论文标题
连贯的带边缘振荡和动态LO声子模式拆分,作为polovsing pallonic耦合的证据
Coherent Band-Edge Oscillations and Dynamic LO Phonon Mode Splitting as Evidence for Polaronic Coupling in Perovskites
论文作者
论文摘要
在复杂系统中长期以来一直在寻求集体模式的相干性,例如声子及其对电子状态的调节,这是光伏和量子电子中的一个跨裁切问题。在基于金属卤化物钙钛矿的光伏细胞和激光器中,具有二极管耦合的存在,即由带电晶格的宏观运动打扮的光载体,在Terahertz(THZ)纵向光学(LO)的辅助方面,已经进行了深入研究,但仍被深入研究。这可能是解释钙钛矿材料的显着特性的关键,例如缺陷耐受性,长电荷寿命和扩散长度。在这里,我们使用强烈的单周期THZ脉冲,峰值电场高达$ e_ {thz} = $ 1000 \,kv/cm在室温下以CH $ _3 $ _3 $ _3 $ _3 $ _3 $ _3 $ pbi $ _3 $驱动连贯的带边缘振荡。我们以$ω_ {\ mathrm {lo}}} \ sim $ 4 Thz的形式揭示了特定量化晶格振动模式的振荡行为,既是偶极子和动量。 THZ驱动的相干动力学表现出显着特征:室温相干振荡以$ω_ {\ mathrm {lo}}} $长于单晶和薄膜的1 ps长度超过1 ps; {\ em模式 - 选择性}由电子phonon($ e $ - $ ph $)辅助的不同带边缘状态的调制; {\ em动态模式拆分}由有机阳离子的熵和非谐度导致的温度控制。我们的结果表明,强烈的THZ驱动的相干带边缘调制是对电子晶体耦合现象的强大探针,并为perovskites的极性相关性提供了令人信服的含义。
The coherence of collective modes, such as phonons, and their modulation of the electronic states are long sought in complex systems, which is a cross-cutting issue in photovoltaics and quantum electronics. In photovoltaic cells and lasers based on metal halide perovskites, the presence of polaronic coupling, i.e., photocarriers dressed by the macroscopic motion of charged lattice, assisted by terahertz (THz) longitudinal optical (LO) phonons, has been intensely studied yet still debated. This may be key for explaining the remarkable properties of the perovskite materials, e.g., defect tolerance, long charge lifetimes and diffusion length. Here we use the intense single-cycle THz pulse with the peak electric field up to $E_{THz}=$1000\,kV/cm to drive coherent band-edge oscillations at room temperature in CH$_3$NH$_3$PbI$_3$. We reveal the oscillatory behavior dominantly to a specific quantized lattice vibration mode at $ω_{\mathrm{LO}}\sim$4 THz, being both dipole and momentum forbidden. THz-driven coherent dynamics exhibits distinguishing features: the room temperature coherent oscillations at $ω_{\mathrm{LO}}$ longer than 1 ps in both single crystals and thin films; the {\em mode-selective} modulation of different band edge states assisted by electron-phonon ($e$-$ph$) interaction; {\em dynamic mode splitting} controlled by temperature due to entropy and anharmonicity of organic cations. Our results demonstrate intense THz-driven coherent band-edge modulation as a powerful probe of electron-lattice coupling phenomena and provide compelling implications for polaron correlations in perovskites.