arXiv subjects

Andrius Baltuška

Publications and source records attributed to Andrius Baltuška.

27 records · Page 2Linked to original sources

arXiv2017

Localizing High-Lying Rydberg Wave Packets with Two-Color Laser Fields

We demonstrate control over the localization of high-lying Rydberg wave packets in argon atoms with phase-locked orthogonally polarized two-color (OTC) laser fields. With a reaction microscope, we measured ionization signals of high-lying Rydberg states induced by a weak dc field and black-body radiation as a function of the relative phase between the two-color fields. We find that the dc-field ionization yields of high-lying Rydberg argon atoms oscillate with the relative two-color phase with a period of $2π$ while the photoionization signal by black-body radiation shows a period of $π$. These observations are a clear signature of the asymmetric localization of electrons recaptured into high-lying Rydberg states after conclusion of the laser pulse and are supported by a semiclassical simulation of argon-OTC laser interaction. Our findings thus open an effective pathway to control the localization of high-lying Rydberg wave packets.

physics.atom-ph↗

arXiv2016

Sub 100-fs, 5.2-$μ$m ZGP Parametric Amplifier Driven by a ps Ho:YAG Chirped Pulse Amplifier and its application to high harmonic generation

We report a 1 kHz repetition-rate mid-IR (MIR) optical parametric amplifier (OPA) system operating at a central wavelength of 5.2 $μ$m with the tail-to-tail spectrum extending over 1.5 $μ$m and delivering 40 $μ$J pulses that are compressed to 99 fs (5.6 optical cycles). Also we develop a novel pulse compression scheme for further pulse compression and wavelength tunability. As the first application of this laser system, we generated high harmonics in bulk ZnSe above the bandgap, dense exciton generation after 10-photon absorption, high order sum- and difference-frequency generation, ultrafast transition in the conduction band, which reflects the structure of conduction bands.

physics.optics↗

arXiv2016

Channel-resolved subcycle interferences of electron wave packets emitted from H$_2$ in two-color laser fields

We report on the observation of subcycle interferences of electron wave packets released during the strong field ionization of H$_2$ with cycle-shaped two-color laser fields. With a reaction microscope, channel-resolved photoelectron momentum distribution are obtained for different final products originating from single ionization of H$_2$. Our results show that the subcycle interference structures of electron wave packet are very sensitive to the cycle-shape of the two-color laser field. The reason is that the ionization time within an optical cycle is determined by the cycle-shape of the laser field. The subcycle interference structures can be further used to get the subcycle dynamics of molecules during strong field interaction.

physics.chem-ph↗

arXiv2016

Direct Observation of Molecular Oxygen Production from Carbon Dioxide

Oxygen ($O_2$) is one of the most important elements required to sustain life. The concentration of $O_2$ on Earth has been accumulated over millions of years and has a direct connection with that of $CO_2$. Further, $CO_2$ plays an important role in many other planetary atmospheres. Therefore, molecular reactions involving $CO_2$ are critical for studying the atmospheres of such planets. Existing studies on the dissociation of $CO_2$ are exclusively focused on the C--O bond breakage. Here we report first experiments on the direct observation of molecular Oxygen formation from $CO_2$ in strong laser fields with a reaction microscope. Our accompanying simulations suggest that $CO_2$ molecules may undergo bending motion during and after strong-field ionization which supports the molecular Oxygen formation process. The observation of the molecular Oxygen formation from $CO_2$ may trigger further experimental and theoretical studies on such processes with laser pulses, and provide hints in studies of the $O_2$ and $CO_2^+$ abundance in $CO_2$-dominated planetary atmospheres.

physics.chem-ph↗

arXiv2016

Coincidence spectroscopy of high-lying Rydberg states produced in strong laser fields

We report on the measurement of electron emission after the interaction of strong laser pulses with atoms and molecules. These electrons originate from high-lying Rydberg states with quantum numbers up to $n \lesssim 120$ formed by frustrated field ionization. Simulations show that both tunneling ionization by a weak dc field and photoionization by the black-body radiation contribute to delayed electron emission on the nano- to microsecond scale. We measured ionization rates from these Rydberg states by coincidence spectroscopy. Further, the dependence of the Rydberg-state production on the ellipticity of the driving laser field proves that such high-lying Rydberg states are populated through electron recapture. The present experiment provides detailed quantitative information on Rydberg production by frustrated field ionization.

physics.atom-ph↗

arXiv2016

Fragmentation of long-lived hydrocarbons after strong field ionization

We experimentally and theoretically investigated the deprotonation process on nanosecond to microsecond timescale in ethylene and acetylene molecules, following their double ionization by a strong femtosecond laser field. In our experiments we utilized coincidence detection with the reaction microscope technique, and found that both the lifetime of the long-lived ethylene dication leading to the delayed deprotonation and the relative channel strength of the delayed deprotonation compared to the prompt one have no evident dependence on the laser pulse duration and the laser peak intensity. Quantum chemical simulations suggest that such delayed fragmentation originates from the tunneling of near-dissociation-threshold vibrational states through a dissociation barrier on a dication electronic state along C--H stretching. Such vibrational states can be populated through strong field double ionization induced vibrational excitation on an electronically excited state in the case of ethylene, and through intersystem crossing from electronically excited states to the electronic ground state in the case of acetylene.

physics.chem-ph↗

arXiv2014

Laser-sub-cycle two-dimensional electron momentum mapping using orthogonal two-color fields

The two-dimensional sub-cycle-time to electron momentum mapping provided by orthogonal two-color laser fields is applied to photoelectron spectroscopy. Using neon as the example we gain experimental access to the dynamics of emitted electron wave packets in electron momenta spectra measured by coincidence momentum imaging. We demonstrate the opportunities provided by this time-to-momentum mapping by investigating the influence of the parent ion on the emitted electrons on laser-sub-cycle times. It is found that depending on their sub-cycle birth time the trajectories of photoelectrons are affected differently by the ion's Coulomb field.

physics.atom-ph↗

arXiv2014

Enhanced multi-colour gating for the generation of high-power isolated attosecond pulses

Isolated attosecond pulses (IAP) generated by high-order harmonic generation are valuable tools that enable dynamics to be studied on the attosecond time scale. The applicability of these IAP would be widened drastically by increasing their energy. Here we analyze the potential of using multi-colour driving pulses for temporally gating the attosecond pulse generation process. We devise how this approach can enable the generation of IAP with the available high-energy kHz-repetition-rate Ytterbium-based laser amplifiers (delivering 180-fs, 1030-nm pulses). We show theoretically that this requires a three-colour field composed of the fundamental and its second harmonic as well as a lower-frequency auxiliary component. We present pulse characterization measurements of such auxiliary pulses generated directly by white-light seeded OPA with the required significantly shorter pulse duration than the that of the fundamental. This, combined with our recent experimental results on three-colour waveform synthesis [Phys. Rev. X 4, 021028 (2014)], proves that the theoretically considered multi-colour drivers for IAP generation can be realized with existing high-power laser technology. The high-energy driver pulses, combined with the strongly enhanced single-atom-level conversion efficiency we observe in our calculations, thus make multi-colour drivers prime candidates for the development of unprecedented high-energy IAP sources in the near future.

physics.atom-ph↗

arXiv2012

Attosecond-recollision-controlled selective fragmentation of polyatomic molecules

Control over various fragmentation reactions of a series of polyatomic molecules (acetylene, ethylene, 1,3-butadiene) by the optical waveform of intense few-cycle laser pulses is demonstrated experimentally. We show both experimentally and theoretically that the responsible mechanism is inelastic ionization from inner-valence molecular orbitals by recolliding electron wavepackets, whose recollision energy in few-cycle ionizing laser pulses strongly depends on the optical waveform. Our work demonstrates an efficient and selective way of pre-determining fragmentation and isomerization reactions in polyatomic molecules on sub-femtosecond time-scales.

physics.chem-ph↗