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The Journal of Chemical Physics

Weakly chirped pulses in frequency resolved coherent spectroscopy

Niklas Christensson, Yuri Avlasevich, Arkady P. Yartsev, Kläus Müllen, Torbjörn Pascher, Tõnu Pullerits

Published May 7, 2010• 16 citations
Publisher

Abstract

The role of weakly chirped pulses (time bandwidth product, DeltanuDeltatau<0.61) on three-pulse photon echo signals has been systematically studied. Pulses with varying chirp were characterized with frequency resolved optical gating (FROG) and used to measure spectrally resolved three-pulse photon echoes of a dye in solution. The weakly chirped pulses give rise to markedly different echo signals for population times below approximately 100 fs. The chirped pulses can decrease or enhance spectral signatures of an excited state absorption transition in the echo signal. Furthermore, the observed dephasing dynamics depend on the phase of the electric fields. Simulations based on a three-level model and the electric fields retrieved from the FROG traces give a good agreement for photon echo experiments with both transform limited and chirped pulses. The simulations also allow for a numerical investigation of effects of chirp in two-dimensional spectroscopy. For a two-level system, the chirped pulses result in nonelliptical two-dimensional spectra that can erroneously be interpreted as spectral heterogeneity with frequency dependent dephasing dynamics. Furthermore, chirped pulses can give rise to "false" cross peaks when strong vibrational modes are involved in the system-bath interaction.

DOI
10.1063/1.3404402

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The role of weakly chirped pulses (time bandwidth product, DeltanuDeltatau<0.61) on three-pulse photon echo signals has been systematically studied. Pulses with varying chirp were characterized with frequency resolved optical gating (FROG) and used to measure spectrally resolved three-pulse photon echoes of a dye in solution. The weakly chirped pulses give rise to markedly different echo signals for population times below approximately 100 fs. The chirped pulses can decrease or enhance spectral signatures of an excited state absorption transition in the echo signal. Furthermore, the observed dephasing dynamics depend on the phase of the electric fields. Simulations based on a three-level model and the electric fields retrieved from the FROG traces give a good agreement for photon echo experiments with both transform limited and chirped pulses. The simulations also allow for a numerical investigation of effects of chirp in two-dimensional spectroscopy. For a two-level system, the chirped pulses result in nonelliptical two-dimensional spectra that can erroneously be interpreted as spectral heterogeneity with frequency dependent dephasing dynamics. Furthermore, chirped pulses can give rise to "false" cross peaks when strong vibrational modes are involved in the system-bath interaction.
Optical dephasing of a cyanine dye chromophore in solution is investigated by time-gated photon echo spectroscopy in a three-pulse scattering geometry. The third-order polarization response is gated by up-conversion with a reference pulse in a nonlinear optical crystal. Time gating establishes two controllable periods of system evolution in an optical coherence. The measurements are compared with numerical simulations employing the measured OKE spectrum of solvent (butanol, DMSO) fluctuations. The time-shift of the time-gated echo signals for several gating forming pulse time delays agrees with simulation while the narrower simulated widths suggest a frequency-dependent solute-solvent interaction and the consideration of chromophore vibronic transitions.
A theoretical analysis is carried out for the recently developed three-pulse photon echo spectroscopy employing dual frequency combs (DFC) as the light sources. In this method, the molecular sample interacts with three pulse trains derived from the DFC, and the generated third-order signal is displayed as a two-dimensional (2D) spectrum that depends on the waiting time introduced by employing the asynchronous optical sampling method. Through the analysis of the heterodyne-detected signal interferogram using a local oscillator derived from one of the optical frequency combs, we show that the 2D spectrum closely matches the spectrum expected from a conventional approach with four pulses derived from a single femtosecond laser pulse, and the waiting time between the second and third field-matter interactions is given by the down-converted detection time of the interferogram. The theoretical result is applied to a two-level model system with solvation effect described by solvatochromic spectral density. The model 2D spectrum reproduces spectral features such as the loss of frequency correlation, dephasing, and spectral shift as a function of the population time. We anticipate that the present theory will be the general framework for quantitative descriptions of DFC-based nonlinear optical spectroscopy.
It is predicted that linearly chirped optical excitation pulses give rise to photon echoes whose shortness is limited only by the total material bandwidth that contributes to the echo signal. The photon echo process acts as a frequency-dependent optical delay line whose dispersion is determined by the chirp rate of the excitation pulses rather than by their bandwidth. Consequently, long and short pulses can be compressed with equal facility without complicated alignment procedure. Accumulated echoes have similar properties and can be used with trains of weak excitation pulses.
Atomic spectroscopy using broadband ultrashort laser pulses with durations in the 100-fs range seems nearly impossible because the large bandwidth of the pulses exceeds the line-width of atomic transitions by several orders of magnitude. Therefore the energy loss of ultrashort pulses crossing a narrow-linewidth medium is very low, even if the center frequency of the pulses is tuned to the transition frequency. For instance, the total absorption of a 100-fs pulse centered at the D/sub 2/-absorption line of Rb near 780 nm is well below 10/sup -3/ if the pulse is sent through a 75-mm-long Rb vapor cell at room temperature. Much more information can be obtained by measurement of the change of the pulse phase rather than the pulse energy after the pulse has crossed the medium. We found that a measurement technique similar to previously published second harmonic generation (SHG) frequency-resolved optical gating (FROG) is very convenient for that purpose. In our first experiments we send light pulses with a duration of 100 fs, a Fourier-limited bandwidth of 10 nm, and a pulse energy of 1 nJ through a 75-mm long Rb vapor cell. The pulses were analyzed with use of a SHG-FROG system composed on a single shot correlator and dispersive optics that depicted temporal and spectral information as two-dimensional images on a CCD sensor. The SHG-FROG signals depended strongly on the Rb vapor pressure inside the cell, which was controlled by the cell temperature. While these experiments analyzed steady states, the new technique principally allows the monitoring of transient states as well. We present first results on the investigation of optical pumped material.
We will demonstrate that four-wave mixing with linearly chirped (phase-modulated) pulses is a unique tool for obtaining information on the dynamics and level structure of a system. Especially, it will be shown that the transient-grating-scattering type of experiment with chirped pulses provides an immediate answer to the question of whether the dynamics of a system occurs on a fast and/or slow time scale. In addition, we present compelling evidence that chirped four-wave mixing in a molecular system is a viable method for measuring excited-state vibrational frequencies. Double-sided Feynman diagrams are used for a third-order perturbative calculation of two-level four-wave-mixing effects and chirped coherent Raman scattering. The diagrams provide a visual representation of the quantum-mechanical pathways that the system can take as a result of the different field interactions. The number of quantum-mechanical pathways that contribute to the signal is shown to depend on the chirp rate compared to the time scale(s) of the system dynamics. A stochastic model is used to describe the optical dynamics of the system. The resulting expressions for the third-order nonlinear polarization are so complex that numerical calculations are necessary to simulate the time dependence of the optical response. It will also be shown that our theoretical results in the appropriate limits converge to those obtained for impulsive or continuous-wave excitation.
We investigate the precision of estimating the interaction strength between a two-level system (TLS) and a single-photon pulse when the latter is subject to chirping. We consider linear, quadratic, and sinusoidal temporal phases applied to Gaussian and exponential temporal profiles. At the asymptotic time, when the TLS has fully decayed to its ground state, the fundamental precision depends solely on the magnitude of its spectral amplitude. For quadratically phase-modulated Gaussian pulses, this is entirely determined by the spectral bandwidth. We provide expressions for evaluating the fundamental precision for general temporal profiles and phase modulations. Finally, we show that experimentally feasible mode-resolved measurements are optimal, or close to it, for chirped, pulsed single-photon spectroscopy. Published by the American Physical Society 2024