固体高次谐波产生、调控及应用

汪洋; 刘煜; 吴成印

doi:10.7498/aps.71.20221319

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摘要

基于超快强激光与物质相互作用的高次谐波产生(high-order harmonic generation, HHG)提供了非微扰区光与物质相互作用的研究平台, 同时也是台式化极紫外光源和阿秒脉冲的主要产生途径. 非微扰区固体HHG涉及超快强场物理、凝聚态物理、材料科学和信息科学等领域的核心内容, 自2011年首次在实验中观察到以来, 迅速成为强场物理和阿秒科学的研究前沿. 本综述从一个实验工作者的角度, 总结了固体HHG的研究进展和重要应用. 首先通过对比高次谐波(high-order harmonic, HH)产率和截止能量对驱动激光参数的依赖关系, 展示固体HHG与气体HHG截然不同的特性. 重点介绍固体HHG调控和应用方面的进展, 包括通过设计靶材结构或者激光光场实现对HH产率、偏振、时空分布等精密调控, 以及固体HH谱学技术在材料结构表征和超快电子动力学研究等领域的应用. 最后对固体HHG的未来发展进行了展望.

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Abstract

The generation of high-order harmonics based on the interaction between ultrafast intense laser and matter provides a platform for studying the light-matter interaction in the non-perturbative region. It is also the main route to generating desktop extreme ultraviolet light source and attosecond pulse. The non-perturbative solid high-order harmonic involves the core content of ultrafast strong field physics, condensed matter physics, materials science, information science and other fields. Since it was first experimentally observed in 2011, it has rapidly become the research frontier of strong field physics and attosecond science. This review summarizes the research progress and important applications of solid high-order harmonics from the perspective of an experimentalist. Firstly, distinct characteristics are shown for solid high-order harmonic by comparing the dependence of harmonic yield and cut-off energy on driving laser parameters with gas high-order harmonic. Then, the progress of manipulation and application are highlighted for solid high-order harmonic, including the precise control of harmonic yield, polarization, space-time distribution through the design of target structure or laser field, as well as the application of solid high-order harmonic spectroscopy in the fields of material structure characterization and ultrafast electron dynamics. Finally, the future is prospected for the study of solid high-order harmonics.

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作者及机构信息

北京大学物理学院, 人工微结构与介观物理国家重点实验室, 北京　100871

通信作者: 吴成印, cywu@pku.edu.cn

基金项目: 国家重点研发计划(批准号: 2018YFA0306302)和国家自然科学基金(批准号: 12174011, 11625414)资助的课题.

Authors and contacts

State Key Laboratory for Mesoscopic Physics, School of Physics, Peking University, Beijing 100871, China

Corresponding author: Wu Cheng-Yin, cywu@pku.edu.cn

Funds: Project supported by the National Key R&D Program of China (Grant No. 2018YFA0306302) and the National Natural Science Foundation of China (Grant Nos. 12174011, 11625414).

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施引文献

图 1 固体高次谐波(high-order harmonic, HH)光谱及其产生机制示意图　(a)金表面反射HH谱^[7]; (b) ZnO晶体透射HH谱^[8]; (c) 固体HHG机制示意图

Fig. 1. Solid high-order harmonic (HH) spectrum and schematic diagram of HHG mechanism: (a) Reflection HH spectrum of Au surface ^[7]; (b) transmission HH spectrum of ZnO crystal ^[8]; (c) schematic diagram of solid HHG mechanism.

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图 2 固体损伤阈值、HH谱及晶向依赖　(a) 不同带隙固体材料的损伤阈值^[42]; (b) 固体Ar的HHG^[32]; (c) ZnO HHG截止能量与驱动激光场强呈线性关系^[8]; (d) ZnO^[8], (e) MgO^[9], (f) 金属TiN薄膜^[46]固体材料HHG的晶向依赖

Fig. 2. Damage threshold and HH spectra in solids with different crystallographic orientations: (a) Damage threshold of solid materials with different bandgaps^[42]; (b) high harmonic spectrum of solid Ar^[32]; (c) linear dependence of the HHG cutoff energy in ZnO with the driving laser field strength^[8]. Crystallographic orientation dependence of solid HHG in solid materials of (d) ZnO^[8]; (e) MgO^[9]; (f) TiN metallic film^[46].

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图 3 纳米结构和界面工程控制HHG. (a), (b)金属-蓝宝石锥增强HHG ^[11]　(a) 蓝宝石锥的扫描电镜显微图像; (b) 测量的HH光谱. (c)—(f) 菲尼尔波带片HHG^[13] (c) 在样品平面记录的三次谐波发射模式; (d)三次和(e)五次谐波聚焦扫描; (f) 焦点强度剖面形状

Fig. 3. Control of solid HHG using nanostructure and interface engineering. (a), (b) Enhancement of HHG on a metal-sapphire nanotip^[11]: (a) Scanning electron microscopy (SEM) image of the tips; (b) measured HH spectra. (c)–(f) HHG from Fresnel zone plate (FZP)^[13]: (c) Third-harmonic emission pattern recorded at the sample plane; (d) third and (e) fifth harmonic focus scanning as a distance to sample plane; (f) focus intensity profiles.

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图 4 光场控制固体HHG　(a) MgO HH对CEP依赖性^[44]; (b) ZnO HH谱与双色场相对延迟关系^[65]; (c) 锁定测量MgO HH谱(青色)和平均光谱(紫色)^[67]; (d) 双色正交激光场的控制GaSe倒空间轨迹示意图^[68]; (e) 双色反向旋圆偏光合成场控制手性HHG示意图^[69]; (f) 驻波场增强MgO HHG示意图^[70]

Fig. 4. Control of solid HHG by manipulating driving laser field: (a) CEP dependence of HH in MgO ^[44]; (b) HH spectra in ZnO versus delay between two-color fields^[65]; (c) normalized oscillating harmonic spectrum of lock measurement (cyan) and normalized average spectrum (purple) of MgO^[67]; (d) schematic diagram of k-space trajectories of electrons in GaSe, driven by perpendicularly polarized two-color field^[68]; (e) schematic diagram of controlling chiral HHG by using synthetic two-color counter-rotating circularly polarized light^[69]; (f) schematic diagram of the enhancement of MgO HHG in the standing wave field^[70].

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图 5 固体HHG应用　(a) $ \rm{S}\rm{i}{\rm{O}}_{2} $阿秒条纹谱^[72]; (b) 双层h-BN的感应电子密度随时间的演化^[76]; (c) ZnO能带重构^[77]; (d) ZnSe HH产率随光强的依赖关系^[78]; (e) α-石英贝利曲率重构^[79]; (f) β-WP₂贝利曲率重构^[24]

Fig. 5. Applications of solid HHG: (a) Attosecond-streaking spectrogram in $ \rm{S}\rm{i}{\rm{O}}_{2} $^[72]; (b) time evolution of induced electronic density for distant bilayer h-BN^[76]; (c)band reconstruction of ZnO^[77]; (d) the power of HHG yield versus driving laser intensity for ZnSe^[78]; (e) retrieved Berry curvature of $ \rm{\alpha } $-quartz^[79]; (f) retrieved Berry curvature of β-WP₂^[24].

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图 6 光波驱动$ \rm{W}{\rm{S}\rm{e}}_{2} $准粒子碰撞^[80]　(a) 高阶边带强度$ {I}_{\rm{H}\rm{S}\rm{G}} $随太赫兹驱动场和带间激发脉冲之间延迟时间$ {t}_{\rm{e}\rm{x}} $的依赖关系; 太赫兹场驱动准粒子碰撞示意图, 对应电子-空穴(b)远离和(c)碰撞湮灭, 发射出边带光子$ {h\nu }_{\rm{H}\rm{S}\rm{G}} $; 不同动量k和时间延迟$ {t}_{\rm{e}\rm{x}} $的电子分布, 对应电子-空穴 (d)远离和(e) 碰撞

Fig. 6. Lightwave driven quasi-particle recollision in WSe₂^[80]: (a) Intensity of high order sideband $ {I}_{\rm{S}\rm{H}\rm{G}} $ as a function of the time delay between the THz driving fields and the interband excitation pulse; schematic diagram of the quasi-particle recollision driven by THz field, corresponding to electron-hole (b) apart and (c) recombine, annihilate and emit a sideband photon $ {h\nu }_{\rm{H}\rm{S}\rm{G}} $; electron distribution as a function of momentum k and time delay $ {t}_{\rm{e}\rm{x}} $, corresponding to electron-hole (d) separation (d) and (e) recollision.

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图 7 MgF₂价电子显微成像^[33]　(a) 强激光场下有效晶体势; (b) $ {\rm{M}\rm{g}}^{2+} $半径测量; (c) 几种材料中最小离子/原子半径; (d) 价电子势和电子密度的重构

Fig. 7. Microscopic imaging of valence charge density in MgF₂^[33]: (a) The effective crystal potential along the^[99] crystal orientation under the intense laser field; (b) radius measurement of $ {\rm{M}\rm{g}}^{2+} $; (c) minimum ion/atom radius in several materials; (d) reconstruction of charge potential and valence charge density.

下载: 全尺寸图片幻灯片

图 8 HHG检测$ \rm{V}{\rm{O}}_{2} $相变^[83] (a)实验光路示意图; (b) HHG产率随泵浦光强度和延时关系. $ \rm{M}\rm{o}{\rm{S}}_{2} $电子-空穴相干性检验^[84] (c) 带隙附近的电子-空穴动力学示意图; (d) 退相干时间拟合结果. 拓扑表面态HHG^[17] (e) 拓扑绝缘体能带示意图; (f) HHG产率对材料解离时间依赖关系

Fig. 8. Detection of $ \rm{V}{\rm{O}}_{2} $ phase transition^[83]: (a) Schematic diagram of experimental setup; (b) relationship of harmonic yield with pump laser intensity and delay. Test on coherence of electron-hole pair in $ \rm{M}\rm{o}{\rm{S}}_{2} $^[84]: (c) Schematic diagram of electron-hole dynamics near bandgap; (d) fitted value for the dephasing time. (e) (f) HHG from topological surface^[17]: (e) Schematic diagram of topological insulator band; (f) the HH yield versus the cleavage time of the sample.

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固体高次谐波产生、调控及应用

北京大学物理学院, 人工微结构与介观物理国家重点实验室, 北京　100871

通信作者: 吴成印, cywu@pku.edu.cn

基金项目: 国家重点研发计划(批准号: 2018YFA0306302)和国家自然科学基金(批准号: 12174011, 11625414)资助的课题.

收稿日期: 2022-07-04

修回日期: 2022-08-05

上网日期: 2022-11-25

刊出日期: 2022-12-05

摘要: 基于超快强激光与物质相互作用的高次谐波产生(high-order harmonic generation, HHG)提供了非微扰区光与物质相互作用的研究平台, 同时也是台式化极紫外光源和阿秒脉冲的主要产生途径. 非微扰区固体HHG涉及超快强场物理、凝聚态物理、材料科学和信息科学等领域的核心内容, 自2011年首次在实验中观察到以来, 迅速成为强场物理和阿秒科学的研究前沿. 本综述从一个实验工作者的角度, 总结了固体HHG的研究进展和重要应用. 首先通过对比高次谐波(high-order harmonic, HH)产率和截止能量对驱动激光参数的依赖关系, 展示固体HHG与气体HHG截然不同的特性. 重点介绍固体HHG调控和应用方面的进展, 包括通过设计靶材结构或者激光光场实现对HH产率、偏振、时空分布等精密调控, 以及固体HH谱学技术在材料结构表征和超快电子动力学研究等领域的应用. 最后对固体HHG的未来发展进行了展望.

关键词:

Generation, manipulation, and application of high-order harmonics in solids

State Key Laboratory for Mesoscopic Physics, School of Physics, Peking University, Beijing 100871, China

Corresponding author: Wu Cheng-Yin, cywu@pku.edu.cn

Fund Project: Project supported by the National Key R&D Program of China (Grant No. 2018YFA0306302) and the National Natural Science Foundation of China (Grant Nos. 12174011, 11625414).

Received Date: 04 July 2022

Accepted Date: 05 August 2022

Available Online: 25 November 2022

Published Online: 05 December 2022

Abstract: The generation of high-order harmonics based on the interaction between ultrafast intense laser and matter provides a platform for studying the light-matter interaction in the non-perturbative region. It is also the main route to generating desktop extreme ultraviolet light source and attosecond pulse. The non-perturbative solid high-order harmonic involves the core content of ultrafast strong field physics, condensed matter physics, materials science, information science and other fields. Since it was first experimentally observed in 2011, it has rapidly become the research frontier of strong field physics and attosecond science. This review summarizes the research progress and important applications of solid high-order harmonics from the perspective of an experimentalist. Firstly, distinct characteristics are shown for solid high-order harmonic by comparing the dependence of harmonic yield and cut-off energy on driving laser parameters with gas high-order harmonic. Then, the progress of manipulation and application are highlighted for solid high-order harmonic, including the precise control of harmonic yield, polarization, space-time distribution through the design of target structure or laser field, as well as the application of solid high-order harmonic spectroscopy in the fields of material structure characterization and ultrafast electron dynamics. Finally, the future is prospected for the study of solid high-order harmonics.

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5. 展　望

自2011年ZnO非微扰HHG报道以来, 固体HHG迅速成为强场物理和阿秒科学的研究前沿. 得益于固体材料的高原子密度, 固体HHG作为一种高效光学频率上转换过程, 产生宽谱超快光源. 固体HH光谱范围覆盖了太赫兹到极紫外波段, 尤其对宽带隙介质(如MgO和石英晶体), 在10—20 eV范围内可以形成较宽的极紫外平台区, 为基于固体HHG的阿秒脉冲产生提供了可能. 且固体HH光源具有多自由度控制的优势, 在实现紧凑化和模块化的同时, 也为多功能定制波长可调谐光源提供了便利. 应当指出的是, 受到固体材料相对低的损伤阈值的限制, 基于固体HHG来制备更高光子能量和更强单脉冲能量的紧凑光源仍面临挑战. 为了克服材料损伤的不利影响, 大带隙材料和超短脉冲等能极大提高材料损伤阈值. 此外, 微纳结构、超表面和掺杂等技术的应用也有望在材料损伤阈值之下增强HHG产率、扩展其光谱覆盖范围. 同时也为固体HHG控制提供了自由度, 使得利用表面修饰和能带工程等技术实现对HH特定波段选择、特殊空间分布设计(如聚焦和散焦)、特定椭偏率和角动量获取等成为可能, 为推进HH光源片上集成提供技术支撑.

此外, 作为一种灵敏的光谱学手段, HH光谱将为材料物性表征和信息科学提供新的手段与平台. HH光谱在表征材料能带、贝利曲率、价电子结构和超快相变等领域的更大潜力等待研究者们进一步发掘. 同时, 与HH偏振和时域特性为自由度的信息科学将蓬勃发展, 并有望超越偏振和时域的二进制, 为多自由度可编程器件提供可能.

最后, 应当强调, 固体HHG研究远没有完备, 诸如HHG机制等许多开放性问题需要实验和理论工作进一步探索. 目前, 固体HHG理论研究主要基于单电子近似含时薛定谔方程、半导体布洛赫方程与含时密度泛函理论. 单电子近似含时薛定谔方程采用静止离子实的周期性势场描述相互作用, 而半导体布洛赫方程采用的能带没有考虑光场作用, 即能带是锁定的, 两者都是处理无相互作用电子波包的绝热演化. 多体相互作用被简单概括进唯象的退相干时间中, 多体作用对固体HHG的影响细节并不清晰. 更准确地描述固体HHG需要考虑电子的多体相互作用和固体HHG过程中的非绝热效应. 受限于计算资源, 对固体HHG进行从头算的量子处理尚无法普及和推广, 发展简明有效的包含多体相互作用的理论描述图像对推动固体HHG更深入理解至关重要.

国内固体HHG研究虽然起步较国外晚, 但是发展非常迅速, 近几年取得了一批优秀成果^{[17,22,29,30,35,49,76,85-106]}. 目前这些成果主要还是集中在理论模拟, 实验方面正迎头赶上^{[17,22,49,85,86]}. 由于固体HHG涉及多学科交叉, 精确的信息提取依赖于准确的理论模拟, 希望国内实验和理论研究者紧密合作, 通过精确的实验测量, 结合高精度的理论计算, 在固体HHG物理和应用方面做出更大贡献.

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