Joint Measurements of Terahertz Wave Generation and High-Harmonic Generation from Aligned Nitrogen Molecules Reveal Angle-Resolved Molecular Structures

Huang, Yindong; Meng, Chao; Wang, Xiaowei; Lü, Zhihui; Zhang, Dongwen; Chen, Wenbo; Zhao, Jianlin; Yuan, Jianmin; Zhao, Zengxiu

doi:10.1103/physrevlett.115.123002

Cited by 38 publications

(24 citation statements)

References 48 publications

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“…Alignment dependent THz yield of molecules is proportional to the square of angular ionization probabilities [81]. Thus, by carrying out the joint detection of HATS from aligned molecules and using the alignment dependent THz yields, the angular differential PICS could be retrieved [21,82].…”

Section: Thz Reference For Molecular Photoionizationmentioning

confidence: 99%

“…The light path for HATS measurement on molecules is analogous to the one in Figure 2a, with an additional beam for molecular alignment [21]. As shown in Figure 6, normalized modulations of HATS are compared under different alignments.…”

Section: Thz Reference For Molecular Photoionizationmentioning

confidence: 99%

“…Furthermore, the joint measurement in HATS allows the in situ simultaneous manipulations on the two ends of emissions, which could be realized by varying the accumulated phase during the electron propagation (e.g., using dual-color laser fields [17]) or varying the potential curve (e.g., varying the molecular alignment [21]). The first experimental demonstration of HATS from gaseous argon was reported in 2012 [17].…”

Section: Introductionmentioning

confidence: 99%

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High-Harmonic and Terahertz Spectroscopy (HATS): Methods and Applications

et al. 2019

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Electrons driven from atom or molecule by intense dual-color laser fields can coherently radiate high harmonics from extreme ultraviolet to soft X-ray, as well as an intense terahertz (THz) wave from millimeter to sub-millimeter wavelength. The joint measurement of high-harmonic and terahertz spectroscopy (HATS) was established and further developed as a unique tool for monitoring electron dynamics of argon from picoseconds to attoseconds and for studying the molecular structures of nitrogen. More insights on the rescattering process could be gained by correlating the fast and slow electron motions via observing and manipulating the HATS from atoms and molecules. We also propose the potential investigations of HATS of polar molecules, and solid and liquid sources.

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Section: Thz Reference For Molecular Photoionizationmentioning

confidence: 99%

Section: Thz Reference For Molecular Photoionizationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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High-Harmonic and Terahertz Spectroscopy (HATS): Methods and Applications

et al. 2019

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“…Other examples include the minimum in PRCS due to multi-electron effects, which appears in the measured HHG spectrum of Xe [31]. For molecules, similar minimum in the harmonic spectra has been observed in aligned N 2 molecules [32][33][34][35][36] and CO 2 molecules [37][38][39][40], and even for unaligned polyatomic molecules [41]. However, the suppression of high harmonics by solely making use of macroscopic phase-matching conditions has not been systematically explored.…”

Section: Introductionmentioning

confidence: 99%

Control of soft X-ray high harmonic spectrum by using two-color laser pulses

Jin

Lin

2018

Photon. Res.

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We demonstrate the suppression of soft X-ray high harmonics generated by two-color laser pulses interacting with Ne gas in a gas cell. We show that harmonic suppression can occur at the proper combination of the propagation distance and gas pressure. The physical mechanism behind is the phase mismatch between "short"-trajectory harmonics generated at the early and later times through the interplay of geometric phase, dispersion, and plasma effects. In addition, we demonstrate that the position and depth of harmonic suppression can be tuned by increasing the gas pressure. Furthermore, the suppression can be extended to other laser focusing configurations by properly scaling macroscopic parameters. Our investigation reveals a simple and novel experimental scheme purely relying on the phase mismatch for selectively controlling soft X-ray tabletop light sources without adopting the filters for applications.

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“…g state (a hole in the HOMO) in partial PICSs [17] but the other way around in angle resolved HHG [8,15,18]. The A 2 Π u state is 1.3 eV higher in energy than the X 2 Σ + g state.…”

Section: Introductionmentioning

confidence: 99%

Contributions of inner-valence molecular orbitals and multiphoton resonances to high-order-harmonic generation ofN2: A time-dependent density-functional-theory study

Chu

Groenenboom

2016

Phys. Rev. A

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Using a TDDFT method, we calculated the high-harmonic generation (HHG) spectra of N 2 in 800 nm and 1300 nm intense lasers. The calculations reproduce the experimentally observed minimum near 40 eV and the shift of the minimum due to interference of different molecular orbitals. They also support the proposed shape resonance near 30 eV. The TDDFT method allows us to analyze the involvement of different electronic configurations in the HHG process. We identified a significant role of Rydberg states and autoionizing states in enhancing HHG. This finding is consistent with studies of photoelectron spectra in a similar energy range. Moreover, we discover a significant contribution of the 2σ g orbital above 40 eV, demonstrating the complexity of electronic structure information contained in molecular HHG. At high energy not only the HOMO and HOMO-1 are important, as suggested by earlier studies, but the HOMO-3 contributes substantially as well.

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Joint Measurements of Terahertz Wave Generation and High-Harmonic Generation from Aligned Nitrogen Molecules Reveal Angle-Resolved Molecular Structures

Cited by 38 publications

References 48 publications

High-Harmonic and Terahertz Spectroscopy (HATS): Methods and Applications

High-Harmonic and Terahertz Spectroscopy (HATS): Methods and Applications

Control of soft X-ray high harmonic spectrum by using two-color laser pulses

Contributions of inner-valence molecular orbitals and multiphoton resonances to high-order-harmonic generation ofN2: A time-dependent density-functional-theory study

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