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Physical Review Letters

Ramsey interference in strongly driven Rydberg systems

R. R. Jones, Chandra Raman, Douglass W. Schumacher, P. H. Bucksbaum

Published Oct 18, 1993• 115 citations
Publisher

Abstract

We have studied the evolution of regular and ``dark'' radial wave packets under the influence of two coherent, temporally separated 100 fs laser pulses. The atomic states are probed by ramped-field ionization. The final state populations exhibit Ramsey oscillations with periods ranging from 2.6--1000 fs as a function of the delay between the two pulses. This time-domain bound-state interferometry reveals several new aspects of the dynamic evolution of wave packets in the presence of strong laser fields. Lowest order perturbation theory is inadequate to describe wave packet formations, even at the lowest intensities studied.

DOI
10.1103/physrevlett.71.2575

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The evolution of atomic systems under the influence of two coherent, temporally separated 100 fs laser pulses has been studied. Ramsey interference fringes are observed in the populations of various energy levels as a function of delay between the two pulses. At high intensities the temporal interferograms are quite complicated and yield information on the couplings between all of the states in the atomic system. A simple three‐level system as well as localized and dark radial Rydberg wavepackets have been studied.

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Observation of quantum features in the evolution of a Rydberg wave packet

John A. Yeazell, Carlos R. Stroud

Quantum mechanical wave packet states can approach the classical ideal of a spatially localized particle traveling along a well-defined trajectory. These states offer a system in which the classical limit of quantum atomic theory can be studied. In this work, a wave packet that is radially localized and whose radial motion occurs at the classical orbital period is studied. Despite these strong classical features, the long-term evolution displays the quantum nature of the state. As the wave packet evolves, it becomes dispersed, and the radial motion becomes irregular. However, the wave packet does not remain dispersed, and classical motion returns with the return of the spatial localization. Both the collapse and revival of the wave packet occur because of the quantized nature of the atom. In this experiment, the wave packet was excited to the Rydberg slates by a short, ultraviolet pulse from the ground state of potassium. The probe pulse delay was scanned, and the resulting photo-ionization signal displayed the evolution of the wave packet. The collapse and revival of the radial wave packet were observed.1

Annual Meeting Optical Society of America•Jan 1, 1990•0 citations
We have studied the evolution of regular and ``dark'' radial wave packets under the influence of two coherent, temporally separated 100 fs laser pulses. The atomic states are probed by ramped-field ionization. The final state populations exhibit Ramsey oscillations with periods ranging from 2.6--1000 fs as a function of the delay between the two pulses. This time-domain bound-state interferometry reveals several new aspects of the dynamic evolution of wave packets in the presence of strong laser fields. Lowest order perturbation theory is inadequate to describe wave packet formations, even at the lowest intensities studied.
The evolution of atomic systems under the influence of two coherent, temporally separated 100 fs laser pulses has been studied. Ramsey interference fringes are observed in the populations of various energy levels as a function of delay between the two pulses. At high intensities the temporal interferograms are quite complicated and yield information on the couplings between all of the states in the atomic system. A simple three‐level system as well as localized and dark radial Rydberg wavepackets have been studied.
Rydberg states in sodium are excited using two identical broadband, dye laser pulses. Each 8 ns pulse has a bandwidth of approximately 45 cm -1 , and Rydberg states with several different principal quantum numbers are simultaneously excited. The number of Rydberg atoms created by each pulse pair is detected as a function of the delay between the two pulses. Strong modulations in the population in each Rydberg level and in the total Rydberg signal are observed. The oscillations are identical to those which would be expected if two transform-limited, 300 fs laser pulses had been used. We show explicitly, in the limit of weak pulses, that these 'bound-state interferograms' acquired using the time-domain, Ramsey separated-oscillatory fields method are only dependent on the excitation cross section and pulse frequency spectrum. Therefore, weak-field interferograms do not in themselves give information on the spatial-distribution of the electron wavefunction. In addition, the benefits of using strong or weak pulses for bound-state interferometry are discussed.
We show that wave-packet interference techniques can reconstruct the quantum state of wave packets excited by strong laser pulses. The measurement may be accomplished even when the strength of the excitation is sufficient to significantly deplete the ground state. The probe of the wave packet can still remain perturbative. An inversion algorithm is also developed that is a generalization of the standard Ramsey fringe probe of a wave packet. The normalized sums and differences of the populations of two of the Rydberg states display Ramsey fringes and from these fringes the relative phase between these two states can be found. The algorithm offers advantages in efficiency over previous interferometric algorithms. The algorithm is not sensitive to the precise nature of the distribution of the phase between the pump and probe pulses.
Following the experiment of Jones et al. [Phys. Rev. Lett. 71, 2575 (1993)], we present a theory of coherent redistribution of population in a model Rydberg atom exposed to a sequence of two identical laser pulses separated in time and shorter in duration than the Rydberg-electron Kepler period. For different initial-population conditions, we solve the problem of redistribution in a fully analytical and rigorously nonperturbative way, thus obtaining discrete-state population amplitudes, dependent on laser intensity, and a time delay between the pulses. Using this solution, we study the population in a given state versus pulse delay (Ramsey fringes), as well as the corresponding Fourier spectrum, for both low and high laser intensities. From the number of frequency components and their positions in the Fourier spectrum, we deduce the redistribution of the initial-state population over a number of states by the first pulse. Within our model calculations we achieve qualitative agreement with the experimental observation of Jones et al. that an increase in laser intensity results in a general increase in the number of frequency components in the Fourier spectrum. Our theoretical results are also consistent with the experimental finding of Noordam et al. [Phys. Rev. Lett. 68, 1496 (1992)] that Raman transitions via the continuum between different Rydberg states are essential for population redistribution. We suggest new experiments to measure the effect of the initial-state depletion on the Fourier spectrum. As follows from our model calculations, some frequency components (both low and optical) present in the low-intensity Fourier spectrum should vanish in the high-intensity spectrum due to complete depletion of the initial state by the first pulse.
Excitation and photoionization of Rydberg wave packets are described. Interference of bound-free transitions from many coherently populated Rydberg levels is shown to affect the dependence of the photoionization probability on the duration of interaction. Strong-field interference effects in such a system are described also. The most important of these is the field-induced interference stabilization of Rydberg atoms in a strong ionizing field. The intensity range in which this effect can exist is determined. The results derived are used for a qualitative model describing supercontinuum emission in the process of multiphoton ionization.
Quantum mechanical wave packet states can approach the classical ideal of a spatially localized particle traveling along a well-defined trajectory. These states offer a system in which the classical limit of quantum atomic theory can be studied. In this work, a wave packet that is radially localized and whose radial motion occurs at the classical orbital period is studied. Despite these strong classical features, the long-term evolution displays the quantum nature of the state. As the wave packet evolves, it becomes dispersed, and the radial motion becomes irregular. However, the wave packet does not remain dispersed, and classical motion returns with the return of the spatial localization. Both the collapse and revival of the wave packet occur because of the quantized nature of the atom. In this experiment, the wave packet was excited to the Rydberg slates by a short, ultraviolet pulse from the ground state of potassium. The probe pulse delay was scanned, and the resulting photo-ionization signal displayed the evolution of the wave packet. The collapse and revival of the radial wave packet were observed.1