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

Wang Yang; Liu Yu; Wu Cheng-Yin

doi:10.7498/aps.71.20221319

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.

Keywords:

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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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

Figure 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

Figure 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

Figure 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]

Figure 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]

Figure 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

Figure 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

Figure 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.

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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

Figure 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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