Quantum control by selective population of dressed states using intense chirped femtosecond laser pulses

Wollenhaupt, M.; Präkelt, A.; Sarpe-Tudoran, C.; Liese, D.; Baumert, Thomas

doi:10.1007/s00340-005-2066-0

Cited by 80 publications

(74 citation statements)

References 25 publications

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“…[1][2][3][4][5][6][7][8][9][10][11] Often, this is accomplished in the strong-field regime where the electric field is on the order of the molecular electric field binding the valence electrons. The interaction of a strong, nonresonant laser field with a molecule is governed by the coupling of the laser field with the molecular electrons in the system.…”

Section: Introductionmentioning

confidence: 99%

Observing the Transition from Stark-Shifted, Strong-Field Resonance to Nonadiabatic Excitation

et al. 2009

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Time-dependent Hartree-Fock simulations for a linear triatomic molecular monocation (CO 2 + ) interacting with a 5 fs, 800 nm, strong field laser pulse were performed to explore the excitation mechanisms in a molecular cation. Fourier analysis of the time-dependent residual dipole moment reveal a nonmonotonic behavior in the amplitude of the 5.18 eV feature in the excitation spectra of the molecular monocation with increasing intensity, suggesting a change in the excitation mechanism. Calculations performed for different carrier frequencies of the laser field reveal that the mechanism changes from resonant multiphoton excitation to nonadiabatic excitation. In the resonant multiphoton excitation regime, a slight variation of the laser pulse duration (fwhm) reveals a nonlinear increase in the peak height of the multiphoton resonant state, and Stark-shifting of the multiphoton resonant state is observed for an increase in intensity. Nonadiabatic excitation from TDHF compares well with the analytical theory for nonadiabatic excitation.

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Section: Introductionmentioning

confidence: 99%

Observing the Transition from Stark-Shifted, Strong-Field Resonance to Nonadiabatic Excitation

et al. 2009

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“…We theoretically propose a π or cubic phase modulation to realize the enhancement and narrowing of REMPI-PS [26][27][28][29]. In theory, the photoelectron spectral modulation was explained by the selective population of dressed states [21][22][23][24], or multiphoton power spectrum [28,29].In our previous works [26][27][28][29], the REMPI-PS was calculated by considering the laser field in time domain; thus the physical control mechanism of the photoelectron spectral modulation cannot be directly explained from this theoretical model, which greatly limits the understanding of the resonance-enhanced multiphoton-ionization process. However, in this paper we develop a theoretical model by considering the laser field in frequency domain and show that the REMPI process involves the on-and near-resonant excitation pathways, and therefore the photoelectron spectral modulation can be well explained by the inter-and intragroup interference involving these on-and near-resonant excitation pathways.…”

mentioning

confidence: 99%

“…Recently, the advent of the femtosecond pulse shaping technique by modulating the laser spectral phase and/or amplitude in the frequency domain opened an opportunity to effectively control the femtosecond REMPI-PS. Various phase modulation schemes have been proposed to enhance or narrow the REMPI-PS [21][22][23][24][25][26][27][28][29], and some schemes have been experimentally realized [21][22][23][24][25]. For example, Wollenhaupt et al experimentally demonstrated the selective excitation of the slow and fast photoelectron components of REMPI-PS by sinusoidal, chirped, or phase-step modulation [21-24].…”

mentioning

confidence: 99%

Quantum control of femtosecond resonance-enhanced multiphoton-ionization photoelectron spectroscopy

Zhang

Jia

et al. 2013

Phys. Rev. A

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We establish a theoretical model based on perturbation theory to show that the resonance-enhanced multiphoton-ionization photoelectron spectroscopy (REMPI-PS) in cesium (Cs) atom can be effectively enhanced and narrowed by appropriately shaping the femtosecond laser pulse, and the corresponding physical control processes can be well illustrated by considering the inter-and intragroup interferences involving on-and near-resonant three-photon excitation pathways. Consequently, a high-resolution REMPI-PS and fine energy-level diagram of the excited states can be obtained in spite of the broad femtosecond laser spectrum. PACS number(s): 32.80. Qk, 32.80.Rm, 42.50.Md Studying the microscopic behaviors of atom and molecule is always an interesting subject of scientists, which is very helpful for understanding and manipulating the macroscopic world. Resonance-enhanced multiphoton-ionization photoelectron spectroscopy (REMPI-PS), involving a resonant single-or multiple-photon absorption to an excited state followed by another photon that ionizes the atom or molecule, has become a powerful technique applied to the atomic and molecular spectroscopy [1][2][3][4][5], and has been widely applied to study the excited or Rydberg state structure and the photoionization and dissociation process [6][7][8][9][10][11][12][13][14]. By observing REMPI-PS, one can determine which excited state is ionized that offers the structure information of the excited states, and also identify the dynamical processes occurring in the excited states that the electrons derive from the ionization of the neutral medium or the dissociation of the parent ion.Nanosecond or picosecond laser pulse was a wellestablished tool to achieve high-resolution REMPI-PS [15-18], but the nanosecond or picosecond REMPI-PS was not suitable to study the dynamical process of the excited state due to the long pulse duration, such as transient population, wavepacket evolution, proton transfer, and so on. The femtosecond laser pulse was considered as an ideal excitation source because of its high laser intensity and short pulse duration [19,20], while an inevitable question for the femtosecond REMPI-PS is poor spectral resolution due to the large laser spectral bandwidth. Recently, the advent of the femtosecond pulse shaping technique by modulating the laser spectral phase and/or amplitude in the frequency domain opened an opportunity to effectively control the femtosecond REMPI-PS. Various phase modulation schemes have been proposed to enhance or narrow the REMPI-PS [21][22][23][24][25][26][27][28][29], and some schemes have been experimentally realized [21][22][23][24][25]. For example, Wollenhaupt et al. experimentally demonstrated the selective excitation of the slow and fast photoelectron components of REMPI-PS by sinusoidal, chirped, or phase-step modulation [21-24]. Krug et al. experimentally achieved the enhancement * sazhang@phy.ecnu.edu.cn † zrsun@phy.ecnu.edu.cnand suppression of REMPI-PS by chirped phase modulation [25]. We theoretically propose a π or cubic p...

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“…76 Strong field quantum control via SPODS using pulse shaping techniques was experimentally demonstrated for the potassium atom by M. Wollenhaupt and T. Baumert. 77 Within their investi gations, they used sinusoidal spectral phase modulation, 78,79 chirped excitation 80 and adaptive optimization of the spectral phase 77 to realize the SPODS scheme. In the following sections we shortly revisit the basics of the SPODS mechanism.…”

Section: Oct To Control the Spods-scheme In The Potassium Dimermentioning

confidence: 99%

Optimal control theory – closing the gap between theory and experiment

Hoff

Thallmair

Kowalewski

et al. 2012

Phys. Chem. Chem. Phys.

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Optimal control theory and optimal control experiments are state of the art tools to control quantum systems. Both methods have been demonstrated successfully for numerous applications in molecular physics, chemistry and biology. Modulated light pulses could be realized, driving these various control processes. Next to the control efficiency, a key issue is the understanding of the control mechanism. An obvious way is to seek support from theory. However, the underlying search strategies in theory and experiment towards the optimal laser field differ. While the optimal control theory operates in the time domain, optimal control experiments optimize the laser fields in the frequency domain. This also implies that both search procedures experience a different bias and follow different pathways on the search landscape. In this perspective we review our recent developments in optimal control theory and their applications. Especially, we focus on approaches, which close the gap between theory and experiment. To this extent we followed two ways. One uses sophisticated optimization algorithms, which enhance the capabilities of optimal control experiments. The other is to extend and modify the optimal control theory formalism in order to mimic the experimental conditions.

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Quantum control by selective population of dressed states using intense chirped femtosecond laser pulses

Cited by 80 publications

References 25 publications

Observing the Transition from Stark-Shifted, Strong-Field Resonance to Nonadiabatic Excitation

Observing the Transition from Stark-Shifted, Strong-Field Resonance to Nonadiabatic Excitation

Quantum control of femtosecond resonance-enhanced multiphoton-ionization photoelectron spectroscopy

Optimal control theory – closing the gap between theory and experiment

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