72 results
Search Results
Now showing 1 - 10 of 72
- ItemFew-cycle laser driven reaction nanoscopy on aerosolized silica nanoparticles([London] : Nature Publishing Group UK, 2019) Rupp, Philipp; Burger, Christian; Kling, Nora G; Kübel, Matthias; Mitra, Sambit; Rosenberger, Philipp; Weatherby, Thomas; Saito, Nariyuki; Itatani, Jiro; Alnaser, Ali S.; Raschke, Markus B.; Rühl, Eckart; Schlander, Annika; Gallei, Markus; Seiffert, Lennart; Fennel, Thomas; Bergues, Boris; Kling, Matthias F.Nanoparticles offer unique properties as photocatalysts with large surface areas. Under irradiation with light, the associated near-fields can induce, enhance, and control molecular adsorbate reactions on the nanoscale. So far, however, there is no simple method available to spatially resolve the near-field induced reaction yield on the surface of nanoparticles. Here we close this gap by introducing reaction nanoscopy based on three-dimensional momentum-resolved photoionization. The technique is demonstrated for the spatially selective proton generation in few-cycle laser-induced dissociative ionization of ethanol and water on SiO2 nanoparticles, resolving a pronounced variation across the particle surface. The results are modeled and reproduced qualitatively by electrostatic and quasi-classical mean-field Mie Monte-Carlo (M3C) calculations. Reaction nanoscopy is suited for a wide range of isolated nanosystems and can provide spatially resolved ultrafast reaction dynamics on nanoparticles, clusters, and droplets.
- ItemRaman gas self-organizing into deep nano-trap lattice([London] : Nature Publishing Group UK, 2016) Alharbi, M.; Husakou, A.; Chafer, M.; Debord, B.; Gérôme, F.; Benabid, F.Trapping or cooling molecules has rallied a long-standing effort for its impact in exploring new frontiers in physics and in finding new phase of matter for quantum technologies. Here we demonstrate a system for light-trapping molecules and stimulated Raman scattering based on optically self-nanostructured molecular hydrogen in hollow-core photonic crystal fibre. A lattice is formed by a periodic and ultra-deep potential caused by a spatially modulated Raman saturation, where Raman-active molecules are strongly localized in a one-dimensional array of nanometre-wide sections. Only these trapped molecules participate in stimulated Raman scattering, generating high-power forward and backward Stokes continuous-wave laser radiation in the Lamb-Dicke regime with sub-Doppler emission spectrum. The spectrum exhibits a central line with a sub-recoil linewidth as low as ∼14 kHz, more than five orders of magnitude narrower than conventional-Raman pressure-broadened linewidth, and sidebands comprising Mollow triplet, motional sidebands and four-wave mixing.
- ItemStable coherent mode-locking based on π pulse formation in single-section lasers([London] : Macmillan Publishers Limited, part of Springer Nature, 2021) Arkhipov, Rostislav; Pakhomov, Anton; Arkhipov, Mikhail; Babushkin, Ihar; Rosanov, NikolayHere we consider coherent mode-locking (CML) regimes in single-section cavity lasers, taking place for pulse durations less than atomic population and phase relaxation times, which arise due to coherent Rabi oscillations of the atomic inversion. Typically, CML is introduced for lasers with two sections, the gain and absorber ones. Here we show that, for certain combination of the cavity length and relaxation parameters, a very stable CML in a laser, containing only gain section, may arise. The mode-locking is unconditionally self-starting and appears due to balance of intra-pulse de-excitation and slow interpulse-scale pump-induced relaxation processes. We also discuss the scaling of the system to shorter pulse durations, showing a possibility of mode-locking for few-cycle pulses.
- ItemIn situ single-shot diffractive fluence mapping for X-ray free-electron laser pulses([London] : Nature Publishing Group UK, 2018) Schneider, Michael; Günther, Christian M.; Pfau, Bastian; Capotondi, Flavio; Manfredda, Michele; Zangrando, Marco; Mahne, Nicola; Raimondi, Lorenzo; Pedersoli, Emanuele; Naumenko, Denys; Eisebitt, StefanFree-electron lasers (FELs) in the extreme ultraviolet (XUV) and X-ray regime opened up the possibility for experiments at high power densities, in particular allowing for fluence-dependent absorption and scattering experiments to reveal non-linear light-matter interactions at ever shorter wavelengths. Findings of such non-linear effects are met with tremendous interest, but prove difficult to understand and model due to the inherent shot-to-shot fluctuations in photon intensity and the often structured, non-Gaussian spatial intensity profile of a focused FEL beam. Presently, the focused beam is characterized and optimized separately from the actual experiment. Here, we present the simultaneous measurement of XUV diffraction signals from solid samples in tandem with the corresponding single-shot spatial fluence distribution on the actual sample. Our in situ characterization scheme enables direct monitoring of the sample illumination, providing a basis to optimize and quantitatively understand FEL experiments.
- ItemMolecular movie of ultrafast coherent rotational dynamics of OCS([London] : Nature Publishing Group UK, 2019) Karamatskos, Evangelos T.; Raabe, Sebastian; Mullins, Terry; Trabattoni, Andrea; Stammer, Philipp; Goldsztejn, Gildas; Johansen, Rasmus R.; Długołecki, Karol; Stapelfeldt, Henrik; Vrakking, Marc J. J.; Trippel, Sebastian; Rouzée, Arnaud; Küpper, JochenRecording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. Here we present the direct experimental recording of very-high-resolution and -fidelity molecular movies over more than one-and-a-half periods of the laser-induced rotational dynamics of carbonylsulfide (OCS) molecules. Utilising the combination of single quantum-state selection and an optimised two-pulse sequence to create a tailored rotational wavepacket, an unprecedented degree of field-free alignment, 〈cos2θ2D〉 = 0.96 (〈cos2θ〉 = 0.94) is achieved, exceeding the theoretical limit for single-pulse alignment. The very rich experimentally observed quantum dynamics is fully recovered by the angular probability distribution obtained from solutions of the time-dependent Schrödinger equation with parameters refined against the experiment. The populations and phases of rotational states in the retrieved time-dependent three-dimensional wavepacket rationalises the observed very high degree of alignment.
- 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.
- ItemStrong-field ionization of clusters using two-cycle pulses at 1.8 μm([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Schütte, Bernd; Ye, Peng; Patchkovskii, Serguei; Austin, Dane R.; Brahms, Christian; Strüber, Christian; Witting, Tobias; Ivanov, Misha Yu; Tisch, John W. G.; Marangos, Jon P.The interaction of intense laser pulses with nanoscale particles leads to the production of high-energy electrons, ions, neutral atoms, neutrons and photons. Up to now, investigations have focused on near-infrared to X-ray laser pulses consisting of many optical cycles. Here we study strong-field ionization of rare-gas clusters (103 to 105 atoms) using two-cycle 1.8 μm laser pulses to access a new interaction regime in the limit where the electron dynamics are dominated by the laser field and the cluster atoms do not have time to move significantly. The emission of fast electrons with kinetic energies exceeding 3 keV is observed using laser pulses with a wavelength of 1.8 μm and an intensity of 1 × 1015 W/cm2, whereas only electrons below 500 eV are observed at 800 nm using a similar intensity and pulse duration. Fast electrons are preferentially emitted along the laser polarization direction, showing that they are driven out from the cluster by the laser field. In addition to direct electron emission, an electron rescattering plateau is observed. Scaling to even longer wavelengths is expected to result in a highly directional current of energetic electrons on a few-femtosecond timescale.
- ItemCationic double K-hole pre-edge states of CS2 and SF6(London : Nature Publishing Group, 2017) Feifel, R.; Eland, J.H.D.; Carniato, S.; Selles, P.; Püttner, R.; Koulentianos, D.; Marchenko, T.; Journel, L.; Guillemin, R.; Goldsztejn, G.; Travnikova, O.; Ismail, I.; Miranda, B. Cunha de; Lago, A.F.; Céolin, D.; Lablanquie, P.; Penent, F.; Piancastelli, M.N.; Simon, M.Recent advances in X-ray instrumentation have made it possible to measure the spectra of an essentially unexplored class of electronic states associated with double inner-shell vacancies. Using the technique of single electron spectroscopy, spectra of states in CS2 and SF6 with a double hole in the K-shell and one electron exited to a normally unoccupied orbital have been obtained. The spectra are interpreted with the aid of a high-level theoretical model giving excellent agreement with the experiment. The results shed new light on the important distinction between direct and conjugate shake-up in a molecular context. In particular, systematic similarities and differences between pre-edge states near single core holes investigated in X-ray absorption spectra and the corresponding states near double core holes studied here are brought out.
- ItemTheoretical analysis of hard x-ray generation by nonperturbative interaction of ultrashort light pulses with a metal(Melville, NY : AIP Publishing LLC, 2015) Weisshaupt, Jannick; Juvé, Vincent; Holtz, Marcel; Woerner, Michael; Elsaesser, ThomasThe interaction of intense femtosecond pulses with metals allows for generating ultrashort hard x-rays. In contrast to plasma theories, tunneling from the target into vacuum is introduced as electron generation step, followed by vacuum acceleration in the laser field and re-entrance into the target to generate characteristic x-rays and Bremsstrahlung. For negligible space charge in vacuum, the Kα flux is proportional to the incident intensity and the wavelength squared, suggesting a strong enhancement of the x-ray flux by mid-infrared driving pulses. This prediction is in quantitative agreement with experiments on femtosecond Cu Kα generation.
- ItemProbing multiphoton light-induced molecular potentials([London] : Nature Publishing Group UK, 2020) Kübel, M.; Spanner, M.; Dube, Z.; Naumov, A.Yu.; Chelkowski, S.; Bandrauk, A.D.; Vrakking, M.J.J.; Corkum, P.B.; Villeneuve, D.M.; Staudte, A.The strong coupling between intense laser fields and valence electrons in molecules causes distortions of the potential energy hypersurfaces which determine the motion of the nuclei and influence possible reaction pathways. The coupling strength varies with the angle between the light electric field and valence orbital, and thereby adds another dimension to the effective molecular potential energy surface, leading to the emergence of light-induced conical intersections. Here, we demonstrate that multiphoton couplings can give rise to complex light-induced potential energy surfaces that govern molecular behavior. In the laser-induced dissociation of H2+, the simplest of molecules, we measure a strongly modulated angular distribution of protons which has escaped prior observation. Using two-color Floquet theory, we show that the modulations result from ultrafast dynamics on light-induced molecular potentials. These potentials are shaped by the amplitude, duration and phase of the dressing fields, allowing for manipulating the dissociation dynamics of small molecules.