| 1. |
- Baev, Alexander
(författare)
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Dynamics of optical and X-ray responses of molecules
- 2002
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Licentiatavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The aim of this licentiatethesis is to investigate by means of theoretical simulationsthe dynamics of light scattering by molecules, with specialemphasis on molecules in gas phase and in solutions.The first part of the thesisconcerns the two-photon absorption (TPA) process in the opticalwavelength region. A new dynamical theory for TPA of moleculesin solutions is developed. The roles of collisions with solventparticles, of pulse duration, of saturation effects and ofpropagation effects on the absorbing capacity of nonlinearmedia are analyzed which can promote a choice of new compoundsfor various applications.The second part addresses thesoft X-ray region of exciting light, namely resonant X-rayRaman scattering (RXS). It is shown that collisional dephasingin solutions changes the physics of X-ray scattering. Anadditional, incoherent contribution to the RXS cross sectioncomes into play, resulting in a doubling of the spectrallines.A theoretical analysis ofdissociative resonant photoelectron spectra of homonucleardiatomic molecules is performed. Special attention is paid tothe electron Doppler effect and to the role of the interferencebetween scattering channels on formation of an atomic-like partof the spectra.The quantum oscillatorybehaviour for the vibrational collapse in the resonant Augerdecay of core excited nitrogen molecule is explored. Aone-phonon model is presented which opens a new possibility todetermine the equilibrium bond distance for a core excitedstates.
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| 2. |
- Baev, Alexander, et al.
(författare)
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Metaphotonics : An emerging field with opportunities and challenges
- 2015
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Ingår i: Physics reports. - : Elsevier. - 0370-1573 .- 1873-6270. ; 594, s. 1-60
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Forskningsöversikt (refereegranskat)abstract
- Metaphotonics is an emerging multidisciplinary field that deals with manipulation of electro-magnetic fields in nanoengineered (meta)materials using both electric and magnetic interactions and their cross-coupling. It offers unprecedented control of both linear and nonlinear optical functions for applications ranging from optical switching, to negative- and near-zero refractive index metamaterials, to chiral bioimaging, to cloaking. However, realization of such applications requires physics-guided nanoengineering of appropriate artificial media with electro-magnetic properties at visible and infrared wavelengths that are tailored to surpass those of any naturally-occurring material. Here, we review metaphotonics with a broadened vision and scope, introduce potential applications, describe the role of theoretical physics through multiscale modeling, review the materials development and current status, and outline opportunities in this fertile emerging field.
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| 3. |
- Baev, Alexander, 1974-
(författare)
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Multi-Photon Interactions with a Time Structure
- 2003
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The present thesis concerns aspects of the interaction ofmatter in gas, liquid and solid phases, with electromagneticradiation, ranging from the optical to the X-ray region. Overthe last decade the availability of ultrashort strong laserpulses as well as of high power synchrotron sources of tunableX-ray radiation has stimulated a rapid development of newexperimental techniques which makes it possible to analysedifferent physical, chemical and biological processes inunprecedented detail. All of this urges a concomitantdevelopment of adequate theoretical language and methodscombined with simulation techniques.The first part of the thesis addresses nonlinear propagationof strong optical pulses. This study is motivated by thebreakthrough in synthesis of novel organic materials possessingprespecified nonlinear optical properties and which has led toa multitude of potential applications such as, for example, 3Dimaging and data storage, optical limiting and photodynamiccancer therapy. In order to clarify the underlying physics, astrict solution has been derived of the density matrixequations of a material aiming at an explicit treatment of itsnonlinear polarization without addressing a conventional Taylorexpansion over field amplitudes. Such a formalism is developedfor many-level molecules, allowing to solve the coupledMaxwell's and density matrix equations for the propagation of afew interacting laser pulses through a nonlinear molecularmedium. The theory presented is capable to account formulti-photon processes of an arbitrary order and for differentsaturation effects. The theory is applied to simulations oftwo- and three-photon absorption as well as to upconvertedstimulated emission of organic molecules in solvents.The second part of the thesis is devoted to resonant X-rayRaman scattering from free molecules, solutions and polymerfilms. The temporal analysis of the spectral profiles isperformed using the technique of scattering duration whichallows to select physical processes with different time scales.The slowing-down/speeding-up of the scattering by frequencydetuning provides insight in the formation of the differentparts of the scattering profile like atomic and molecularbands, resonant and vertical scattering channels, anomalousenhancement of the Stokes doubling effect. The lifetimevibrational interference (LVI), playing a crucial role inresonant scattering, is found to strongly influence thedispersion of the Auger resonances of polymers in agreementwith experiment. An almost complete quenching of the scatteringcross section by LVI is observed for the N2molecule. It is found that the interferenceelimination of the scattering amplitude gives valuableinformation on molecular geometry. The electron Doppler effectis minutely studied making use of a wave packet technique. Thesimulations show an "interference burning" of a narrow hole onthe top of the Doppler broadened profile of the Auger spectraof molecular oxygen. For the SF6molecule the Auger Doppler effect is found to besensitive to the detuning due to the scattering anisotropy. Inall of these studies the temporal language was foundconstructive and enormously helpful for understanding theunderlying physical processes. Most theoretical predictionsmade have been verified by experiments.
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| 4. |
- Baev, Alexander, et al.
(författare)
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Optical limiting properties of Zinc- and Platinum-based organometallic compounds
- 2004
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Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 108:36, s. 7406-7416
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Tidskriftsartikel (refereegranskat)abstract
- Optical power limiting is theoretically studied using an approach that combines quantum electronic structure calculations of multiphoton excitations and classical calculations of dynamical wave propagation. We illustrate the capability of such a combined approach by presenting results for a couple of organometallic compounds; basic metal-base porphyrins, vinylphenylamine porhyrin, and the so-called type IVc platinum compound. A comparative analysis of their electronic properties related to nonlinear absorption of electromagnetic radiation and their optical limiting capability has been performed based on dynamical simulations of the nonlinear pulse propagation taking account of resonant as well as off-resonant effects. Several key features and rate-limiting steps in the transmission have been examined in relation to various characteristics of the pulse. It is found that the resonant vs off-resonant conditions, the saturation conditions and the dephasing play critical roles for the nonlinear transmission. The saturation effects are sensitive to the pulse duration, the inter-system crossing rate and the quenching of the higher triplet state. The inter-system crossing rate has to be comparable with the inverse pulse duration in order to boost the stepwise two-photon channel associated with singlet-singlet followed by triplet-triplet transitions. It is illustrated that structure-to-property relations of the rate-limiting steps serve as important criteria for choices of compounds suitable for the application of interest.
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| 5. |
- Baev, Alexander, et al.
(författare)
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Theoretical Simulations of clamping levels in optical power limiting
- 2006
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Ingår i: Journal of Physical Chemistry B. - : American Chemical Society (ACS). - 1520-6106 .- 1520-5207 .- 1520-5215. ; 110:42, s. 20912-20916
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Tidskriftsartikel (refereegranskat)abstract
- Multiphysics modeling, combining quantum mechanical and classical wave mechanical theories, of clamping levels has been performed for a platinum(II) organic compound in a sol-gel glass matrix. A clamping level of 2.5 mu J is found for a pulse duration of 10 ns. The excited-state absorption in the triplet manifold is shown to be crucial for clamping to occur.
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| 6. |
- Baev, Alexander, et al.
(författare)
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Upconverted lasing based on many-photon absorption : an all dynamic description
- 2004
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Ingår i: Journal of the Optical Society of America. B, Optical physics. - 0740-3224 .- 1520-8540. ; 21:2, s. 384-396
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Tidskriftsartikel (refereegranskat)abstract
- A theory is developed for the propagation through a nonlinear medium of strong pump and amplifiedspontaneous-emission pulses. The theory is based on a solution of the density matrix equations that aims at providing an adequate treatment of the nonlinear polarization of the material without addressing the Taylor expansion over the powers of intensity. The theory has been applied for modeling of three-photon absorption induced upconverted stimulated emission of organic molecules in solvents. Numerical results are presented for the organic chromophore 4-[N-(2-hydroxyethyl)-N-(methyl)amino phenyl]-4'-(6-hydroxyhexyl sulfonyl) stilbene dissolved in dimethyl sulfoxide. The results are in good agreement with available experimental results.
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| 7. |
- Carrete, Jesus, et al.
(författare)
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Thermoelectric Properties of Hybrid Organic-Inorganic Superlattices
- 2012
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 116:20, s. 10881-10886
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Tidskriftsartikel (refereegranskat)abstract
- We theoretically evaluate the thermoelectric transport coefficients of hybrid thiophene/SiGe superlattices and the effect of their chemical tuning via phenyl groups. Owing to the interplay between alloy scattering and phonon transmission at the molecular layers, very low thermal conductivities under 1 W/(m K) and values of ZT more than twice as large as those of bulk SiGe can be attained. These results highlight exciting possibilities of organic-inorganic hybrid systems, as compared to traditional inorganic thermoelectrics.
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| 8. |
- Feifel, R., et al.
(författare)
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Generalization of the duration-time concept for interpreting high-resolution resonant photoemission spectra
- 2004
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 69:2, s. 022707-
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Tidskriftsartikel (refereegranskat)abstract
- The duration-time concept, vastly successful for interpreting the frequency dependence of resonant radiative and nonradiative x-ray scattering spectra, is tested for fine-scale features that can be obtained with state of the art high-resolution spectroscopy. For that purpose resonant photoelectron (RPE) spectra of the first three outermost singly ionized valence states X (2)Sigma(g)(+), A (2)Pi(u), and B (2)Sigma(u)(+), are measured for selective excitations to different vibrational levels (up to n=13) of the N 1s-->pi(*) photoabsorption resonance in N-2 and for negative photon frequency detuning relative to the adiabatic 0-0 transition of this resonance. It is found that different parts of the RPE spectrum converge to the spectral profile of direct photoionization (fast scattering) for different detunings, and that the RPE profiles are asymmetrical as a function of frequency detuning. The observed asymmetry contradicts the picture based on the simplified notation of a common scattering duration time, but is shown to agree with the here elaborated concept of partial and mean duration times. Results of the measurements and the simulations show that the duration time of the scattering process varies for different final electronic and different final vibrational states. This owes to two physical reasons: one is the competition between the fast vertical and the slow resonant scattering channels and the other is the slowing down of the scattering process near the zeros of the real part of the scattering amplitude.
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| 9. |
- Feifel, R., et al.
(författare)
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Profile of resonant photoelectron spectra versus the spectral function width and photon frequency detuning
- 2004
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 70:3
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Tidskriftsartikel (refereegranskat)abstract
- The outermost, singly ionized valence state of N-2, the X (2)Sigma(g)(+) state, is investigated in detail as a function of the photon frequency bandwidth for core excitation to the N 1s-->pi(*) resonance, where the photon frequency is tuned in between the first two vibrational levels of this bound intermediate electronic state. We find a strong, nontrivial dependence of the resulting resonant photoemission spectral profile on the monochromator function width and the frequency of its peak position. For narrow bandwidth excitation we observe a well resolved vibrational fine structure in the final electron spectrum, which for somewhat broader bandwidths gets smeared out into a continuous structure. For even broader monochromator bandwidths, it converts again into a well resolved vibrational progression. In addition, spectral features appearing below the adiabatic transition energy of the ground state of N-2(+) are observed for broadband excitation. A model taking into account the interplay of the partial scattering cross section with the spectral function is presented and applied to the X (2)Sigma(g)(+) final state of N-2(+).
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| 10. |
- Feifel, R., et al.
(författare)
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Role of stray light in the formation of high-resolution resonant photoelectron spectra : an experimental and theoretical study of N-2
- 2004
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Ingår i: Journal of Electron Spectroscopy and Related Phenomena. - : Elsevier BV. - 0368-2048 .- 1873-2526. ; 134:1, s. 49-65
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Tidskriftsartikel (refereegranskat)abstract
- We show that the undular stray light, diffusely scattered by the optical system of a synchrotron beamline, can play an important role in the formation of high-resolution resonant photoelectron (RPE) spectra. The influence of the stray light is mediated through the Stokes doubling effect, with the Lorentzian tail of the spectral function being replaced by a more complicated form. This effect is shown to appear in the high-resolution resonant photoelectron spectrum of the N-2 molecule in which the spectral shape of the non-Raman (NR) bands differs qualitatively for the A(2)Pi(u) and X(2)Sigma(g)(+) final states. A particularly large enhancement of the non-Raman Stokes line is observed for the A-state while the picture is inverted for the X-state where the non-Raman band is suppressed. It is shown that the resonant photoemission profile is affected by two qualitatively different detunings, the detuning of the monochromatized line relative to the photoabsorption line and the detuning of the undulator harmonic relative to the same reference line. The experimental data show that the relative intensity of the non-Raman line strongly depends on the tuning of the undulator harmonic with respect to the selected monochromator bandpass, leading to a strong decrease of the Stokes line intensity for certain undulator detunings. A clear red-shift asymmetry for the decrease in the Stokes line intensity is observed when the monochromator line is detuned towards negative photon frequencies, whereas the picture is reverted for the situation of a positively detuned monochromator line. The results show the necessity to control the stray light and to investigate both the Raman and non-Raman contributions to the spectral profiles in order to avoid misinterpretation and in order to make full use of the information available in resonant photoemission spectra of molecules.
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| 11. |
- Fomin, Alexey, et al.
(författare)
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Fiber Laser Intracavity Spectroscopy of hot water for temperature and concentration measurements
- 2015
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Ingår i: Applied Physics B. - : Springer Science and Business Media LLC. - 0946-2171 .- 1432-0649. ; 121:3, s. 345-351
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Tidskriftsartikel (refereegranskat)abstract
- The feasibility of temperature and concentration measurements using near-IR (similar to 1.5 mu m) water spectra obtained by fiber laser intracavity spectroscopy was evaluated. The spectra were registered with water vapor heated in a tubular oven at temperatures between 1000 and 1300 K and in adiabatic flames where temperatures were above 1800 K. Adiabatic flames of methane were stabilized on the heat flux burner. For temperature and concentration evaluation, the observed spectra were fitted by simulated spectra calculated utilizing the HITEMP database. Several discrepancies between HITEMP data and the experiments leading to significant errors in evaluation were found. After small corrections to the database better, accuracy of the temperature (+/- 70 K) and concentration (+/- 20 %) measurements is obtained. A more precise spectroscopic assignment is needed to improve the accuracy of the results.
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| 12. |
- Friedlein, Rainer, et al.
(författare)
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Role of electronic localization and charge-vibrational coupling in resonant photoelectron spectra of polymers : Application to poly(para-phenylenevinylene)
- 2004
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Ingår i: Physical Review B. Condensed Matter and Materials Physics. - 1098-0121 .- 1550-235X. ; 69:12
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Tidskriftsartikel (refereegranskat)abstract
- A combination of x-ray absorption and resonant photoemission (RPE) spectroscopy has been used to study the electronic structure of the one-dimensional conjugated polymer poly (para-phenylenevinylene) in nonordered (as prepared) thin films. The dispersion of RPE features for the decay to localized and delocalized bands are qualitatively different. A theory for band dispersion of RPE in polymers is given, showing the important roles of electronic state localization and vibrational (phonon) excitations for the character of the dispersion.
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| 13. |
- He, Guang S., et al.
(författare)
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Twisted pi-System Chromophores for All-Optical Switching
- 2011
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 133:17, s. 6675-6680
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Tidskriftsartikel (refereegranskat)abstract
- Molecular chromophores with twisted pi-electron systems have been shown to possess unprecedented values of the quadratic hyperpolarizability, beta, with very large real parts and much smaller imaginary parts. We report here an experimental and theoretical study which shows that these twisted chromophores also possess very large values of the real part of the cubic hyperpolarizability, gamma, which is responsible for nonlinear refraction. Thus, for the two-ring twisted chromophore TMC-2 at 775 nm, relatively close to one-photon resonance, n(2) extrapolated to neat substance is large and positive (1.87 x 10(-13) cm(2)/W), leading to self-focusing. Furthermore, the third-order response includes a remarkably low two-photon absorption coefficient, which means minimal nonlinear optical losses: the T factor, alpha(2)lambda/n(2), is 0.308. These characteristics are attributed to closely spaced singlet biradical and zwitterionic states and offer promise for applications in all-optical switching.
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| 14. |
- Jiang, Xiantao, et al.
(författare)
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Two-dimensional MXenes : From morphological to optical, electric, and magnetic properties and applications
- 2020
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Ingår i: Physics reports. - : Elsevier. - 0370-1573 .- 1873-6270. ; 848
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Forskningsöversikt (refereegranskat)abstract
- MXenes, generally referring to two-dimensional (2D) transition-metal carbides, nitrides, and carbonitrides, have received tremendous attention since the first report in 2011. Extensive experimental and theoretical studies have unveiled their enormous potential for applications in optoelectronics, photonics, catalysis, and many other areas. Because of their intriguing mechanical and electronic properties, together with the richness of elemental composition and chemical decoration, MXenes are poised to provide a new 2D nanoplatform for advanced optoelectronics. This comprehensive review, intended for a broad multidisciplinary readership, highlights the state-of-the-art progress on MXene theory, materials synthesis techniques, morphology modifications, opto-electromagnetic properties, and their applications. The efforts exploring the device performance limits, steric configurations, physical mechanisms, and novel application boundaries are comprehensively discussed. The review is concluded with a compelling perspective, outlook as well as non-trivial challenges in future investigation of MXene-based nano-optoelectronics.
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| 15. |
- Kaplan, Alexander, et al.
(författare)
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An analysis of the heat transfer from a moving elliptical cylinder
- 1997
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Ingår i: Journal of Physics D. - : IOP Publishing. - 0022-3727 .- 1361-6463. ; 30, s. 1190-1196
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Tidskriftsartikel (refereegranskat)abstract
- A theoretical analysis of the heat transfer from a moving elliptical cylinder is carried out and general solutions in elliptical coordinates are obtained for aspect ratios β, both β and β. The heat-flux distribution and total heat-flow rate are calculated, investigated for a wide range of parameters and presented graphically. The results obtained are useful for applications concerning thermal processes (laser cutting, welding, heat treatment and so on). A comparison of a moving circular cylinder with a numerical model of laser cutting is considered and discussed.
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| 16. |
- Kimberg, Victor, et al.
(författare)
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Dynamics of cavityless lasing generated by ultrafast multiphoton excitation
- 2006
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 74:3
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 17. |
- Lim, Chang-Keun, et al.
(författare)
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Plasmon-enhanced two-photon-induced isomerization for highly-localized light-based actuation of inorganic/organic interfaces
- 2016
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Ingår i: Nanoscale. - : Royal Society of Chemistry. - 2040-3364 .- 2040-3372. ; 8:7, s. 4194-4202
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Tidskriftsartikel (refereegranskat)abstract
- Two-photon initiated photo-isomerization of an azobenzene moiety adsorbed on silver nanoparticles (Ag NPs) is demonstrated. The azobenzene is linked to a materials-binding peptide that brings it into intimate contact with the Ag NP surface, producing a dramatic enhancement of its two-photon absorbance. An integrated modeling approach, combining advanced conformational sampling with Quantum Mechanics/Capacitance Molecular Mechanics and response theory, shows that charge transfer and image charges in the Ag NP generate local fields that enhance two-photon absorption of the cis isomer, but not the trans isomer, of adsorbed molecules. Moreover, dramatic local field enhancement is expected near the localized surface plasmon resonance (LSPR) wavelength, and the LSPR band of the Ag NPs overlaps the azobenzene absorbance that triggers cis to trans switching. As a result, the Ag NPs enable two-photon initiated cis to trans isomerization, but not trans to cis isomerization. Confocal anti-Stokes fluorescence imaging shows that this effect is not due to local heating, while the quadratic dependence of switching rate on laser intensity is consistent with a two-photon process. Highly localized two-photon initiated switching could allow local manipulation near the focal point of a laser within a 3D nanoparticle assembly, which cannot be achieved using linear optical processes.
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| 18. |
- Macak, Peter, et al.
(författare)
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Two-photon excitations in molecules
- 2003
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Ingår i: Non-linear optical responses of molecules,solids and liquids: Methods and applications. - : Plenum Publishing.
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Bokkapitel (refereegranskat)abstract
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| 19. |
- Reddy, I. V. A. K., et al.
(författare)
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Pulsed response theory prediction of ZnO nanocluster polarizabilities : A benchmark study
- 2021
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Ingår i: Chemical Physics Letters. - : Elsevier. - 0009-2614 .- 1873-4448. ; 778
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Tidskriftsartikel (refereegranskat)abstract
- Motivated by the interest in zinc oxide nanostructures and their properties, we calculate in this work molecular polarizabilities and hyperpolarizabilities of a series of zinc oxide nanoclusters using modern response theory in the form of damped and pulsed response for both Hartree-Fock and DFT reference states. We show that as the size of the cluster grows, both real and imaginary parts of polarizability, computed with these two distinct approaches, asymptotically converge. We also show the importance of eliminating the dangling bonds in small clusters for predicting the correct trend in the values of the HOMO/LUMO gap. Finally, we calculate the hyperpolarizability tensors, associated with the second order nonlinear optical effects, in the hexagonal (wurtzite) phase of ZnO nanoclusters and demonstrate a highly nonlinear growth of this quantity with the cluster size.
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| 20. |
- Rinkevicius, Zilvinas, et al.
(författare)
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Novel Pathways for Enhancing Nonlinearity of Organics Utilizing Metal Clusters
- 2010
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Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 114:28, s. 7590-7594
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Tidskriftsartikel (refereegranskat)abstract
- We show that ultrasmall metallic nanoparticles can be combined with large second- and third-order response organic chromophores to enhance the overall third-order response of the system. This approach can be used in combination with microscopic cascading to generate exceptionally large third-order response. Intermolecular charge-transfer coupling between the molecules and the metal clusters enhances the real part of the nonlinearity at telecommunication wavelengths, while avoiding plasmonic enhancement of one- and two-photon absorption, and minimizing optical losses. The results of density functional calculations for a molecule with large second-order response, (para)nitroaniline, show that use of a gold cluster as a link between molecular entities enhances third-order nonlinearity. Varying size and shape of the metal cluster as well as the distance between the clusters and the molecules allows fine-tuning of nonlinear response over a large range of magnitudes.
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| 21. |
- Ågren, Hans, et al.
(författare)
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Multiphysics modelling of optical materials
- 2006
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Ingår i: Optical Materials in Defence Systems Technology III. - BELLINGHAM, WA : SPIE-INT SOC OPTICAL ENGINEERING. - 9780819464996 ; , s. U8-U24
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Konferensbidrag (refereegranskat)abstract
- We review multiphysics modeling of pulse propagation in non-linear media and highlight some recent applications on optical materials containing organic or organometallic chromophores.
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