Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userImaging ultrafast molecular wavepackets with a single chirped UV pulse
72
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
We show how to emulate a conventional pump-probe scheme using a single frequency-chirped ultrashort UV pulse to obtain a time-resolved image of molecular ultrafast dynamics. The chirp introduces a spectral phase in time that encodes the delay between the pump and the probe frequencies contained in the pulse. By comparing the results of full dimensional ab initio calculations for the H$^+_2$ molecule with those of a simple sequential model, we demonstrate that, by tuning the chirp parameter, two-photon energy-differential ionization probabilities directly map the wave packet dynamics generated in the molecule. As a result, one can also achieve a significant amount of control of the total ionization yields, with a possible enhancement by more than an order of magnitude.
rate research
Read More
Photoionization of molecular species is, essentially, a multi-path interferometer with both experimentally controllable and intrinsic molecular characteristics. In this work, XUV photoionization of impulsively aligned molecular targets ($N_2$) is used to provide a time-domain route to complete photoionization experiments, in which the rotational wavepacket controls the geometric part of the photoionization interferometer. The data obtained is sufficient to determine the magnitudes and phases of the ionization matrix elements for all observed channels, and to reconstruct molecular frame interferograms from lab frame measurements. In principle this methodology provides a time-domain route to complete photoionization experiments, and the molecular frame, which is generally applicable to any molecule (no prerequisites), for all energies and ionization channels.
We demonstrate an ultrafast voltage sampling technique using a stream of electron wavepackets. Electrons are emitted from a single-electron pump and travel through electron waveguides towards a detector potential barrier. Our electrons sample an instantaneous voltage on the gate upon arrival at the detector barrier. Fast sampling is achieved by minimising the duration that the electrons interact with the barrier, which can be made as small as a few picoseconds. The value of the instantaneous voltage can be determined by varying the gate voltage to match the barrier height to the electron energy, which is used as a stable reference. The test waveform can be reconstructed by shifting the electron arrival time against it. We argue that this method has scope to increase the bandwidth of voltage sampling to 100 GHz and beyond.
The recent demonstration of isolated attosecond pulses from an X-ray free-electron laser (XFEL) opens the possibility for probing ultrafast electron dynamics at X-ray wavelengths. An established experimental method for probing ultrafast dynamics is X-ray transient absorption spectroscopy, where the X-ray absorption spectrum is measured by scanning the central photon energy and recording the resultant photoproducts. The spectral bandwidth inherent to attosecond pulses is wide compared to the resonant features typically probed, which generally precludes the application of this technique in the attosecond regime. In this paper we propose and demonstrate a new technique to conduct transient absorption spectroscopy with broad bandwidth attosecond pulses with the aid of ghost imaging, recovering sub-bandwidth resolution in photoproduct-based absorption measurements.
In contrast with imaging using position-resolving cameras, single-pixel imaging uses a bucket detector along with spatially structured illumination for image recovery. This emerging imaging technique is a promising candidate for a broad range of applications due to high signal-to-noise ratio (SNR) and sensitivity, and applicability in a wide range of frequency bands. Here, inspired by single-pixel imaging in the spatial domain, we demonstrate a temporal single-pixel imaging (TSPI) system that covers frequency bands including both terahertz (THz) and near-infrared (NIR) region. By implementing a programmable temporal fan-out (TFO) gate based on a digital micromirror device (DMD), we can deterministically prepare temporally structured pulses with a temporal sampling size down to 16.00$pm$0.01 fs. By inheriting the advantages in detection efficiency and sensitivity from spatial single-pixel imaging, TSPI enables the compressive recovery of a 5 fJ THz pulse and two NIR pulses with over 97$%$ fidelity. We demonstrate that the TSPI is robust against temporal distortions in the probe pulse train as well. As a direct application, we apply TSPI to machine-learning-aided THz spectroscopy and demonstrate a high sample identification accuracy (97.5$%$) even under low SNRs (SNR $sim$ 10).
Tunnel ionization of room-temperature D$_2$ in an ultrashort (12 femtosecond) near infra-red (800 nm) pump laser pulse excites a vibrational wavepacket in the D2+ ions; a rotational wavepacket is also excited in residual D2 molecules. Both wavepacket types are collapsed a variable time later by an ultrashort probe pulse. We isolate the vibrational wavepacket and quantify its evolution dynamics through theoretical comparison. Requirements for quantum computation (initial coherence and quantum state retrieval) are studied using this well-defined (small number of initial states at room temperature, initial wavepacket spatially localized) single-electron molecular prototype by temporally stretching the pump and probe pulses.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
