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Scientific Reports volume 14, Article number: 24457 (2024 ) Cite this article cr39 lens material
We demonstrated an inline synthesizer for generating ultrashort pulses in the ultraviolet (UV) range. The inline UV pulse synthesizer comprised three nonlinear crystals located in the propagation path of the fundamental driving laser pulse. Second-harmonic signals with central wavelengths of 420, 375, and 345 nm were generated in turn in the three BBO crystals, resulting in a synthesized UV pulse subsequent to the final nonlinear crystal. Its temporal amplitude and phase could be manipulated easily by changing the relative positions of the crystals, allowing for flexibility of the waveform. The minimum pulse duration of the synthesized UV pulse was 4.7 fs, which was close to the Fourier-transform-limited pulse duration. This ultrashort UV pulse with 19 \(\upmu\) J energy can be utilized in various applications such as high harmonic generation and frustrated tunneling ionization.
Ultrashort-pulse lasers have been developed to investigate several light-matter interactions in real time with high temporal resolution1,2,3,4. In fact, they have been used to capture moments of material changes, such as above-threshold ionization and high-harmonic generation (HHG), where the atomic state is changed within a half-cycle pulse5,6,7,8,9,10. In particular, ultrashort laser pulses in the ultraviolet (UV) region facilitate the study of phonon vibrational modes that require high photon energies. As a useful tool for nonlinear time-resolved spectroscopy in the UV region, they have been utilized to investigate ultrafast electronics and vibrational dynamics in molecules and graphene with high bandgaps11,12,13 and to observe fast charge-carrier dynamics in semiconductors on a femtosecond time scale. Furthermore, an ultrashort UV pulse enables high-yield HHG signal generation and frustrated tunneling ionization, which is useful for studying the atomic dynamics of the Rydberg state near the ionization energy of a material14,15,16,17.
One of the most common methods for generating ultrashort UV pulses is spectral broadening through propagation in a gas-filled hollow-core fiber18,19,20,21. Nibbering et al. obtained a 20 fs, 20 \(\upmu\) J UV pulse by first generating a 50 fs, 400 nm UV pulse with 100 \(\upmu\) J energy through frequency doubling of a 32 fs, 800 nm pulse, and then extending its spectral width to 70 nm with an argon-filled hollow-core fiber22. However, the UV pulse duration was limited to 20 fs owing to uncompensated higher-order dispersions. Later, Liu et al. generated a sub 10 fs, 400 nm UV pulse by compensating for higher-order dispersions using chirped mirrors. But the final pulse energy was as low as 4 \(\upmu\) J due to significant energy loss caused by the chirped mirrors with limited spectral bandwidths and several aluminum-coated mirrors23. Recently, Travers et al. generated ultrashort UV pulses with high energy of 16 \(\upmu\) J through a soliton self-compression using resonant dispersive-wave emission in a gas-filled hollow-core fiber stage without chirped mirrors24. The soliton self-compression fiber stage requires a long space due to a long hollow-core fiber as well as elaborate handling of a beam pointing and a gas pressure for its stable operation. Thus, an efficient method for generating a high-energy ultrashort UV pulse needs to be implemented handily on a small scale for facilitating expansion of its application scope.
A synthesis method was used to generate an ultrashort laser pulse25. Krauss et al. obtained a 4.3 fs infrared (IR) pulse by synthesizing two longer IR pulses with different central wavelengths. Here a 7.8 fs IR pulse with a spectral range from 900 to 1400 nm and a 31 fs IR pulse with a spectral range from 1600 to 2000 nm were generated using highly nonlinear fibers, and they were temporally synthesized using a variable delay line. This synthesis method can be applied for the generation of ultrashort UV pulses. First, longer UV pulses can be generated through frequency doubling of an IR pulse in inline multiple nonlinear crystals with different phase-matching conditions, and an ultrashort UV pulse can be obtained by synthesizing longer UV pulses through their temporal matching. In this inline configuration, there is no instability induced by temporal jitters among longer UV pulses during their synthesis. Furthermore, chirped mirrors for dispersion control are not required; thus, the energy loss induced by them can be avoided. But, there will be a limit to energy scalability due to the limit of the size of the nonlinear crystal because the crystal must grow in size to prevent its optical damage as the seed IR pulse energy increases. Consequently, this inline synthesis method is efficient for obtaining high-energy ultrashort pulses in the UV region, and can be implemented with a compact setup composed of multiple nonlinear crystals.
In this letter, we present an inline synthesizer for generating high-energy sub-5 fs pulses in the UV region. Three nonlinear crystals were serially placed in the propagation path of a broadband IR laser pulse to generate UV pulses with different central wavelengths through second-harmonic (SH) generation. A 4.7 fs UV pulse was obtained by synthesizing three SH signals through the time delay adjustment of each SH signal. Time-delay adjustments were enabled by controlling the relative positions of the nonlinear crystals. Here the temporal waveform of the synthesized UV pulse could be manipulated easily just through the time delay adjustment. This synthesis of SH signals obviates the need for several chirped mirrors for dispersion compensation, resulting in a low energy loss. The waveform of the synthesized UV pulse was measured and its characteristics were investigated by conducting an HHG experiment.
An ultrashort UV pulse can be obtained by generating SH pulses with UV central wavelengths and then synthesizing them in the time domain. SH pulses with different central wavelengths were obtained by adjusting the phase-matching bandwidth of each nonlinear crystal. Temporal coincidence of SH pulses can be achieved by precisely controlling their temporal delays. To achieve efficient temporal coincidence, a close quantitative analysis of the time lags among them should be prioritized.
The time delays of the SH signals from the nonlinear crystals were calculated analytically. Beta-barium borate (BBO) crystals were used as nonlinear crystals to generate SH signals. Three BBO crystals with thicknesses of \(L_1\) , \(L_2\) and \(L_3\) were arranged in succession to generate SH signals with central wavelengths of \(\lambda _1\) , \(\lambda _2\) and \(\lambda _3\) , respectively. The phase delay as well as the group delay of each SH signal has a decisive effect on the temporal waveform of the synthesized pulse. Here the phase delay could be adjusted just through fine tuning of the group delay. The group delay of each SH signal immediately after the third crystal can be expressed as
Time delays of spectral components of the fundamental signal and the second-harmonic signals in inline UV pulse synthesizer.
Here \(\tau _{2 \lambda _{n}}\) is the time delay of the fundamental partial pulse with a central wavelength of \(2 \lambda _n\) before the nth BBO crystal. \(\tau _{2\lambda _1}\) was set to be zero because the origin of the time-frame was the position of the fundamental partial pulse with a central wavelength of 2\(\lambda _1\) before the first BBO crystal. \(v_{BBO_m}(\lambda _n)\) is the group velocity of the SH signal with a central wavelength of \(\lambda _n\) during passage through the \(\it \hbox {m}\) th BBO crystal along the extraordinary axis. \(v_{air}(\lambda _n)\) is the group velocity of the SH signal with a central wavelength of \(\lambda _n\) in air. \(L_{1,2}(L_{2,3})\) is the separation between the first (second) and second (third) BBO crystal in air. The time delays of the SH signals after the third BBO crystal were predicted using analytical calculations, as shown in Fig. 1. When the fundamental chirp-free pulse passes through the first BBO crystal, an SH signal with a central wavelength of \(\lambda _1 (\hbox {UV}_1\,\, \hbox {signal})\) is generated. An SH signal with a central wavelength of \(\lambda _2 (\hbox {UV}_2\,\, \hbox {signal})\) is generated after the second BBO crystal and it will precede or lag behind the \(\hbox {UV}_1\) signal immediately after the second BBO crystal according to the air separation distance of \(L_{1,2}\) . Similarly, an SH signal with a central wavelength of \(\lambda _3 (\hbox {UV}_3\,\, \hbox {signal})\) precedes or lags behind the \(\hbox {UV}_1\) signal and the \(\hbox {UV}_2\) signal immediately after the third BBO crystal. As a result, the temporal delays of the three UV signals vary according to the air lengths \(L_{1,2}\) and \(L_{2,3}\) , and the temporal profile of a synthesized UV pulse depends on the air lengths.
Experimental setup for synthesized UV pulse generation. SM silver mirror, MCM multiple chirped mirror, CM chirped mirror, DM dichroic mirror, FM focus mirror, AM aluminum mirror, AFM aluminum focus mirror.
A few-cycle IR pulse with a central wavelength of 730 nm was generated using a gas-filled hollow-core fiber. A 25 fs, 1.2 mJ laser pulse from a 1 kHz Ti:sapphire laser was focused at the entrance of the hollow-core fiber with an inner diameter of 500 \(\upmu\) m and a length of 2 m, as shown in Fig. 2. Its spectral width was broadened through a self-phase modulation effect in the pressure-gradient neon-filled hollow-core fiber, as shown in Fig. 3a. The broadband laser pulse was collimated after a spherical mirror, and its second-order dispersion was compensated using an array of chirp mirrors and one pair of fused silica wedges26. Finally, the compressed laser pulse with a 320 \(\upmu\) J energy and a 5 fs duration was used as a broadband seed pulse of an inline UV pulse synthesizer.
The UV pulse synthesizer consists of a single iris, three BBO crystals, a thin wedge pair, a dichroic mirror, and two UV chirp mirrors, as shown in Fig. 2. The iris was used to reduce the beam diameter from 15 mm to 8 mm, considering the 10 mm diameter BBO crystals. After the iris, the laser pulse with 120 \(\upmu\) J energy was made incident to three BBO crystals. The first, second, and third BBO crystals had thicknesses of 100, 100, and 200 \(\upmu m\) , respectively. Here the third BBO crystal was thicker than other crystals to increase the conversion efficiency of the \(\hbox {UV}_3\) signal for a low intensity of the fundamental partial pulse with a central wavelength of 2\(\lambda _3\) . UV pulses with central wavelengths of 420, 375, and 345 nm were produced by the SH generation in the first, second, and third BBO crystals, respectively, as shown in Fig. 3b. A thin-wedge pair was used to control the dispersion of the synthesized UV pulse minutely. The synthesized UV pulse, which was separated from the fundamental IR pulse using a dichroic mirror, was introduced into the target chamber for the HHG experiment or into a temporal characterization device. Two UV chirp mirrors were installed after the dichroic mirror to compensate for the total group delay dispersion originating from the materials, including the thin wedge, window of the target chamber, and air after the third BBO crystal.
Measured spectra of (a) fundamental input signal and (b) second harmonic signal.
The waveform of the synthesized UV pulse immediately after the third BBO crystal is theoretically calculated to estimate the temporal profile. The optical waveform can be described as follows:
where \(t_1(t_2)\) represents the time delay of the \(\hbox {UV}_2\) signal (\(\hbox {UV}_3\) signal) with respect to the \(\hbox {UV}_1\) signal. \(\tau _1, \tau _2\) and \(\tau _3\) represent the temporal durations of \(\hbox {UV}_1\) signal, \(\hbox {UV}_2\) signal and \(\hbox {UV}_3\) signal, respectively. To prioritize the temporal coincidence between the \(\hbox {UV}_1\) signal and \(\hbox {UV}_3\) signal, the separation distance between the first and third BBO crystals was calculated to be approximately 210 mm. Under the condition of temporal coincidence between the \(\hbox {UV}_1\) signal and \(\hbox {UV}_3\) signal, the temporal profile of the synthesized pulse was sensitive to the relative position of the second BBO crystal, which determined the temporal lag between the \(\hbox {UV}_1\) signal and \(\hbox {UV}_2\) signal, as shown in Fig. 4. Consequently, the separation distance between the three BBO crystals had a decisive effect on the temporal profile of the synthesized pulse.
The temporal profile of the synthesized UV pulse was measured using tunneling ionization with perturbation for the time-domain observation of an electric field (TIPTOE) device27. First, the temporal durations of \(\hbox {UV}_1\) signal, \(\hbox {UV}_2\) , and \(\hbox {UV}_3\) signals were 12, 20, and 30 fs, respectively. Figure 4 shows the temporal profiles measured according to the time delay between the \(\hbox {UV}_1\) signal and \(\hbox {UV}_2\) signal when the \(\hbox {UV}_1\) signal and \(\hbox {UV}_3\) signal were synthesized. When the time delay between the \(\hbox {UV}_1\) signal and the \(\hbox {UV}_2\) signal was set to zero and the separation distance between the first and second BBO crystals was approximately 100 mm, the temporal profile of the synthesized UV pulse was optimized, as shown in Fig. 4a. Here the pulse duration was measured to be 4.7 fs (FWHM). At a small time delay (0.65 fs corresponding to a separation distance of 124 mm), the temporal profile deviated significantly from the optimized one, resulting in double peaks, as shown in Fig. 4b. At a time delay of 1.3 fs corresponding to a separation distance of 148 mm, the temporal profile approached the optimized profile, as shown in Fig. 4c. The adjustment range of the time delay between the \(\hbox {UV}_1\) signal and the \(\hbox {UV}_2\) signal for temporal optimization of the synthesized UV pulse was of the order of an optical cycle at the central wavelength of the fundamental IR pulse. These measured profiles, which agree well with the calculated profiles, show that the temporal profile of the synthesized UV pulse can be controlled by adjusting the relative positions of the BBO crystals.
Measured temporal intensity profiles (solid blue line) and calculated profiles (dotted red line) of the synthesized pulse when time delays between the first and second UV pulse were (a) zero, (b) 0.65 fs and (c) 1.3 fs under temporal coincidence between the first and the third UV pulse.
The rate of air ionization induced by the synthesized UV pulses was measured using a TIPTOE device with no perturbation signal channel27. The synthesized UV pulse was focused on the air gap between the copper plates of the TIPTOE device and the air ionization rate was measured. The air ionization rate, which is proportional to the integral value of the 8th power of the incident optical waveform, can be calculated by using the Equation (2)28. Figure 5 shows the air ionization rate as a function of the position of the second BBO crystal relative to that of the first BBO crystal under temporal coincidence between the \(\hbox {UV}_1\) signal and \(\hbox {UV}_3\) signal. The measured air ionization rate agreed well with the calculated rate. Consequently, inline UV pulse synthesis is demonstrated to be a reliable method for generating ultrashort UV pulses.
Air ionization rate depending on time delay between the first UV signal and the second UV signal under temporal coincidence between the first and the third UV pulse.
An HHG experiment was conducted to prove the utility of the synthesized sub-5 fs UV pulses. At first, the synthesized UV pulse with a 19 \(\upmu\) J energy was directed at a vacuum chamber for the HHG experiment. The temporal profile was controlled by varying the insertion length of the glass wedge. Figure 6a shows the spectra of the HHG signals measured as a function of the insertion length of the glass wedge when the synthesized UV pulses were focused onto a krypton gas target in the vacuum chamber. When the insertion length was 0.4 mm, the temporal profile of the synthesized UV pulse was optimized and its HHG signal was observed up to 23 eV, as shown by the green line of Fig. 6b. In contrast, when the insertion length was approximately 0 mm, the synthesized UV pulse with a negative chirp had few peaks, and its HHG signal was observed up to 17 eV owing to its lower peak intensity, as shown by the red line in Fig. 6b. This experimental result shows that the synthesized UV pulse can be efficiently utilized to generate HHG signals, the characteristics of which depend on the temporal profile of the synthesized UV pulse.
Measured spectra of high harmonic signals as a function of insertion length of glass wedge when synthesized UV pulses were focused into a krypton gas target.
In conclusion, we demonstrated the inline synthesis of three UV pulses with central wavelengths of 420, 375, and 345 nm to generate a high-energy sub-5 fs UV pulse. The synthesized UV pulse was generated through three BBO crystals with different phase-matching conditions, and the waveform was controlled by adjusting the relative positions of the three crystals. The temporal waveform of the synthesized UV pulse was measured using a TIPTOE device, with a minimum duration of 4.7 fs. This 4.7 fs UV pulse with a 19 \(\upmu\) J energy was efficiently utilized in the HHG experiment. To the best of our knowledge, this inline UV pulse synthesis is the first synthesis technique applied to the UV region. We anticipate that this inline synthesis method will be highly effective for generating high-energy ultrashort UV pulses and useful for studying atomic dynamics in the UV region.
All data generated or analyzed during this study are included in this published article.
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This work was supported by the Institute for Basic Science (IBS-R012-D1) and the Ultrashort Quantum Beam Facility operation program (No. 140011) through Advanced Photonics Research Institute, Gwangju Institute of Science and Technology.
Center for Relativistic Laser Science, Institute for Basic Science, Gwangju, 61005, Korea
Sung In Hwang, Wosik Cho, Kyung Taec Kim, Jin Woo Yun, Seong Ku Lee & Jae Hee Sung
Advanced Photonics Research Institute, Gwangju Institute of Science and Technology, Gwangju, 61005, Korea
Sung In Hwang, Hyeok Yun, Jin Woo Yun, Seong Ku Lee & Jae Hee Sung
Department of Physics and Photon Science, Gwangju Institute of Science and Technology, Gwangju, 61005, Korea
Wosik Cho & Kyung Taec Kim
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Wosik Cho provided assistance of optical waveform measurement based on the TIPTOE , while Hyeok Yun provided helps for the high harmonic generation experiements. Kyung Taec Kim, Jin Woo Yun and Seong Ku Lee gave valuable advice for the manuscript. Sung In Hwang and Jae Hee Sung performed data analysis and wrote the manuscript.
Correspondence to Jae Hee Sung.
The authors declare no competing interests.
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Hwang, S.I., Cho, W., Yun, H. et al. Inline UV pulse synthesizer. Sci Rep 14, 24457 (2024). https://doi.org/10.1038/s41598-024-75415-z
DOI: https://doi.org/10.1038/s41598-024-75415-z
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