| 1. |
- Manschwetus, Bastian, et al.
(författare)
-
Self-Probing Spectroscopy of the SF6 Molecule: A Study of the Spectral Amplitude and Phase of the High Harmonic Emission
- 2015
-
Ingår i: The Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory. - : American Chemical Society (ACS). - 1520-5215. ; 119:23, s. 6111-6122
-
Tidskriftsartikel (refereegranskat)abstract
- We present characterizations of the attosecond pulse train produced in the high harmonic generation (HHG) from SF6 molecules irradiated by a strong pulsed laser field at 800 nm. At harmonic order 17, we observe a minimum in the amplitude of the emitted spectrum and a corresponding distortion in the phase. Our experimental results are compared to two models: a multicenter interference model focused on the effect of the structure of the SF6 molecule in HHG and a model focused on the interferences between multiple ionization channels in HHG. We find that the experimental results agree very well with the multiple ionization channels model, illustrating that HHG in molecules can be very complex and that it provides insights of the intramolecular electron dynamics during the interaction process.
|
|
| 2. |
- Allum, Felix, et al.
(författare)
-
Coulomb explosion imaging of CH3I and CH2CII photodissociation dynamics
- 2018
-
Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 149:20
-
Tidskriftsartikel (refereegranskat)abstract
- The photodissociation dynamics of CH3I and CH2CII at 272 nm were investigated by time-resolved Coulomb explosion imaging, with an intense non-resonant 815nmprobe pulse. Fragment ion momenta over a widem/z range were recorded simultaneously by coupling a velocity map imaging spectrometer with a pixel imaging mass spectrometry camera. For both molecules, delay-dependent pump-probe features were assigned to ultraviolet-induced carbon-iodine bond cleavage followed by Coulomb explosion. Multi-mass imaging also allowed the sequential cleavage of both carbon-halogen bonds in CH2ClI to be investigated. Furthermore, delay-dependent relative fragment momenta of a pair of ions were directly determined using recoil-frame covariance analysis. These results are complementary to conventional velocity map imaging experiments and demonstrate the application of time-resolved Coulomb explosion imaging to photoinduced real-time molecular motion.
|
|
| 3. |
- Brasse, Felix, et al.
(författare)
-
Time-resolved inner-shell photoelectron spectroscopy : From a bound molecule to an isolated atom
- 2018
-
Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - 2469-9926 .- 2469-9934. ; 97:4
-
Tidskriftsartikel (refereegranskat)abstract
- Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH3I) is investigated by ionization above the iodine 4d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.
|
|
| 4. |
- Burt, Michael, et al.
(författare)
-
Coulomb-explosion imaging of concurrent CH2BrI photodissociation dynamics
- 2017
-
Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - 2469-9926 .- 2469-9934. ; 96:4
-
Tidskriftsartikel (refereegranskat)abstract
- The dynamics following laser-induced molecular photodissociation of gas-phase CH2BrI at 271.6 nm were investigated by time-resolved Coulomb-explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment momenta reveal that CH2BrI undergoes C-I cleavage, depositing 65.6% of the available energy into internal product states, and that absorption of a second UV photon breaks the C-Br bond of C(H)2Br. Simulations confirm that this mechanism is consistent with previous data recorded at 248 nm, demonstrating the sensitivity of Coulomb-explosion imaging as a real-time probe of chemical dynamics.
|
|
| 5. |
- He, Xinkui, et al.
(författare)
-
Spatial and spectral properties of the high-order harmonic emission in argon for seeding applications
- 2009
-
Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 79:6
-
Tidskriftsartikel (refereegranskat)abstract
- We characterize and control the harmonic emission in the spectral and spatial domains in order to define in which conditions the harmonic radiation can be a high-quality seed for soft x-ray and x-ray free-electron lasers. The length of the gas cell, where harmonics are generated, was optimized and the energy per pulse was determined in absolute value with a calibrated x-ray photodiode. The beam spatial profile was measured and, in some conditions, a very collimated beam with a half-angle divergence below 1 mrad could be obtained. We also show that increasing the intensity of the fundamental laser field leads to a considerable broadening of the bandwidth of the harmonic radiation, allowing us to cover a large spectral range. This effect is due to fundamental reshaping leading to an efficient phase matching of both short- and long-trajectory contributions.
|
|
| 6. |
- Kimel, Alexey, et al.
(författare)
-
The 2022 magneto-optics roadmap
- 2022
-
Ingår i: Journal of Physics D. - : Institute of Physics (IOP). - 0022-3727 .- 1361-6463. ; 55:46
-
Tidskriftsartikel (refereegranskat)abstract
- Magneto-optical (MO) effects, viz. magnetically induced changes in light intensity or polarization upon reflection from or transmission through a magnetic sample, were discovered over a century and a half ago. Initially they played a crucially relevant role in unveiling the fundamentals of electromagnetism and quantum mechanics. A more broad-based relevance and wide-spread use of MO methods, however, remained quite limited until the 1960s due to a lack of suitable, reliable and easy-to-operate light sources. The advent of Laser technology and the availability of other novel light sources led to an enormous expansion of MO measurement techniques and applications that continues to this day (see section 1). The here-assembled roadmap article is intended to provide a meaningful survey over many of the most relevant recent developments, advances, and emerging research directions in a rather condensed form, so that readers can easily access a significant overview about this very dynamic research field. While light source technology and other experimental developments were crucial in the establishment of today's magneto-optics, progress also relies on an ever-increasing theoretical understanding of MO effects from a quantum mechanical perspective (see section 2), as well as using electromagnetic theory and modelling approaches (see section 3) to enable quantitatively reliable predictions for ever more complex materials, metamaterials, and device geometries. The latest advances in established MO methodologies and especially the utilization of the MO Kerr effect (MOKE) are presented in sections 4 (MOKE spectroscopy), 5 (higher order MOKE effects), 6 (MOKE microscopy), 8 (high sensitivity MOKE), 9 (generalized MO ellipsometry), and 20 (Cotton–Mouton effect in two-dimensional materials). In addition, MO effects are now being investigated and utilized in spectral ranges, to which they originally seemed completely foreign, as those of synchrotron radiation x-rays (see section 14 on three-dimensional magnetic characterization and section 16 on light beams carrying orbital angular momentum) and, very recently, the terahertz (THz) regime (see section 18 on THz MOKE and section 19 on THz ellipsometry for electron paramagnetic resonance detection). Magneto-optics also demonstrates its strength in a unique way when combined with femtosecond laser pulses (see section 10 on ultrafast MOKE and section 15 on magneto-optics using x-ray free electron lasers), facilitating the very active field of time-resolved MO spectroscopy that enables investigations of phenomena like spin relaxation of non-equilibrium photoexcited carriers, transient modifications of ferromagnetic order, and photo-induced dynamic phase transitions, to name a few. Recent progress in nanoscience and nanotechnology, which is intimately linked to the achieved impressive ability to reliably fabricate materials and functional structures at the nanoscale, now enables the exploitation of strongly enhanced MO effects induced by light–matter interaction at the nanoscale (see section 12 on magnetoplasmonics and section 13 on MO metasurfaces). MO effects are also at the very heart of powerful magnetic characterization techniques like Brillouin light scattering and time-resolved pump-probe measurements for the study of spin waves (see section 7), their interactions with acoustic waves (see section 11), and ultra-sensitive magnetic field sensing applications based on nitrogen-vacancy centres in diamond (see section 17). Despite our best attempt to represent the field of magneto-optics accurately and do justice to all its novel developments and its diversity, the research area is so extensive and active that there remains great latitude in deciding what to include in an article of this sort, which in turn means that some areas might not be adequately represented here. However, we feel that the 20 sections that form this 2022 magneto-optics roadmap article, each written by experts in the field and addressing a specific subject on only two pages, provide an accurate snapshot of where this research field stands today. Correspondingly, it should act as a valuable reference point and guideline for emerging research directions in modern magneto-optics, as well as illustrate the directions this research field might take in the foreseeable future.
|
|
| 7. |
- Kockert, Hansjochen, et al.
(författare)
-
UV-induced dissociation of CH2BrI probed by intense femtosecond XUV pulses
- 2022
-
Ingår i: JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 55:1
-
Tidskriftsartikel (refereegranskat)abstract
- The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump-XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C-I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.
|
|
| 8. |
- Mansten, Erik, et al.
(författare)
-
Broadband attosecond pulse shaping
- 2007
-
Ingår i: Optics Letters. - 0146-9592. ; 32:11, s. 1353-1355
-
Tidskriftsartikel (refereegranskat)abstract
- We use semiconductor (Si) and metallic (Al, Zr) transmission filters to shape, in amplitude and phase, high-order harmonics generated from the interaction of an intense titanium sapphire laser field with a pulsed neon gas target. Depending on the properties of the filter, the emitted attosecond pulses can be optimized in bandwidth and/or pulse length. We demonstrate the generation of attosecond pulses centered at energies from 50 to 80 eV, with bandwidths as large as 45 eV and with pulse durations compressed to 130 as. (c) 2007 Optical Society of America.
|
|
| 9. |
- Mansten, Erik, et al.
(författare)
-
Spectral signature of short attosecond pulse trains.
- 2009
-
Ingår i: Physical Review Letters. - 1079-7114. ; 102:8
-
Tidskriftsartikel (refereegranskat)abstract
- We report experimental measurements of high-order harmonic spectra generated in Ar using a carrier-envelope-offset (CEO) stabilized 12 fs, 800 nm laser field and a fraction (less than 10%) of its second harmonic. Additional spectral peaks are observed between the harmonic peaks, which are due to interferences between multiple pulses in the train. The position of these peaks varies with the CEO and their number is directly related to the number of pulses in the train. An analytical model, as well as numerical simulations, support our interpretation.
|
|
| 10. |
- Mauritsson, Johan, et al.
(författare)
-
Coherent electron scattering captured by an attosecond quantum stroboscope.
- 2008
-
Ingår i: Physical Review Letters. - 1079-7114. ; 100:7
-
Tidskriftsartikel (refereegranskat)abstract
- We demonstrate a quantum stroboscope based on a sequence of identical attosecond pulses that are used to release electrons into a strong infrared (IR) laser field exactly once per laser cycle. The resulting electron momentum distributions are recorded as a function of time delay between the IR laser and the attosecond pulse train using a velocity map imaging spectrometer. Because our train of attosecond pulses creates a train of identical electron wave packets, a single ionization event can be studied stroboscopically. This technique has enabled us to image the coherent electron scattering that takes place when the IR field is sufficiently strong to reverse the initial direction of the electron motion causing it to rescatter from its parent ion.
|
|
| 11. |
- Ruchon, Thierry, et al.
(författare)
-
Macroscopic effects in attosecond pulse generation
- 2008
-
Ingår i: New Journal of Physics. - : IOP Publishing. - 1367-2630. ; 10
-
Tidskriftsartikel (refereegranskat)abstract
- We examine how the generation and propagation of high-order harmonics in a partly ionized gas medium affect their strength and synchronization. The temporal properties of the resulting attosecond pulses generated in long gas targets can be significantly influenced by macroscopic effects, in particular by the intensity in the medium and the degree of ionization which control the dispersion. Under some conditions, the use of gas targets longer than the absorption length can lead to the generation of compressed attosecond pulses. We show these macroscopic effects experimentally, using a 6 mm-long argon-filled gas cell as the generating medium.
|
|
| 12. |
- Ruchon, Thierry, et al.
(författare)
-
Momentum shearing interferometry of electron waves
- 2007
-
Ingår i: Proceedings of SPIE - The International Society for Optical Engineering. - : SPIE. - 1996-756X .- 0277-786X. ; 6460, s. 4600-4600
-
Konferensbidrag (refereegranskat)abstract
- We analyse recent experiments on momentum shearing interferometry of electron wave packets1,2 by using an optical analogy with shearing interferometry for optical waves. This analogy offers a convenient point of view to discuss the capabilities and difficulties of this technique used to access the phase of electron wave packets.
|
|
| 13. |
- Swoboda, Marko, et al.
(författare)
-
Intensity dependence of laser-assisted attosecond photoionization spectra
- 2009
-
Ingår i: Laser Physics. - 1054-660X. ; 19:8, s. 1591-1599
-
Tidskriftsartikel (refereegranskat)abstract
- We study experimentally the influence of the intensity of the infrared (IR) probe field on attosecond pulse train (APT) phase measurements performed with the RABITT method (Reconstruction of Attosecond Beating by Interference in Two-Photon Transitions). We find that if a strong IR field is applied, the attosecond pulses will appear to have lower-than-actual chirp rates. We also observe the onset of the streaking regime in the breakdown of the weak-field RABITT conditions. We perform a Fourier-analysis of harmonic and sideband continuum states and show that the mutual phase relation of the harmonics can be extracted from higher Fourier components.
|
|
| 14. |
- Varju, Katalin, et al.
(författare)
-
Angularly resolved electron wave packet interferences
- 2006
-
Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 39:18, s. 3983-3991
-
Tidskriftsartikel (refereegranskat)abstract
- We study experimentally the ionization of argon atoms by a train of attosecond pulses in the presence of a strong infrared laser field, using a velocity map imaging technique. The recorded momentum distribution strongly depends on the delay between the attosecond pulses and the laser field. We interpret the interference patterns observed for different delays using numerical and analytical calculations within the strong field approximation.
|
|
