有机半导体/金属杂化纳米结构中的强耦合相互作用及超快动力学特性

王卫, 张红. 有机半导体/金属杂化纳米结构中的强耦合相互作用及超快动力学特性[J]. 光电工程, 2017, 44(2): 161-171. doi: 10.3969/j.issn.1003-501X.2017.02.004
引用本文: 王卫, 张红. 有机半导体/金属杂化纳米结构中的强耦合相互作用及超快动力学特性[J]. 光电工程, 2017, 44(2): 161-171. doi: 10.3969/j.issn.1003-501X.2017.02.004
Wang Wei, Zhang Hong. Strong coupling and ultrafast dynamics in organic semiconductor/metal hybrid nanostructures[J]. Opto-Electronic Engineering, 2017, 44(2): 161-171. doi: 10.3969/j.issn.1003-501X.2017.02.004
Citation: Wang Wei, Zhang Hong. Strong coupling and ultrafast dynamics in organic semiconductor/metal hybrid nanostructures[J]. Opto-Electronic Engineering, 2017, 44(2): 161-171. doi: 10.3969/j.issn.1003-501X.2017.02.004

有机半导体/金属杂化纳米结构中的强耦合相互作用及超快动力学特性

  • 基金项目:
    国家自然科学基金(61675139, 11374217, 11474210, 11474207)资助项目
详细信息

Strong coupling and ultrafast dynamics in organic semiconductor/metal hybrid nanostructures

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  • 有源表面等离光子学(active plasmonics)是目前表面等离子体光子学研究的一个重要分支,其基本思想是利用“增益”物质和纳米金属结构相结合形成杂化金属纳米结构,从而克服表面等离子体激元(surface plasmon polariton,SPP)的耗散问题以及实现对SPP光子的外部操作和调制。本文主要针对有机半导体/金属杂化纳米结构,介绍其相关研究结果。结合色散补偿的光谱相干法和超快泵浦-探测瞬态光谱测量技术,分析了J-凝聚/光栅杂化金属纳米结构的静态和瞬态光学特性,揭示了X-SPP的强耦合过程中的相干和非相干相互作用通道,杂化能态的sub/super-radiance现象,以及有机半导体染料中的激子和SPP之间的瞬态相干能量交换过程:“拉比”振荡。实现了10 fs量级的SPP光学特性的外部相干调制。

  • Abstract: Metallic nanostructures can support the strongly confined interface waves: surface plasmon polaritons (SPPs). SPPs have recently been used in a variety of applications due to their abilities to guide light in the scale of nanometer. Whereas, intrinsic weak optical nonlinearities and short propagation lengths of SPPs hinder their applications in novel active plasmonic devices.

    One promising solution is to couple SPPs to nonlinear optical resonances, such as excitons (Xs) in molecular or semiconducting nanostructures. Consequently, hybrid nanostructures containing J-aggregate molecules and metallic nanostructures have attracted considerable interest. In these systems, vacuum field fluctuations lead to a coherent exchange of energy between ensembles of excitons and plasmons and the formation of new hybrid polariton states. Strong coupling between Xs and SPPs enables an efficient transfer of the strong optical nonlinearities of the excitonic emitters to the passive plasmonic nanostructures on the ultrashort time scale of femtosecond.

    Here, we give a brief review of our studies in the area of active plasmonics. We focus on hybrid J-aggregate/metal nanostructures consisting of J-aggregate excitons and surface plasmon polaritons supported by metallic nanogroove arrays. We first introduce two experimental methods used in our study: chrip-compensated spectral interferometry and nonlinear pump-probe spectroscopy. The strong coupling between J-aggregate excitons and SPPs is studied in detail by probing both the static optical properties and ultrafast dynamics of the strongly coupled X-SPP systems. We show that two different energy transfer channels: a coherent resonant dipole-dipole interaction and an incoherent exchange of photons, are coexisting in the hybrid system. The interplay between both pathways results in a pronounced modification of the radiative damping due to the formation of super- and subradiant polariton states.

    We also investigate the coherent energy exchange, Rabi oscillations between the excitonic and the SPP systems in real time. Using nonlinear pump-probe spectroscopy, coherent polariton dynamics of the hybrid X-SPP systems is studied. It is found that the optical response of the individual resonances is drastically altered by the optical dipole coupling between excitons and SPPs. Coherent X-SPP population transfer induces transient oscillations in exciton density, leading to a periodic modulation of the normal mode splitting and thus optical nonlinearity in a 10 fs timescale.

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  • 图 1  (a1)无机半导体量子阱-金属杂化纳米结构示意图. (a2)角度分辨的远场反射谱的计算值,其中空气-金属界面激发的SPP用AM表示,半导体-金属界面激发的SPP用SM表示. (b1)硒化镉量子点-银膜杂化结构以及全反射激发实验装置示意图,蓝色曲线表示正入射情况下的吸收谱线. (b2)测量得到的角度分辨的反射谱.图中结果来自文献[25]和[26].

    Figure 1.  (a1) Schematic of the metal-semiconductor hybrid structure consisting of a gold nanoslit grating deposited on a GaAs QW. (a2) Calculated angle-resolved far-field reflectivity spectra of this structure. Dispersion relations for different AM and SM SPP resonances are indicated as dashdotted lines. (b1) Normal incidence absorption spectrum of a CdSe film, ~25 nm in thickness spin coated onto a glass slide. (b2) Reflectivity spectra plotted as a function of the angle of incidence external to the prism (right). Reproduced with permission from Ref. [25-26].

    图 2  有机染料分子的分子式(a)及其单体(蓝色)和J-凝聚(红色)吸收谱线(b). J-凝聚的吸收谱线的半高宽变小并明显红移. (c)金属纳米光栅结构. (d) J-凝聚/金属光栅杂化纳米结构.

    Figure 2.  (a) Molecular structure of J-aggregated dye. (b) Absorption spectra of monomer molecules (blue) and their corresponding J-aggregate form (red) measured at room temperature. (c) Schematic of gold groove array deposited on glass substrate and (d) the hybrid nanostructure consisting of J-aggregate dye film spin-coated on the gold groove array.

    图 3  (a) 光谱相干法原理图:宽波段的激光被第一个分光片分成两束光,其中一束光通过样品,另一束则作为参考光,两束光在第二个分波片上汇合,然后进入光谱仪。光谱仪测量得到两束光的干涉条纹. (b)高精度色散补偿相干测量示意图:宽波段白光光源通过分束器产生两束光,一束经过样品,样品放在真空环境中; 光谱仪测量其和另一束参考光的干涉条纹.

    Figure 3.  (a) Principle of spectral interferometry setup. The broadband laser pulses are split by the first beam splitter (BS1) and sent through the two arms of a Mach-Zehnder interferometer. The one passing through the sample are modulated by its complex response function. The other beam is the undisturbed delayed reference beam with respect to the sample arm. The two beams are then combined after the second beam splitter (BS2) and sent to the detector where the interfering field intensity is recorded. (b) Schematic of angle-resolved spectral interferometry setup.

    图 4  泵浦-探测光谱测量光路示意图.宽波段脉冲激光被分光片分为泵浦光(pump)和探测光(probe).探测光相对泵浦光有时间延迟τ.探测光信号随时间延迟的变化强度反映出待测样品的超快动力学性质.

    Figure 4.  Schematic of a generic setup for pump-probe measurements. An ultrafast laser is split into pump and probe beams. They are both sent to the sample with the probe delayed by a time of τ. The signal of the probe beam is recorded by a detector as a function of delay to monitor the real-time dynamics of the sample.

    图 5  反射式角度分辨泵浦-探测光谱测量光路示意图.宽波段脉冲激光输出6 fs的脉冲激光,经过棱镜组和色散补偿镜进行色散预补偿(chirp pre-compensation).泵浦光和探测光都用声光调制器(AOM)进行调制.样品固定在真空室内并用液氮冷却.旋转镜片安装在旋转位移台上,通过平动位移台的移动可以得到0.2°的角分辨能力.安装有二极管阵列(PD)的光谱仪(spectrometer)用来记录探测光随时间延迟(time delay)的强度变化.

    Figure 5.  Angle-resolved pump probe setup. The sample is mounted inside a cryostat, which can provide vacuum environment and is cooled with liquid nitrogen or helium. A 6-fs pulse is first compressed using chirped mirrors, a prism compressor and a pulse shaper (not shown) before split into pump and probe. A delay stage is used to delay the probe beam relative to the pump beam. Both beams are modulated using AOMs at different frequencies. The pump beam can be spectrally narrowed by using a short-pass filter. Computer controlled angle tuning platform is used for excitation and detection angle.

    图 6  (a) SPP和J-凝聚激子强耦合相互作用示意图.激子看作三能级系统,含有基态、单激子激发态|X〉和双激子激发态|XX〉; SPP系统用光子模式|P〉表示, 真空连续态表示为|V〉; 虚线代表相干耦合通道,实线代表非相干耦合通道. (b)杂化能级UP和LP随角度变化的谱线半高宽度的实验测量值(圆圈)和计算值(蓝色和红色实线).绿色实线是SPP和X色散曲线的计算值. (c) UP和LP布居数衰减ħγ' (实线)和退激发效应ħγ*(虚线)的计算值.所示结果来源于文献[17].

    Figure 6.  (a) Schematic of a strongly coupled X-SPP system. The excitonic system is modeled as a three-level system consisting of a ground state, a single exciton state |X〉 and a biexciton state |XX〉. The plasmon system is represented as a photonic mode |P〉. The continuum of vacuum states is denoted as |V〉. The solid arrows denote the incoherent X-SPP coupling through vacuum field. (b) Spectral widths of the UP/LP modes obtained from experiment (circles) and oscillator model (solid lines). (c) Calculated population damping (solid) and pure dephasing (dash-dot) of the UP (blue) and LP (red). Results are taken from Ref. [17].

    图 7  X-SPP共振情况下UP (a)和LP (b)附近探测光反射谱变化率. (c)共振激发UP(1.84 eV,蓝色)、第一激发态激子(1.8 eV,黑色)和LP(1.74 eV,红色)情况下探测光反射谱变化率的测量值(圆圈、方块和三角)和拟合值(实线). (d)共振激发下UP和LP辐射衰减在不同入射角度的测量值(圆圈)和耦合谐振子模型的计算值(实线),虚线代表不考虑非耦合相干项的计算结果, 绿线代表X和SPP的辐射衰减计算值.图片摘自文献[17].

    Figure 7.  Time-resolved differential reflectivity signal (∆R/R) (a) for UP and LP mode (b) for resonant excitation. (c) ∆R/R dynamics (logarithmic scale) at the X resonance of the bare dye film, and near the LP (1.74 eV) and UP (1.84 eV) resonances of the hybrid structure. (d) Measured polariton population damping term as a function of detuning angle (circles) compared to predictions of the coupled oscillator model (solid). Dashed lines denote the results in the absence of incoherent photon exchange. Green: damping rates of uncoupled X and SPP modes. Results are taken from Ref. [17].

    图 8  X-SPP强耦合系统的拉比振荡. (a)时序为15 fs的超快泵浦光和探测光平行θ=39°入射情况下,在p=430 nm光栅周期杂化纳米结构上的反射图谱(ΔR/R)(ωpr, τ)的测量值. (b)在τ=0时实验值(红色曲线)和密度矩阵的模拟值(黑色虚线)比较. (c) LP附近反射谱信号ΔR/R在不同入射角度下的时间演变。(d), (e) θ=39°时反射图谱(ΔR/R)(ωpr, τ)的模拟值以及SPP和X布居数动力学特征. (f)振荡周期的测量值(三角)和模拟值(黑色实线)比较,红色实线代表UP和LP的共振波长位置的计算值.图片摘自文献[39].

    Figure 8.  Coherent dynamics of X-SPP Rabi oscillations. (a) Measured differential reflectivity map (ΔR/R)(ωpr, τ) for a hybrid structure with p=430 nm, recorded using two nearly collinearly propagating 15 fs pulses with time delay τ at an incidence angle of θ=39°. (b) Comparison between measured (solid line) and simulated (dashed line) differntial spectra. (c) Time evolution of the ΔR/R signal near the LP resonance measured at two different angles. (d), (e) Simulated (ΔR/R)(ωpr, τ) map (d) and pump-induced SPP and exciton population dynamics atθ=39°(e). (f) Comparison between observed (open symbols) and calculated (solid lines, error bars taken as standard deviation of Fouriertransformed ΔR (ωpr, τ) traces) oscillation periods and LP resonance energies. Results are taken from Ref. [39].

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出版历程
收稿日期:  2016-11-04
修回日期:  2016-12-24
刊出日期:  2017-02-15

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