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Physical Review A

Relationship between second-harmonic generation and electric-field-induced second-harmonic generation

Raanan Bavli, Y. B. Band

Published Jan 1, 1991• 23 citations
Publisher

Abstract

We calculate the electric-field-induced second-harmonic-generation (EFISH) susceptibility of a homogeneously broadened two-level system with permanent dipole moments. This susceptibility has contributions from the second-harmonic-generation (SHG) susceptibility of the same system without the presence of a dc field and the four-wave-mixing (FWM) component of the susceptibility ${\ensuremath{\gamma}}_{\mathit{e}}$(-2\ensuremath{\omega};\ensuremath{\omega},\ensuremath{\omega},0). The magnitude and phase of the various contributions to EFISH arising from SHG and from FWM depend on the frequency of the fundamental optical field, the transition dipole moment ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}$, the permanent dipole moment of the ground-state level ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{a}}$, and the difference of the ground- and excited-state dipole moments \ensuremath{\Delta}\ensuremath{\mu}. We present non-rotating-wave-approximation results for both the quasi-steady-state in systems where the dephasing time ${\mathit{T}}_{2}$ is much shorter than the population decay time ${\mathit{T}}_{1}$, so the polarization is in a steady state but the population is not, and for the complete steady state. Extraction of the SHG susceptibility from EFISH measurements is considered.

DOI
10.1103/physreva.43.507

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Nonlinear Dynamics in Optical Systems•Jan 1, 1990•0 citations
We calculate the electric-field-induced second-harmonic-generation (EFISH) susceptibility of a homogeneously broadened two-level system with permanent dipole moments. This susceptibility has contributions from the second-harmonic-generation (SHG) susceptibility of the same system without the presence of a dc field and the four-wave-mixing (FWM) component of the susceptibility \ensuremathγe{\ensuremath{\gamma}}_{\mathit{e}}\ensuremathγe​(-2\ensuremath{\omega};\ensuremath{\omega},\ensuremath{\omega},0). The magnitude and phase of the various contributions to EFISH arising from SHG and from FWM depend on the frequency of the fundamental optical field, the transition dipole moment \ensuremathμab{\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}\ensuremathμab​, the permanent dipole moment of the ground-state level \ensuremathμaa{\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{a}}\ensuremathμaa​, and the difference of the ground- and excited-state dipole moments \ensuremath{\Delta}\ensuremath{\mu}. We present non-rotating-wave-approximation results for both the quasi-steady-state in systems where the dephasing time T2{\mathit{T}}_{2}T2​ is much shorter than the population decay time T1{\mathit{T}}_{1}T1​, so the polarization is in a steady state but the population is not, and for the complete steady state. Extraction of the SHG susceptibility from EFISH measurements is considered.
We calculate the third-order nonlinear absorption and dispersion (self-phase-modulation and cross-phase modulation) of a homogeneously broadened two-level molecular system with permanent dipole moments interacting with (1) an optical field of frequency \ensuremath{\omega}, and (2) two optical fields of frequency ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$, i.e., the susceptibilities ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-\ensuremath{\omega};\ensuremath{\omega},-\ensuremath{\omega},\ensuremath{\omega}) and ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-${\mathrm{\ensuremath{\omega}}}_{1}$;${\mathrm{\ensuremath{\omega}}}_{1}$,-${\mathrm{\ensuremath{\omega}}}_{2}$,${\mathrm{\ensuremath{\omega}}}_{2}$). Sharp features in the nonlinear absorption and dispersion appear whenever one- or two-photon resonance conditions are met. Only features corresponding to one-photon resonance arise if the difference between the permanent dipole moments of the levels, \ensuremath{\Delta}\ensuremath{\mu}, vanishes. The ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-\ensuremath{\omega};\ensuremath{\omega},-\ensuremath{\omega},\ensuremath{\omega}) spectrum has two features, one at frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$ dominated by contributions proportional to ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}^{4}$, where ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}$ is the transition dipole moment of the two levels with transition frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$, and the other at frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$/2 dominated by contributions proportional to (\ensuremath{\Delta}\ensuremath{\mu})2{)}^{2})2${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}^{2}$. Sharp features in ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-${\mathrm{\ensuremath{\omega}}}_{1}$;${\mathrm{\ensuremath{\omega}}}_{2}$,-${\mathrm{\ensuremath{\omega}}}_{2}$,${\mathrm{\ensuremath{\omega}}}_{1}$) appear when ${\mathrm{\ensuremath{\omega}}}_{2}$ is near ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$,${\mathrm{\ensuremath{\omega}}}_{1}$,${\mathrm{\ensuremath{\omega}}}_{1}$+${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$, and \ensuremath{\Vert}${\mathrm{\ensuremath{\omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$\ensuremath{\Vert}.
The interaction between radiation and a two-level molecular system in the presence of permanent dipole moments is analyzed. It is found that the nonzero difference between permanent dipoles induces a polarization that oscillates at frequencies /spl omega/, 2/spl omega/, 3/spl omega/, etc., where /spl omega/ is the frequency of the electromagnetic field resonant with the two-level system. An analysis of the propagation equation of the harmonics shows that even harmonics are amplified while odd harmonics are absorbed.
We calculate the sum- and difference-frequency-generation (SFG and DFG) susceptibilities, ${\mathrm{\ensuremath{\chi}}}^{(2)}$(-(${\mathrm{\ensuremath{\omega}}}_{1}$+${\mathrm{\ensuremath{\omega}}}_{2}$);${\mathrm{\ensuremath{\omega}}}_{1}$,${\mathrm{\ensuremath{\omega}}}_{2}$) and ${\mathrm{\ensuremath{\chi}}}^{(2)}$(-(${\mathrm{\ensuremath{\omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{2}$);${\mathrm{\ensuremath{\omega}}}_{1}$,-${\mathrm{\ensuremath{\omega}}}_{2}$), of a homogeneously broadened two-level system with permanent dipole moments in the presence of pump fields at frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$. Both SFG and DFG susceptibilities have two maxima at frequencies corresponding to the one- and two-photon resonances of the two-level system. Knowledge of the magnitude of one of the maxima of either SFG or DFG is sufficient for determining the magnitude of the second peak of that process and also the two peaks of the other process. In both processes the peak at the two-photon resonance has dominant contributions arising from off-diagonal elements of the density matrix. The interference between these contributions is constructive in SFG and destructive in DFG. Therefore, SFG is more efficient at the two-photon resonance than DFG. An expression for the ratio between these peaks is obtained. The peak of the spectrum of each process corresponding to the one-photon resonance has two main contributions, one of which is diagonal and the other off diagonal. In DFG the interference between the two contributions is constructive and in SFG the interference is destructive. Hence, DFG is more efficient in the vicinity of the one-photon resonance. However, since the off-diagonal contributions to SFG and DFG on the one-photon resonance are equal in magnitude (and differ by a phase difference of \ensuremath{\sim}\ensuremath{\pi}) the efficiencies of the two processes are equal when the duration of the pulses is comparable to or shorter than T1{\mathit{T}}_{1}T1​.
Properties of the resonance peaks associated with the non-degenerate four-wave mixing signal in a two-level molecular system with non-zero permanent dipole moments are studied in the space defined by the pump ( omega 1 ) and probe ( omega 2 ) frequencies. An analytical expression for the Fourier components of the nonlinear homogeneous macroscopic polarization are obtained, where the terms responsible for the oscillation (at frequency omega 3 =2 omega 1 - omega 2 ) of the populations and coherences are also identified. Topological properties of the resulting nonlinear spectra are studied in frequency space using three-dimensional curves and contour plots. We have additionally identified the dominant contributions of the coherence and/or population that determine the intensity and the spectral linewidth. The critical quantities for the present analysis are the transition and permanent dipole moments when the rotating-wave approximation (RWA) is not considered.
The theory of three wave mixing was formulated in a classic paper by Armstrong, Bloembergen, Ducuing, and Pershan over 25 years ago.1 A theoretical description of three wave mixing for multimode time-dependent input fields (as opposed to cw single frequency time independent input fields) has recently been presented.2 Analytic solutions were developed for die time-dependent intensities of the output fields. These solutions differ dramatically from those for single-mode fields. New frequencies in the sum-frequency output spectrum and in the input-field output spectrum are created and grow in magnitude as the input intensities are increased. The output spectrum broadens under conditions of strong nonlinear coupling, ultimately reaching the phasematched bandwidth limit. Here, we review the results presented in Ref. 2 for sum frequency generation (SFG) and explicidy compare these results with those for second harmonic generation (SHG). We show that SHG cannot be described as a limit of the SFG formalism for multimode fields. The SFG formulation for the interaction of photons close to frequency ω1 with photons close to frequency ω2 producing photons close to frequency ω 3= ω 1+ ω 2 does not allow ω1(ω2) photons to interact with each other to produce photons close to frequency 2ω1(2ω2). This self interaction is crucial for SHG and must be incorporated. Therefore, a separate formulation is used to describe SHG with multimode input fields.