### Abstract

Discussion on wavelength dependent "anharmonic" effects in a pump-probe signal for a system of wavepacket on one- and two-dimensional harmonic potentials was given. The Fourier power spectrum of the signal, calculated for a model composed of a three-state electronic system coupled to a set of displaced harmonic oscillators, depends on the pulse duration. Condition under which the wavepacket motion in the harmonic potential substantially deviates from that of the classical point mass is derived. The Fourier power spectrum has enhanced components with frequencies of harmonics even in a system composed of ideally harmonic potentials. Utility of the Fourier analysis of the spectrum for clarification of the squeezed molecular vibrational state is discussed. Calculated oscillatory behavior in phase of a pump-probe signal, as a function of probe frequency, was discussed in terms of a two-dimensional effect on a pump-probe signal.

Original language | English |
---|---|

Pages (from-to) | 189-199 |

Number of pages | 11 |

Journal | Chemical Physics |

Volume | 341 |

Issue number | 1-3 |

DOIs | |

Publication status | Published - Nov 15 2007 |

Externally published | Yes |

### Fingerprint

### Keywords

- Fourier power spectrum
- Molecular dynamics
- Molecular vibration
- Phase
- Phonon
- Pump-probe spectroscopy
- Transient spectrum
- Ultra-fast phenomena
- Vibrational modes
- Wavepacket

### ASJC Scopus subject areas

- Physics and Astronomy(all)
- Physical and Theoretical Chemistry

### Cite this

**Anomalous phase behavior and apparent anharmonicity of the pump-probe signal in a two-dimensional harmonic potential system.** / Taneichi, T.; Kobayashi, Tatsuo.

Research output: Contribution to journal › Article

*Chemical Physics*, vol. 341, no. 1-3, pp. 189-199. https://doi.org/10.1016/j.chemphys.2007.07.047

}

TY - JOUR

T1 - Anomalous phase behavior and apparent anharmonicity of the pump-probe signal in a two-dimensional harmonic potential system

AU - Taneichi, T.

AU - Kobayashi, Tatsuo

PY - 2007/11/15

Y1 - 2007/11/15

N2 - Discussion on wavelength dependent "anharmonic" effects in a pump-probe signal for a system of wavepacket on one- and two-dimensional harmonic potentials was given. The Fourier power spectrum of the signal, calculated for a model composed of a three-state electronic system coupled to a set of displaced harmonic oscillators, depends on the pulse duration. Condition under which the wavepacket motion in the harmonic potential substantially deviates from that of the classical point mass is derived. The Fourier power spectrum has enhanced components with frequencies of harmonics even in a system composed of ideally harmonic potentials. Utility of the Fourier analysis of the spectrum for clarification of the squeezed molecular vibrational state is discussed. Calculated oscillatory behavior in phase of a pump-probe signal, as a function of probe frequency, was discussed in terms of a two-dimensional effect on a pump-probe signal.

AB - Discussion on wavelength dependent "anharmonic" effects in a pump-probe signal for a system of wavepacket on one- and two-dimensional harmonic potentials was given. The Fourier power spectrum of the signal, calculated for a model composed of a three-state electronic system coupled to a set of displaced harmonic oscillators, depends on the pulse duration. Condition under which the wavepacket motion in the harmonic potential substantially deviates from that of the classical point mass is derived. The Fourier power spectrum has enhanced components with frequencies of harmonics even in a system composed of ideally harmonic potentials. Utility of the Fourier analysis of the spectrum for clarification of the squeezed molecular vibrational state is discussed. Calculated oscillatory behavior in phase of a pump-probe signal, as a function of probe frequency, was discussed in terms of a two-dimensional effect on a pump-probe signal.

KW - Fourier power spectrum

KW - Molecular dynamics

KW - Molecular vibration

KW - Phase

KW - Phonon

KW - Pump-probe spectroscopy

KW - Transient spectrum

KW - Ultra-fast phenomena

KW - Vibrational modes

KW - Wavepacket

UR - http://www.scopus.com/inward/record.url?scp=35948986764&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=35948986764&partnerID=8YFLogxK

U2 - 10.1016/j.chemphys.2007.07.047

DO - 10.1016/j.chemphys.2007.07.047

M3 - Article

AN - SCOPUS:35948986764

VL - 341

SP - 189

EP - 199

JO - Chemical Physics

JF - Chemical Physics

SN - 0301-0104

IS - 1-3

ER -