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Phase-sensitive wave-packet dynamics caused by a breakdown of the rotating-wave approximation
KTH, Skolan för bioteknologi (BIO).ORCID-id: 0000-0003-1269-8760
KTH, Skolan för bioteknologi (BIO), Teoretisk kemi (stängd 20110512).
KTH, Skolan för bioteknologi (BIO), Teoretisk kemi (stängd 20110512).
KTH, Skolan för bioteknologi (BIO), Teoretisk kemi (stängd 20110512).
2006 (engelsk)Inngår i: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 73, nr 2, artikkel-id 023409Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

The water dimer driven by strong infrared field is studied in the two-vibrational mode approximation. A pump pulse excites the OH vibrational modes and creates a coherent superposition of vibrational states of the low-frequency OO mode. The solution of the Schrodinger equation in the adiabatic approximation shows a strong sensitivity of the OO vibrational wave-packet dynamics to the absolute phase of the pump field. This effect appears due to a break down of the rotating-wave approximation when the Rabi frequency of the OH vibrational transition approaches the frequency of the OH mode. The violation of the rotating wave approximation modifies considerably the interaction of the probe radiation with the laser-driven molecule.

sted, utgiver, år, opplag, sider
2006. Vol. 73, nr 2, artikkel-id 023409
Emneord [en]
Approximation theory, Infrared radiation, Laser pulses, Nonlinear equations, Water
HSV kategori
Identifikatorer
URN: urn:nbn:se:kth:diva-5491DOI: 10.1103/PhysRevA.73.023409ISI: 000235668100132Scopus ID: 2-s2.0-33144456310OAI: oai:DiVA.org:kth-5491DiVA, id: diva2:9874
Merknad

QC 20100825

Tilgjengelig fra: 2006-03-15 Laget: 2006-03-15 Sist oppdatert: 2017-11-21bibliografisk kontrollert
Inngår i avhandling
1. Pulse Propagation in Nonlinear Media and Photonic Crystals
Åpne denne publikasjonen i ny fane eller vindu >>Pulse Propagation in Nonlinear Media and Photonic Crystals
2006 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

The present thesis is devoted to theoretical studies of pulse propagation of light through linear and nonlinear media, and of light-induced nuclear dynamics.

The first part of the thesis addresses propagation of light pulses in linear periodical media - photonic crystals. The main accent was put on studies of the angular properties of two qualitatively different types of photonic crystals: holographic photonic crystals, and impurity band based photonic crystals. The anisotropy of band structure, group velocity and pulse delay with respect to the light polarization are analyzed.

In the second part of the thesis a strict theory of nonlinear propagation of a few strong interacting light beams is presented. The key idea of this approach is a self-consistent solution of the nonlinear wave equation and the density matrix equations of the material. This technique is applied to studies of dynamics of cavityless lasing generated by ultra-fast multi-photon excitation. It is shown that interaction of co- and counter-propagating pulses of amplified spontaneous emission (ASE) affects the dynamics and efficiency of nonlinear conversion. Our dynamical theory allows to explain the asymmetric spectral properties of the forward and backward ASE pulses, which were observed in recent experiment with different dye molecules. It is shown that the ASE spectral profile changes drastically when the pump intensity approaches the threshold level. The effect of the temporal self-pulsation of ASE is studied in detail.

The third part of the thesis is devoted to light-induced nuclear dynamics. Time- and frequency-resolved X-ray spectroscopy of molecules driven by strong and coherent infrared (IR) pulses shows that the phase of the IR field strongly influences the trajectory of the nuclear wave packet, and hence, the X-ray spectrum. Such a dependence arises due to the interference of one (X-ray) and two-photon (X-ray + IR) excitation channels. The phase of the light influences the dynamics also when the Rabi frequency approaches the vibrational frequency, breaking down the rotating-wave approximation. The probe X-ray spectra are also sensitive to the delay time, the duration, and the shape of the pulses. The evolution of the nuclear wave packets in the dissociative core-excited state affects the dynamics of resonant Auger scattering from fixed-in-space molecules. One of the important dynamical effects is the atomic-like resonance which experiences electronic Doppler shift. We predict that the scattering of the Auger electrons by nearby atoms leads to new Doppler shifted resonances. These extra resonances show sharp maxima in the bond directions, which makes them very promising as probes for local molecular structure using energy and angular resolved electron-ion coincidence techniques. Our theory provides prediction of several new effects, but also results that are in good agreement with the available experimental data.

sted, utgiver, år, opplag, sider
Stockholm: KTH, 2006. s. x, 49
Emneord
Photonic Crystals, Nonlinear optics, X-ray spectroscopy
HSV kategori
Identifikatorer
urn:nbn:se:kth:diva-3886 (URN)91-7178-275-3 (ISBN)
Disputas
2006-03-31, FB42, AlbaNova, Roslagstullsbaken 21, Stockholm, 10:00
Opponent
Veileder
Merknad
QC 20100906Tilgjengelig fra: 2006-03-15 Laget: 2006-03-15 Sist oppdatert: 2011-11-23bibliografisk kontrollert

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