Divergence and efficiency optimization in polarization-controlled two-color high-harmonic generation

Abbing, Sylvianne D.C. Roscam; Campi, Filippo; Zeltsi, Alexandra; Smorenburg, P.W.; Kraus, Peter M.

doi:10.1038/s41598-021-03657-2

Cited by 14 publications

(9 citation statements)

References 52 publications

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“…Briefly, higher harmonics of an 800 nm pump laser running at 2 kHz are generated in a finite gas cell with argon (22–42 eV) or with neon (42–70 eV). By combining the 800 nm source with the frequency doubled 400 nm output, odd and even harmonics are produced in the case of high-harmonic generation from argon, to increase the spectral coverage. , The spectra of the irradiance at the sample in the two energy ranges are shown in Figure S1 (Supporting Information).…”

Section: Methodsmentioning

confidence: 99%

XUV Absorption Spectroscopy and Photoconversion of a Tin-Oxo Cage Photoresist

Sadegh,

Evrard,

Kraus

et al. 2024

J. Phys. Chem. C

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Extreme ultraviolet lithography has recently been introduced in high-volume production of integrated circuits for manufacturing the smallest features in high-end computer chips. Hybrid organic/inorganic materials are considered as the next generation of photoresists for this technology, but detailed knowledge about the response of such materials to the ionizing radiation used (13.5 nm, 92 eV) is still scarce. In the present work, we use broadband high-harmonic radiation in the energy range 22−70 eV for absorption spectroscopy and photobleaching (that is, the decrease of absorbance) of thin films of an n-butyltin oxocage, a representative of the class of metal-based EUV photoresist. The shape of the absorption spectrum in the range 22−92 eV matches well with the spectrum predicted using tabulated atomic cross sections. The photobleaching results are consistent with loss of the butyl side groups due to the breaking of Sn−C bonds following photoionization. Bleaching is strongest in the low-energy range (<40 eV), where the absorption is largely due to the carbon atoms in the organic groups. At higher energies (42−70 eV), absorption is dominated by the tin atoms, and since these remain in the film after photoconversion, the absorption change in this region is smaller. It is estimated that after prolonged irradiation (up to ∼3 J cm −2 in the range 22−40 eV) about 70% of the hydrocarbon groups are removed from the film. The rate of bleaching is high at the beginning of exposure, but it rapidly decreases with increasing conversion. We rationalize this using density functional theory calculations: the first Sn−C bonds are efficiently cleaved (quantum yield Φ ≈ 0.9), because the highest occupied molecular orbitals (HOMOs) (from which an electron is removed after photoionization) are located on Sn−C sigma bonds. In the photoproducts, the HOMO is localized on tin atoms that have lost their hydrocarbon group (formally reduced to the Sn(II) oxidation state), and holes formed on those tin atoms lead to less efficient cleavage reactions. Our results reveal the primary reaction steps following excitation with ionizing radiation of tin-oxo cages. Our methodology represents a systematic approach of studying and quantitatively assessing the performance of new photoresists and as such enables the development of future EUV photoresists.

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Section: Methodsmentioning

confidence: 99%

XUV Absorption Spectroscopy and Photoconversion of a Tin-Oxo Cage Photoresist

Sadegh,

Evrard,

Kraus

et al. 2024

J. Phys. Chem. C

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“…This generates broadband XUV radiation through the high-order harmonic generation (HHG) process. 23 − 26 A representative spectrum generated at peak intensities of ∼1.5 × 10 14 W/cm 2 is shown in Figure 1 A. The XUV radiation is refocused with a toroidal mirror onto the sample mounted on a sample stage.…”

Section: Methodsmentioning

confidence: 99%

“…Briefly, 1.1 mJ is split from the output of a 2 kHz titanium:sapphire (Ti:Sa) laser (Solstice ACE, Spectra Physics, 800 nm, 35 fs, 7 W) and focused into a noble gas target in vacuum. This generates broadband XUV radiation through the high-order harmonic generation (HHG) process. − A representative spectrum generated at peak intensities of ∼1.5 × 10 14 W/cm 2 is shown in Figure A. The XUV radiation is refocused with a toroidal mirror onto the sample mounted on a sample stage.…”

Section: Methodsmentioning

confidence: 99%

Extreme-Ultraviolet Excited Scintillation of Methylammonium Lead Bromide Perovskites

et al. 2022

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Inorganic–Organic lead halide materials have been recognized as potential high-energy X-ray detectors because of their high quantum efficiencies and radiation hardness. Surprisingly little is known about whether the same is true for extreme-ultraviolet (XUV) radiation, despite applications in nuclear fusion research and astrophysics. We used a table-top high-harmonic generation setup in the XUV range between 20 and 45 eV to photoexcite methylammonium lead bromide (MAPbBr 3 ) and measure its scintillation properties. The strong absorbance combined with multiple carriers being excited per photon yield a very high carrier density at the surface, triggering photobleaching reactions that rapidly reduce the emission intensity. Concurrent to and in spite of this photobleaching, a recovery of the emission intensity as a function of dose was observed. X-ray photoelectron spectroscopy and X-ray diffraction measurements of XUV-exposed and unexposed areas show that this recovery is caused by XUV-induced oxidation of MAPbBr 3 , which removes trap states that normally quench emission, thus counteracting the rapid photobleaching caused by the extremely high carrier densities. Furthermore, it was found that preoxidizing the sample with ozone was able to prolong and improve this intensity recovery, highlighting the impact of surface passivation on the scintillation properties of perovskite materials in the XUV range.

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“…On the experimental side, many studies have investigated HHG driven by two‐ and multi‐color fields with parallel [ 6,20,23,77,160,162,168–180 ] or perpendicular [ 181–186 ] polarizations. In particular, experiments with parallel‐polarized fields revealed HHG yield enhancement, energy cutoff extension, attosecond coherent control, and direct IAP generation.…”

Section: Applications Of Waveform Synthesismentioning

confidence: 99%

“…In the opposite scenario, where the strong, fundamental field was fixed at 0.8 µm and a longer-wavelength, weaker field served as the assisting field; HHG enhancements were found only a few times lower than the original 𝜔-3𝜔 optimization. [167] Experimental Works: On the experimental side, many studies have investigated HHG driven by two-and multi-color fields with parallel [6,20,23,77,160,162,[168][169][170][171][172][173][174][175][176][177][178][179][180] or perpendicular [181][182][183][184][185][186] polarizations. In particular, experiments with parallel-polarized fields revealed HHG yield enhancement, energy cutoff extension, attosecond coherent control, and direct IAP generation.…”

Section: Attosecond Pulse Generation Driven By Multi-color and Synthe...mentioning

confidence: 99%

Optical Waveform Synthesis and Its Applications

Cirmi

Mainz

Silva‐Toledo

et al. 2023

Laser & Photonics Reviews

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The quest for ever‐shorter optical pulses has been ongoing for over half a century. Although few‐cycle pulses have been generated for nearly 40 years, pulse lengths below the single‐cycle limit have remained an elusive goal for a long time. For this purpose, optical waveform synthesizers, generating high‐energy, high‐average‐power pulses via coherent combination of multiple pulses covering different spectral regions, have been recently developed. They allow unprecedented control over the generated optical waveforms, spanning an extremely broad spectral range from ultraviolet to infrared. Such control allows for steering strong‐field interactions with increased degrees of freedom. When driving high‐harmonic generation, tailored waveforms can produce bright attosecond pulse trains and even isolated attosecond pulses with tunable spectra up to the soft X‐ray range. In this paper recent progress on parametric and hollow‐core fiber waveform synthesizers is discussed. Newly developed seeding schemes; absolute, relative, and spectral phase measurement; and control techniques suitable for synthesizers are described. The progress on serial and parallel waveform synthesis based on Ti:sapphire and Ytterbium laser systems and their latest applications in high‐harmonic generation in gaseous and solid media, attosecond science, and laser wakefield acceleration is discussed.

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Divergence and efficiency optimization in polarization-controlled two-color high-harmonic generation

Cited by 14 publications

References 52 publications

XUV Absorption Spectroscopy and Photoconversion of a Tin-Oxo Cage Photoresist

XUV Absorption Spectroscopy and Photoconversion of a Tin-Oxo Cage Photoresist

Extreme-Ultraviolet Excited Scintillation of Methylammonium Lead Bromide Perovskites

Optical Waveform Synthesis and Its Applications

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