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

Sato, Shin‐ichiro

doi:10.1021/ct7000073

Cited by 9 publications

(11 citation statements)

References 11 publications

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“…An alternative way to retrieve coherent dynamics is by making use of the statistical variance of interferometric noise following randomly phased pulse-pair excitation (known as coherence observation by interference noise, or COIN) [9,10]. In contrast, here we report selective enhancement or suppression of fluorophores based on direct observation of the QI signal only [12][13][14], without any deliberate attempt to unravel pure coherent dynamics.…”

Section: Methodsmentioning

confidence: 96%

“…In a recent experiment, Brinks et al implemented a single-molecule fluorescencedetection technique to disentangle this spectral inhomogeneity under phase-locked pulse-pair excitation [31]. Taking into account the spectral line shape of absorption (which turns out to be a Voigt profile when both the homogeneous contribution with Lorentzian line shape as well as the inhomogeneous contribution with Gaussian line shape are present) and laser pulse (Gaussian profile), the QI signal under periodically phase-modulated pulse-pair excitation has shown to be varied for two different scenarios [13]: (1) if the pulse spectral width is at least an order of magnitude larger than the absorption linewidth, one expects the fringe frequency to be the inverse of the frequency width of the absorption profile and (2) at the other extreme, if a narrow pulse spectrum excites a subpopulation of the broad inhomogeneous absorption line shape, then the temporal fringe oscillations occur at a pulse carrier-wave frequency analogous to ultrafast hole-burning experiments [9,32]. For an intermediate situation (which happens to be the case in our experiment), the QI signal is neither given by the inverse of the spectral width nor follows the optical field oscillations [13,14]; for partial pulse-pair overlapping zone the QI signal differs from optical field oscillations due to nuclear dynamics i.e.…”

Section: Methodsmentioning

confidence: 99%

“…strong overlapping region) by periodically modulating the interpulse phase. This approach has been utilized in controlled gas-phase molecularfragmentation experiments [12] and studied in detail taking into account broadening of the spectral line shape as well as pulse profile, which is crucial in a condensed-phase environment [13,14]. In this Brief Report, we describe solutionphase fluorophore discrimination based on high-frequency QI observation and discuss its possible implementation in fluorescence microscopy.…”

Section: Introductionmentioning

confidence: 99%

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Fluorophore discrimination by tracing quantum interference in fluorescence microscopy

Roy

Goswami

2011

Phys. Rev. A

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Section: Methodsmentioning

confidence: 96%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Fluorophore discrimination by tracing quantum interference in fluorescence microscopy

Roy

Goswami

2011

Phys. Rev. A

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“…[23,26] The optical-phase-controlled pulse pair was generated by splitting femtosecond pulses (844 nm, % 40 fs, 80 MHz) from a Ti:sapphire laser (Tsunami, Spectra Physics) into two equal parts by means of a Michelson interferometer. A delay time t d of the pulse pair was determined by the difference in the optical path lengths of the two arms of the interferometer.…”

Section: Methodsmentioning

confidence: 99%

“…The detailed theoretical treatment of the QI measurements in condensed media has been described elsewhere. [26] Fitting of both the QI signal and the steady-state electronic spectra to Voigt functions was carried out simultaneously to eliminate the ambiguity that arises from estimating the homogeneous dephasing time and the inhomogeneous linewidth values (for details of the fitting procedure, see the Supporting Information.) As a result, we found the best parameter set for reconstructing the steady-state spectra and the time profile consistently.…”

Section: A C H T U N G T R E N N U N G [Cmmentioning

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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Brillouin shift and temperature measurement by spontaneous Rayleigh‐Brillouin scattering profiles using different models

Yan

et al. 2022

Micro & Optical Tech Letters

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Spontaneous Rayleigh-Brillouin scattering spectra in nitrogen have been measured in the pressure range from 4 to 7 bar at a wide temperature from 291 to 399 K with a scattering angle of about 90°, and then fitted to different theoretical models (S6, V3, and G3). The result of the root-mean-square errors of fitting residuals shows that the V3 and G3 models have good fitting performance. However, compared to the predicted Brillouin shift, the maximum relative errors in deducing the Brillouin shift from fitted data are 0.6% for the S6, 3.3% for the V3 and 4.6% the G3 models.The S6 model is the most accurate model in retrieving temperature for the absolute error below 3.5 K while the absolute error is less than 25 K for the V3 model and 35 K for the G3 model. Although the V3 and G3 models may not be suitable for the atmospheric temperature measurement, they are more potential for the hightemperature measurement of unknown environmental pressures.

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

Cited by 9 publications

References 11 publications

Fluorophore discrimination by tracing quantum interference in fluorescence microscopy

Fluorophore discrimination by tracing quantum interference in fluorescence microscopy

Cyclodextrin Nanocavity Caging Effect on Electronic Dephasing

Brillouin shift and temperature measurement by spontaneous Rayleigh‐Brillouin scattering profiles using different models

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