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International Conference on Ultrafast Phenomena

Stimulated Emission Pumping and Selective Excitation by Adiabatic Passage with Frequency Modulated Picosecond Laser Pulses

Joseph S. Melinger, Anand Hariharan, Suketu R. Gandhi, Warren S. Warren

Published Jan 1, 1992• 0 citations
Publisher

Abstract

Optical excitation of material transitions by adiabatic passage with frequency modulated (chirped) laser pulses is a useful spectroscopic tool.1,2 Here we demonstrate that picosecond frequency modulated laser pulses produce more efficient population transfer, and more selective excitation than equivalent (same spectral bandwidth) nearly transform limited laser pulses. We apply frequency modulated pulses to gas-phase and condensed phase systems. We also point out the "robustness", or insensitivity of the properties of the material excitation to the parameters of the laser field, that is inherent to the adiabatic process. The robustness obtainable by adiabatic passage will ultimately prove useful to laboratory applications of theoretical schemes which require frequency modulated ultrashort laser pulses to control chemical reaction dynamics.3

DOI
10.1364/up.1992.tuc17

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Optical excitation of material transitions by adiabatic passage with frequency modulated (chirped) laser pulses is a useful spectroscopic tool.1,2 Here we demonstrate that picosecond frequency modulated laser pulses produce more efficient population transfer, and more selective excitation than equivalent (same spectral bandwidth) nearly transform limited laser pulses. We apply frequency modulated pulses to gas-phase and condensed phase systems. We also point out the "robustness", or insensitivity of the properties of the material excitation to the parameters of the laser field, that is inherent to the adiabatic process. The robustness obtainable by adiabatic passage will ultimately prove useful to laboratory applications of theoretical schemes which require frequency modulated ultrashort laser pulses to control chemical reaction dynamics.3
Calculations indicate that high vibrational states of oxygen and chlorine can be excited using a series of nonresonant Raman pulses, where both the pump and the Stokes pulses are chirped with linear frequency sweeps. Most of the previously reported coherent processes (such as simple adiabatic passage) are seriously degraded when rotational effects are included. However, we find that the laser pulse parameters (intensity and bandwidth) required to invert population into high vibrational states via Raman chirped adiabatic passage are achievable using technology that is currently available. Applications to homonuclear diatomic molecules are discussed in detail.
We study the dynamics of chirped adiabatic passage (CHIRAP) with temporally delayed pulses to selectively and fully transfer population in atoms and molecules. We show that the transfer of population via stimulated Raman adiabatic passage (STIRAP) and stimulated two-photon adiabatic absorption with temporally delayed laser pulses is not adversely affected by applying a chirp to the pulses, provided the intensity of the laser is sufficiently large to allow adiabatic passage. We then proceed to consider systems in which a near degeneracy of terminal state levels results in nonselective population of the terminal levels using nonchirped STIRAP or two-photon absorption stimulated passage, because the dynamics within the nearly degenerate pair of levels is not adiabatic. However, the CHIRAP process selectively populates only one of the terminal levels.
We propose a method to control population transfer and coherence in a multimode system using a transform-limited pump and a linearly chirped Stokes pulse in stimulated Raman scattering. Simultaneously applied pump and Stokes pulse are shown to induce the ac Stark shifts that result in nonadiabatic coupling of the dressed states, through which the pulse chirp governs population distribution. The method may be applied to selectively excite Raman transitions having the frequency difference less than the bandwidth of a transform-limited pulse.
We propose and experimentally demonstrate the method of population transfer by piecewise adiabatic passage between two quantum states. Coherent excitation of a two-level system with a train of ultrashort laser pulses is shown to reproduce the effect of an adiabatic passage, conventionally achieved with a single frequency-chirped pulse. By properly adjusting the amplitudes and phases of the pulses in the excitation pulse train, we achieve complete and robust population transfer to the target state. The piecewise nature of the process suggests a possibility for the selective population transfer in complex quantum systems.
The difficulty in combining high fidelity with fast operation times and robustness against sources of noise is the central challenge of most quantum control problems, with immediate implications for the realization of quantum devices. We theoretically propose a protocol, based on the widespread stimulated Raman adiabatic passage technique, which achieves these objectives for quantum state transfers in generic three-level systems. Our protocol realizes accelerated adiabatic following through the application of additional control fields on the optical excitations. These act along frequency sidebands of the principal adiabatic pulses, dynamically counteracting undesired transitions. The scheme facilitates experimental control, not requiring new hardly-accessible resources. We show numerically that the method is efficient in a very wide set of control parameters, bringing the timescales closer to the quantum speed limit, also in the presence of environmental disturbance. These results hold for complete population transfers and for many applications, e.g., for realizing quantum gates, both for optical and microwave implementations. Furthermore, extensions to adiabatic passage problems in more-level systems are straightforward.
We have considered a coherent population transfer to a higher excited singlet state ( S2 ) of molecules with anomalous fluorescence in molecular assemblies (e.g., a dense medium). A direct excitation to S2 requires light in the UV region. Because of this, the transition is conveniently realized by a two-step (two-photon) process: S0→S1→S2 , where transitions S0→S1 and S1→S2 correspond to the optical region. We have shown that efficient stimulated Raman adiabatic passage (STIRAP) in the ladder configuration can be realized in this case, using suitably chirped pulses, to compensate a change of the two-photon transition frequency in time, induced by the pulses themselves, due to near dipole-dipole interactions. We have provided a reduced state formulation of the optical control process. Chirping the “pump” pulse that excites transition S0→S1 is nonequivalent to chirping the “Stokes” pulse that excites transition S1→S2 , with respect to the population of the intermediate state ( S1 ) in the pulse nonadiabatic regime. We have also shown that with suitably chirped pulses, efficient STIRAP still persists even for a rather large decay of the intermediate state.