複雜性過渡金屬氧化物(complex transition-metal oxides)具有十分迥異且豐富的物理性質，其中包含多鐵性(multiferroicity)、龐磁阻、高溫超導、焦電、介電、熱電、導/半導性與光性等等，是以在固態物理的領域中備受關注。其複雜性來源為在不同晶格位置上關聯性電子間(correlated electrons)的電荷、自旋與軌道自由度間不可忽視的交互作用。這些交互作用項能量相近並彼此競爭，使得同個複雜性氧化物系統在不同條件下能表現出完全不同的電性、磁性等物理特性。在過往的探索中，主要是透過外加電場、磁場與應力等因素的施加來調控複雜性氧化物的強關聯物理現象。而本篇研究論文則將專注於使用光來控制強關聯系統中各種豐富的功能性，希望透過此額外的調控自由度，產生新穎的物理現象並擴展複雜性氧化物的應用性。
本研究的第一個主題為深入開發一個具有優異光致伸縮特性的複雜性氧化物系統，銥酸鍶(SrIrO3)磊晶薄膜。我們藉由拉曼光譜學分析照光下之銥酸鍶薄膜的光學聲子變化，並計算出此材料在室溫下能產生約2 %的光致應變，極具應用價值。過程中我們首次對銥酸鍶薄膜不同振動模態的光學聲子進行詳細標定與對稱性分析，並報導了連結聲子能量與光致應變的關鍵係數。而藉由超快動力學的分析我們得知其光致伸縮的機制為光激發載子以熱彈性波(thermoelastic wave)的形式將能量轉移至晶格，其反應時間約為50皮秒，遠快於傳統的光致伸縮材料。第二個主題是關於新穎的光控鐵電/反鐵磁/鐵磁的多位元非揮發記憶體開發。鐵酸鉍(BiFeO3)在室溫下具有相互共存且耦合的鐵電、反鐵磁以及弱鐵磁矩。透過適當的磊晶應力調製，能形成類長方晶相(T-like)與類菱長方晶相(R-like)共存的混相結構。研究中我們透過聚焦可見連續光的照射，成功在混相鐵酸鉍薄膜中實現晶相與多鐵有序疇結構的微區操控。藉由拉曼光譜學、X光繞射結構分析與與相場模擬的探討，發現其調控機制為微區加熱與晶格形變所造成的撓電場，過程中的結構相變是打破原本堅固疇結構的關鍵。而照光對於空間上的晶相切換也同時對應了包含鐵電、反鐵磁與鐵磁的記憶寫入效果，還能伴隨著表面形貌、介電係數、壓電系數與導電率等基本物理特性的改變，皆透過掃描探針顯微與光電子顯微術進行觀察與驗證。而作為延伸，本論文的第三部分則專注於探討此光控多鐵性的操控速度極限。研究發現即使雷射脈衝時間縮短至奈秒到飛秒尺度，混相BFO到T-like相BFO的轉變依然能直接被驅動，實現高速且非揮發之晶相與多鐵有序操控，相關結果皆透過掃描探針顯微術與次微米軟X光能譜所驗證。而有限元分析之熱傳導模擬以及超快雷射動力學結果顯示此單向相變的機制可能為光致暫態應力脈衝。此脈衝的產生可歸因於脈衝光的電場分量所引起的電致伸縮效應(electrostrictive effect)，發生於5.2皮秒後，使得光控鐵多鐵記憶體的概念能允許高速的資料寫入。這些研究成果示範了以光調控複雜性氧化物系統之物理性質的潛力，為多功能性材料的光調控提供了廣泛適用的方法。

Complex transition-metal oxides (complex oxides) have attracted enormous attention in the field of solid-state physics due to their rich physical properties, such as multiferroicity, colossal magnetoresistance, high-temperature superconductivity, thermoelectric, and optical sensitivity, etc. Their intrinsic complexities come from the non-negligible interaction between the charge, spin, and orbital degrees of freedom of correlated electrons at different lattice sites. These interactions including exchange interaction, crystal field, and etc., are comparable in energy scale and compete with each other. Therefore, the exhibiting electronic and magnetic properties of certain complex oxide systems can be completely distinct under different conditions. In the past explorations, it was mainly through the application of external electric field, magnetic field, and stress to control the strong correlation phenomena of complex oxides. In contrast, light illumination will be adopted in our research to modulate the abundant functionalities in the strongly correlated system. We hope this additional degree of freedom, i.e. light illumination, can promote the emergence of novel physical phenomena and extent the applicability for complex oxides.
In the first part of this dissertation, strontium iridate (SrIrO3) epitaxial films with excellent photostrictive properties were developed. Power-dependent Raman spectroscopy was utilized to investigate the optical phonon changes of the SIO films under illumination. We found the photostrictive strains reach a value of about 2% at room temperature, which is of great application prospect. Besides, detailed symmetry analysis and associated phonon assignments of the SIO films were performed. The coefficients for connecting the measured phonon energies and corresponding light-induced strains were also provided. The mechanism for photostriction of SIO films can be attributed to the energy transferring from photon-excited carriers to the lattice in the form of thermoelastic waves according to the analysis from ultrafast pump-probe spectroscopy. The response time is about 50 picoseconds, which is faster than most of the traditional photostrictive materials.
The second topic is about the development of novel optically-controllable multiferroic memory. Bismuth ferrites (BiFeO3) exhibit coupled ferroelectric, antiferromagnetic, and weak ferromagnetic moments at room temperature. Through applying a moderate epitaxial strain (~4 %), phase mixtures constructed with tetragonal-like phase (T-like) and rhombohedral-like phase (R-like) forms. By the illumination of a focused CW green laser, we succeeded in a deterministic manipulation of both crystal phases and multiferroic domains in mixed-phase BFO films. Through the investigation of Raman spectroscopy, X-ray diffraction structure analysis, and phase-field simulation, we noticed that the flexoelectric field caused by local heating and lattice deformation plays a focal role. The transition of structural phase during illumination serves as the key event breaking the original robust domain structure. Note that the phase alteration in mixed-phase BFO films by light illumination corresponds to the changes in ferroelectric, antiferromagnetic, and ferromagnetic orderings. It also accompanies modification in the physical properties such as surface morphology, dielectric coefficient, piezoelectric coefficient, and electrical conductivity. The associated characteristic evolutions are observed and verified through scanning probe microscopy and photoelectron microscopy, accordingly.
As an extension, the third part of this dissertation focuses on the operation speed of the light-controllable multiferroics. Remarkably, we found the transition from mixed-phase to T-like phase BFO can be stimulated even if the duration for a single optical pulse illumination is scaled down to nanosecond and femtosecond regime, achieving high-speed and non-volatile manipulation of both phases and multiferroic orderings. The relevant results were verified by scanning probe microscopy and submicron soft X-ray spectroscopy. A combination of finite element analysis for heat conduction simulation and ultrafast pump-probe spectroscopy indicates that the mechanism for the unidirectional phase transition can be attributed to the light-induced transient strain pulses. The strain pulses appear after 5.2 picoseconds due to the electrostrictive effect caused by the electric field component of the intense light pulse, allowing high-speed optical encoding in multiferroic memory. These demonstrations point out the potential for tuning the physical properties in complex oxides by optical means, providing a widely applicable method for optical control of multifunctional materials.

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