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Physical review. B, Condensed matter

Cooperative optical absorption

Theodore D. Holstein, R. Orbach, S. Alexander

Published Oct 15, 1982• 11 citations
Publisher

Abstract

We demonstrate that vibrational overtone (second-harmonic) absorption must be treated as a resonance in the presence of vibrational two-exciton band excitations, as outlined earlier by two of us (T.H. and R.O.) in a manuscript with Luiz C. Scavarda do Carmo and Fritz L\"uty. Explicit calculations are made for a three-dimensional body-centered cubic and a one-dimensional lattice. The behavior of the position and intensity of the overtone absorption with exciton bandwidth and vibrational anharmonicity is studied in detail. Substantial cooperative vibrational absorption intensity is seen to be inconsistent with significant overtone splitting on the scale of the cooperative vibrational absorption bandwidth. Because no extrinsic impurity is required to provide a matrix element for two-exciton absorption, we suggest that the exciton band absorption associated with overtone absorption may be a very clean technique to observe exciton dispersion in solids.

DOI
10.1103/physrevb.26.4721

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On The Excitonic Absorption Of CuCl Microcrystallites In A Glass Matrix Under High Resonant Excitation Conditions

P. Gilliot, J.‐C. Merle, Michele Robino +1 more

We present new experimental results concerning the optical nonlinearities of CuCl microcrystallites embedded in a glass matrix. Using a "pump and probe" technique, the induced absorption is measured in the spectral range of the Z3 exciton. We observe two phenomena: first, a bleaching of the excitonic resonance accompanied by the generation of a new absorption band at higher photon energies when the test probes the sample during the pump pulse; secondly, a weak shift of the excitonic resonance towards higher photon energies when probing the sample during and after the pump excitation. We vary the intensity and the photon energy of the pump beam as well as the delay between the pump and the probe pulses. Thus we can show that the pump beam populates excitonic states, which leads to a complete bleaching of the excitonic absorption. In addition, excitons can be created at higher energies, inducing the new absorption band. Its energy depends on the number of states already occupied in the microcrystallites. The shift of the excitonic resonance, on the contrary, can be explained by the heating of the microcrystallites through this high population of excitons and its non radiative decay during and after the excitation pulse.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Dec 22, 1989•4 citations
We demonstrate that vibrational overtone (second-harmonic) absorption must be treated as a resonance in the presence of vibrational two-exciton band excitations, as outlined earlier by two of us (T.H. and R.O.) in a manuscript with Luiz C. Scavarda do Carmo and Fritz L"uty. Explicit calculations are made for a three-dimensional body-centered cubic and a one-dimensional lattice. The behavior of the position and intensity of the overtone absorption with exciton bandwidth and vibrational anharmonicity is studied in detail. Substantial cooperative vibrational absorption intensity is seen to be inconsistent with significant overtone splitting on the scale of the cooperative vibrational absorption bandwidth. Because no extrinsic impurity is required to provide a matrix element for two-exciton absorption, we suggest that the exciton band absorption associated with overtone absorption may be a very clean technique to observe exciton dispersion in solids.
We examine the third-overtone absorption of diatomic molecules in the presence of a tunable field in near-third-overtone resonance using a one-dimensional anharmonic-oscillator model. We find that the tunable mode causes modulation of the absorption as a result of an intensity-induced quenching effect. At high intensities the absorption diminishes accompanied with the disappearance of the modulation. Our investigations also show that these effects are insensitive to the dephasing of the interaction.
Abstract The amplitudes and the excitation profiles of coherent resonant Raman scattering (coherent anti‐Stokes and Stokes Raman scattering (CARS and CSRS)) by impurity centers in crystals and/or molecules in solutions are studied, taking into account the coherence of the excited mode and the inhomogeneity of the environment. The CARS and CSRS excitation profiles can directly be related to one‐photon absorption when using the transform theory known from spontaneous resonant Raman scattering. The enlargement of the amplitude of the active mode reveals itself in an enhancement of the vibrational overtones. At large amplitudes, a splitting in the profiles caused by the contribution of two turning points of a strong coherent vibration is observed. The inhomogeneous broadening is different in the excitation profiles of CARS and CSRS. The overlapping contributions to spectrally narrow and broad transitions lead to Fano peculiarities. The effects are illustrated by model calculations. Copyright © 2011 John Wiley & Sons, Ltd.
We present new experimental results concerning the optical nonlinearities of CuCl microcrystallites embedded in a glass matrix. Using a "pump and probe" technique, the induced absorption is measured in the spectral range of the Z3 exciton. We observe two phenomena: first, a bleaching of the excitonic resonance accompanied by the generation of a new absorption band at higher photon energies when the test probes the sample during the pump pulse; secondly, a weak shift of the excitonic resonance towards higher photon energies when probing the sample during and after the pump excitation. We vary the intensity and the photon energy of the pump beam as well as the delay between the pump and the probe pulses. Thus we can show that the pump beam populates excitonic states, which leads to a complete bleaching of the excitonic absorption. In addition, excitons can be created at higher energies, inducing the new absorption band. Its energy depends on the number of states already occupied in the microcrystallites. The shift of the excitonic resonance, on the contrary, can be explained by the heating of the microcrystallites through this high population of excitons and its non radiative decay during and after the excitation pulse.