15 results
Search Results
Now showing 1 - 10 of 15
- ItemMultidimensional high harmonic spectroscopy of polyatomic molecules: detecting sub-cycle laser-driven hole dynamics upon ionization in strong mid-IR laser fields(Cambridge [u.a.] : Soc., 2016) Bruner, Barry D.; Mašín, Zdeněk; Negro, Matteo; Morales, Felipe; Brambila, Danilo; Devetta, Michele; Faccialà, Davide; Harvey, Alex G.; Ivanov, Misha; Mairesse, Yann; Patchkovskii, Serguei; Serbinenko, Valeria; Soifer, Hadas; Stagira, Salvatore; Vozzi, Caterina; Dudovich, Nirit; Smirnova, OlgaHigh harmonic generation (HHG) spectroscopy has opened up a new frontier in ultrafast science, where electronic dynamics can be measured on an attosecond time scale. The strong laser field that triggers the high harmonic response also opens multiple quantum pathways for multielectron dynamics in molecules, resulting in a complex process of multielectron rearrangement during ionization. Using combined experimental and theoretical approaches, we show how multi-dimensional HHG spectroscopy can be used to detect and follow electronic dynamics of core rearrangement on sub-laser cycle time scales. We detect the signatures of laser-driven hole dynamics upon ionization and reconstruct the relative phases and amplitudes for relevant ionization channels in a CO2 molecule on a sub-cycle time scale. Reconstruction of channel-resolved complex ionization amplitudes on attosecond time scales has been a long-standing goal of high harmonic spectroscopy. Our study brings us one step closer to fulfilling this initial promise and developing robust schemes for sub-femtosecond imaging of multielectron rearrangement in complex molecular systems.
- ItemAll-optical Stückelberg spectroscopy of strongly driven Rydberg states(College Park, MD : APS, 2022) Bengs, Ulrich; Patchkovskii, Serguei; Ivanov, Misha; Zhavoronkov, NickolaiThe AC Stark shift of electronic levels is ubiquitous in the interaction of intense light fields with atoms and molecules. As the light intensity changes on the rising and falling edges of a femtosecond laser pulse, it shifts the Rydberg states in and out of multiphoton resonances with the ground state. The two resonant pathways for transient excitation arising at the leading and the trailing edges of the pulse generate Young's type interference, generally referred to as the Stückelberg oscillations. Here we report the observation of the Stückelberg oscillations in the intensity of the coherent free-induction decay following resonant multiphoton excitation. Moreover, combining the experimental results with accurate numerical simulations and a simple model, we use the Stückelberg oscillations to recover the population dynamics of strongly driven Rydberg states inside the laser pulse by all-optical measurements after the end of the pulse. We demonstrate the potential of this spectroscopy to characterize lifetimes of Rydberg states dressed by laser fields with strengths far exceeding the Coulomb field between the Rydberg electron and the core.
- ItemPopulation transfer to high angular momentum states in infrared-assisted XUV photoionization of helium(Bristol : IOP Publ., 2020) Mayer, Nicola; Peng, Peng; Villeneuve, David M.; Patchkovskii, Serguei; Ivanov, Misha; Kornilov, Oleg; Vrakking, Marc J.J.; Niikura, HiromichiAn extreme-ultraviolet (XUV) laser pulse consisting of harmonics of a fundamental near-infrared (NIR) laser frequency is combined with the NIR pulse to systematically study two-color photoionization of helium atoms. A time-resolved photoelectron spectroscopy experiment is carried out where energy- A nd angle-resolved photoelectron distributions are obtained as a function of the NIR intensity and wavelength. Time-dependent Schrödinger equation calculations are performed for the conditions corresponding to the experiment and used to extract residual populations of Rydberg states resulting from excitation by the XUV + NIR pulse pair. The residual populations are studied as a function of the NIR intensity (3.5 × 1010-8 × 1012 W cm-2) and wavelength (760-820 nm). The evolution of the photoelectron distribution and the residual populations are interpreted using an effective restricted basis model, which includes the minimum set of states relevant to the features observed in the experiments. As a result, a comprehensive and intuitive picture of the laser-induced dynamics in helium atoms exposed to a two-color XUV-NIR light field is obtained. © 2020 The Author(s). Published by IOP Publishing Ltd.
- ItemEnantio-sensitive unidirectional light bending([London] : Nature Publishing Group UK, 2021) Ayuso, David; Ordonez, Andres F.; Decleva, Piero; Ivanov, Misha; Smirnova, OlgaStructured light, which exhibits nontrivial intensity, phase, and polarization patterns in space, has key applications ranging from imaging and 3D micromanipulation to classical and quantum communication. However, to date, its application to molecular chirality has been limited by the weakness of magnetic interactions. Here we structure light’s local handedness in space to introduce and realize an enantio-sensitive interferometer for efficient chiral recognition without magnetic interactions, which can be seen as an enantio-sensitive version of Young’s double slit experiment. Upon interaction with isotropic chiral media, such chirality-structured light effectively creates chiral emitters of opposite handedness, located at different positions in space. We show that if the distribution of light’s handedness breaks left-right symmetry, the interference of these chiral emitters leads to unidirectional bending of the emitted light, in opposite directions in media of opposite handedness, even if the number of the left-handed and right-handed emitters excited in the medium is exactly the same. Our work introduces the concepts of polarization of chirality and chirality-polarized light, exposes the immense potential of sculpting light’s local chirality, and offers novel opportunities for efficient chiral discrimination, enantio-sensitive optical molecular fingerprinting and imaging on ultrafast time scales.
- ItemTopological protection versus degree of entanglement of two-photon light in photonic topological insulators([London] : Nature Publishing Group UK, 2021) Tschernig, Konrad; Jimenez-Galán, Álvaro; Christodoulides, Demetrios N.; Ivanov, Misha; Busch, Kurt; Bandres, Miguel A.; Perez-Leija, ArmandoTopological insulators combine insulating properties in the bulk with scattering-free transport along edges, supporting dissipationless unidirectional energy and information flow even in the presence of defects and disorder. The feasibility of engineering quantum Hamiltonians with photonic tools, combined with the availability of entangled photons, raises the intriguing possibility of employing topologically protected entangled states in optical quantum computing and information processing. However, while two-photon states built as a product of two topologically protected single-photon states inherit full protection from their single-photon “parents”, a high degree of non-separability may lead to rapid deterioration of the two-photon states after propagation through disorder. In this work, we identify physical mechanisms which contribute to the vulnerability of entangled states in topological photonic lattices. Further, we show that in order to maximize entanglement without sacrificing topological protection, the joint spectral correlation map of two-photon states must fit inside a well-defined topological window of protection.
- ItemFemtosecond Field‐Driven On‐Chip Unidirectional Electronic Currents in Nonadiabatic Tunneling Regime(Weinheim : Wiley VCH, 2021) Shi, Liping; Babushkin, Ihar; Husakou, Anton; Melchert, Oliver; Frank, Bettina; Yi, Juemin; Wetzel, Gustav; Demircan, Ayhan; Lienau, Christoph; Giessen, Harald; Ivanov, Misha; Morgner, Uwe; Kovacev, MilutinRecently, asymmetric plasmonic nanojunctions have shown promise as on-chip electronic devices to convert femtosecond optical pulses to current bursts, with a bandwidth of multi-terahertz scale, although yet at low temperatures and pressures. Such nanoscale devices are of great interest for novel ultrafast electronics and opto-electronic applications. Here, the device is operated in air and at room temperature, revealing the mechanisms of photoemission from plasmonic nanojunctions, and the fundamental limitations on the speed of optical-to-electronic conversion. Inter-cycle interference of coherent electronic wavepackets results in a complex energy electron distribution and birth of multiphoton effects. This energy structure, as well as reshaping of the wavepackets during their propagation from one tip to the other, determine the ultrafast dynamics of the current. It is shown that, up to some level of approximation, the electron flight time is well-determined by the mean ponderomotive velocity in the driving field.
- ItemKinematic origin for near-zero energy structures in mid-IR strong field ionization(Bristol : IOP Publ., 2016) Pisanty, Emilio; Ivanov, MishaWe propose and discuss a kinematic mechanism underlying the recently discovered 'near-zero energy structure' in the photoionization of atoms in strong mid-infrared laser fields, based on trajectories which revisit the ion at low velocities exactly analogous to the series responsible for low-energy structures. The different scaling of the new series, as $E\sim {I}_{p}^{2}/{U}_{p}$, suggests that the near-zero energy structure can be lifted to higher energies, where it can be better resolved and studied, using harder targets with higher ionization potential.
- ItemAttosecond recorder of the polarization state of light([London] : Nature Publishing Group UK, 2018) Jiménez-Galán, Álvaro; Dixit, Gopal; Patchkovskii, Serguei; Smirnova, Olga; Morales, Felipe; Ivanov, MishaHigh harmonic generation in multi-color laser fields opens the opportunity of generating isolated attosecond pulses with high ellipticity. Such pulses hold the potential for time-resolving chiral electronic, magnetization, and spin dynamics at their natural timescale. However, this potential cannot be realized without characterizing the exact polarization state of light on the attosecond timescale. Here we propose and numerically demonstrate a complete solution of this problem. Our solution exploits the extrinsic two-dimensional chirality induced in an atom interacting with the chiral attosecond pulse and a linearly polarized infrared probe. The resulting asymmetry in the photoelectron spectra allows to reconstruct the complete polarization state of the attosecond pulse, including its possible time dependence. The challenging problem of distinguishing circularly polarized, partially polarized, or unpolarized pulses in the extreme ultraviolet range is also resolved. We expect this approach to become the core ingredient for attosecond measurements of chiral-sensitive processes in gas and condensed phase.
- ItemSub-cycle valleytronics: control of valley polarization using few-cycle linearly polarized pulses(Washington, DC : OSA, 2021) Jiménez-Galán, Álvaro; Silva, Rui E. F.; Smirnova, Olga; Ivanov, MishaSo far, it has been assumed that selective excitation of a desired valley in the Brillouin zone of a hexagonal two-dimensional material has to rely on using circularly polarized fields. We theoretically demonstrate a way to control the valley excitation in hexagonal 2D materials on a few-femtosecond timescale using a few-cycle, linearly polarized pulse with controlled carrier–envelope phase. The valley polarization is mapped onto the strength of the perpendicular harmonic signal of a weak, linearly polarized pulse, which allows to read this information all-optically without destroying the valley state and without relying on the Berry curvature, making our approach potentially applicable to inversion-symmetric materials. We show applicability of this method to hexagonal boron nitride and MoS2.
- ItemRotational quantum beat lasing without inversion(Washington, DC : OSA, 2020) Richter, Maria; Lytova, Marianna; Morales, Felipe; Haessler, Stefan; Smirnova, Olga; Spanner, Michael; Ivanov, MishaIn standard lasers, light amplification requires population inversion between an upper and a lower state to break the reciprocity between absorption and stimulated emission. However, in a medium prepared in a specific superposition state, quantum interference may fully suppress absorption while leaving stimulated emission intact, opening the possibility of lasing without inversion. Here we show that lasing without inversion arises naturally during propagation of intense femtosecond laser pulses in air. It is triggered by the combination of molecular ionization and molecular alignment, both unavoidable in intense light fields. The effect could enable inversionless amplification of broadband radiation in many molecular gases, opening unusual opportunities for remote sensing. © 2020 Optical Society of America