基于钛酸铜钙、铌酸锂铁电材料的太赫兹波调制特性研究
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摘要
太赫兹功能器件是太赫兹研究领域中非常重要的一部分，其中基于铁电材料的太赫兹波调制器件，由于其重要的研究和应用价值而受到广泛关注。本论文着重于研究基于钛酸铜钙陶瓷和不同掺杂近化学计量比铌酸锂晶体等铁电材料在太赫兹波段的调制特性。通过建立模型，分析了太赫兹波与铁电材料相互作用的物理机制。利用太赫兹时域光谱系统对钛酸铜钙和不同掺杂近化学计量比铌酸锂晶体在太赫兹波段的物理性质和介电响应进行了研究，重点采用光控手段对这些铁电材料在太赫兹波段的介电常数进行调制，调制幅度分别达到了7%和5.5%，并且探讨了影响铁电材料在太赫兹波段介电响应的各种微观机制以及实验中观测到的光铁电现象。具体研究内容如下：
（1）介绍了太赫兹技术和铁电体的基本概念。对太赫兹波的应用系统结构和太赫兹时域光谱技术进行了简介。讨论了铁电微观机制中的软模理论，它认为铁电相变是由晶体布里渊区中心的某个光学横模振动频率的下降引起的。我们利用德拜弛豫模型和振子模型来探讨铁电体的介电响应频谱，它们分别对应于有序无序型铁电体和位移型铁电体。介绍了一些常见的光铁电现象，重点讨论了反常光生伏打效应和光折变效应。
（2）采用实验方法测量了室温下钛酸铜钙（CCTO）陶瓷在太赫兹波段的光谱特性。通过数据处理和计算得到了钛酸铜钙陶瓷在太赫兹波段的复介电常数色散曲线。CCTO在太赫兹波段的介电常数数值约为65~75，并没有表现出较强的巨介电性质。当对样品材料施加不同强度的外光场时，我们实现了对CCTO介电常数的调制，调制幅度可达7%。我们观察到样品折射率的变化与外加光场的强度成线性关系，这些变化被认为是由材料中光生载流子导致的自发极化的改变引起的。
（3）采用实验方法测量了室温下掺铁近化学计量比铌酸锂单晶和掺铈近化学计量比铌酸锂单晶在太赫兹波段的光谱特性。通过数据处理和计算得到了两种晶体在太赫兹波段的复介电常数、吸收系数、复折射率色散曲线。在太赫兹波段，掺铁近化学计量比铌酸锂单晶的介电常数约为42~46，折射率约为6.5~6.8；吸收系数约为60~100cm~(-1)，略大于无掺杂的近化学计量比铌酸锂单晶。在太赫兹波段，掺铈近化学计量比铌酸锂单晶的介电常数约为39~43，折射率约为6.3~6.6；吸收系数约为70~120cm~(-1)，略大于无掺杂的近化学计量比铌酸锂单晶。
（4）利用外加光场的方法实现了对掺铁近化学计量比铌酸锂单晶和掺铈近化学计量比铌酸锂单晶在太赫兹波段的介电常数和吸收系数的调制，对介电常数的调制幅度分别达到3%和1.8%，对吸收系数的调制幅度分别达到5.5%和4%。当光强较小时，晶体的折射率变化量随着外加光场强度的变化成线性关系，这一现象被认为是由光折变效应引起的，即光生载流子的空间位移在晶体内部产生了空间电荷场，它通过线性电光效应引起了晶体折射率的变化。其中掺铁近化学计量比铌酸锂单晶的光折变效应明显强于掺铈近化学计量比铌酸锂单晶。另外，当光强达到一定程度后，我们在两种晶体当中均观测到光折变效应的突然减弱，引起这一现象的原因被归结为光致畴反转。在掺铁近化学计量比铌酸锂单晶观察到光致畴反转现象所需的光强要低于掺铈近化学计量比铌酸锂单晶。
The terahertz functional device is an important part in the area of terahertz research.Especially, the terahertz modulation characteristics based on ferroelectric materials haveattracted much attention of researchers because of its unique physical property andapplication value. This manuscript focused on the dielectric behavior of CaCu_3Ti_4O_(12)(CCTO) ceramic and different doped near-stoichiometric LiNbO3(near-SLN) crystals inthe terahertz range. We analyses the physical mechanisms of the interaction betweenterahertz wave and ferroelectric materials. By employing a terahertz time-domainspectroscopy system, we measured the complex dielectric constants of CCTO and dopednear-SLN. When applying an external optical field, we have modulated the dielectricconstants of both CCTO and doped near-SLN, the modulation depths reached up to7%and5.5%, respectively. We discussed the micro mechanisms behind the observed effectsand some photo-ferroelectric phenomena. The details of my work are listed as following:
(1) We introduced the concepts of THz technology and ferroelectrics. Then we talkedabout the THz application system structure and the THz time-domain spectroscopy system.We investigated the soft-mode theory, which is the most important micromechanism inferroelectric phase transition. The theory indicated that the phase transition was caused bythe frequency drop of an optical transverse mode in the center of Brillouin zone. Weinvestigated the Debye relaxation model and oscillator model for the dielectric behavior offerroelectrics, which corresponded to the displacement ferroelectrics and theorder-disorder ferroelectrics, respectively. We introduced some common photo-ferroelectric phenomena, emphatically talked about anomalous photovoltaic (APV) effectand photorefraction.
(2) The dielectric properties of1050°C/12h sintered CaCu_3Ti_4O_(12)(CCTO) ceramicshave been investigated by using terahertz time domain spectroscopy in the frequencyrange of0.2~(-1).6THz at room temperature. CCTO do not show giant permittivityproperties in the THz range. When applying an external optical field, an obvious variationof dielectric constant was observed and reached up to7%. From the results, we found thatthe change of refractive index has a linear relationship on scale with the applied light intensity. These findings were attributed to the change of spontaneous polarization in theceramic caused by the excited free carriers.
(3) The dielectric properties of near-stoichiometric LiNbO_:Fe and near-stoichiometric LiNbO_:Ce single crystals have been investigated by using a terahertz timedomain spectroscopy (THz-TDS) in a frequency range of0.7~(-1).6THz at room temperature.Through a Fourier transform, we got the transmission spectra and the intrinsic phase shiftsof the samples. The complex refractive index and permittivity were calculated from theTHz transmission spectra. In the terahertz range, the dielectric constant of near-SLN:Fe isabout42-46(corresponding refractive index is6.5-6.8), and the dielectric constant ofnear-SLN:Ce is about40-43(corresponding refractive index is6.3-6.6). The absorptioncoefficient of near-SLN:Fe in the terahertz range is about60~(-1)00cm~(-1), and the absorptioncoefficient of near-SLN:Ce in the terahertz range is about70~(-1)20cm~(-1). They are bothhigher than that of undoped CLN.
(4) When coupled with an applied external optical field, obvious photorefractiveeffects were observed, resulting in the modulation of the complex dielectric constants forboth near-SLN:Fe and near-SLN:Ce. The variation of refractive index|Δn|has a linearrelationship on scale with the applied light intensity accompanied with a steplike decrease.These findings were attributed to the internal space charge field of photorefraction and thelight-induced domain reversal in the crystals. The light intensity at which the steplikedecrease of photorefraction takes place in near-SLN:Ce is a little higher than that ofnear-SLN:Fe crystal. It means that the coercive field of near-SLN:Ce is a little larger thanthat of near-SLN:Fe, which can also be attributed to the photorefraction resistancebehavior of near-SLN:Ce crystal.
（1）介绍了太赫兹技术和铁电体的基本概念。对太赫兹波的应用系统结构和太赫兹时域光谱技术进行了简介。讨论了铁电微观机制中的软模理论，它认为铁电相变是由晶体布里渊区中心的某个光学横模振动频率的下降引起的。我们利用德拜弛豫模型和振子模型来探讨铁电体的介电响应频谱，它们分别对应于有序无序型铁电体和位移型铁电体。介绍了一些常见的光铁电现象，重点讨论了反常光生伏打效应和光折变效应。
（2）采用实验方法测量了室温下钛酸铜钙（CCTO）陶瓷在太赫兹波段的光谱特性。通过数据处理和计算得到了钛酸铜钙陶瓷在太赫兹波段的复介电常数色散曲线。CCTO在太赫兹波段的介电常数数值约为65~75，并没有表现出较强的巨介电性质。当对样品材料施加不同强度的外光场时，我们实现了对CCTO介电常数的调制，调制幅度可达7%。我们观察到样品折射率的变化与外加光场的强度成线性关系，这些变化被认为是由材料中光生载流子导致的自发极化的改变引起的。
（3）采用实验方法测量了室温下掺铁近化学计量比铌酸锂单晶和掺铈近化学计量比铌酸锂单晶在太赫兹波段的光谱特性。通过数据处理和计算得到了两种晶体在太赫兹波段的复介电常数、吸收系数、复折射率色散曲线。在太赫兹波段，掺铁近化学计量比铌酸锂单晶的介电常数约为42~46，折射率约为6.5~6.8；吸收系数约为60~100cm~(-1)，略大于无掺杂的近化学计量比铌酸锂单晶。在太赫兹波段，掺铈近化学计量比铌酸锂单晶的介电常数约为39~43，折射率约为6.3~6.6；吸收系数约为70~120cm~(-1)，略大于无掺杂的近化学计量比铌酸锂单晶。
（4）利用外加光场的方法实现了对掺铁近化学计量比铌酸锂单晶和掺铈近化学计量比铌酸锂单晶在太赫兹波段的介电常数和吸收系数的调制，对介电常数的调制幅度分别达到3%和1.8%，对吸收系数的调制幅度分别达到5.5%和4%。当光强较小时，晶体的折射率变化量随着外加光场强度的变化成线性关系，这一现象被认为是由光折变效应引起的，即光生载流子的空间位移在晶体内部产生了空间电荷场，它通过线性电光效应引起了晶体折射率的变化。其中掺铁近化学计量比铌酸锂单晶的光折变效应明显强于掺铈近化学计量比铌酸锂单晶。另外，当光强达到一定程度后，我们在两种晶体当中均观测到光折变效应的突然减弱，引起这一现象的原因被归结为光致畴反转。在掺铁近化学计量比铌酸锂单晶观察到光致畴反转现象所需的光强要低于掺铈近化学计量比铌酸锂单晶。
The terahertz functional device is an important part in the area of terahertz research.Especially, the terahertz modulation characteristics based on ferroelectric materials haveattracted much attention of researchers because of its unique physical property andapplication value. This manuscript focused on the dielectric behavior of CaCu_3Ti_4O_(12)(CCTO) ceramic and different doped near-stoichiometric LiNbO3(near-SLN) crystals inthe terahertz range. We analyses the physical mechanisms of the interaction betweenterahertz wave and ferroelectric materials. By employing a terahertz time-domainspectroscopy system, we measured the complex dielectric constants of CCTO and dopednear-SLN. When applying an external optical field, we have modulated the dielectricconstants of both CCTO and doped near-SLN, the modulation depths reached up to7%and5.5%, respectively. We discussed the micro mechanisms behind the observed effectsand some photo-ferroelectric phenomena. The details of my work are listed as following:
(1) We introduced the concepts of THz technology and ferroelectrics. Then we talkedabout the THz application system structure and the THz time-domain spectroscopy system.We investigated the soft-mode theory, which is the most important micromechanism inferroelectric phase transition. The theory indicated that the phase transition was caused bythe frequency drop of an optical transverse mode in the center of Brillouin zone. Weinvestigated the Debye relaxation model and oscillator model for the dielectric behavior offerroelectrics, which corresponded to the displacement ferroelectrics and theorder-disorder ferroelectrics, respectively. We introduced some common photo-ferroelectric phenomena, emphatically talked about anomalous photovoltaic (APV) effectand photorefraction.
(2) The dielectric properties of1050°C/12h sintered CaCu_3Ti_4O_(12)(CCTO) ceramicshave been investigated by using terahertz time domain spectroscopy in the frequencyrange of0.2~(-1).6THz at room temperature. CCTO do not show giant permittivityproperties in the THz range. When applying an external optical field, an obvious variationof dielectric constant was observed and reached up to7%. From the results, we found thatthe change of refractive index has a linear relationship on scale with the applied light intensity. These findings were attributed to the change of spontaneous polarization in theceramic caused by the excited free carriers.
(3) The dielectric properties of near-stoichiometric LiNbO_:Fe and near-stoichiometric LiNbO_:Ce single crystals have been investigated by using a terahertz timedomain spectroscopy (THz-TDS) in a frequency range of0.7~(-1).6THz at room temperature.Through a Fourier transform, we got the transmission spectra and the intrinsic phase shiftsof the samples. The complex refractive index and permittivity were calculated from theTHz transmission spectra. In the terahertz range, the dielectric constant of near-SLN:Fe isabout42-46(corresponding refractive index is6.5-6.8), and the dielectric constant ofnear-SLN:Ce is about40-43(corresponding refractive index is6.3-6.6). The absorptioncoefficient of near-SLN:Fe in the terahertz range is about60~(-1)00cm~(-1), and the absorptioncoefficient of near-SLN:Ce in the terahertz range is about70~(-1)20cm~(-1). They are bothhigher than that of undoped CLN.
(4) When coupled with an applied external optical field, obvious photorefractiveeffects were observed, resulting in the modulation of the complex dielectric constants forboth near-SLN:Fe and near-SLN:Ce. The variation of refractive index|Δn|has a linearrelationship on scale with the applied light intensity accompanied with a steplike decrease.These findings were attributed to the internal space charge field of photorefraction and thelight-induced domain reversal in the crystals. The light intensity at which the steplikedecrease of photorefraction takes place in near-SLN:Ce is a little higher than that ofnear-SLN:Fe crystal. It means that the coercive field of near-SLN:Ce is a little larger thanthat of near-SLN:Fe, which can also be attributed to the photorefraction resistancebehavior of near-SLN:Ce crystal.
引文
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