Spectroscopy heterodyne detection technique

The description of pump-probe signals presented in the preceding section can be immediately generalized to heterodyne-detected transient grating spectroscopy as well as to other four-wave mixing techniques. Heterodyne detection involves mixing the scattered field with an additional heterodyne field 4(r). The signal in the ks direction can then be written in terms of the polarization Ts(t) as... 

The following section contains a more detailed treatment of the theory behind the nonresonant spectroscopy of liquids. This will be followed by a description of the experimental implementation and data analysis techniques for a common OKE scheme, optical-heterodyne-detected Raman-induced Kerr-effect spectroscopy (22). We will then discuss the application of this technique to the study of the temperature-dependent dynamics of simple liquids composed of symmetric-top molecules. 

In this contribution we present two laser spectroscopic methods that use coherent resonance Raman scattering to detect rf-or laser -induced Hertzian coherence phenomena in the gas phase these novel coherent double resonance techniques for optical heterodyne detection of sublevel coherence clearly extend the above mentioned previous methods using incoherent light sources. In the case of Doppler broadened optical transitions new signal features appear as a result of velocity-selective optical excitation caused by the narrow-bandwidth laser. We especially analyze the potential and the limitations of the new detection schemes for the study of collision effects in double resonance spectroscopy. In particular, the effect of collisional velocity changes on the Hertzian resonances will be investigated. 

Besides various detection mechanisms (e.g. stimulated emission or ionization), there exist moreover numerous possible detection schemes. For example, we may either directly detect the emitted polarization (oc PP, so-called homodyne detection), thus measuring the decay of the electronic coherence via the photon-echo effect, or we may employ a heterodyne detection scheme (oc EP ), thus monitoring the time evolution of the electronic populations In the ground and excited electronic states via resonance Raman and stimulated emission processes. Furthermore, one may use polarization-sensitive detection techniques (transient birefringence and dichroism spectroscopy ), employ frequency-integrated (see, e.g. Ref. 53) or dispersed (see, e.g. Ref. 54) detection of the emission, and use laser fields with definite phase relation. On top of that, there are modern coherent multi-pulse techniques, which combine several of the above mentioned options. For example, phase-locked heterodyne-detected four-pulse photon-echo experiments make it possible to monitor all three time evolutions inherent to the third-order polarization, namely, the electronic coherence decay induced by the pump field, the djmamics of the system occurring after the preparation by the pump, and the electronic coherence decay induced by the probe field. For a theoretical survey of the various spectroscopic detection schemes, see Ref. 10. 

A new technique to measure low-frequency spectra is optical-heterodyne-detected Raman-induced Kerr-effect spectroscopy (OHD-RIKES). A recent publication by Chang and Cast-ner contains references to previous work within this field [18]. OHD-RIKES is based on a four-wave mixing of femtosecond laser pulses. Spectra obtained by OHD-RIKES reflect the anisotropic part of the Raman polarizability. Thus, the information obtained by OHD-RIKES is very similar to that obtained by low-frequency Raman scattering in an scattering configuration. From a theoretical point of view, the spectral representation obtained from OHD-RIKES measurements corresponds to the I v) representation given in Eq. (3). In Fig. 4 is shown an OHD-RIKES spectrum of liquid A-methylformamide (NMF). In Fig. 5 are shown low-frequency Raman spectra of liquid NMF together with the R(i>),... 

According to the literature, narrow band detection in the THz regime often involves heterodyne techniques or Fourier transform spectroscopy, both of which require exotic supplementary hardware. " Our tuned detector involves just a few modifications to the... 

New absorption methods, like intracavity spectroscopy, cavity-ring-down and cavity-enhanced spectroscopy, have demonstrated very high sensitivities in laboratory measurements with DLs. An ultrasensitive technique that combines external cavity enhancement and FM spectroscopy has been developed recently. This method, which has been called NICE-OHMS. or noise-immune cavity-enhanced optical heterodyne molecular spectroscopy, is based on frequency modulation of the laser at the cavity free-spectral-range frequency or its multiple. The MDA of 5x 10 1 X 10 cm ) in the detection of narrow... 

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