Shift Of Cavity Modes Research Articles

Strong coupling-induced frequency shifts of highly detuned photonic modes in multimode cavities.

Strong coupling between light and molecules is a fascinating topic exploring the implications of the hybridization of photonic and molecular states. For example, many recent experiments have explored the possibility that strong coupling of photonic and vibrational modes might modify chemical reaction rates. In these experiments, reactants are introduced into a planar cavity, and the vibrational mode of a chemical bond strongly couples to one of the many photonic modes supported by the cavity. Some experiments quantify reaction rates by tracking the spectral shift of higher-order cavity modes that are highly detuned from the vibrational mode of the reactant. Here, we show that the spectral position of these cavity modes, even though they are highly detuned, can still be influenced by strong coupling. We highlight the need to consider this strong coupling-induced frequency shift of cavity modes if one is to avoid underestimating cavity-induced reaction rate changes. We anticipate that our work will assist in the re-analysis of several high-profile results and has implications for the design of future strong coupling experiments.

Self-calibrated NICE-OHMS based on an asymmetric signal: theoretical analysis and experimental validation.

As an ultra-sensitive detection technique, the noise-immune cavity enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) technique has great potential for assessment of the concentration of trace gases. To determine gas concentrations at the ppt or lower level with high accuracy, it is desirable that the technique exhibits self-calibration (or calibration-free) capabilities. Although being sensitive, NICE-OHMS has so far not demonstrated any such ability. To remedy this, this paper provides a self-calibrated realization of NICE-OHMS that is based on a switching of the feedback target of the DeVoe-Brewer (DVB) locking procedure from the modulation frequency of the frequency modulation spectroscopy (FMS) to the cavity length, which creates an asymmetrical signal whose form and size can be used to unambiguously assess the gas concentration. A comprehensive theoretical model for self-calibrated NICE-OHMS is established by analyzing the shift of cavity modes caused by intracavity absorption, demonstrating that gas absorption information can be encoded in both the laser frequency and the NICE-OHMS signal. To experimentally verify the methodology, we measure a series of dispersion signals under different levels of absorbance using a built experimental setup. An instrument factor and the partial pressure are obtained by fitting the measured signal through theoretical expressions. Our results demonstrate that fitted values are more accurate for higher partial pressures than for lower. To improve on the accuracy at low partial pressures, it is shown that the instrument factor obtained by fitting the signal at large partial pressures (in this case, above 7.8 µTorr) can be set to a fixed value for all fits. By this, the partial pressures can be assessed with a relative error below 0.65%. This technique has the potential to enable calibration-free ultra-sensitive gas detection.

Ultrafast Lasing Dynamics in a CsPbBr3 Perovskite Microplate

The perovskite microlaser is a competitive candidate of light source for optical communication and integrated photonic circuits. Understanding the fundamental mechanism of lasing is crucial for the upcoming devices. The ultrafast establishment of lasing modes within a 2D perovskite microplate cavity at room temperature is investigated. The transient red shift of lasing modes can be found. Analysis based on electron–hole plasma (EHP) and a dynamic Drude‐like model are carried out with simulations on the transient dielectric response and the mode shift. In addition, the integrated lasing gain profile have a red shift at high excitation intensity, which is explained with EHP‐induced bandgap renormalization. The conflict between the experimental phenomena and the exciton–polariton theory confirms that under intense excitation, the exciton–polariton is ruled out for the origin of lasing. These results provide a direct understanding of the lasing evolving in a 2D perovskite microcavity. Suppressing the EHP‐related transient shift of cavity modes will advance the lasing applications.

Measurement of molecular absorption spectrum with a laser locked on a high-finesse cavity

High-resolution and high-sensitivity molecular spectroscopy is widely used in fundamental molecular physics, atmospheric studies, remote sensing, industrial process monitoring, and medical diagnostics. Accurate determination of the parameters of molecule absorption lines, such as line positions, line strengths, line widths and profiles, is essential to support these studies and applications. For example, in order to retrieve the column density of carbon dioxide with a precision of one part per million (ppm), we need laboratory data of line positions with a uncertainty lower than 0.3 MHz and line intensities with a relative accuracy better than 0.5%. Here we present precision spectroscopy of molecules using a laser locked with a high-finesse cavity. The cavity made of invar is thermo-stabilized to reduce the drifts of its length and the cavity mode frequencies. The frequency of the probe laser is locked on a longitudinal mode of the cavity by using the Pound-Drever-Hall method. Another beam from the probe laser, which is frequency shifted and on resonance with a nearby longitudinal mode of the cavity, is used for cavity ring-down spectrum (CRDS) measurement. The CRDS absorption spectrum is recorded by stepping the modulation frequency of a fiber electro-optic modulator in increment of the mode spacing of the cavity. Note that the cavity mode frequencies are shifted due to the dispersion introduced by the absorption lines. Prior to the CRDS measurements, the transmittance spectra of the cavity modes are recorded by scanning the probe laser frequencies over the resonance, which allows the determination of the cavity mode frequencies with an accuracy at a Hz level. Therefore, a dispersion spectrum is also obtained using the same setup by measuring the frequency shifts of cavity modes of the samples with and without absorption. The absolute frequency of the probe laser is determined by an optical frequency comb referring to a GPS-disciplined rubidium clock. The long term drift of beat frequency between the optical frequency comb and the probe laser is measured to be about 1.8 MHz per hour, which is consistent with the thermal expansion of the cavity under a temperature drift of 50 mK. The performance of the spectrometer is demonstrated by measuring the Doppler-broadened spectra of CO2 around 6470.42 cm-1. Precise spectroscopic parameters are derived from both the absorption and dispersion spectra recorded by the same spectrometer. The line position is determined with an accuracy of 0.18 MHz, which is over one order of magnitude better than those given in previous studies and spectral databases.

Ultrafast photoinduced shift of cavity modes in semiconductor microcavity under femtosecond excitations

Ultrafast photoinduced changes of interference (cavity) modes frequencies in ZnSe films on metal substrates were investigated by femtosecond pump-supercontinuum probe spectroscopy. For the pumping energy below the energy gap of ZnSe the laser pulse excites mainly electrons of the metal, i.e. the boundary of the cavity. Nonequilibrium carriers of the metal penetrate into ZnSe film through the Schottky electron barrier and change dielectric function of the semiconductor microcavity. Photoinduced changes in the boundary condition and in optical thickness of the microcavity lead to observable ultrafast shifts of cavity modes with time less the time for establishment of the Fabry-Perot cavity modes. (© 2005 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)