光电工程

单光子泵浦下基于光子晶体微腔的CsPbBr₃量子点低阈值放大自发辐射

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冯全红 , 李云霄 , 刘正豪 , 程晨 ^*^,^*

光电工程 | 科研论文 2026,53(7): 260101-1

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光电工程 |科研论文 2026 , 53 (7) : 260101 -1

单光子泵浦下基于光子晶体微腔的CsPbBr₃量子点低阈值放大自发辐射

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程晨 (1989-)，男，博士，副教授，研究方向包括超快激光与物质相互作用、集成光子器件等。在‌IEEE J. Sel. Top. Quantum Electron.‌、ACS Photonics和Appl. Phys. Lett.等同行评审期刊上发表论文50余篇。此外，主持了由国家自然科学基金、国家重点研发计划以及山东省自然科学基金资助的多项科研项目。E-mail：drccheng@sdnu.edu.cn drccheng@sdnu.edu.cn

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冯全红, 李云霄, 刘正豪, 程晨^*^,^*

作者信息

山东师范大学物理与光电学院，山东济南 250300

通讯作者:

程晨，drccheng@sdnu.edu.cn

作者简介:

作者贡献

冯全红：论文撰写、数据收集；李云霄：模拟仿真、实验指导；刘正豪：数据收集；程晨：论文指导选题、论文撰写与审核。

冯全红 (2001-)，女，硕士研究生。研究聚焦钙钛矿微纳光子器件和钙钛矿发光机制机理。E-mail：2024317064@stu.sdnu.edu.cn 2024317064@stu.sdnu.edu.cn

Low-threshold amplified spontaneous emission in CsPbBr₃ quantum dots via photonic crystal microcavities under single-photon pumping

Quanhong Feng, Yunxiao Li, Zhenghao Liu, Chen Cheng

Affiliations

School of Physics and Optoelectronics, Shandong Normal University, Jinan, Shandong 250300, China

Corresponding Author:

drccheng@sdnu.edu.cn

出版时间: 2026-07-25 doi: 10.12086/oee.2026.260101

文章导航

摘要

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全无机卤化物钙钛矿CsPbX₃（X = Cl, Br, I）量子点（quantum dots, QDs）因其极高的荧光量子产率和带隙可调等特性，已成为新一代激光增益介质的研究焦点。然而，在全无机体系中实现超低阈值放大自发辐射（amplified spontaneous emission, ASE）仍是当前光电子器件走向实用化的核心挑战之一。本研究提出将CsPbBr₃ QDs与SiO₂基光子晶体（photonic crystals, PCs）集成的协同策略，构建CsPbBr₃-QD-PCs复合微腔结构，以显著提升光学增益。通过时域有限差分法（FDTD）仿真优化微腔设计，采用真空辅助自组装法制备复合薄膜，并系统表征了其结构、稳态光谱及超快动力学特性。结果表明，得益于Purcell效应为核心的微腔增强，CsPbBr₃-QD-PCs的光致发光 (photoluminescence, PL)强度增强至纯QDs薄膜的3.8倍，PL寿命从1.96 ns缩短至1.24 ns。在400 nm飞秒激光泵浦下，该复合体系实现了低至8.7 μJ/cm²的ASE阈值；瞬态吸收光谱揭示微腔使光学增益寿命从1924 ps大幅缩短至618 ps，显著加速了粒子数反转的建立。本研究阐明了光子晶体微腔增强钙钛矿光学增益的物理机制，为低功耗全无机受激发射器件提供了关键技术平台。

关键词

钙钛矿 / 光子晶体 / 量子点 / 放大自发辐射

Abstract

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Objective

All-inorganic CsPbX₃ quantum dots (QDs) are promising gain media for next-generation lasers due to their excellent optoelectronic properties and superior stability. However, achieving ultralow-threshold amplified spontaneous emission (ASE) remains a challenge. While hybrid perovskites integrated with photonic crystals (PCs) suffer from environmental instability, the integration of stable CsPbX₃ QDs with PC microcavities is still in its infancy. Here, we engineer a PC microcavity that synergistically couples with CsPbBr₃ QDs to enhance the spontaneous emission rate via the Purcell effect, thereby dramatically reducing the ASE threshold under single-photon pumping and elucidating the underlying gain dynamics.

Methods

A strategy that integrates CsPbBr₃ QDs with SiO₂-based PCs to construct a composite microcavity (CsPbBr₃-QD-PCs) was proposed. The PC microcavity was first optimized using the finite-difference time-domain (FDTD) method. The physical model consisted of close-packed SiO₂ microspheres (refractive index n=1.46) on a quartz substrate (n=1.54), coated with CsPbBr₃ QDs (n=2.3–2.5). The resonance wavelength was governed by a modified Bragg diffraction equation, and the Purcell factor F_p was computed to quantify spontaneous emission enhancement. The simulation parameter space included SiO₂ microsphere diameters d=50–1000 nm, diffraction orders m=1 and 2, and QD overlayer thickness increments ΔH. Experimentally, CsPbBr₃ QDs were synthesized via the ligand-assisted reprecipitation (LARP) method at room temperature, using CsBr and PbBr₂ as precursors with oleic acid and oleylamine as ligands dissolved in DMF/DMSO, followed by a two-step centrifugation purification. The PC template was fabricated via an SDS-assisted lifting method using SiO₂ microspheres of approximately 253 nm diameter, forming a hexagonal close-packed periodic structure. CsPbBr₃ QD solution was infiltrated into the PC template under low vacuum (0.3–0.6 Pa). A dense CsPbBr₃ QD film on quartz served as the control. Characterizations included XRD, SEM, steady-state absorption and PL spectroscopy, time-resolved photoluminescence (TRPL), and femtosecond transient absorption (TA) spectroscopy. The pump source was a Ti:sapphire femtosecond laser amplifier (Spectra-Physics Solstice Ace) frequency-doubled via a BBO crystal to produce 400 nm pulses (~35 fs, 1 kHz).

Results and Discussions

FDTD simulations revealed three key features of F_p within the CsPbBr₃ QD emission window (λ=500–550 nm): 1) high F_p at diffraction orders m=1 and m=2; 2) the F_p peak red-shifts with increasing SiO₂ diameter d owing to variations in the lattice constant and filling fraction; 3) the maximum F_p exhibits a near-periodic distribution with m. Fine spectral scans identified d=170 nm (m=1) and d=250 nm (m=2) as optimal diameters, both with F_p peaking near 540 nm. The d=250 nm design was selected for its superior robustness: the ΔH tolerance range maintaining F_p > 2.5 was approximately 300 nm, substantially broader than the ~200 nm range for d=170 nm, attributable to stronger electric field localization.

XRD confirmed the orthorhombic phase of CsPbBr₃ QDs. SEM revealed the periodic hexagonal close-packed structure and uniform QD coverage, with a continuous QD layer (D₁≈436 nm) fully encapsulating the SiO₂ microspheres (D₂≈253 nm), yielding ΔH≈183 nm consistent with FDTD optimization. Despite lower absorption due to the SiO₂ volume, the PL intensity of CsPbBr₃-QD-PCs was enhanced 3.8-fold compared with bare QD films, accompanied by a PL redshift of approximately 15 nm. This redshift is primarily attributed to the spectrally selective Purcell enhancement (F_p peaking at λ≈540 nm), with additional contributions from the modified local dielectric environment and enhanced reabsorption of shorter-wavelength photons. TRPL measurements showed that the PL lifetime was shortened from 1.96 ns (bare QDs) to 1.24 ns (QD-PCs), directly evidencing the Purcell-enhanced spontaneous emission rate.

Under 400 nm femtosecond laser pumping, CsPbBr₃-QD-PCs exhibited clear ASE: a narrow emission peak emerged at ~540 nm with superlinear intensity growth. The ASE threshold was determined to be 8.7 μJ/cm², with the FWHM narrowing to approximately 6.7 nm. Bare CsPbBr₃ QD films showed no ASE under identical conditions, confirming the essential role of the PC microcavity.

TA spectroscopy further elucidated the gain dynamics. Both samples shared four spectral features: excited-state absorption (470–500 nm), ground-state bleaching (GSB, 500–530 nm), transient photoinduced absorption (530–550 nm), and its subsequent inversion into stimulated emission. The PC microcavity shifted the GSB center wavelength consistently with the PL redshift and accelerated the GSB rise time from 1501 ps to 960 ps, indicating Purcell-enhanced carrier relaxation to the band edge. Critically, the optical gain lifetime at ~540 nm was drastically shortened from 1924 ps (bare QDs) to 618 ps (QD-PCs), a ~3.1-fold acceleration. This demonstrates that the PC structure activates a highly efficient stimulated emission channel, enabling the excited state to be rapidly depleted via stimulated emission and outcompeting nonradiative recombination. A systematic comparison with reported CsPbBr₃-based gain media—including thermally evaporated films (~35 μJ/cm²), spin-coated films (26–100 μJ/cm²), and glass-embedded nanocrystals (~54.5 μJ/cm²)—confirms the competitiveness of the 8.7 μJ/cm² threshold achieved here. The solution-based self-assembly approach offers the advantage of large-area, low-cost fabrication without complex lithography.

Conclusions

In summary, we have demonstrated ultralow-threshold ASE by integrating CsPbBr₃ QDs with a PC microcavity. FDTD optimization yielded a CsPbBr₃-QD-PCs composite with F_p > 2.5 and strong electric field confinement, fabricated via vacuum-assisted self-assembly. The PC microcavity enhanced the PL intensity 3.8-fold, shortened the PL lifetime from 1.96 ns to 1.24 ns, and accelerated the optical gain lifetime from 1924 ps to 618 ps, enabling an ASE threshold of 8.7 μJ/cm² under single-photon pumping. This work elucidates the Purcell effect-driven mechanism by which PC microcavities enhance perovskite optical gain, and provides a platform for developing low-power, high-performance all-inorganic perovskite laser devices.

Key words

perovskite / photonic crystals / quantum dots / amplified spontaneous emission

引用本文

冯全红, 李云霄, 刘正豪, 程晨. 单光子泵浦下基于光子晶体微腔的CsPbBr₃量子点低阈值放大自发辐射. 光电工程, 2026 , 53 (7) : 260101 -1 . DOI: 10.12086/oee.2026.260101

Quanhong Feng, Yunxiao Li, Zhenghao Liu, Chen Cheng. Low-threshold amplified spontaneous emission in CsPbBr₃ quantum dots via photonic crystal microcavities under single-photon pumping[J]. Opto-Electronic Engineering, 2026 , 53 (7) : 260101 -1 . DOI: 10.12086/oee.2026.260101

正文

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1　引　言

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全无机卤化物钙钛矿量子点，特别是CsPbX₃ (X = Cl， Br， I)，因其极高的光致发光量子产率、带隙易于调控以及可低温合成等优异特性，在光电子学领域引起了广泛关注^[1-5]，其卓越的发光性能和不断提升的热稳定性使其在高性能白光发光二极管等领域展现出巨大的应用潜力^[6]，为了满足高性能器件对量子点高质量、规模化制备的需求，研究人员致力于开发和优化包括热注射法、配体辅助再沉淀法，以及超声化学辅助法等在内的多种低成本、高效率的量子点本征制备工艺^[7]。在高性能激光器开发中，CsPbX₃作为增益介质展现出卓越的非线性光学潜力^[8-11]。放大自发辐射是实现激光输出的先决条件，它为激光的产生提供了必要的光学放大过程^[12-14]。ASE阈值直接反映了材料以最小能量输入实现并维持粒子数反转的能力，因此实现低阈值放大自发辐射 (amplified spontaneous emission, ASE)对于开发实用型激光器至关重要^[15]。为了突破增益介质固有自发辐射特性的限制，研究人员们致力于研究各类微纳尺度下的工程化光学微腔，如利用钙钛矿自然结晶形成的单晶纳米线 (法布里-珀罗腔)^[16]和纳米板 (回音壁模式腔)^[17]结构的固有光学限域效应，已成功实现激光输出。除了这些天然的几何结构外，研究人员还探索了回音壁微球腔^[18]、垂直腔^[19]以及光子晶体^[20]等人工谐振腔，以进一步增强光与物质的相互作用。在诸多谐振腔结构中，光子晶体的独特优势在于能够通过高品质因子 (Q)与小模式体积 (V_m)调控Purcell效应，进而调节自发辐射速率，从而有效提高光学增益并实现低阈值ASE乃至激光输出。

尽管现有研究取得了一定进展，但在基于CsPbX₃的系统中实现超低的ASE阈值仍然存在挑战。虽然MAPBX₃ (有机-无机杂化钙钛矿)光子晶体已经实现了单模激光^[15,21]和分布反馈激光^[22]，但它们的环境不稳定性阻碍了实际应用。相比之下，全无机CsPbX₃量子点展现出更为卓越的环境稳定性、热稳定性，以及优异的非线性光学特性，但将其与高分辨率微纳结构进行深度集成或大规模图案化组装的研究仍处于起步阶段^[23]，如何兼顾器件集成度与材料本征稳定性是当前的核心挑战之一^[24]。目前针对CsPbX₃-PCs的研究主要集中于单光子泵浦的ASE^[25]，而在揭示微腔设计、增益动力学与阈值降低之间的内在耦合机制方面，尚存在巨大的探索空间。

本文提出了一种将CsPbBr₃量子点与SiO₂基光子晶体相结合的协同策略 (CsPbBr₃-QD-PCs)，在单光子泵浦下实现了超低的ASE阈值。基于时域有限差分模拟的仿真结果，我们精确设计了具有优化的Purcell因子 (

$ {F}_{\rm{p}} $

> 2.5)和强电场限域效应的光子晶体微腔。通过真空辅助自组装技术，利用直径253 nm的SiO₂微球的真空辅助自组装技术成功制备了CsPbBr₃-QD-PCs，结果表明，该复合体系PL强度增强至原始量子点的3.8倍，且荧光寿命较原始量子点有所缩短 (从1.96 ns降至1.24 ns)。TA光谱进一步证实，该结构加速了光学增益的过程 (增益寿命从1924 ps缩短至618 ps)，从而极大地促进了受激辐射粒子数反转的建立。据此，本文方法成功实现了单光子泵浦下低至8.7 μJ/cm²的ASE阈值，在开发实用化、低阈值钙钛矿激光器领域取得了重要进展。

2　仿真模拟

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CsPbBr₃-QD-PCs的结构优化采用了时域有限差分法，该计算方法因其能精确解析电磁场分布而被广泛应用于光子器件设计。首先在仿真软件中进行物理建模：将密堆积的SiO₂微球 (折射率n = 1.46)紧密放置在石英基底 (折射率n = 1.54)上，并用CsPbBr₃-QDs (折射率n = 2.3~2.5)包覆SiO₂微球。光子晶体微腔的谐振波长

$ {\lambda }_{\rm{c}} $

由布拉格衍射决定，修正后的布拉格衍射方程式 (1)所示^[24]。衍射波长取决于晶格常数a、介质填充率f、介质折射率n、入射光角θ和衍射级m。

$ m{\lambda }_{\rm{c}}=2a\sqrt{{ ({{f}_{1}}{{n}_{1}}+\left (1-{f}_{1}\right){{n}_{2}})}^{2}-{\sin }^{2} \theta } \;.$

(1)

式 (1)表明可以通过改变a和f₁来调控

$ {\lambda }_{\rm{c}} $

，使光谱对准CsPbBr₃-QDs的荧光波段 (λ= 500~550 nm)^[26-27]。材料在腔内的自发辐射速率

$\varGamma \left (\lambda \right) $

、Purcell因子(

$ F_{\mathrm{p}} $

)分别由式 (2)、 (3)给出，其中

$ {\varGamma }_{0}\left (\lambda \right) $

为材料在没有腔结构时的自发辐射速率，

$ L\left(\lambda\right)=1/\left(1+4Q^2\left(\lambda/\lambda\mathrm{_c}-1\right)^2\right) $

是PCs微腔的洛伦兹谱，

$ \psi =E\mu /\left| {E}_{\max}\right| \left| \mu \right| $

表示偶极辐射

$ \mu $

和腔内电场E对自发辐射率的影响因素，

$ {F}_{\text{leak}} $

是PCs微腔的辐射泄漏损耗^[26]。如式 (2)所示，具有高

$ F_{\mathrm{p}} $

的PCs微腔能够显著提升自发辐射速率。自发辐射速率的提升有利于提高材料的光学增益，降低ASE阈值，进而促进激光的产生^[28-31]。

$ \varGamma \left (\lambda \right)={\varGamma }_{0}\left (\lambda \right)[F_{\rm{p}}L\left (\lambda \right){\left| \psi \right| }^{2}]+{F}_{\text{leak}}\;, $

(2)

$ F_{\rm{p}}=(3\lambda_{\rm{c}}^3Q)/(4\pi^2n^3V\mathrm{_m})\; . $

(3)

利用FDTD对CsPbBr₃-QD-PCs薄膜的Purcell因子进行仿真，仿真结果如图1所示。图1(a)展示了当ΔH = 0 (ΔH表示CsPbBr₃-QDs薄膜高出SiO₂微球上表面的厚度)时，在扫描步长为5 nm的设置下，

$ {F}_{\rm{p}} $

随SiO₂微球直径 (d)和衍射级数 (m)的变化情况。在图1中可以观察到

$ {F}_{\rm{p}} $

的三个关键特征： 1)如图1(a)的插图所示，CsPbBr₃-QDs的荧光发射波段衍射级次m = 1和m = 2时观察均能观察到较高的

$ {F}_{\rm{p}} $

值； 2)对于固定的m，随着d的增大，

$ {F}_{\rm{p}} $

峰发生红移。这是由于a和f的比例发生变化导致了光子晶体微腔谐振波长的红移 (如式 (1)所示)； 3)

$ {F}_{\rm{p}} $

的最大值随m的增加呈现近周期性分布，该分布受与微球直径d相关的a及f的共同调制。尽管增加ΔH会对

$ {F}_{\rm{p}} $

的峰值引入微小扰动，但SiO₂微球的直径仍是影响

$ {F}_{\rm{p}} $

的主要因素。

图1(b)和1(c)分别给出了m = 1和m = 2时，扫描步长为1 nm的精细

$ {F}_{\rm{p}} $

光谱。通过精细扫描结果可以明显看出，当d = 170 nm和d = 250 nm时，CsPbBr₃-QD-PCs在量子点发射波段内表现出较高的

$ {F}_{\rm{p}} $

，且其

$ {F}_{\rm{p}} $

峰值在

$ \lambda $

= 540 nm附近 (图1(f))。其中，d = 250 nm的CsPbBr₃-QD-PCs表现出更优异的鲁棒性，能够在更宽的厚度变化范围内将Purcell因子维持在

$ {F}_{\rm{p}}> $

2.5 (见图1(d)与1(e))。当d = 170 nm 时，随着ΔH的增加，Purcell因子峰值呈现周期性分布。在CsPbBr₃-QDs的荧光波段内，存在特定的ΔH范围对应高Purcell因子，ΔH可调范围约为200 nm。当d = 250 nm 时，随着ΔH的增加，Purcell因子峰值同样呈现周期性分布。值得注意的是，具有高Purcell因子的ΔH可调范围约为300 nm，远大于d = 170 nm时的可调范围。因此d = 250 nm的钙钛矿光子晶体在更宽广的薄膜可调范围表现出了高Purcell因子，这可以作为选择该结构的原因之一。电场强度分布图 (图1(g))表明，这种对厚度变化的稳健性归因于其更强的电场局域效应。

3　实　验

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本研究采用配体辅助再沉淀法 (ligand-assisted reprecipitation‌, LARP)在室温大气环境下合成全无机CsPbBr₃量子点。将适量溴化铯 (CsBr，西安浴光日能科技有限公司，规格：99.999%)、溴化铅 (PbBr₂，西安浴光日能科技有限公司，规格：99.999%)以及油酸 (oleic acid, OA，西格玛奥德里奇贸易有限公司，规格：99.9%)与油胺 (oleylamine, OAm，韶远科技，规格：95.6%)配体溶解于N,N-二甲基甲酰胺 (DMF，毕得医药，规格：97%)和二甲基亚砜 (DMSO，西格玛奥德里奇贸易有限公司，规格：99.9%)的混合溶剂中，剧烈搅拌至完全溶解，得到前驱体溶液。随后，将前驱体迅速注入剧烈搅拌的无水甲苯中，溶液瞬间转为黄绿色，表明量子点快速成核生长。为去除大尺寸杂质、未反应的前驱体盐及高沸点溶剂，对粗溶液进行双步离心纯化：先经低速离心弃去大颗粒沉淀，保留上清液；随后在上清液中加入适量乙酸乙酯作为反溶剂，静置后高速离心以洗脱残留的DMF/DMSO和过剩配体。最终收集高纯度CsPbBr₃量子点沉淀，并重新分散于无水甲苯中备用^[32]。

如图2所示，本研究采用真空辅助自组装法制备了CsPbBr₃-QD-PCs样品。首先，采用十二烷基硫酸钠 (sodium dodecyl sulfate, SDS)辅助提升法制备了紧密堆积的光子晶体模板，形成周期性的六方紧密堆积结构。随后，在低真空度 (0.3~0.6 Pa)条件下，将CsPbBr₃量子点溶液逐渐滴加到PCs表面，以确保溶液的均匀渗透并形成高质量的薄膜。作为对比，另一组实验中，直接将量子点溶液滴涂在清洗后的石英衬底上，并进行相同的低压处理，制备了一层致密的CsPbBr₃-QDs薄膜。随后，采用X射线衍射 (X-ray diffraction, XRD)和扫描电子显微镜 (scanning electron microscope, SEM)对CsPbBr₃-QD-PCs的结构性质进行了表征。

图3(a)显示了PCs和CsPbBr₃-QD-PCs的XRD图谱。CsPbBr₃-QD-PCs薄膜中的主要衍射峰分别对应于CsPbBr₃正交相的 (100)、 (110)、 (200)和 (210)晶面，表明CsPbBr₃-QDs在PCs上具有较高的结晶质量，SEM成像进一步验证了PCs和CsPbBr₃-QD-PCs的结构完整性。图3(b)显示了SiO₂微球的周期性六方紧密堆积结构，而图3(c)显示了CsPbBr₃-QDs已均匀覆盖在PCs表面。横截面SEM图像 (图3(d))显示，量子点形成了厚度为D₁ ≈ 436 nm的连续层，完全包裹了直径D₂ ≈ 253 nm的SiO₂微球 (如白圈所示)。如图3(e)和3(g)所示，上述连续层与SiO₂微球的厚度偏差 (ΔH ≈ 183 nm)与FDTD优化参数一致，从而确保了系统具备高的

$ {F}_{\rm{p}} $

和强电场局域效应。

图3(e)展示了CsPbBr₃-QD-PCs和CsPbBr₃-QDs薄膜的吸收光谱。由于SiO₂基PCs占据了CsPbBr₃-QDs薄膜的部分体积，CsPbBr₃-QD-PCs的吸收强度明显低于CsPbBr₃-QDs。尽管吸收减弱理论上会导致发射减弱，但在相同的400 nm飞秒激光激发条件下，CsPbBr₃-QD-PCs的发光强度仍是CsPbBr₃-QDs薄膜的3.8倍 (图3(f))，且CsPbBr₃-QD-PCs的PL发射峰表现出15 nm的红移。随后，测量了时间分辨光致发光 (time-resolved photoluminescence，TRPL)寿命。如图3(g)所示，CsPbBr₃-QDs的PL寿命为1.96 ns，而CsPbBr₃-QD-PCs的PL寿命缩短至1.24 ns。PL寿命的缩短直观反映了微腔对自发辐射速率的提升，这是导致PL增强的重要因素^[33-36]。同时如图1(f)所示，CsPbBr₃-QD-PCs在其荧光光谱的高波段范围内 (530~550 nm)具有较高的

$ {F}_{\rm{p}} $

，并在540 nm处达到峰值。这一高

$ {F}_{\rm{p}} $

不仅为自发辐射速率的提升提供了理论支持 (如式 (2)所示)，也解释了实验中观测到的PL峰红移现象。

为研究PCs结构对ASE性能的影响，记录了在400 nm的飞秒激光泵浦下CsPbBr₃-QD-PCs和CsPbBr₃-QDs的光致发光光谱。泵浦光源为钛宝石飞秒激光放大器 (spectra-physics solstice ace)经BBO倍频模块产生的400 nm脉冲，脉宽约35 fs，重复频率1 kHz。图4(a)展示了在单光子飞秒泵浦下CsPbBr₃-QD-PCs的发射光谱随泵浦密度的演变。可以清晰地看到，随着泵浦强度的增加，在540 nm处出现了一个极窄的发射峰，且其峰值强度随泵浦通量的增加呈非线性迅速放大，这是ASE的一个典型特征。图4(b)进一步量化了这一特性：当泵浦密度达到8.7 μJ/cm²时，输出强度曲线的斜率发生了明显的转折 (即阈值行为)，同时半高全宽 (full width at half maximum, FWHM)迅速收窄至约为6.7 nm。相比之下，如图4(c)所示，CsPbBr₃-QDs薄膜在相同泵浦条件下并未出现ASE现象。这表明CsPbBr₃-QD-PCs薄膜的ASE的实现高度依赖于光子晶体结构的作用，其核心驱动力源于Purcell效应驱动^[28-29]。

$ {F}_{\rm{p}} $

在ASE的中心波长处达到峰值 (如图1(f)所示)这一事实，进一步印证了上述物理机制。

为了深入探究PCs结构对CsPbBr₃-QDs光学增益动力学的影响，我们在400 nm泵浦下获得了CsPbBr₃-QD-PCs和CsPbBr₃-QDs的瞬态吸收光谱。图5(a)和图5(b)分别展示了CsPbBr₃-QD-PCs和CsPbBr₃-QDs的二维伪彩色瞬态吸收(transient absorption，TA)光谱，图5(c)和图5(d)则分别提取了在0.2 ~7000 ps的不同延迟时间范围内的TA信号。通过对比分析发现，两者具有四个共同的光谱特征： 1)在470~500 nm范围内有光诱导激发态吸收； 2)在500~530 nm范围内存在明显的基态漂白信号； 3)在530~550 nm范围内，初始阶段观察到瞬态光吸收信号； 4)随着延迟时间的增加，该光吸收信号迅速反转为受激辐射信号。然而，PCs微腔的引入也导致了两者的TA光谱呈现显著差异：首先，可以清楚地观察到基态漂白信号中心波长发生了偏移(图5(c)和图5(d))，这与PCs结构引起的CsPbBr₃-QD-PCs的稳态PL峰的红移(图3(f))是一致的。至此，CsPbBr₃-QD-PCs的PL红移可归因于以下机制的协同作用：1) Purcell因子的光谱选择性增强是主导因素——本PC结构的

$ {F}_{\rm{p}} $

在λ ≈ 540 nm处达到峰值且在530~550 nm波段维持较高水平，这导致QD发射波段内长波长侧的自发辐射速率被选择性增强，从而在表观上拉动PL峰位向长波方向移动；2) PC结构改变了QD周围的局部介电环境 (有效折射率增大)，介电屏蔽的变化可引起激子结合能的微小改变，导致带边跃迁能量红移，这与TA光谱中观测到的基态漂白峰中心波长偏移一致；3) CsPbBr₃-QD-PCs的光散射增强使得PL光子在逃逸表面前经历更多的重吸收——短波长光子因吸收截面较大而被优先消耗，也会使表观PL峰位红移。综合而言，Purcell增强的光谱选择性是最主要的物理机制，介电环境变化和重吸收效应为辅助贡献。

瞬态动力学曲线进一步揭示了两者在激发态弛豫过程中的差异。如图5(e)所示，CsPbBr₃-QD-PCs的基态漂白信号建立时间约为960 ps，显著快于CsPbBr₃-QDs的1501 ps (如图5(f))。这种加速的基态漂白动力学过程表明，CsPbBr₃-QD-PCs中载流子的辐射复合速率得到了提升，使得载流子能够从高能态更快速地弛豫至能带边缘，这一物理过程极为有利于ASE的产生^[13]。图5(g)和图5(h)分别展示了两者在ASE波长 (约540 nm)处的TA动力学衰减曲线。纯CsPbBr₃-QDs的光学增益寿命为1924 ps，而在引入PCs结构后，CsPbBr₃-QD-PCs的增益寿命大幅缩短至618 ps。需特别指出，此处的光学增益寿命 (由TA动力学在高激发密度下测量)与前述TRPL寿命 (在低激发密度下测量)是两种不同物理过程的度量，二者的差异具有明确的物理含义。PL寿命 (1.24~1.96 ns)反映的是低激发密度下 (远低于ASE阈值)的自发辐射衰减过程，其特征时间为自发辐射寿命

$ \tau\mathrm{_r} $

；光学增益寿命 (618~1924 ps)反映的是高激发密度下 (>ASE阈值、存在粒子数反转)受激辐射与自发辐射共同作用的衰减过程。增益寿命远短于PL寿命是受激辐射通道打开的直接标志——ASE建立后腔内光子密度急剧增大，受激辐射速率与光子密度成正比，远大于自发辐射速率，因此总衰减大幅加速。值得关注的是，纯CsPbBr₃-QDs薄膜的增益寿命 (1924 ps)与其PL寿命 (1.96 ns)接近，表明在无PC反馈的条件下受激辐射通道低效，增益衰减以自发辐射为主导，这与图4(c)中纯QD薄膜未出现ASE的实验事实自洽。相反，CsPbBr₃-QD-PCs中增益寿命从1924 ps大幅缩短至618 ps (约3.1倍加速)，说明PC结构通过Purcell增强与Bragg反馈成功激活了高效的受激辐射通道，使激发态能以受激辐射的方式被迅速消耗^[18,25]。这一更为迅捷的增益建立与衰减过程表明，CsPbBr₃-QD-PCs中，激子通过辐射复合释放能量的速率成功竞争过了陷阱态捕获、声子散射和俄歇复合等非辐射复合通道^[21,35]。这证明了CsPbBr₃-QD-PCs能够更迅速地实现并消耗激发态粒子数反转，快速建立起稳定的增益状态，从而实现对产生ASE至关重要的高效光放大过程。

为了客观评估本研究CsPbBr₃-QD-PCs的ASE性能水平，将本文实验结果与近年来报道的CsPbBr₃基增益介质的ASE阈值进行了系统对比。结果表明，本研究实现的8.7 μJ/cm²阈值在溶液法CsPbBr₃量子点体系中处于领先水平。例如，热蒸发法制备的CsPbBr₃薄膜ASE阈值约为35 μJ/cm^{2 [36]}，溶液旋涂法制备的CsPbBr₃薄膜阈值通常在26~100 μJ/cm²范围内^[37]，而嵌入玻璃基质中的CsPbBr₃纳米晶阈值约为54.5 μJ/cm^{2 [38]}。本研究采用的光子晶体微腔策略展现出独特的物理优势：Purcell效应在增强自发辐射速率的同时，还加速了光学增益的建立过程 (如瞬态吸收光谱所证实)。

4　结　论

收起

本研究中通过将CsPbBr₃量子点与光子晶体微腔结构相集成，成功实现了超低阈值的放大自发辐射。利用时域有限差分法进行仿真与结构优化，设计并制备了具有高Purcell因子和强电场限域效应的CsPbBr₃-QD-PCs复合体系。基于自组装光子晶体模板，采用真空辅助组装工艺确保了量子点在微腔间隙中的均匀渗透与高质量成膜。实验表征结果表明，得益于微腔增强效应，CsPbBr₃-QD-PCs的PL寿命从1.96 ns显著缩短至1.24 ns，PL发光强度提升至纯量子点薄膜的3.8倍。瞬态吸收动力学分析揭示，PCs微腔使光学增益寿命从1924 ps大幅缩短至618 ps，极大地加速了激发态粒子数反转的建立过程。凭借以上性能优势，该体系在单光子泵浦条件下，实现了低至8.7 μJ/cm²的ASE阈值。本研究不仅深入剖析了光子晶体微腔增强钙钛矿材料光学增益的内在物理机制，也为开发新一代低功耗、高性能的全无机钙钛矿激光器件提供了重要的理论依据与技术支撑。

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2026年第53卷第7期

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doi: 10.12086/oee.2026.260101

接收时间：2026-04-28
首发时间：2026-10-22
出版时间：2026-07-25

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收稿日期：2026-04-28
修回日期：2026-07-13
录用日期：2026-07-14

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山东师范大学物理与光电学院，山东济南 250300

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程晨，drccheng@sdnu.edu.cn

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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