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Selective Strong-Field Enhancement and Attenuation of Excitation and Ionization with Short Laser Pulses

N. A. Hart

Published May 12, 2015• 0 citations
OpenAlex

Abstract

The coherent control of atomic energy level population is important for several areas physics and engineering including fluorescent spectroscopy, resonantly enhanced multiphoton ionization, harmonic generation, remote sensing and lasing. At low intensities where the Stark shift can be neglected, coherent control mechanisms usually exploit resonances created from stationary energy states dressed by integer multiples of the photon energy. However, in the strong field limit where large laser pulse intensities lead to significant Stark shifts, the resonant conditions are dynamic both in time and space and will likely not be satisfied for the entire laser pulse or beam.\n\nIn this research, we experimentally and theoretically demonstrate coherent control of atomic energy level population in sodium vapor as well as the selective excitation of sodium Rydberg levels using high intensity laser pulses. We also make a direct measurement of the ponderomotive shift of the continuum. While techniques based on resonance interferences and rapid adiabatic passage have been introduced for selective excitation, the conditions that must be satisfied for these phenomena can be hampered by short femtosecond pulse durations and large Stark shifts. In contrast, a technique referred to here as Resonance Sampling, uses the AC Stark shifts to selectively induce Freeman resonances and is resilient to changes in the spectral phase. Freeman resonances established in this way can result in population inversion of the excited state, and may lead to new lasing mediums and remote sensing applications.\n\n\nIn this research, we experimentally and theoretically demonstrate coherent control of atomic energy level population in sodium vapor as well as the selective excitation of sodium Rydberg levels using high intensity laser pulses. While techniques based on resonance interferences and rapid adiabatic passage have been introduced for selective excitation, the conditions that must be satisfied for these phenomena can be hampered by short femtosecond pulse durations and large Stark shifts. In contrast, a technique referred to here as Resonance Sampling, uses the AC Stark shifts to selectively induce Freeman resonances and is resilient to changes in the spectral phase. Freeman resonances established in this way can result in population inversion of the excited state, and may lead to new lasing mediums and remote sensing applications.

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The coherent control of atomic energy level population is important for several areas physics and engineering including fluorescent spectroscopy, resonantly enhanced multiphoton ionization, harmonic generation, remote sensing and lasing. At low intensities where the Stark shift can be neglected, coherent control mechanisms usually exploit resonances created from stationary energy states dressed by integer multiples of the photon energy. However, in the strong field limit where large laser pulse intensities lead to significant Stark shifts, the resonant conditions are dynamic both in time and space and will likely not be satisfied for the entire laser pulse or beam.\n\nIn this research, we experimentally and theoretically demonstrate coherent control of atomic energy level population in sodium vapor as well as the selective excitation of sodium Rydberg levels using high intensity laser pulses. We also make a direct measurement of the ponderomotive shift of the continuum. While techniques based on resonance interferences and rapid adiabatic passage have been introduced for selective excitation, the conditions that must be satisfied for these phenomena can be hampered by short femtosecond pulse durations and large Stark shifts. In contrast, a technique referred to here as Resonance Sampling, uses the AC Stark shifts to selectively induce Freeman resonances and is resilient to changes in the spectral phase. Freeman resonances established in this way can result in population inversion of the excited state, and may lead to new lasing mediums and remote sensing applications.\n\n\nIn this research, we experimentally and theoretically demonstrate coherent control of atomic energy level population in sodium vapor as well as the selective excitation of sodium Rydberg levels using high intensity laser pulses. While techniques based on resonance interferences and rapid adiabatic passage have been introduced for selective excitation, the conditions that must be satisfied for these phenomena can be hampered by short femtosecond pulse durations and large Stark shifts. In contrast, a technique referred to here as Resonance Sampling, uses the AC Stark shifts to selectively induce Freeman resonances and is resilient to changes in the spectral phase. Freeman resonances established in this way can result in population inversion of the excited state, and may lead to new lasing mediums and remote sensing applications.
We experimentally demonstrate robust selective excitation and attenuation of atomic Rydberg level populations in sodium vapor (Na i) using intense laser pulses in the strong-field limit (>1012W/cm2)(>{10}^{12}\phantom{\rule{0.16em}{0ex}}\mathrm{W}/\mathrm{c}{\mathrm{m}}^{2})(>1012W/cm2). Coherent control of the atomic population and related ionization channels is realized for intensities above the over-the-barrier ionization intensity. Moreover, atomic excitation selectivity and high ionization yield are simultaneously achieved without the need to tailor the spectral phase of the laser. A qualitative model confirms that this strong-field coherent control arises through the manifestation of a Freeman resonance.
We investigate AC Stark-shifted resonances in argon with ultrashort near-infrared pulses. Using 30 fs pulses, we observe periodic enhancements of the excitation yield in the intensity regions corresponding to the absorption of 13 and 14 photons. By reducing the pulse duration to 6 fs with only a few optical cycles, we also demonstrate that the enhancements are significantly reduced beyond what is measurable in the experiment. Comparing these to numerical predictions, which are in quantitative agreement with experimental results, we find that even though the quantum state distribution can be broad, the enhancements are largely due to the efficient population of a select few AC Stark-shifted resonant states rather than the closing of an ionization channel. Because these resonances are dependent on the frequency and intensity of the laser field, the broad bandwidth of the 6 fs pulses means that the resonance condition is fulfilled across a large range of intensities. This is further exaggerated by volume-averaging effects, resulting in excitation of the 5g5g5g state at almost all intensities and reducing the apparent magnitude of the enhancements. For 30 fs pulses, volume averaging also broadens the quantum state distribution, but the enhancements are still large enough to survive. In this case, selectivity of excitation to a single state is reduced below 25% of the relative population. However, an analysis of time-dependent Schr\"odinger equation simulations indicates that excitation of up to 60% into a single state is possible if volume averaging can be eliminated and the intensity can be precisely controlled.
The energy levels of atoms and molecules exposed to intense, short, high-frequency laser pulses undergo time-dependent distortion known as dynamic Stark shift (DSS). These level shifts are induced by the coupling with nonresonant (nonessential) states and follow the temporal intensity profile of the laser pulse. Owing to the different DSSs of the individual atomic levels, transient resonance suppressions and enhancements significantly modify the multiphoton ionization pathway, leaving clear fingerprints (asymmetry, splitting, and shifting) in the energy spectrum of emitted photoelectrons. Here we investigate this phenomenon by solving the time-dependent Schr\"odinger equation of the valence electron of Na and Li in increasing levels of complexity: (i) developing minimal models for two-photon transition and (2+12+12+1)-photon ionization, (ii) applying a spectral method without continuum-continuum couplings, and (iii) propagating the electron wave packet on a large spatial grid accounting for all possible couplings. We show that appropriately detuned transform limited pulses provide a high level of control in strong-field excitation, when the atomic levels are dynamically shifted. Furthermore, we demonstrate the role of DSSs in the multipeak structure of the Autler-Townes doublet, found when several Rabi oscillations are induced during the strong-field resonant ionization.
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←←3s, 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.
We have measured the energy spectrum of photoelectrons emitted in multiphoton ionization of atoms by a short-pulse, tunable laser. The spectrum shows prominent resonances, confirming the observations of Freeman et al. [Phys. Rev. Lett. 59, 1092 (1987)]. The study of the position and intensity of such resonances, as a function of laser wavelength and intensity, probes the structure of the atom in the presence of the strong electromagnetic field and allows their spectroscopic assignment. A systematic study of the ac Stark shift of one of the resonances, the 7s[3/2]\ifmmode^\circ\else\textdegree\fi{} level of xenon, is presented.
We show that coherent control of multiphoton transitions is possible in the strong field limit, even in the presence of large dynamic Stark shifts. By tailoring the phase of an ultrafast laser pulse, one can compensate for the dynamic Stark shift during the atom-field interaction to achieve efficient population transfer in two-photon absorption. Numerical simulations for atomic sodium reveal efficient population transfer from the $\ensuremath{\mid}3s⟩$ ground state to the $\ensuremath{\mid}4s⟩$ excited state using an appropriately shaped ultrafast laser pulse. The theory and simulations provide insight into coherent control of more complicated multiphoton processes.