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Pulse Propagation in Nonlinear Media and Photonic Crystals
KTH, Skolan för bioteknologi (BIO).ORCID-id: 0000-0003-1269-8760
2006 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
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.

Ort, förlag, år, upplaga, sidor
Stockholm: KTH , 2006. , s. x, 49
Nyckelord [en]
Photonic Crystals, Nonlinear optics, X-ray spectroscopy
Nationell ämneskategori
Teoretisk kemi
Identifikatorer
URN: urn:nbn:se:kth:diva-3886ISBN: 91-7178-275-3 (tryckt)OAI: oai:DiVA.org:kth-3886DiVA, id: diva2:9877
Disputation
2006-03-31, FB42, AlbaNova, Roslagstullsbaken 21, Stockholm, 10:00
Opponent
Handledare
Anmärkning
QC 20100906Tillgänglig från: 2006-03-15 Skapad: 2006-03-15 Senast uppdaterad: 2011-11-23Bibliografiskt granskad
Delarbeten
1. Angular properties of band structures in one-dimensional holographic photonic crystals
Öppna denna publikation i ny flik eller fönster >>Angular properties of band structures in one-dimensional holographic photonic crystals
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2004 (Engelska)Ingår i: Journal of Optics. A, Pure and applied optics, ISSN 1464-4258, E-ISSN 1741-3567, Vol. 6, nr 10, s. 991-996Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

One-dimensional photonic crystals with continuous distribution of the dielectric constant were fabricated by the use of photopolymer materials and laser holography. The angular dependence of light propagation through the system was studied experimentally and theoretically. It is shown that the Brewster angles for different bands are different, in contrast to the conventional two-layer Bragg reflector with a step-like distribution of the dielectric constant. Comparison of the theory with experimental data allowed us to define the parameters of the hologram-the dielectric contrast and the shrinkage of the structure.

Ort, förlag, år, upplaga, sidor
Institute of Physics Publishing (IOPP), 2004
Nyckelord
photonic crystal, holographic lithography, photonic band gap, materials
Nationell ämneskategori
Annan fysik
Identifikatorer
urn:nbn:se:kth:diva-5483 (URN)10.1088/1464-4258/6/10/009 (DOI)000224970900010 ()2-s2.0-6344237670 (Scopus ID)
Anmärkning

QC 20100830 QC 20110922

Tillgänglig från: 2006-03-15 Skapad: 2006-03-15 Senast uppdaterad: 2017-11-21Bibliografiskt granskad
2. Angular anisotropy of the delay time of short pulses in impurity band based photonic crystals
Öppna denna publikation i ny flik eller fönster >>Angular anisotropy of the delay time of short pulses in impurity band based photonic crystals
2005 (Engelska)Ingår i: Journal of Optics. A, Pure and applied optics, ISSN 1464-4258, E-ISSN 1741-3567, Vol. 7, nr 3, s. 118-122Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

We investigate the transmission of short pulses through one-dimensional impurity band based photonic crystals. We found a strong dependence of the delay time on the angle of incidence. The delay time is larger for larger incident angles for the transverse electrical mode, while the delay time of the transverse magnetic mode has a qualitatively different angular dependence, especially in the region below the Brewster angle. The strong anisotropy of the delay time is traced to the anisotropy of the group velocity which is directly related to the angular dependence of the impurity band structure.

Nyckelord
photonic crystal, impurity band, optical delay lines
Nationell ämneskategori
Annan fysik
Identifikatorer
urn:nbn:se:kth:diva-5484 (URN)10.1088/1464-4258/7/3/004 (DOI)000228114600004 ()2-s2.0-14844322820 (Scopus ID)
Anmärkning
QC 20100830Tillgänglig från: 2006-03-15 Skapad: 2006-03-15 Senast uppdaterad: 2017-11-21Bibliografiskt granskad
3. Nonlinear propagation of strong multi-mode fields
Öppna denna publikation i ny flik eller fönster >>Nonlinear propagation of strong multi-mode fields
2003 (Engelska)Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics, ISSN 0953-4075, E-ISSN 1361-6455, Vol. 36, s. 3761-3774Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

We develop a strict theory of nonlinear propagation of few interacting stronglight beams. The key idea of our approach is a self-consistent solution ofthe nonlinear wave equation and the density matrix equations of the materialbeyond the rotatory wave approximation. We assume a Fourier expansion ofthe density matrixwhich goes beyond the conventionalTaylor expansions of thepolarization over the field amplitudeswhich is inadequate for the field strengthsthat we are interested in. Two qualitatively different situations are considered,with and without phase matching. Unlike in our previous paper (Baev et al2003 J. Opt. Soc. Am. B at press) devoted to the three-photon (TP) absorptioninduced upconverted lasing, we obtain here a strict solution for the nonlinearinteraction between different light beams. The general theory is applied to anumerical study of the role of saturation in TP photoabsorption by an organicchromophore in solution.

Nyckelord
2-photon excitation, absorption, dynamics, memory, pulses, media
Nationell ämneskategori
Teoretisk kemi
Identifikatorer
urn:nbn:se:kth:diva-5485 (URN)10.1088/0953-4075/36/18/305 (DOI)000185966200006 ()
Anmärkning
QC 20100906Tillgänglig från: 2006-03-15 Skapad: 2006-03-15 Senast uppdaterad: 2017-11-21Bibliografiskt granskad
4. Bi-directional description of amplified spontaneous emission induced by three-photon absorption
Öppna denna publikation i ny flik eller fönster >>Bi-directional description of amplified spontaneous emission induced by three-photon absorption
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2005 (Engelska)Ingår i: Journal of the Optical Society of America. B, Optical physics, ISSN 0740-3224, E-ISSN 1520-8540, Vol. 22, nr 2, s. 385-393Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

 A semiclassical dynamic theory of the nonlinear propagation of a few interacting intense light pulses is applied to study the nonlinear counterpropagation of amplified spontaneous emission (ASE) induced by three-photon absorption of short intense laser pulses in a chromophore solution. Several important results from the modeling are reached for the ASE process developing in the regime of strong saturation. Accounting for ASE in both forward and backward directions with respect to the pump pulse results in a smaller efficiency of nonlinear conversion for the forward ASE compared with the case in which forward emission is considered alone, something that results from the partial repump of the absorbed energy to the backward ASE component; the overall efficiency is nevertheless higher than for the forward emission considered alone. The efficiency of nonlinear conversion of the pump energy to the counterpropagating ASE pulses is strongly dependent on the concentration of active molecules so that a particular combination of concentration versus cell length optimizes the conversion coefficient. Under certain specified conditions, the ASE effect is found to be oscillatory; the origin of oscillations is dynamical competition between stimulated emission and off-resonant absorption. This result can be considered one of the possible explanations of the temporal fluctuations of the forward ASE pulse [Nature 415, 767 (2002)].

Nyckelord
Laser pulses, Light absorption, Light propagation, Mathematical models, Maxwell equations, Optical frequency conversion, Optical materials, Optical pumping, Oscillations, Photons, Spontaneous emission, Wave equations
Nationell ämneskategori
Fysik
Identifikatorer
urn:nbn:se:kth:diva-5486 (URN)10.1364/JOSAB.22.000385 (DOI)000226967800012 ()2-s2.0-15044350805 (Scopus ID)
Anmärkning
QC 20100901Tillgänglig från: 2006-03-15 Skapad: 2006-03-15 Senast uppdaterad: 2017-11-21Bibliografiskt granskad
5. Dynamics of cavityless lasing generated by ultrafast multiphoton excitation
Öppna denna publikation i ny flik eller fönster >>Dynamics of cavityless lasing generated by ultrafast multiphoton excitation
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2006 (Engelska)Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 74, nr 3, artikel-id 033814Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

A dynamical theory is developed with the purpose of explaining recent experimental results on multiphoton-excited amplified stimulated emission (ASE). Several conspicuous features of this experiment are analyzed, like the threshold dependence of the spectral profile on the pump intensity, and spectral shifts of the ASE pulses co- and counterpropagating relative to the pump pulse. Two models are proposed and evaluated, one based on the isolated molecule and another which involves solvent interaction. The spectral shift between the forward and backward ASE pulses arises in the first model through the competition between the ASE transitions from the pumped vibrational levels and from the bottom of the excited-state well, while in the solvent-related model the dynamical solute-solvent interaction leads to a relaxed excited state, producing an additional ASE channel. In the latter model the additional redshifted ASE channel makes the dynamics of ASE essentially different from that in the molecular model because the formation of the relaxed state takes a longer time. The variation of the pump intensity influences strongly the relative intensities of the different ASE channels and, hence, the spectral shape of ASE in both models. The regime of ASE changes character when the pump intensity crosses a threshold value. Such a phase transition occurs when the ASE rate approaches the rate of vibrational relaxation or the rate of solute-solvent relaxation in the first excited state.

Nyckelord
Cavitation; Electric excitation; Laser applications; Mathematical models; Optical pumping; Photons; Solvents; Stimulated emission; Vibration control; Amplified stimulated emission (ASE); Multiphoton excitation; Solute-solvent relaxation; Vibrational relaxation; Ultrafast phenomena
Nationell ämneskategori
Biokemi och molekylärbiologi
Identifikatorer
urn:nbn:se:kth:diva-6994 (URN)10.1103/PhysRevA.74.033814 (DOI)000241067100139 ()2-s2.0-33748950997 (Scopus ID)
Anmärkning

QC 20100813. Tidigare titel: Dynamics of cavityless lasing generated by ultra-fast multi-photon excitation. Titel ändrad 20100813.

Tillgänglig från: 2007-04-20 Skapad: 2007-04-20 Senast uppdaterad: 2017-12-14Bibliografiskt granskad
6. Self-sustained pulsation of amplified spontaneous emission of molecules in solution
Öppna denna publikation i ny flik eller fönster >>Self-sustained pulsation of amplified spontaneous emission of molecules in solution
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2006 (Engelska)Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics, ISSN 0953-4075, E-ISSN 1361-6455, Vol. 39, nr 2, s. 215-227Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Temporal oscillations of amplified spontaneous emission of molecules are studied theoretically. From the proposed theory and numerical simulations, it is found that the self-pulsations originate in an interplay between stimulated emission and saturable absorption. A stability analysis demonstrates the crucial role of the photoabsorption in this process, which can be regulated by a proper choice of buffer molecules. Variations in the saturable absorption mediate a transition from damped oscillations to self-sustained pulsations. The role of propagation effects as well as of the interaction of co- and counter-propagating pulses is also investigated. Numerical simulations, demonstrating the theoretical findings, are performed for a model 3-level system and for an organic chromophore; 4-[N-(2-hydroxyethyl)-N-(methyl)amino phenyl]-4'-(6-hydroxyhexyl sulphonyl) stilbene.

Nyckelord
Computer simulation; Damping; Light absorption; Mathematical models; Molecular dynamics; Oscillations; Stimulated emission; Buffer molecules; Damped oscillations; Self-sustained pulsation; Stability analysis; Spontaneous emission
Nationell ämneskategori
Industriell bioteknik
Identifikatorer
urn:nbn:se:kth:diva-5488 (URN)10.1088/0953-4075/39/2/002 (DOI)000235457800005 ()2-s2.0-29144478864 (Scopus ID)
Anmärkning
QC 20100813Tillgänglig från: 2006-03-15 Skapad: 2006-03-15 Senast uppdaterad: 2017-11-21Bibliografiskt granskad
7. Two-color phase-sensitive x-ray pump-probe spectroscopy
Öppna denna publikation i ny flik eller fönster >>Two-color phase-sensitive x-ray pump-probe spectroscopy
2004 (Engelska)Ingår i: Phys. Rev. A, ISSN 1050-2947, Vol. 70, s. 062504-Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

X-ray pump-probe spectroscopy is studied theoretically. It is shown that two-color-optical+x-ray-excitation with constant phase of the pump radiation exhibits strong interference between the one- and two-photon excitation channels. This effect is found to be large for both long and short pump pulses, while the interference vanishes for x-ray pulses longer than one cycle of the pump field. It is predicted that the spectral shape of x-ray absorption is strongly influenced by the absolute phase of the pump light. A strong sensitivity of the x-ray absorption and/or photoionization profile to the phase and detuning of the pump field is predicted, as well as to the duration of the x-ray pulse. Our simulations display oscillations of x-ray absorption as a function of the delay time. This effect allows the synchronization of the x-ray pulse relative to the "comb" of the pump radiation. The interference pattern copies the temporal and space distribution of the pump field. We pay special attention to the role of molecular orientation for the interference effect.

Nyckelord
absorption spectroscopy; excited lithium; laser; photoionization; molecules; pulses; dynamics; fields; states; atoms
Nationell ämneskategori
Teoretisk kemi
Identifikatorer
urn:nbn:se:kth:diva-5489 (URN)10.1103/PhysRevA.70.062504 (DOI)000226418900058 ()2-s2.0-42749106716 (Scopus ID)
Anmärkning
QC 20100825Tillgänglig från: 2006-03-15 Skapad: 2006-03-15 Senast uppdaterad: 2010-09-06Bibliografiskt granskad
8. Phase sensitive x-ray absorption driven by strong infrared fields
Öppna denna publikation i ny flik eller fönster >>Phase sensitive x-ray absorption driven by strong infrared fields
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2005 (Engelska)Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 71, nr 4, artikel-id 043407Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

In this paper it is demonstrated that electron vibrational absorption of molecules driven by strong IR field provides rich physical interpretations of dynamical processes on a short time scale. The phase of an infrared field influences strongly the trajectory of the nuclear wave packet and the probing spectrum. It is shown that the probe spectrum keeps memory of the infrared phase even after that the pump field left the system. The phase effect takes maximum value when the duration of the probe pulse is of the order of the infrared field period, and can be enhanced by a proper control of the duration and intensity of the pump pulse. The phase effect is different for oriented and disordered molecules and depends strongly on the intensity of pump radiation. It can be an effective tool to study charge transfer processes like proton transfer in hydrogen bonded networks.

Nyckelord
synchrotron-radiation; laser; pulses; molecules
Nationell ämneskategori
Teoretisk kemi
Identifikatorer
urn:nbn:se:kth:diva-5490 (URN)10.1103/PhysRevA.71.043407 (DOI)000228752700085 ()2-s2.0-26944469351 (Scopus ID)
Anmärkning

QC 20100825

Tillgänglig från: 2006-03-15 Skapad: 2006-03-15 Senast uppdaterad: 2017-11-21Bibliografiskt granskad
9. Phase-sensitive wave-packet dynamics caused by a breakdown of the rotating-wave approximation
Öppna denna publikation i ny flik eller fönster >>Phase-sensitive wave-packet dynamics caused by a breakdown of the rotating-wave approximation
2006 (Engelska)Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 73, nr 2, artikel-id 023409Artikel i tidskrift (Refereegranskat) 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.

Nyckelord
Approximation theory, Infrared radiation, Laser pulses, Nonlinear equations, Water
Nationell ämneskategori
Teoretisk kemi
Identifikatorer
urn:nbn:se:kth:diva-5491 (URN)10.1103/PhysRevA.73.023409 (DOI)000235668100132 ()2-s2.0-33144456310 (Scopus ID)
Anmärkning

QC 20100825

Tillgänglig från: 2006-03-15 Skapad: 2006-03-15 Senast uppdaterad: 2017-11-21Bibliografiskt granskad
10. Structure determination through measurements of Doppler-split Augerresonances in fixed-in-space molecules
Öppna denna publikation i ny flik eller fönster >>Structure determination through measurements of Doppler-split Augerresonances in fixed-in-space molecules
2004 (Engelska)Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 69, nr 2, s. 020501(R)-Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Auger resonances of dissociating atoms in randomly oriented molecules experience large electronic Dopplershifts. We predict that when fixed-in-space molecules are considered there will appear extra Doppler resonancesresulting from the diffractional scattering of the Auger electrons by the surrounding atoms. Theseresonances show sharp maxima in bond directions, something that makes them very promising as probes forlocal molecular structure using current energy- and angular-resolved electron-ion coincidence experiments.

Nyckelord
FEMTOSECOND DISSOCIATION, ANGULAR-DISTRIBUTION, ELECTRONS, SPECTRA, DECAY
Nationell ämneskategori
Teoretisk kemi
Identifikatorer
urn:nbn:se:kth:diva-5492 (URN)10.1103/PhysRevA.69.020501 (DOI)000189386300003 ()2-s2.0-1942540520 (Scopus ID)
Anmärkning
QC 20100906Tillgänglig från: 2006-03-15 Skapad: 2006-03-15 Senast uppdaterad: 2017-11-21Bibliografiskt granskad
11. X-ray Doppler spectroscopy of ultrafast fragmentation
Öppna denna publikation i ny flik eller fönster >>X-ray Doppler spectroscopy of ultrafast fragmentation
2004 (Engelska)Ingår i: Chemical Physics, ISSN 0301-0104, E-ISSN 1873-4421, Chem. Phys., Vol. 299, s. 253-258Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Doppler effects are now commonly observed for Auger resonances of dissociating atoms in randomly oriented molecules. The physics behind the, yet not observed, Doppler effect for fixed-in-space molecules is different in that there will appear extra Doppler resonances resulting from the diffractional scattering of the Auger electrons by the surrounding atoms. It is argued that as these resonances will show maxima in the bond directions their measurement by current energy and angular resolved electron-ion coincidence experiments will provide structural probing. It is also shown that the electronic Doppler effect caused by nuclear vibrations can be observed also for bound nuclear states making use of electron-ion coincidence measurements. Optimal conditions for such measurements prevail when the scattering duration is comparable with a vibrational period.

Nyckelord
33.70.Ca; 33.80.Eh; 34.50.Gb; Doppler effect; Ultrafast fragmentation; X-ray spectroscopy
Nationell ämneskategori
Teoretisk kemi
Identifikatorer
urn:nbn:se:kth:diva-5493 (URN)10.1016/j.chemphys.2003.11.017 (DOI)000220525200012 ()2-s2.0-1642414131 (Scopus ID)
Anmärkning
QC 20100906Tillgänglig från: 2006-03-15 Skapad: 2006-03-15 Senast uppdaterad: 2017-11-21Bibliografiskt granskad

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