Coherent transients involving 2P excitons in ZnSe

Mitsumori, Yasuyoshi; Mizuno, Misao; Tanji, S.; Kuroda, Takashi; Minami, F.

doi:10.1016/s0022-2313(97)00189-0

Cited by 7 publications

(4 citation statements)

References 5 publications

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“…This has been demonstrated before in atomic systems [7] and in bulk ZnSe [8]. This has been demonstrated before in atomic systems [7] and in bulk ZnSe [8].…”

supporting

confidence: 60%

Coherent Control of Two-Photon Transitions

Garro

Kennedy

Heberle

et al. 2000

phys. stat. sol. (b)

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“…This has been demonstrated before in atomic systems [7] and in bulk ZnSe [8]. This has been demonstrated before in atomic systems [7] and in bulk ZnSe [8].…”

supporting

confidence: 60%

Coherent Control of Two-Photon Transitions

Garro

Kennedy

Heberle

et al. 2000

phys. stat. sol. (b)

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“…Control of quantum interference (QI) of molecular wavefunctions excited by a pair of femtosecond laser pulses that have a definite optical phase is one of the basic schemes for the control of versatile quantum systems including chemical reactions. The QI technique with the pulse pair, or the double pulse, has been applied to several atomic, molecular systems in the gas phase 1-3 and condensed phases. − A basic theory of the double-pulse QI experiment for a two-level molecular system in the gas phase has been given in the original paper by Scherer et al , In their beautiful work, they derived the expression for the QI signal from a two-level system including a molecular vibration. However, the effect of inhomogeneous broadening, which is not very significant in the gas phase, has not been taken into account.…”

Section: Introductionmentioning

confidence: 99%

Theory for Quantum Interference Signal from an Inhomogeneously Broadened Two-Level System Excited by an Optically Phase-Controlled Laser-Pulse Pair

Sato

2007

J. Chem. Theory Comput.

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A useful expression for the quantum interference (QI) signal was derived for an inhomogeneously broadened two-level system when it was excited by an optically phase-controlled laser-pulse pair. It was shown that the QI signal oscillates as a function of a relative optical phase, with the reduced angular frequency given by the relation ωa = (Γ(2)ω0 + γg(2)Ω)/(γg(2) + Γ(2)), where γg and Γ are standard deviations of the system's absorption and the laser spectra both having a Gaussian line shape, respectively, and ω0 and Ω are the center angular frequency of the system absorption and the carrier angular frequency of the laser, respectively.

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“…A method to induce QI of molecular wavefunctions by a pair of phaselocked pulses has been originally developed by Scherer et al and successfully applied to I 2 molecules in the gas phase. [14] The QI technique was successfully applied to various systems, such as GaAs quantum dots, [15,16] ZnSe films, [17] the Rydberg atom, [18,19] Cl 2 in an Ar matrix, [20] I 2 in the gas phase, [21,22] and a microcrystalline powder of a linked anthracene dimer.[23] Figure 1 shows the steady-state fluorescence and fluorescence-excitation spectra of perylene in both a g-CD aqueous solution and a tetrahydrofuran (THF) solution. Because of the low solubility of perylene in water (ca.…”

mentioning

confidence: 99%

Cyclodextrin Nanocavity Caging Effect on Electronic Dephasing

et al. 2008

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The ability to control molecular wavefunctions may lead to novel quantum technologies, such as bond-selective chemistry and quantum computing. [1][2][3] An understanding of the coherent-loss process is essential for the realization of these quantum technologies using quantum-interference (QI) effects in condensed media. Although the overwhelming majority of chemical reactions take place in solution, there have been very few experimental studies on the coherent reaction control of polyatomic molecules in condensed media, because of the rapid decoherence of wavefunctions. These fast quantumphase relaxations are thought to be caused by solute-solvent interactions. [4,5] Thus, an understanding of the roles of solvent molecules in the dephasing mechanism is strongly required. It is noted that the inhibition of dephasing is necessary for the development of coherent control techniques for more general reactions. Therefore, the protection of molecular wavefunctions from the surrounding environment becomes an important issue for the realization of quantum-control techniques in condensed phases. Here, we aimed to protect the quantum phase of a guest molecule by using the size-fit nanospace of a cyclodextrin nanocavity.Cyclodextrins (a-, b-, or g-CD), which are oligosaccharides with hydrophobic interiors and hydrophilic exteriors, are used as nanocavities. The ability of CDs to encapsulate organic and inorganic molecules in aqueous solution has led to intensive studies of their inclusion complexes.[6] We intuitively imagined that the confinement of a guest molecule within the CD nanocavity would reduce perturbations from the surrounding environment, which cause the decoherence. Several studies on CD complexes with aromatic compounds, performed using timeresolved spectroscopy, have been reported. [6][7][8][9][10][11][12][13] To our knowledge, however, no experiments have been reported on CD inclusion to suppress decoherence. As far as we know, this is the first report on the CD encapsulation effect that moderates the decoherence of the molecular wavefunction at room temperature.Herein, we report the moderation of electronic decoherence of perylene in g-CD at room temperature, as measured by an optical-phase-controlled pulse-pair quantum interferometer, [14][15][16][17][18][19][20][21][22][23] combined with spectral lineshape analysis. A method to induce QI of molecular wavefunctions by a pair of phaselocked pulses has been originally developed by Scherer et al. and successfully applied to I 2 molecules in the gas phase. [14] The QI technique was successfully applied to various systems, such as GaAs quantum dots, [15,16] ZnSe films, [17] the Rydberg atom, [18,19] Cl 2 in an Ar matrix, [20] I 2 in the gas phase, [21,22] and a microcrystalline powder of a linked anthracene dimer.[23] Figure 1 shows the steady-state fluorescence and fluorescence-excitation spectra of perylene in both a g-CD aqueous solution and a tetrahydrofuran (THF) solution. Because of the low solubility of perylene in water (ca. 1.6 10 À9 m), [24] we could n...

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Coherent transients involving 2P excitons in ZnSe

Cited by 7 publications

References 5 publications

Coherent Control of Two-Photon Transitions

Coherent Control of Two-Photon Transitions

Theory for Quantum Interference Signal from an Inhomogeneously Broadened Two-Level System Excited by an Optically Phase-Controlled Laser-Pulse Pair

Cyclodextrin Nanocavity Caging Effect on Electronic Dephasing

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