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Conference on Lasers and Electro-Optics

Time-gated photoionization spectroscopy of cesium Rydberg wave packets

Lambertus D. Noordam, G. M. Lankhuijzen, F. Robicheaux

Published Nov 27, 2002• 0 citations
Publisher

Abstract

Summary form only given.We introduce a new type of spectroscopy that provides the time of electron emission versus wavelength. In the time-gated photoionization spectroscopy (TGS) technique an atomic streak camera is used to measure the electron flux leaving the excited atoms.
DOI
10.1109/iqec.1998.680293

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An atomic streak camera has been constructed that operates from the near to the far infrared. The photocathode used in conventional streak cameras for the conversion of photons to electrons has been replaced by gas-phase atoms in a Rydberg state. The low binding energy of the electron in a Rydberg atom combined with the large photoionization cross section of a Rydberg atom makes Rydberg atoms suitable for use in an infrared streak camera. Operation of the streak camera is demonstrated at 2.6 microm, well beyond the spectral range of any conventional streak camera.
A group at Oak Ridge National Laboratory reports that by means of the new technique of resonance ionization spectroscopy they have observed single atoms of cesium. They say that one atom in an environment of 1019 atoms or molecules of another kind can be measured with their method, and they do not believe this to be a limit. In subsequent experiments, the group has observed density fluctuations of atoms, absolute photodissociation cross sections, time-resolved diffusion and chemical reaction of atoms, and the detection of cesium atoms from the spontaneous fission of californium nuclei.
We theoretically study time-resolved photoemission in atoms as probed by attosecond streaking. We review recent advances in the study of the photoelectric efect in the time domain and show that the experimentally accessible time shifts can be decomposed into distinct contributions that stem from the feld-free photoionization process itself and from probe-field induced corrections. We perform accurate quantum-mechanical as well as classical simulations of attosecond streaking for efective one-electron systems and determine all relevant contributions to the time delay with attosecond precision. In particular, we investigate the properties and limitations of attosecond streaking for the transition from short-ranged potentials (photodetachment) to long-ranged Coulomb potentials (photoionization). As an example for a more complex system, we study time-resolved photoionization for endohedral fullerenes A @C 60 and discuss how streaking time shifts are modifed due to the interaction of the C 60 cage with the probing infrared streaking field.
Laser-dressed photoemission spectroscopy has established itself as the gold standard of attosecond temporal metrology.In this technique, the attosecond structure of an extreme-ultraviolet pulse is retrieved from the wave function of the electron wave packet released during photoionization.Here, we show that this electron wave packet should rather be described using the density matrix formalism, thus allowing one to account for all processes that can affect its coherence, from the attosecond pulse generation to the photoemission and the measurement processes.Using this approach, we reconstruct experimentally a partially coherent electron wave packet with a purity of 0.11 (1 for full coherence).Comparison with theoretical models then allows us to identify the origins of this decoherence and to overcome several limitations such as beam-line instabilities or spectrometer resolution.Furthermore, we show numerically how this method gives access to the coherence and eigencomponents of complex photoelectron wave packets.It thus goes beyond the current measurement of photoionization time delays and provides a general framework for the analysis and understanding of complex photoemission processes.
It is well known that the application of a pulse to a molecular electronic transition leaves the molecules vibrational modes in different electronic states in well-localized states, or wave packets[1]. One method of detecting the wave packets is via the time-dependent spectra of spontaneous emission from the excited molecule[2]. The emission consists in general of two parts, an incoherent part that depends only on the wave packet in the excited state, and a coherent part, that depends on the wave packets in both excited and ground electronic states (of a two-state molecule). This can be seen from the following simple calculation.
Spectroscopy of atoms in Rydberg states was an object of extensive investigation (see for example [1-5] and references therein). Usually necessary population of Rydberg states is achieved by means of multi-stage pulse laser pumping. That is why useful signal of ionization current from Single Channel Electron Multiplier (CEM or channeltron) is also pulse signal. Essential temporal instability of this signal is one of the main problems during its registration. More over in order to investigate Rydberg spectra of elements with high value of ionization potential (Al, Cu, Au etc.) it is necessary to apply high-temperature source of atoms (up to 2000 3000K). That is why there appears effect of redistribution of population by means of black body radiation. This effect makes additional difficulties to study ionization spectra. In order to overcome these obstacles we propose to apply time-dependent registration of ionization current from CEM. First of all such approach will allow us to store individual time-dependent realizations and to provide averaging of these realizations numerically excluding temporal instability. In addition after improvement of the receiving system it will be possible to detect ionization spectra resolving Rydberg states populated by means of black body radiation.