broad class of many-body systems.
}, address = {1200 East California Boulevard, Pasadena, California 91125}, advisor = {Hsieh, David}, } @phdthesis{10.7907/Z9VD6WHV, author = {Chu, Hao}, title = {Nonlinear and Ultrafast Optical Investigations of Correlated Materials}, school = {California Institute of Technology}, year = {2017}, doi = {10.7907/Z9VD6WHV}, url = {https://resolver.caltech.edu/CaltechTHESIS:06092017-141136995}, abstract = {This thesis comprises studies of 3d-5d transition metal oxides with various degrees of electronic correlation using nonlinear harmonic generation rotational anisotropy as well as time-resolved optical reflectivity methods. Specifically, we explored photo-induced phase transition in Ca2RuO4 and Sr2IrO4, discovered novel electronic phases in doped Sr2IrO4 and Sr3Ir2O7, and investigated different types of antiferromagnetic orders in transition metal trichalcogenides MPX3.
}, address = {1200 East California Boulevard, Pasadena, California 91125}, advisor = {Hsieh, David}, }