Two-photon excitation spectroscopy of 1,5--Diphenyl-1,3,5-hexatriene using phase modulation

We have used two-photon Fourier transform spectroscopy to investigate the first singlet excited state (S1) of a prototypical polyene molecule 1,5 -- Diphenyl-1,3,5-hexatriene. As the S1 state in the polyenes is a one-photon forbidden transition, its structure of the vibrational levels cannot be studied using resonant linear excitation. Although this level is accessible with two-photon excitation, previous studies done by using wavelength tunable pulsed lasers did not have enough resolution to investigate the details of the vibrational levels. In Fourier transform spectroscopy, one uses a pair of laser beams to excite the sample. The measurements are done by varying the time delay between the pulses. The spectral resolution is given by the inverse of the maximum time delay rather than the spectral width of the pulses. We have used the method to investigate the vibrational levels of the S1 state. In our implementation, we have used a phase modulation technique to carry out the measurements in the rotating frame, which require fewer data points along the time delay thereby significantly reducing the measurement time

Direct Measurement of Fast Transients by Using Boot-strapped Waveform Averaging

An approximation to coherent sampling, also known as boot-strapped waveform averaging, is presented. The method uses digital cavities to determine the condition for coherent sampling. It can be used to increase the effective sampling rate of a repetitive signal and the signal to noise ratio simultaneously. The method is demonstrated by using it to directly measure the fluorescence lifetime from rhodamine 6G by digitizing the signal from a fast avalanche photodiode. The obtained lifetime of 4.4+-0.1 ns is in agreement with the known values

The nature of relaxation processes revealed by the action signals of phase modulated light fields

We introduce a generalized theoretical approach to study action signals induced by the absorption of two-photons from two phase modulated laser beams and subject it to experimental testing for two types of photoactive samples, solution of rhodamine 6G and GaP photodiode. In our experiment, the phases of the laser beams are modulated at the frequencies f1 and f2, respectively. The action signals, such as photoluminescence and photocurrent, which result from the absorption of two photons, are isolated at frequencies m f (f=|f1-f2|, m=0,1,2...). We demonstrate that the ratio of the amplitudes of the secondary (m=2) and the primary (m=1) signals is sensitive to the type of relaxation process taken place in the system and thus can be used for its identification. Such sensitivity originates from cumulative effects of non-equilibrated state of the system between the light pulses. When the cumulative effects are small, i.e. the relaxation time is much shorter then the laser repetition rate or the laser intensity is high enough to dominate the system behavior, the ratio achieves its reference value 1:4 (the signature of two-photon absorption). In the intermediate regimes the ratio changes rapidly with the growth of intensity from zero value in case of second order relaxation process, while it demonstrates slow monotonic decrease for linear relaxation. In the article we also determine the value of the recombination rate in a GaP photodiode by using the above approach

Probing Silicon Carbide with Phase-Modulated Femtosecond Laser Pulses: Insights into Multiphoton Photocurrent

Wide bandgap semiconductors are widely used in photonic technologies due to their advantageous features, such as large optical bandgap, low losses, and fast operational speeds. Silicon carbide is a prototypical wide bandgap semiconductor with high optical nonlinearities, large electron transport, and a high breakdown threshold. Integration of silicon carbide in nonlinear photonics requires a systematic analysis of the multiphoton contribution to the device functionality. Here, multiphoton photocurrent in a silicon carbide photodetector is investigated using phase-modulated femtosecond pulses. Multiphoton absorption is quantified using a 1030 nm phase-modulated pulsed laser. Our measurements show that although the bandgap is less than the energy of three photons, only four-photon absorption has a significant contribution to the photocurrent. We interpret the four-photon absorption as a direct transition from the valance to the conduction band at the {\Gamma} point. More importantly, silicon carbide withstands higher excitation intensities compared to other wide bandgap semiconductors making it an ideal system for high-power nonlinear applications.Comment: 14 pages, 4 figure

Compressed Sensing for Reconstructing Coherent Multidimensional Spectra

We apply two sparse reconstruction techniques, the least absolute shrinkage and selection operator (LASSO) and the sparse exponential mode analysis (SEMA), to two-dimensional (2D) spectroscopy. The algorithms are first tested on model data, showing that both are able to reconstruct the spectra using only a fraction of the data required by the traditional Fourier-based estimator. Through the analysis of a sparsely sampled experimental fluorescence detected 2D spectra of LH2 complexes, we conclude that both SEMA and LASSO can be used to significantly reduce the required data, still allowing to reconstruct the multidimensional spectra. Of the two techniques, it is shown that SEMA offers preferable performance, providing more accurate estimation of the spectral line widths and their positions. Furthermore, SEMA allows for off-grid components, enabling the use of a much smaller dictionary than the LASSO, thereby improving both the performance and lowering the computational complexity for reconstructing coherent multidimensional spectra

Effects of impurity band on multiphoton photocurrent from InGaN and GaN photodetectors

Multiphoton absorption of wide band-gap semiconductors has shown great prospects in many fundamental researches and practical applications. With intensity-modulated femtosecond lasers by acousto-optic frequency shifters, photocurrents and yellow luminescence induced by two-photon absorption of InGaN and GaN photodetectors are investigated experimentally. Photocurrent from InGaN detector shows nearly perfect quadratic dependence on excitation intensity, while that in GaN detector shows cubic and higher order dependence. Yellow luminescence from both detectors show sub-quadratic dependence on excitation intensity. Highly nonlinear photocurrent from GaN is ascribed to absorption of additional photons by long-lived electrons in traps and impurity bands. Our investigation indicates that InGaN can serve as a superior detector for multiphoton absorption, absent of linear and higher order process, while GaN, which suffers from absorption by trapped electrons and impurity bands, must be used with caution

Molecular properties of astaxanthin in water/ethanol solutions from computer simulations

Astaxanthin (AXT) is a reference model of xanthophyll carotenoids, which is used in medicine and food industry, and has potential applications in nanotechnology. Because of its importance, there is a great interest in understanding its molecular properties and aggregation mechanism in water and mixed solvents. In this paper, we report a novel model of AXT for molecular dynamics simulation. The model is used to estimate different properties of the molecule in pure solutions and in water/ethanol mixtures. The calculated diffusion coefficients of AXT in pure water and ethanol are (3.22+/- 0.01)10^{-6} cm^{2}s^{-1} and (2.7+/-0.4) 10^{-6} cm^{2}s^{-1}, respectively. Our simulations also show that the content of water plays a clear effect on the morphology of the AXT aggregation in water/ethanol mixture. In up to 75\% (v/v) water concentration, loosely connected network of dimers and trimers, and two-dimensional array structures are observed. At higher water concentrations, AXT molecules form more compact three-dimensional structures that are preferentially solvated by the ethanol molecules. The ethanol preferential binding and the formation of a well connected hydrogen bonding network on these AXT clusters, suggest that such preferential solvation can play an important role in controlling the aggregate structure

High Precision Measurements Using High Frequency Signals

Generalized lock-in amplifiers use digital cavities with Q-factors as high as 5X10^8. In this letter, we show that generalized lock-in amplifiers can be used to analyze microwave (giga-hertz) signals with a precision of few tens of hertz. We propose that the physical changes in the medium of propagation can be measured precisely by the ultra-high precision measurement of the signal. We provide evidence to our proposition by verifying the Newton's law of cooling by measuring the effect of change in temperature on the phase and amplitude of the signals propagating through two calibrated cables. The technique could be used to precisely measure different physical properties of the propagation medium, for example length, resistance, etc. Real time implementation of the technique can open up new methodologies of in-situ virtual metrology in material design

Increasing the density of modes in an optical frequency comb by cascaded four-wave mixing in a nonlinear optical fiber

Here, it is shown that when two optical frequency combs with identical mode spacing but different offset frequencies copropagate through a nonlinear optical fiber, four-wave mixing between them generates new modes. Although the spacings between the new modes depend on the difference of the offset frequencies, they appear irregular because of the large number of possible four-wave-mixing processes. However, when the difference in the offset frequencies is an integer fraction of the mode spacing of the original combs, the cascaded four-wave mixing generates a new comb with a fixed mode spacing given by the difference in the offset frequencies. This process can be used to substantially increase the mode density of a frequency comb. The method can be used in conjunction with new sources of frequency combs, such as quantum cascade lasers and microresonators, which have large mode spacing of tens of GHz. Decreasing the mode spacing of such sources is likely to increase their applicability