Research progress of single quantum-dot  spectroscopy and exciton dynamics

Li Bin; Zhang Guo-Feng; Chen Rui-Yun; Qin Cheng-Bing; Hu Jian-Yong; Xiao Lian-Tuan; Jia Suo-Tang

doi:10.7498/aps.71.20212050

Abstract

Colloidal semiconductor quantum dots (QDs) have strong light absorption, continuously adjustable narrowband emission, and high photoluminescence quantum yields, thereby making them promising materials for light-emitting diodes, solar cells, detectors, and lasers. Single-QD photoluminescence spectroscopy can remove the ensemble average to reveal the structure information and exciton dynamics of QD materials at a single-particle level. The study of single-QD spectroscopy can provide guidelines for rationally designing the QDs and giving the mechanism basis for QD-based applications. We can also carry out the research of the interaction between light and single QDs on a nanoscale, and prepare QD-based single-photon sources and entangled photon sources. Here, we review the recent research progress of single-QD photoluminescence spectroscopy and exciton dynamics, mainly including photoluminescence blinking dynamics, and exciton and multi-exciton dynamics of single colloidal CdSe-based QDs and perovskite QDs. Finally, we briefly discuss the possible future development trends of single-QD spectroscopy and exciton dynamics.

Keywords:

Authors and contacts

1.
Key Laboratory of Spectral Measurement and Analysis of Shanxi Province, College of Physics and Information Engineering, Shanxi Normal University, Taiyuan 030031, China
2.
State Key Laboratory of Quantum Optics and Quantum Optics Devices, Institute of Laser Spectroscopy, Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan 030006, China

Corresponding author: Zhang Guo-Feng, guofeng.zhang@sxu.edu.cn ; Xiao Lian-Tuan, xlt@sxu.edu.cn ;

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 62127817, 62075120, 62075122, 61875109, 91950109, 62105193), the Joint Research Fund of the NSFC and STINT (Grant No. 62011530133), the Applied Basic Research Program in Shanxi Province (Grant No. 202103021223254), the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi Province, China (Grant No. 2021L257), the Scientific Research Project for Returned Chinese Scholars of Shanxi Province, China (Grant No. HGKY2019002), and the Program for Middle-aged and Young Innovative Talents of Higher Education Institutions of Shanxi Province, China.

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Cited By

图 1 3种类型的光致发光闪烁　(a)俄歇型闪烁（Auger-blinking）的光致发光强度轨迹^[22]; (b)俄歇型闪烁的光致发光寿命-强度分布图^[22]; (c)带边载流子型闪烁（BC-blinking）的光致发光强度轨迹^[22]; (d)带边载流子型闪烁的光致发光寿命-强度分布图^[22]; (e)热载流子型闪烁（HC-blinking）的光致发光强度轨迹^[23]; (f)热载流子型闪烁的光致发光寿命-强度分布图^[23]

Figure 1. Three types of photoluminescence (PL) blinking: (a) PL intensity trace of Auger-blinking^[22]; (b) fluorescence lifetime-intensity distribution (FLID) map of Auger-blinking^[22]; (c) PL intensity trace of band-edge carrier (BC) blinking^[22]; (d) FLID map of BC blinking^[22]; (e) PL intensity trace of hot-carrier (HC) blinking^[23]; (f) FLID map of HC blinking^[23].

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图 2 带正电激子态与带负电激子态　(a)典型的单量子点的光致发光强度轨迹, 其中亮态(Bright state)、灰态(Gray state)和暗态(Dark state)分别为中性激子态、带负电激子态和带正电激子态; (b)相应的亮态、灰态和暗态的光致发光强度衰减曲线; (c)相应的二阶关联函数曲线; (d)带正电激子态与带负电激子态的形成示意图^[30]

Figure 2. Positive trion state and negative trion state: (a) PL intensity trace of a typical single quantum dot (QD). Bright state, gray state, and dark state represent the neutral exciton state, negative trion state, and positive trion state, respectively. (b) PL decay curves of bright state, gray state, and dark state. (c) Corresponding second-order correlation function (g⁽²⁾) curve. (d) Schematic diagram of the formation of positive and negative trion states^[30].

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图 3 量子点壳层结构对带正电激子态与带负电激子态的影响　(a), (d) CdSe₆₃₀/8CdS单量子点和CdSe₆₃₀/4CdS单量子点的光致发光强度轨迹和相应的强度分布图, 蓝色和红色阴影区域分别对应于带正电激子态和带负电激子态; (b), (e)两类单量子点带正电激子态和带负电激子态的光致发光衰减曲线图; (c), (f)两类单量子点的带正电激子态和带负电激子态的量子产率和俄歇速率的对应关系^[32]

Figure 3. Effect of the shell structure of QDs on positive and negative trion states: (a), (d) PL intensity traces and corresponding histograms of CdSe₆₃₀/8CdS and CdSe₆₃₀/4CdS single QDs. The blue and red shaded regions correspond to positive and negative trion states, respectively. (b), (e) PL decay curves of positive and negative trion states of two kinds of single QDs. (c), (f) Quantum yield and Auger rate of the positive trions versus those of negative trions of two kinds of single QDs^[32].

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图 4 (a) CsPbI₃钙钛矿单量子点的时间依赖的光致发光光谱成像, XX^–, XX, X^2–, X^–和X分别表示带电双激子态、双激子态、高阶带电激子态、带电激子态和单激子态; (b)—(f)相应的X, XX, X^–, XX^–和X^2–的光致发光光谱^[34]

Figure 4. (a) Time-dependent PL spectral image of a single CsPbI₃ perovskite QD. XX^–, XX, X^2–, X^–, and X represent charged biexciton state, biexciton state, higher-order charged exciton state, trion state, and single exciton state, respectively. The PL spectra of X, XX, X^–, XX^–, and X^2– are plotted in (b)–(f), respectively ^[34].

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图 5 CH₃NH₃PbBr₃钙钛矿单量子点的量子限域Stark效应　(a)典型的单量子点的光致发光强度轨迹, 红色和绿色直线区域表示强度不同的中性激子态的光致发光强度; (b)图(a)中红色和绿色直线区域的光致发光强度衰减曲线, 表明较低的光致发光强度对应较大的寿命; (c)相应的二阶关联函数曲线; (d)相应的光致发光寿命-强度分布图; (e)相应的光致发光量子产率与总的复合速率(辐射与非辐射复合速率之和)的分布图^[37]

Figure 5. Intrinsic quantum-confined Stark effect of single CH₃NH₃PbBr₃ perovskite QDs: (a) PL intensity trace of a typical single QD. Red and green lines represent PL intensities of neutral and surface-charged states, respectively. (b) PL decay curves of the PL areas marked by red and green lines. (c) Corresponding g⁽²⁾ curve. (d) Corresponding FLID map. (e) Corresponding distribution of PL quantum yield versus total recombination rate ^[37].

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图 6 (a)不同激发功率下CdSe/CdS单量子点的光致发光强度轨迹和相应的强度分布图; (b)相应的光致发光寿命-强度分布图, “B”和“D”分别代表亮态和灰态; (c)充电速率r_(B→D)和放电速率r_(D→B)随激发条件$ \langle N \rangle$的变化, 其中$\langle N \rangle $表示单个量子点吸收每个激光脉冲中的平均光子数; (d)充电速率r_(B→D)和放电速率r_(D→B)随脉冲光重复频率f的变化^[24]

Figure 6. (a) PL intensity traces and corresponding histograms of a single CdSe/CdS QD under various excitation conditions. (b) Corresponding FLID in color scale. “B” and “D” represent bright states and dim states, respectively. (c) Charging and discharging rates versus $\langle N \rangle $ with a fixed laser repetition frequency ($ f $), where $\langle N \rangle $ is the average number of photons absorbed per QD per pulse. (d) Charging and discharging rates versus f at a given $\langle N \rangle $^[24].

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图 7 (a), (b)核壳界面势陡峭的单量子点(QD1)和核壳界面势平滑的单量子点(QD2)的光致发光强度轨迹和强度分布图, QD2的光致发光闪烁比QD1更剧烈; (c), (d)强度轨迹中的两个高亮区域的光致发光衰减曲线及单指数拟合, 其中灰色曲线为仪器响应函数; (e), (f) QD1和QD2的光致发光闪烁率统计图, QD2的光致发光闪烁率比QD1更高; (g), (h)相应的亮、暗态的概率密度分布图^[46]

Figure 7. (a), (b) Typical PL trajectories for single QDs with sharp interface potential (QD1) and a single QD with smooth interface potential (QD2). The right panels show the corresponding PL intensity histograms. The PL blinking of QD2 is more frequent than that of QD1. (c), (d) Corresponding PL decay curves obtained from the PL regions marked in respective colors on PL intensity trajectories of panel (a) and panel (b), respectively. The solid gray lines are the instrument response function of the system. (e), (f) Histograms of PL blinking rates for the single QD1 and single QD2 obtained under the same excitation. The PL blinking rate of QD2 is higher than that of QD1. (g), (h) Normalized on-state probability densities for the single QD1 and single QD2^[46].

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图 8 利用对苯二胺(PPD)和二甲基苯胺(DMA)抑制单个CdSe类量子点的光致发光闪烁　(a), (b)发射波长为525和622 nm的CdSe/ZnS单量子点、发射波长为800 nm的CdSeTe/ZnS单量子点的典型光致发光强度轨迹; (c), (d)相应的在PPD或DMA作用下的单量子点的光致发光强度轨迹^[30]

Figure 8. Suppression of the PL blinking of single CdSe-based QDs with p-phenylenediamine (PPD) and N, N-dimethylaniline (DMA): (a), (b) Typical PL intensity trajectories of the single CdSe-based QDs with emission wavelengths of 525, 622, and 800 nm in glycerol (cetene), respectively; (c), (d) typical PL intensity trajectories of the single QDs in glycerol with PPD (in cetene with DMA), respectively^[30].

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图 9 (a) CdSeTe/ZnS单量子点在玻片表面和ITO中的光致发光强度轨迹和相应的强度分布图; (b), (c) CdSeTe/ZnS单量子点在玻片表面和ITO中的光致发光闪烁率和亮态比例的统计分布图^[52]

Figure 9. (a) Typical PL intensity trajectories and intensity histograms for the single CdSeTe/ZnS QDs on glass coverslips and encased in ITO, respectively; (b), (c) histograms of blinking rates and proportion of on-state for single QDs on glass coverslips and encased in ITO, respectively^[52].

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图 10 (a)左: Hanbury-Brown-Twiss (HBT)实验装置示意图. 右: 弱光激发条件下双激子和单激子的量子产率之比约等于二阶关联函数零延时处的中心峰面积与边峰面积之比($ g^{(2)}_0 $)^[62]. (b)不同的光致发光强度区域对应的二阶关联函数(g⁽²⁾)^[63]. (c)单光子探测事件与双光子探测事件的示意图^[65]. (d)溶液环境下用于单量子点测量的HBT实验装置示意图^[67]

Figure 10. (a) Left panel: Schematic diagram of Hanbury-Brown-Twiss (HBT) experimental scheme. Right panel: The ratio of quantum yields between biexciton and single exciton excited under weak excitation conditions is approximately equal to the ratio between central peak area and side peak area of g⁽²⁾ function^[62]. (b) g⁽²⁾ functions for different PL intensity regions^[63]. (c) Schematic diagram of single-photon events and two-photon events^[65]. (d) Schematic diagram of HBT experimental scheme for single QDs in solution environment^[67].

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图 11 (a)不同激发条件下的单量子点的光致发光强度轨迹, 红色虚线以上部分定义为光致发光强度轨迹的亮态; (b)相应的强度轨迹的亮态的光致发光衰减曲线, 通过双指数拟合获得双激子寿命^[14]

Figure 11. (a) PL intensity traces of a single QD under different excitation conditions. Bright and dim states are separated by red dashed lines. (b) Corresponding PL decay curves of bright states, and the biexciton lifetime is obtained by biexponential fitting ^[14].

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图 12 (a)带电双激子态和中性双激子态的辐射速率之比、俄歇非辐射速率之比的统计分布图; (b) CdSe/ZnS量子点带电双激子态的辐射复合(红色箭头)和俄歇非辐射复合(黑色箭头)示意图; (c)双激子态和单激子态的辐射速率之比α、通过表面俘获的非辐射复合速率之比β的统计分布图; (d)双激子态的辐射复合(红色箭头)、俄歇非辐射复合(黑色箭头)和表面非辐射复合(灰色箭头)示意图^[22]

Figure 12. (a) Statistical distribution of the ratio of radiative rates and of Auger rates between charged and neutral biexciton states; (b) schematic of radiative recombination pathways (red arrows) and nonradiative Auger recombination (black arrows) of the charged biexciton state for a CdSe-based QD; (c) statistical distributions of the radiative rate ratio (α) and of the surface nonradiative rate ratio (β) between biexciton and single exciton; (d) schematic of radiative recombination pathways (red arrows), Auger recombination pathway (black arrows), and surface nonradiative recombination processes (gray arrows) for the biexciton state^[22]

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图 13 (a)利用4个单光子探测器同时进行HBT探测的共聚焦实验装置; (b)单光子与双光子事件示意图; (c)双激子衰减曲线(绿色)及单指数拟合, 插入图为脉冲光激发下的g⁽²⁾函数; (d)脉冲光激发下的g⁽³⁾函数; (e)三激子衰减曲线(绿色)及单指数拟合; (f) CdSe类量子点三激子复合示意图^[74]

Figure 13. (a) Confocal scanning microscopy equipped with four single-photon detectors for HBT detection. (b) Schematic diagram of single-photon events and two-photon events. (c) PL decay curve of biexciton (green) and corresponding fitted curve. The inset is pulse resolved g⁽²⁾ function. (d) Pulse resolved g⁽³⁾ function. (e) PL decay curve of triexciton (green) and corresponding fitted curve. (f) Model of triexciton recombination of CdSe QD^[74].

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图 14 (a)通过调整PMMA薄膜厚度改变单量子点与金纳米棒之间的距离并测量了$ g^{(2)}_0 $值随距离的变化^[77]; (b)通过原子力显微镜针尖控制金纳米块和单量子点的距离并测量了$ g^{(2)}_0 $值随距离的变化^[78]; (c)核壳界面势调控单量子点双激子俄歇复合速率^[46]

Figure 14. (a) Distance between single QDs and gold nanorods was modulated by PMMA film thickness, and the $ g^{(2)}_0 $ values are measured^[77]; (b) distance between gold nanoparticles and single QD was controlled by AFM tip, and the $ g^{(2)}_0 $ values are measured^[78]; (c) effect of core-shell interface potentials on biexciton Auger rates of single QDs^[46].

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图 15 共聚焦扫描成像过程中单量子点的快速识别　(a), (b)单量子点的单光子和双光子事件成像; (c)相应的时间门控作用后的双光子事件成像; (d)成像图中圆圈C区域中各像素对应的光致发光强度轨迹; (e)每个激发脉冲下单光子事件的探测概率f₁和双光子事件的探测概率f₂以及量子点个数n值的实验与理论关系曲线; (f)共聚焦成像中的量子点个数n值分布图, 其中数字1和2分别表示单量子点和量子点团簇. 图中各标尺长度为3 μm^[65]

Figure 15. Fast recognition of single QDs during confocal scanning imaging: (a), (b) A typical example of images of single-photon and two-photon events of QDs on a glass coverslip; (c) corresponding time-gated two-photon events imaging; (d) PL intensity trace corresponding to each pixel in the circle C region in the image; (e) corresponding experimental and theoretical relationship of the detection probability f₁ of single-photon event, the detection probability f₂ of two-photon event, and the number n of QDs for each excitation pulse; (f) distribution of the number n of QDs in the confocal image. The 1 and 2 represent for single QD and QD clusters, respectively. The scale bars are 3 μm^[65].

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