When the collective coupling of the rovibrational states in organic molecules and confined electromagnetic modes is sufficiently strong, the system enters into vibrational strong coupling, leading to the formation of hybrid light-matter quasiparticles. In this work we demonstrate theoretically how this hybridization in combination with stimulated Raman scattering can be utilized to widen the capabilities of Raman laser devices. We explore the conditions under which the lasing threshold can be diminished and the system can be transformed into an optical parametric oscillator. Finally, we show how the dramatic reduction of the many final molecular states into two collective excitations can be used to create an all-optical switch with output in the mid-infrared.
The vibrational properties of a series of push-pull polyynes have been studied by infrared and Raman spectroscopy. The simultaneous activation of a strong infrared and Raman mode, i.e. the collective vibration of CC bonds of the sp carbon chain, highlights the effectiveness of a polyyne bridge in promoting charge transfer between the electron donor (D) and acceptor (A) ends, thus suggesting that ad-hoc functionalized polyynes are worth being explored as building blocks of organic materials with attractive first-order optical nonlinearity. The optical, electronic, and vibrational properties of …
Spontaneous Raman Scattering under Vibrational Strong Coupling: The Critical Role of Polariton Spatial Mode Coherence
Université de Strasbourg, CNRS, Institut de Physique et Chimie des Matériaux de Strasbourg（斯特拉斯堡大学）；Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière（里昂第一大学）
We present vibrational properties of Franckeite, which is a naturally occurring van der Waals heterostructure consisting of two different semiconducting layers. Franckeite is a complex layered crystal composed of alternating SnS$_2$ like pseudohexagonal and PbS-like pseudotetragonal layers stacked on top of each other, providing a unique platform to study vibrational properties and thermal transport across layers with mass density and phonon mismatches. By using micro-Raman spectroscopy and first-principles Raman simulations, we found that the PbS-like pseudotetragonal structure is mostly comp…
Vibrational Spectra of Pb2Bi2Te3, PbBi2Te4 and PbBi4Te7 Topological Insulators: Temperature Dependent Raman and Theoretical Insight from DFT Simulations
我们提出了温度依赖的频率偏移和线加宽的声子模式的原子层的插入在原型3D拓扑绝缘体Bi 2 Te 3的Pb和PbTe，使用拉曼光谱。用改进的Bridgman法生长了Pb 2Bi 2 Te 3、PbBi 2 Te 4和PbBi 4 Te 7单晶。Pb_2Bi_2 Te_3、Pb_Bi_2 Te_4和Pb_Bi_4 Te_7的拉曼模式随温度从298 K降低到93 K而逐渐发生蓝移，这是由于晶格的非谐振动以及Bi-Te共价相互作用强度的增加。实验结果得到了广泛的密度泛函理论计算的补充，其中一个合理的匹配之间的实验和计算数据被发现。化学压力，诱导的插入的Pb和PbTe层的Bi 2 Te 3，修改的相互作用的边界处的五层，这是显而易见的从模式的演变。在低温下观察到面外Bi-Te振动相对于面内Bi-Te振动的增强。
We report resonant Raman spectroscopy of neutral excitons X$^0$ and intravalley trions X$^-$ in hBN-encapsulated MoS$_2$ monolayer embedded in a nanobeam cavity. By temperature tuning the detuning between Raman modes of MoS$_2$ lattice phonons and X$^0$/X$^-$ emission peaks, we probe the mutual coupling of excitons, lattice phonons and cavity vibrational phonons. We observe an enhancement of X$^0$-induced Raman scattering and a suppression for X$^-$-induced, and explain our findings as arising from the tripartite exciton-phonon-phonon coupling. The cavity vibrational phonons provide intermedia…
Adsorption-Driven Symmetry Lowering in Single Molecules Revealed by Ångstrom-scale Tip-Enhanced Raman Imaging
Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences（捷克科学院有机化学与生物化学研究所）；Institute of Physics, Czech Academy of Sciences（捷克科学院物理研究所）；Instituto de Ciencia de Materiales de Madrid（马德里材料科学研究所）；Departamento de Química, Universidad Autónoma de Madrid（马德里自治大学化学系）；Faculty of Mathematics and Physics, Charles University（查理大学数学与物理学院）；Institute for Advanced Research in Chemical Sciences (IAdChem), Universidad Autónoma de Madrid（马德里自治大学化学高级研究院）
Talc is an insulating layered material that is stable at ambient conditions and has high-quality basal cleavage, which is a major advantage for its use in van der Waals heterostructures. Here, we use near-field synchrotron infrared nanospectroscopy, Raman spectroscopy, and first-principles calculations to investigate the structural and vibrational properties of talc crystals, ranging from monolayer to bulk, in the 300-750 cm-1 and <60 cm-1 spectral windows. We observe a symmetry crossover from mono to bilayer talc samples, attributed to the stacking of adjacent layers. The in-plane lattice par…
Present study explores the observation of topological non-hexagonal rings (NHR) and Stone Wale (SW) defects by Raman experiments in both single (SLG) and multi-layer graphene (MLG) after they are irradiated with 100- 300 eV Ar ions. Although predicted by theoretical studies, here it is experimentally shown for the first time that graphene SW/NHR defects have a signature in Raman. Broad bandwidth of the pertinent Raman features suggests the presence of more than one SW/NHR defect mode, in agreement with the DFT studies. Variations in the SW/NHR related Raman mode intensities demonstrate the ann…
Vibrational and electronic heating in nanoscale junctions
理解和控制热流是纳米电子学的一个主要挑战。当一个结被光或电荷的流动驱动而脱离平衡时，振动和电子的自由度一般不再由单一的温度来描述[1-6]。此外，表征稳态振动和电子分布{ \it in situ}极具挑战性。在这里，我们表明，表面增强拉曼发射可用于确定在用分子装饰的偏置金属纳米级结中振动模式和流动电子的有效温度[7]。分子振动通过光激发[8]和直流电流[9]显示出模式特定的泵浦，有效温度超过几百开尔文。反斯托克斯电子拉曼发射\cite [10，11]表明，在几百mV的偏置电压下，电子有效温度也增加到其无电流值的三倍。虽然精确的有效温度依赖于模型，但作为偏置条件的函数的趋势是稳健的，并且允许与纳米级加热理论进行直接比较。
Understanding the stability limitations and defect formation mechanisms in 2D magnets is essential for their utilization in spintronic and memory technologies. Here, we correlate defects in mono- to multilayer CrSBr with their structural, vibrational and magnetic properties. We use resonant Raman scattering to reveal distinct vibrational defect signatures. In pristine CrSBr, we show that bromine atoms mediate vibrational interlayer coupling, allowing for distinguishing between surface and bulk defect modes. We show that environmental exposure causes drastic degradation in monolayers, with the …
In the bilayer ReS$ _{2} $ channel of a field-effect transistor (FET), we demonstrate using Raman spectroscopy that electron doping (n) results in softening of frequency and broadening of linewidth of the in-plane vibrational modes, leaving out-of-plane vibrational modes unaffected. Largest change is observed for the in-plane Raman mode at $\sim$ 151 cm$^{-1} $, which also shows doping induced Fano resonance with the Fano parameter 1/q = -0.17 at doping concentration of $\sim 3.7\times10^{13}$ cm$^{-2} $. A quantitative understanding of our results is provided by first-principles density funct…
Graphdiyne, atomically-thin 2D carbon nanostructure based on sp-sp2 hybridization, is an appealing system potentially showing outstanding mechanical and optoelectronic properties. Surface-catalyzed coupling of halogenated sp-carbon-based molecular precursors represents a promising bottom-up strategy to fabricate extended 2D carbon systems with engineered structure on metallic substrates. Here, we investigate the atomic-scale structure and electronic and vibrational properties of an extended graphdiyne-like sp-sp2 carbon nanonetwork grown on Au(111) by means of on-surface synthesis. The formati…
