Complete Photoionization Experiments via Ultrafast Coherent Control with Polarization Multiplexing II: Numerics & Analysis Methodologies

The feasibility of complete photoionization experiments, in which the full set of photoionization matrix elements are determined, using multiphoton ionization schemes with polarization-shaped pulses has recently been demonstrated [Hockett et. al., Phys. Rev. Lett. 112, 223001 (2014)]. Here we extend on our previous work to discuss further details of the numerics and analysis methodology utilised, and compare the results directly to new tomographic photoelectron measurements, which provide a more sensitive test of the validity of the results. In so doing we discuss in detail the physics of the photoionziation process, and suggest various avenues and prospects for this coherent multiplexing methodology

Maximum information photoelectron metrology

Photoelectron interferograms, manifested in photoelectron angular distributions (PADs), are a high-information, coherent observable. In order to obtain the maximum information from angle-resolved photoionization experiments it is desirable to record the full, 3D, photoelectron momentum distribution. Here we apply tomographic reconstruction techniques to obtain such 3D distributions from multiphoton ionization of potassium atoms, and fully analyse the energy and angular content of the 3D data. The PADs obtained as a function of energy indicate good agreement with previous 2D data and detailed analysis [Hockett et. al., Phys. Rev. Lett. 112, 223001 (2014)] over the main spectral features, but also indicate unexpected symmetry-breaking in certain regions of momentum space, thus revealing additional continuum interferences which cannot otherwise be observed. These observations reflect the presence of additional ionization pathways and, most generally, illustrate the power of maximum information measurements of this coherent observable

Coherent strong-field control of multiple states by a single chirped femtosecond laser pulse

We present a joint experimental and theoretical study on strong-field photo-ionization of sodium atoms using chirped femtosecond laser pulses. By tuning the chirp parameter, selectivity among the population in the highly excited states 5p, 6p, 7p and 5f, 6f is achieved. Different excitation pathways enabling control are identified by simultaneous ionization and measurement of photoelectron angular distributions employing the velocity map imaging technique. Free electron wave packets at an energy of around 1 eV are observed. These photoelectrons originate from two channels. The predominant 2+1+1 Resonance Enhanced Multi-Photon Ionization (REMPI) proceeds via the strongly driven two-photon transition $4s\leftarrow\leftarrow3s$, and subsequent ionization from the states 5p, 6p and 7p whereas the second pathway involves 3+1 REMPI via the states 5f and 6f. In addition, electron wave packets from two-photon ionization of the non-resonant transiently populated state 3p are observed close to the ionization threshold. A mainly qualitative five-state model for the predominant excitation channel is studied theoretically to provide insights into the physical mechanisms at play. Our analysis shows that by tuning the chirp parameter the dynamics is effectively controlled by dynamic Stark-shifts and level crossings. In particular, we show that under the experimental conditions the passage through an uncommon three-state "bow-tie" level crossing allows the preparation of coherent superposition states

Bichromatic phase-control of interfering Autler-Townes spectra

We propose a new scheme to control the shape of the Autler-Townes (AT) doublet in the photoelectron spectrum from atomic resonance-enhanced multiphoton ionization (REMPI). The scheme is based on the interference of two AT doublets created by ionization of the strongly driven atom from the ground and the resonantly excited state using tailored bichromatic femtosecond (fs) laser pulses. In this scheme, the quantum phase of the photoelectrons is crucial for the manipulation of the AT doublet. The laser polarization state and the relative optical phase between the two colors are used to manipulate the interference pattern. We develop an analytical model to describe the bichromatic REMPI process and provide a physical picture of the control mechanism. To validate the model, the results are compared to an ab initio calculation based on the solution of the 2D time-dependent Schr\"odinger equation for the non-perturbative interaction of an atom with intense polarization-shaped bichromatic fs-laser pulses. Our results indicate that the control mechanism is robust with respect to the laser intensity facilitating its experimental observation.Comment: 13 pages, 5 figure

Interference in the resonance fluorescence of two incoherently coupled transitions

The fluorescence light emitted by a 4-level system in $J=1/2$ to $J=1/2$ configuration driven by a monochromatic laser field and in an external magnetic field is studied. We show that the spectrum of resonance fluorescence emitted on the $\pi$ transitions shows a signature of spontaneously generated interference effects. The degree of interference in the fluorescence spectrum can be controlled by means of the external magnetic field, provided that the Land\'e g-factors of the excited and the ground state doublet are different. For a suitably chosen magnetic field strength, the relative weight of the Rayleigh line can be completely suppressed, even for low intensities of the coherent driving field. The incoherent fluorescence spectrum emitted on the $\pi$ transitions exhibits a very narrow peak whose width and weight depends on the magnetic field strength. We demonstrate that the spectrum of resonance fluorescence emitted on the $\sigma$ transitions show an indirect signature of interference. A measurement of the relative peak heights in the spectrum from the $\sigma$ transitions allows to determine the branching ratio of the spontaneous decay of each excited state into the $\sigma$ channel

Orbital angular momentum superposition states in transmission electron microscopy and bichromatic multiphoton ionization

The coherent control of electron beams and ultrafast electron wave packets dynamics have attracted significant attention in electron microscopy as well as in atomic physics. In order to unify the conceptual pictures developed in both fields, we demonstrate the generation and manipulation of tailored electron orbital angular momentum (OAM) superposition states either by employing customized holographic diffraction masks in a transmission electron microscope or by atomic multiphoton ionization utilizing pulse-shaper generated carrier-envelope phase stable bichromatic ultrashort laser pulses. Both techniques follow similar physical mechanisms based on Fourier synthesis of quantum mechanical superposition states allowing the preparation of a broad set of electron states with uncommon symmetries. We describe both approaches in a unified picture based on an advanced spatial and spectral double slit and point out important analogies. In addition, we analyze the topological charge and discuss the control mechanisms of the free-electron OAM superposition states. Their generation and manipulation by phase tailoring in transmission electron microscopy and atomic multiphoton ionization is illustrated on a 7-fold rotationally symmetric electron density distribution.Comment: K. Eickhoff and C. Rathje contributed equally to this wor

A composite double-/single-stranded RNA-binding region in protein Prp3 supports tri-snRNP stability and splicing

Prp3 is an essential U4/U6 di-snRNP-associated protein whose functions and molecular mechanisms in pre-mRNA splicing are presently poorly understood. We show by structural and biochemical analyses that Prp3 contains a bipartite U4/U6 di-snRNA-binding region comprising an expanded ferredoxin-like fold, which recognizes a 3′-overhang of U6 snRNA, and a preceding peptide, which binds U4/U6 stem II. Phylogenetic analyses revealed that the single-stranded RNA-binding domain is exclusively found in Prp3 orthologs, thus qualifying as a spliceosome-specific RNA interaction module. The composite double-stranded /single-stranded RNA-binding region assembles cooperatively with Snu13 and Prp31 on U4/U6 di-snRNAs and inhibits Brr2-mediated U4/U6 di-snRNA unwinding in vitro. RNP-disrupting mutations in Prp3 lead to U4/U6•U5 tri-snRNP assembly and splicing defects in vivo. Our results reveal how Prp3 acts as an important bridge between U4/U6 and U5 in the tri-snRNP and comparison with a Prp24-U6 snRNA recycling complex suggests how Prp3 may be involved in U4/U6 reassembly after splicing