Yunpei Deng

Generation of carrier-envelope-phase-stable 2-cycle 740-μJ pulses at 2.1-μm carrier wavelength

We produce carrier-envelope-phase-stable 15.7-fs (2-cycle) 740-μJ pulses at the 2.1-μm carrier wavelength, from a three-stage optical parametric chirped-pulse amplifier system, pumped by an optically synchronized 49-ps 11-mJ Nd:YLF laser. A novel seed pulse spectral shaping method is used to ascertain the true amplified seed energy and the parametric superfluorescence levels.

Carrier-envelope-phase-stable, 1.2 mJ, 1.5 cycle laser pulses at 2.1 μm

We produce 1.5 cycle (10.5 fs), 1.2 mJ, 3 kHz carrier-envelope-phase-stable pulses at 2.1 μm carrier wavelength, from a three-stage optical parametric chirped-pulse amplifier system, pumped by an optically synchronized 1.6 ps Yb:YAG thin disk laser. A chirped periodically poled lithium niobate crystal is used to generate the ultrabroad spectrum needed for a 1.5 cycle pulse through difference frequency mixing of spectrally broadened pulse from a Ti:sapphire amplifier. It will be an ideal tool for producing isolated attosecond pulses with high photon energies.

Subfemtosecond steering of hydrocarbon deprotonation through superposition of vibrational modes

Subfemtosecond control of the breaking and making of chemical bonds in polyatomic molecules is poised to open new pathways for the laser-driven synthesis of chemical products. The break-up of the C-H bond in hydrocarbons is an ubiquitous process during laser-induced dissociation. While the yield of the deprotonation of hydrocarbons has been successfully manipulated in recent studies, full control of the reaction would also require a directional control (that is, which C-H bond is broken). Here, we demonstrate steering of deprotonation from symmetric acetylene molecules on subfemtosecond timescales before the break-up of the molecular dication. On the basis of quantum mechanical calculations, the experimental results are interpreted in terms of a novel subfemtosecond control mechanism involving non-resonant excitation and superposition of vibrational degrees of freedom. This mechanism permits control over the directionality of chemical reactions via vibrational excitation on timescales defined by the subcycle evolution of the laser waveform.

Active stabilization for optically synchronized optical parametric chirped pulse amplification

The development of new high power laser sources tends toward optical parametric chirped pulse amplification (OPCPA) in recent years. One of the difficulties in OPCPA is the the temporal overlap between pump and seed pulses. In this work we characterize our timing jitter on a single-shot basis using spectrally resolved cross-correlation in combination with a position sensitive detector. A commercial beam stabilization is adapted to actively enhance temporal overlap. This delay-stabilizer reduces the RMS jitter from σ = 127 fs down to σ = 24 fs. The enhanced temporal overlap is demonstrated in our frontend and we propose the scheme to be applicable in many optically synchronized high-repetition-rate OPCPA systems.

Strong-field control of the dissociative ionization of N2O with near-single-cycle pulses

The dissociative ionization of N2O by near-single-cycle laser pulses is studied using phase-tagged ion–ion coincidence momentum imaging. Carrier–envelope phase (CEP) dependences are observed in the absolute ion yields and the emission direction of nearly all ionization and dissociation pathways of the triatomic molecule. We find that laser-field-driven electron recollision has a significant impact on the dissociative ionization dynamics and results in pronounced CEP modulations in the dication yields, which are observed in the product ion yields after dissociation. The results indicate that the directional emission of coincident + N and + NO ions in the denitrogenation of the dication can be explained by selective ionization of oriented molecules. The deoxygenation of the dication with the formation of coincident + N 2 + + O ions exhibits an additional shift in its CEP dependence, suggesting that this channel is further influenced by laser interaction with the dissociating dication. The experimental

Coherent control of D2/H2 dissociative ionization by a mid-infrared two-color laser field

Steering the electrons during an ultrafast photo-induced process in a molecule influences the chemical behavior of the system, opening the door to the control of photochemical reactions and photobiological processes. Electrons can be efficiently localized using a strong laser field with a well-designed temporal shape of the electric component. Consequently, many experiments have been performed with laser sources in the near-infrared region (800 nm) in the interest of studying and enhancing the electron localization. However, due to its limited accessibility, the mid-infrared (MIR) range has barely been investigated, although it allows to efficiently control small molecules and even more complex systems. To push further the manipulation of basic chemical mechanisms, we used a MIR two-color (1800 and 900 nm) laser field to ionize H2 and D2 molecules and to steer the remaining electron during the photo-induced dissociation. The study of this prototype reaction led to the simultaneous control of four fragmentation channels. The results are well reproduced by a theoretical model solving the time-dependent Schrodinger equation for the molecular ion, identifying the involved dissociation mechanisms. By varying the relative phase between the two colors, asymmetries (i.e., electron localization selectivity) of up to 65% were obtained, corresponding to enhanced or equivalent levels of control compared to previous experiments. Experimentally easier to implement, the use of a two-color laser field leads to a better electron localization than carrier-envelope phase stabilized pulses and applying the technique in the MIR range reveals more dissociation channels than at 800 nm.

Sub-cycle electron control in the photoionization of xenon using a few-cycle laser pulse in the mid-infrared

Using few-cycle laser pulses generated by optical parametric chirped pulse amplification, sub-cycle light-wave control of electrons was achieved at a carrier wavelength of 2.1 μm. We demonstrate the sub-cycle light-wave control in the case of strong field ionization of xenon atoms. Angle-resolved spectra of electrons emitted in the photoionization process were recorded as a function of the carrier-envelope phase (CEP) using an electron imaging technique. We observed a clear CEP-dependent asymmetry in the electron momentum distribution.

Non-sequential double ionization of Ar: from the single-to the many-cycle regime

The transition from the near-single to the multi-cycle regime in non-sequential double ionization of argon is investigated experimentally. Argon atoms are exposed to intense laser pulses with a center wavelength around 790 nm and the momenta of electrons and ions generated in the double ionization process are measured in coincidence using a reaction microscope. The duration of the near transform-limited pulses is varied from 4 to 30 fs. We observe an abrupt collapse of the cross-shaped two-electron momentum distribution [17] in the few-cycle regime. The transition to longer pulses is further accompanied by a strong increase in the fraction of anti-correlated to correlated electrons.

Ultrafast Excitation of an Inner-Shell Electron by Laser-Induced Electron Recollision.

Yunpei Deng, Zhinan Zeng Zhengmao Jia, Pavel Komm, Yinhui Zheng, Xiaochun Ge, Ruxin Li and Gilad Marcus SwissFEL, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland. State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800, China. IFSA Collaborative Innovation Center, Shanghai Jiao Tong University, Shanghai 200240, China. School of Physical Science and Technology, ShanghaiTech University, Shanghai 200031,China. and Department of Applied Physics, The Benin School of Engineering and Computer Science, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.

Inner Shell Excitations through Laser Induced Electron Recollision

Sub-femtosecond excitation of inner-shell electrons is a prerequisite step toward time domain “pump-probe” study of core-hole dynamics. By using a few cycles 1800nm source, we show that the recolliding electron might provide this necessary step.