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Optical Properties of Semiconducting Two-Dimensional Transition Metal Dichalcogenide and Magnetic Materials Artificial van der Waals Heterostructures

Zhang, Yan 京都大学 DOI:10.14989/doctor.k24116

2022.05.23

概要

Atomically thin two-dimensional (2D) monolayer transition metal dichalcogenides (1L-TMDs) have been extensively studied due to their intriguing optical and electrical properties. Semiconducting 1L-TMDs with a direct band gap exhibits novel excitonic states such as tightly bound electron-hole pair by Coulomb interaction (excitons) because of the strong quantum confinement and reduced dielectric screening effect. Moreover, strong spin-orbit coupling and broken spatial inversion symmetry in 1L-TMDs give rise to doubly degenerate but inequivalent valleys (K+ and K− valley) located at corners of Brillouin zone in the momentum space and an effective coupling of spin and valley. The spin-valley polarized excitons accompanied with direct interband transitions at K+ and K− valley are optically generated by σ+ and σ− circularly polarized light, respectively, which also allows to control valley degree of freedom by circularly polarized light. The semiconducting 1L- TMDs with strong-light matter interaction will provide us novel platform to study and control emerging valley-physical properties.

2D materials including semiconducting 1L-TMDs can be freely stacked with other layered materials, which realizes artificial stacking van der Waals (vdW) heterostructures. The artificial vdW heterostructures provide us the opportunities of great number of material combinations with different physical properties, such as semiconducting, insulating, metallic, superconducting, and magnetic materials. The emerging optical phenomena of interactions between optical excitonic states and magnetic spins including magnetic elementary excitations are expected in the artificial semiconducting and magnetic material vdW heterostructures. These heterostructures push me to study novel light-matter interaction and its modulation by magnetic interactions.

In this thesis, I have studied the optical properties of excitonic states in monolayer MoSe2 (1L-MoSe2), and its magnetic vdW heterostructures. At first, I described the dynamics of valley polarized excitons and trions of 1L-MoSe2 under strong magnetic field to understand the fundamental valley-physics as a model system. Then, I have proposed new semiconducting and ferro-magnetic vdW heterostructures (1L- MoSe2/(La0.8Nd0.2)1.2Sr1.8Mn2O7)) with magnetic phase transition properties to reveal charge transfer and magnetic proximity effect. The photoluminescence (PL) properties of 1L-MoSe2 can be strongly influenced and controlled by the electronic and magnetic properties of Mn oxide underneath, and h-BN spacer between semiconducting and Mn oxide. Moreover, I have demonstrated that the valley Zeeman splitting and polarization of 1L-MoSe2 are significantly enhanced in the semiconducting and magnetic vdW heterostructures. I have also investigated the semiconducting and antiferromagnetic vdW heterostructures (1L-MoSe2/MnPS3). The fine spectral peaks in the low temperature PL spectra have been observed, which is attributed to intralayer moiré trion–magnon complexes. It is revealed that the intralayer moiré trion–magnon complexes keep the C3 symmetry and have longer lifetime and coherence time.

These discoveries and findings on novel optical properties in monolayer semiconductor, and its magnetic vdW heterostructures will provide deeper understanding of valley physics and a perspective for the optical functionalities by magnetic control. These fundamental studies are very important to realize spin- and valley- based applications with low energy cost.

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Optical Properties of Semiconducting Two-Dimensional Transition Metal Dichalcogenide and Magnetic Materials Artificial van der Waals Heterostructures

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Temperature dependence of the Raman spectra of multilayer graphene nanoribbons fabricated by unzipping method

二次元遷移金属ダイカルコゲナイドのエピタキシャル成長、化学ドーピング、及びデバイス応用

Studies on the Dimensional Extension of Halogen-Bridged Transition-Metal Chain: Nanotube and Three-Dimensional Network

<Advanced Energy Conversion Division> Functional Materials Science and Engineering Research Section

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Optical Properties of Semiconducting Two-Dimensional Transition Metal Dichalcogenide and Magnetic Materials Artificial van der Waals Heterostructures

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Temperature dependence of the Raman spectra of multilayer graphene nanoribbons fabricated by unzipping method

二次元遷移金属ダイカルコゲナイドのエピタキシャル成長、化学ドーピング、及びデバイス応用

Studies on the Dimensional Extension of Halogen-Bridged Transition-Metal Chain: Nanotube and Three-Dimensional Network

<Advanced Energy Conversion Division> Functional Materials Science and Engineering Research Section

<Advanced Energy Conversion Division> Optical Nano-science Research Section

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