光与电子自旋相互作用及其超快动力学特性的研究
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摘要
近年来，超短激光脉冲的发展为人们在极端时间尺度上研究光与物质的相互作用提供了有效工具。半导体和铁磁性薄膜中的超快自旋动力学研究已成为凝聚态物理研究的热点，促进了自旋电子学的发展。然而，顺磁性材料、多铁性薄膜和反铁磁体系中的光与电子自旋的相互作用尚处于起步阶段，亟待大量原创性的实验和理论工作。本论文基于飞秒激光抽运-探测技术，选取三类典型的材料体系作为研究对象，从逆法拉第效应，三温度光磁唯象模型，自旋的相干控制等基本问题入手，开展的研究工作主要有：
(1)利用圆偏振的飞秒激光脉冲，对磁光晶体NaTb(WO_4)_2、铽镓石榴石（TGG）和顺磁流体1-丁基-3-甲基咪唑四氯化铁盐（[bmim]FeCl_4）中的逆法拉第效应进行了系统研究。室温下，在NaTb(WO_4)_2中发现了近500fs的全光磁开关时间，通过对晶体磁光性质的裁剪，调制其开关幅度；系统研究了任意椭圆偏振的飞秒激光激发下，TGG和[bmim]FeCl_4的非线性光学性质，得到光学克尔效应和逆法拉第效应各自的权重；在[bmim]FeCl_4中发现了1.8THz的高频振荡，可归结为受激拉曼散射导致基态能级的量子相干。研究结果表明，逆法拉第效应使得顺磁性磁光晶体在全光通信系统中有潜在的应用价值。
(2)通过瞬态抽运-探测光谱，发现铁酸铋（BiFeO_3）薄膜的电子-声子相互作用与其薄膜的晶格结构有关；通过镧和铌共掺杂实现了BiFeO_3薄膜中瞬态光致应变效应的加强；通过三温度模型分析了锰酸钇（YMO_3）薄膜中的自旋-晶格相互作用。电子、自旋及晶格间的瞬态动力学信息为发展基于铁电-铁磁集成效应的新型超快信息存储及处理器件等提供了必要的参考。
(3)利用THz脉冲的磁场分量，“非热”地激发了倾角反铁磁晶体DyFeO_3中的准铁磁共振模式（FM，0.38THz）和准反铁磁共振模式（AFM，0.52THz）；通过两束具有时间延迟的THz脉冲，实现了FM和AFM模式的相干相消和相干相长控制；在两种磁共振模式同时激发的情况下，实现对任一模式的相干操控；利用YFeO_3单晶本征介电各向异性，通过旋转晶体（改变晶轴与THz偏振的夹角），仅以单个脉冲实现THz自旋波的有效相干控制。
Recently, the development of ultrashort pulse laser technology provides aneffective tool for investigating the interaction of light and matter on criticaltimescales. The studies on spin dynamics in semiconductors and ferromagnetic filmshave become a new forefront of condensed matter physics, which promotes theprocesses in spintronics. However, the basic issues related to the interaction ofelectron spin and photon in paramagnetic, multiferroic, and antiferromagneticmaterial systems have not been understood completely yet, more originalexperimental and theoretical investigations are needed. In this thesis, these threekinds of materials are chosen for study the fundamental issues, such as inverseFaraday effect, three temperature mode and coherent control of spins. The mainresearch work is summaried as follows:
(1) We report all-optical femtosecond time-resolved measurements of the ultrafastinverse Faraday effect in paramagnetic NaTb(WO_4)_2, terbium gallium garnet (TGG)and magnetic ionic liquid1-butyl-3-methylimidazolium tetrachloroferrate([bmim]FeCl_4). The operation of all-optical magnetic switching based on theNaTb(WO_4)_2demonstrates that the switching time can be as fast as~500fs at roomtemperature. The switching amplitude is proportional to the magnetization inducedby the circularly polarized light and modulated by tailoring the magneto-opticalproperties; The transient rotation and ellipticity of polarization of the probe pulseinduced by pump pulse allows us perform a systematic study of the full nonlinearoptical response in TGG and [bmim]FeCl_4. The magneto-optical contributionsattributed to the inverse Faraday effect and the optical Kerr effect are then extractedby thoroughly studying the dependence of the signal upon the pump polarization;The observation of about1.8THz coherent superposition between magneticsublevels of the Fe3+-ion’s ground-state multiplet is assigned to the impulsivelystimulated Raman scattering in the magnetic ion liquid.
(2) The electronic energy relaxation of polycrystalline BiFeO_3films is studied usingtwo-color pump-probe spectroscopy. The fast relaxation of photo-excited electrons isattributed to scattering of electrons with lattice-vibration modes. Due to thestructural strain and symmetry breaking, the electron-phonon interaction strength oftetragonal BiFeO_3films is larger than that of rhombohedral counterparts; Thegeneration mechanism of coherent longitudinal acoustic (LA) phonons in BiFeO_3films is attributed to the transient photostriction effect, which is strongly connectedwith the ferroelectric polarization and significantly enhanced by La and Nb codoping;The spin-lattice interaction in YMnO_3film is identified from the slow component ofthe transient transmittance change with the excitation energies close to Mn3+ions d-dtransition, which is strongly connected with the type of transition and enhanced byspin ordering.
(3) We present the magnetic dipole transition at0.38THz for quasi-ferromagneticmode (FM) and0.52THz for quasi-antiferromagnetic mode (AFM) excited bymagnetic component of terahertz electromagnetic pulse in an antiferromagneticDyFeO_3crystal, without disturbances such as electronic excitation and heating.Magnetic field perpendicular to the magnetization for exciting the FM mode, andmagnetic field parallel to the magnetization for the AFM mode; Coherent control ofthe precession motion of FM and AFM is demonstrated by choosing an appropriateinterval of double terahertz pulses. In addition, we can selectively choose any spinmode when these two magnetic resonances were excited simultaneously; Theintrinsic dielectric anisotropy of YFeO_3crystal in the THz range allows for coherentcontrol of both the amplitude and the phase of the excited spin wave, by varying thepolarization of the incident single THz pulse with respect to the crystal axes.
(1)利用圆偏振的飞秒激光脉冲，对磁光晶体NaTb(WO_4)_2、铽镓石榴石（TGG）和顺磁流体1-丁基-3-甲基咪唑四氯化铁盐（[bmim]FeCl_4）中的逆法拉第效应进行了系统研究。室温下，在NaTb(WO_4)_2中发现了近500fs的全光磁开关时间，通过对晶体磁光性质的裁剪，调制其开关幅度；系统研究了任意椭圆偏振的飞秒激光激发下，TGG和[bmim]FeCl_4的非线性光学性质，得到光学克尔效应和逆法拉第效应各自的权重；在[bmim]FeCl_4中发现了1.8THz的高频振荡，可归结为受激拉曼散射导致基态能级的量子相干。研究结果表明，逆法拉第效应使得顺磁性磁光晶体在全光通信系统中有潜在的应用价值。
(2)通过瞬态抽运-探测光谱，发现铁酸铋（BiFeO_3）薄膜的电子-声子相互作用与其薄膜的晶格结构有关；通过镧和铌共掺杂实现了BiFeO_3薄膜中瞬态光致应变效应的加强；通过三温度模型分析了锰酸钇（YMO_3）薄膜中的自旋-晶格相互作用。电子、自旋及晶格间的瞬态动力学信息为发展基于铁电-铁磁集成效应的新型超快信息存储及处理器件等提供了必要的参考。
(3)利用THz脉冲的磁场分量，“非热”地激发了倾角反铁磁晶体DyFeO_3中的准铁磁共振模式（FM，0.38THz）和准反铁磁共振模式（AFM，0.52THz）；通过两束具有时间延迟的THz脉冲，实现了FM和AFM模式的相干相消和相干相长控制；在两种磁共振模式同时激发的情况下，实现对任一模式的相干操控；利用YFeO_3单晶本征介电各向异性，通过旋转晶体（改变晶轴与THz偏振的夹角），仅以单个脉冲实现THz自旋波的有效相干控制。
Recently, the development of ultrashort pulse laser technology provides aneffective tool for investigating the interaction of light and matter on criticaltimescales. The studies on spin dynamics in semiconductors and ferromagnetic filmshave become a new forefront of condensed matter physics, which promotes theprocesses in spintronics. However, the basic issues related to the interaction ofelectron spin and photon in paramagnetic, multiferroic, and antiferromagneticmaterial systems have not been understood completely yet, more originalexperimental and theoretical investigations are needed. In this thesis, these threekinds of materials are chosen for study the fundamental issues, such as inverseFaraday effect, three temperature mode and coherent control of spins. The mainresearch work is summaried as follows:
(1) We report all-optical femtosecond time-resolved measurements of the ultrafastinverse Faraday effect in paramagnetic NaTb(WO_4)_2, terbium gallium garnet (TGG)and magnetic ionic liquid1-butyl-3-methylimidazolium tetrachloroferrate([bmim]FeCl_4). The operation of all-optical magnetic switching based on theNaTb(WO_4)_2demonstrates that the switching time can be as fast as~500fs at roomtemperature. The switching amplitude is proportional to the magnetization inducedby the circularly polarized light and modulated by tailoring the magneto-opticalproperties; The transient rotation and ellipticity of polarization of the probe pulseinduced by pump pulse allows us perform a systematic study of the full nonlinearoptical response in TGG and [bmim]FeCl_4. The magneto-optical contributionsattributed to the inverse Faraday effect and the optical Kerr effect are then extractedby thoroughly studying the dependence of the signal upon the pump polarization;The observation of about1.8THz coherent superposition between magneticsublevels of the Fe3+-ion’s ground-state multiplet is assigned to the impulsivelystimulated Raman scattering in the magnetic ion liquid.
(2) The electronic energy relaxation of polycrystalline BiFeO_3films is studied usingtwo-color pump-probe spectroscopy. The fast relaxation of photo-excited electrons isattributed to scattering of electrons with lattice-vibration modes. Due to thestructural strain and symmetry breaking, the electron-phonon interaction strength oftetragonal BiFeO_3films is larger than that of rhombohedral counterparts; Thegeneration mechanism of coherent longitudinal acoustic (LA) phonons in BiFeO_3films is attributed to the transient photostriction effect, which is strongly connectedwith the ferroelectric polarization and significantly enhanced by La and Nb codoping;The spin-lattice interaction in YMnO_3film is identified from the slow component ofthe transient transmittance change with the excitation energies close to Mn3+ions d-dtransition, which is strongly connected with the type of transition and enhanced byspin ordering.
(3) We present the magnetic dipole transition at0.38THz for quasi-ferromagneticmode (FM) and0.52THz for quasi-antiferromagnetic mode (AFM) excited bymagnetic component of terahertz electromagnetic pulse in an antiferromagneticDyFeO_3crystal, without disturbances such as electronic excitation and heating.Magnetic field perpendicular to the magnetization for exciting the FM mode, andmagnetic field parallel to the magnetization for the AFM mode; Coherent control ofthe precession motion of FM and AFM is demonstrated by choosing an appropriateinterval of double terahertz pulses. In addition, we can selectively choose any spinmode when these two magnetic resonances were excited simultaneously; Theintrinsic dielectric anisotropy of YFeO_3crystal in the THz range allows for coherentcontrol of both the amplitude and the phase of the excited spin wave, by varying thepolarization of the incident single THz pulse with respect to the crystal axes.
引文
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