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Register a new userPhotoelectron holographic interferometry to probe the longitudinal momentum offset at the tunnel exit
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Laser-induced electron tunneling underlies numerous emerging spectroscopic techniques to probe attosecond electron dynamics in atoms and molecules. The improvement of those techniques requires an accurate knowledge of the exit momentum for the tunneling wave packet. Here we demonstrate a photoelectron interferometric scheme to probe the electron momentum longitudinal to the tunnel direction at the tunnel exit by measuring the photoelectron holographic pattern in an orthogonally polarized two-color laser pulse. In this scheme, we use a perturbative 400-nm laser field to modulate the photoelectron holographic fringes generated by a strong 800-nm pulse. The fringe shift offers a direct experimental access to the intermediate canonical momentum of the rescattering electron, allowing us to reconstruct the momentum offset at the tunnel exit with high accuracy. Our result unambiguously proves the existence of nonzero initial longitudinal momentum at the tunnel exit and provides fundamental insights into the non-quasi-static nature of the strong-field tunneling.
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We report on the non-adiabatic offset of the initial electron momentum distribution in the plane of polarization upon single ionization of argon by strong field tunneling and show how to experimentally control the degree of non-adiabaticity. Two-color counter- and co-rotating fields (390 and 780 nm) are compared to show that the non-adiabatic offset strongly depends on the temporal evolution of the laser electric field. We introduce a simple method for the direct access to the non-adiabatic offset using two-color counter- and co-rotating fields. Further, for a single-color circularly polarized field at 780 nm we show that the radius of the experimentally observed donut-like distribution increases for increasing momentum in the light propagation direction. Our observed initial momentum offsets are well reproduced by the strong-field approximation (SFA). A mechanistic picture is introduced that links the measured non-adiabatic offset to the magnetic quantum number of virtually populated intermediate states.
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Ultrafast dynamical processes in photoexcited molecules can be observed with pump-probe measurements, in which information about the dynamics is obtained from the transient signal associated with the excited state. Background signals provoked by pump and/or probe pulses alone often obscure these excited state signals. Simple subtraction of pump-only and/or probe-only measurements from the pump-probe measurement, as commonly applied, results in a degradation of the signal-to-noise ratio and, in the case of coincidence detection, the danger of overrated background subtraction. Coincidence measurements additionally suffer from false coincidences. Here we present a probabilistic approach based on Bayesian probability theory that overcomes these problems. For a pump-probe experiment with photoelectron-photoion coincidence detection we reconstruct the interesting excited-state spectrum from pump-probe and pump-only measurements. This approach allows to treat background and false coincidences consistently and on the same footing. We demonstrate that the Bayesian formalism has the following advantages over simple signal subtraction: (i) the signal-to-noise ratio is significantly increased, (ii) the pump-only contribution is not overestimated, (iii) false coincidences are excluded, (iv) prior knowledge, such as positivity, is consistently incorporated, (v) confidence intervals are provided for the reconstructed spectrum, and (vi) it is applicable to any experimental situation and noise statistics. Most importantly, by accounting for false coincidences, the Bayesian approach allows to run experiments at higher ionization rates, resulting in a significant reduction of data acquisition times. The application to pump-probe coincidence measurements on acetone molecules enables novel quantitative interpretations about the molecular decay dynamics and fragmentation behavior.
Based on the strong-field approximation, we obtain analytical expressions for the initial momentum at the tunnel exit and instantaneous ionization rate of tunneling ionization in elliptically polarized laser fields with arbitrary ellipticity. The tunneling electron reveals a nonzero offset of the initial momentum at the tunnel exit in the elliptically polarized laser field. We find that the transverse and longitudinal components of this momentum offset with respect to the instantaneous field direction are directly related to the time derivatives of the instantaneous laser electric field along the angular and radial directions, respectively. We further show that the nonzero initial momentum at the tunnel exit has a significant influence on the laser phase dependence of the instantaneous ionization rate in the nonadiabatic tunneling regime.
This paper employs Bayesian probability theory for analyzing data generated in femtosecond pump-probe photoelectron-photoion coincidence (PEPICO) experiments. These experiments allow investigating ultrafast dynamical processes in photoexcited molecules. Bayesian probability theory is consistently applied to data analysis problems occurring in these types of experiments such as background subtraction and false coincidences. We previously demonstrated that the Bayesian formalism has many advantages, amongst which are compensation of false coincidences, no overestimation of pump-only contributions, significantly increased signal-to-noise ratio, and applicability to any experimental situation and noise statistics. Most importantly, by accounting for false coincidences, our approach allows running experiments at higher ionization rates, resulting in an appreciable reduction of data acquisition times. In addition to our previous paper, we include fluctuating laser intensities, of which the straightforward implementation highlights yet another advantage of the Bayesian formalism. Our method is thoroughly scrutinized by challenging mock data, where we find a minor impact of laser fluctuations on false coincidences, yet a noteworthy influence on background subtraction. We apply our algorithm to data obtained in experiments and discuss the impact of laser fluctuations on the data analysis.
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