A well-known quantum interference phenomenon is combined with laser-induced collisional energy transfer to create a coherently controlled excitation involving two species. From one viewpoint the process involves a laser induced catalyst. An experimental demonstration is performed in mixtures of Xe and Kr gases.
Since its inception, a primary focus of resonance ionization spectroscopy has been sensitive detection of atomic species in one form on another. But RIS has found many applications in spectroscopy where the nature of a resonant transition was of interest, and RIS provided a very useful tool for measuring a given feature. A large set of examples from this category can be found in studies of quantum interferences as they affect multiphoton-resonant transitions in gases and vapors. In many instances RIS has been used to show various effects that can be produced when two different optical paths simultaneously link a resonant transition in a gaseous system. We note that RIS has been used to show dramatic effects of wave mixing interferences on certain multi-photon driven resonant excitation processes. These include: (1) Complete destructive interference from a FWM field can reduce to zero the odd-photon-mediated excitation probability of a dipole allowed transition [1–4]; (2) For dual beam pumping the resonant excitation probability is restored but at a shifted frequency, [2]; (3) Separate resonant excitation profiles of a given transition can be produced under multi-beam pumping, all in conformance with theoretical predictions [3]; Quantum interference can suppress an ac Stark shift [4].
We report the observation of coherent control of the ionization rate in four-photon resonant, five-photon ionization schemes in Kr and Xe. The intermediate resonance is excited via different interfering channels involving four-photon absorption of the fundamental laser frequency ( ionization) as well as one third harmonic and one fundamental frequency photon absorption ( excitation), a particular aspect of the scheme being that interference occurs at a virtual level. By varying the relative phase of the two electromagnetic fields, a large modulation depth has been observed which is due to the chosen non-linear excitation scheme. In the Xe excitation experiment the interference between the different channels could be additionally probed through the modulation of the third-harmonic signal.
Coherent control provides a quantum interference based method for controlling atomic and molecular dynamics. We report two experimental observations of different ways to achieve such a control in atomic photoionization continuum. One is the photoionization of sodium atoms, initially prepared in the 3P1/2 excited state, by a non resonant three-photon interaction with 1064-nm laser light and by a one-photon interaction with the third-harmonic field, at 355 nm. Interference between the two transition paths allows the control of the total ionization rate by varying the relative phase of the laser fields. The second experiment is the observation of the modification of the ionization continua of xenon through laser induced continuum structure (LICS). The multiphoton radiative decay of the xenon ground state into the two electronic continua, that correspond to the two fine structure levels of the ground state of the xenon ion, is varied by electromagnetically embedding a bound state of the atom into the two continua. Both experiments are performed on an atomic beam apparatus which uses a time-of-flight spectrometer for energy analyzing the emitted photoelectrons.
Atoms irradiated with combined femtosecond laser and extreme ultraviolet (XUV) fields ionize through multiphoton processes, even when the energy of the XUV photon is below the ionization potential. However, in the presence of two different XUV photons and an intense laser field, it is possible to induce full electromagnetic transparency. Taking helium as an example, the laser field modifies its electronic structure, while the presence of two different XUV photons and the laser field leads to two distinct ionization pathways that can interfere destructively. This work demonstrates a new approach for coherent control in a regime of highly excited states and strong optical fields.