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Physical Review A

Mode-selective excitation using ultrafast chirped laser pulses

Svetlana Malinovskaya

Published Mar 20, 2006• 23 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.73.033416

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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 study the effect of coupling between molecular vibrational modes attendant the excitation of Raman transitions using ultrafast chirped laser pulses. We model Raman-active vibrational modes by two-level systems (TLSs) with nondegenerate ground states and a predetermined initial relative phase. Chirp of the pump and Stokes pulses is the same in magnitude and opposite in sign for the whole pulse duration. To reveal the nonadiabatic effects induced by the coupling between the vibrational modes, we compare the model of two uncoupled TLSs with the one of two TLSs coupled by the external fields. The first model shows population inversion. Within the second model, the coupling induces nonadiabatic effects leading to a mixed population distribution. By introducing the time delay between the Stokes and pump pulses, nearly complete population transfer is realized in both coupled TLSs.
Abstract We study the effects of coupling between molecular vibrational modes attendant the excitation of Raman transitions. Raman active vibrational modes are described by two two‐level systems (TLSs) with nondegenerate ground states. The population inversion is investigated under the condition of zero relative phase between initially populated states. We use two ultrafast laser pulses for the pump and the Stokes fields that have chirps the same in the magnitude and opposite in the sign. Within this model, the coupling induces nonadiabatic effects leading to a diverse population distribution. By introducing the time delay between the Stokes and the pump pulse, we realized a complete population transfer in both coupled TLSs. We demonstrated the population inversion in a more generic case of the averaged initial relative phase. © 2012 Wiley Periodicals, Inc.
We propose a selective, efficient, and robust way to realize control of coherent population transfer in a $\ensuremath{\Lambda}$-type four-level system with a closely spaced doublet in the final state with time-separated chirped pump pulse and Stokes pulse pair by merging stimulated Raman adiabatic passage, temporal coherent control, and chirped adiabatic passage techniques. Moreover, an arbitrary coherent superposition between the final doublet, or between the intermediate state and either of the doublets can be created. This method holds the ability to ``control with control'' and has potential applications in coherent control of chemical reactions and quantum information processing.
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
We present the experimental demonstration of a novel, efficient, and selective technique to prepare population inversion. The technique is an extension of Stark-chirped rapid adiabatic passage (SCRAP), i.e., SCRAP among three states. In this process a Lambda-type quantum system is driven by two laser pulses, the pump and Stokes pulses, which are appropriately detuned from transition frequencies. A third laser pulse induces a dynamic Stark shift in the upper energy level, and the timing of all three pulses is controlled in order to prepare population inversion between the two lower states in the Lambda-type level scheme. Our data on population transfer in nitric oxide (NO) molecules clearly show that SCRAP among three states provides an advantageous alternative to such techniques as stimulated Raman adiabatic passage.
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.