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International Conference on Ultrafast Phenomena

Photon-echo spectroscopy with 5-fs pulses

Maxim S. Pshenichnikov, Andrius Baltuška, Douwe A. Wiersma

Published Jan 1, 2000• 0 citations
Publisher

Abstract

The formalism for transient photon-echo spectroscopy with extremely short laser pulses that consist of only a few optical cycles is discussed. The pure dephasing time of the hydrated electron is measured as ~1.6 fs which is consistent with the absorption line width.
DOI
10.1364/up.2000.mc4

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International Conference on Ultrafast Phenomena•Jan 1, 1996•0 citations
Summary form only given. A very high temporal resolution and a broad bandwidth are but two advantages provided by the use of extremely short sub-5-fs pulses in a nonlinear spectroscopic experiment. However, the applicability of the standard theoretical description becomes questionable for the pulses that consist merely of a couple of optical oscillations. Far instance, the conventionally employed slowly varying envelope approximation, implying that the change of the pulse amplitude on the duration of an optical cycle is negligible compared to the magnitude of the amplitude itself, can no longer be maintained. Furthermore, the phase-matching bandwidth that is limited due to dispersion in the nonlinear medium rapidly gains importance with the increase of the spectral width of the pulse. Another point of serious concern is the frequency-dependent variation in the sensitivity of signal photodetectors. In combination, these features result in what is known as a spectral-filter effect. Finally, artificial lengthening of the experimental transients is a direct consequence of the noncollinear geometry employed in spectroscopic experiments. We present a theoretical analysis which thoroughly reexamines the formalism of ultrafast photon echo spectroscopy. We obtain a general expression for the echo signal, which is valid even for single-cycle-pulse applications. The derived formalism is applied to photon-echo spectroscopy on the hydrated electron with 5-fs pulses.
Until now all reported studies of transient spectroscopy with incoherent light, including photon echo and pump-probe spectroscopy, were concerned with two-level systems where quasi-monochromatic light of only one frequency couples the two levels.[1-4] However, there exist various coherent transient phenomena where light of two or more frequencies are concerned, and time resolution of the transient spectroscopies using these phenomena are also expected to be limited not by the duration of used light pulses but by the correlation time of the radiation fields.[5]
Recently we have reported[1] on the measurements of electronic dephasing (T_2) and radiationless decay (T_1) in molecules using emission spectroscopy as a probe for the detection of the photon echo. This right-angle photon echo utilizes a single mode of a narrow-band (~MHz) cw dye laser and an intracavity electro-optical (EO) element that modulates the frequency of the laser.[2] Applying voltage pulses into the EO crystal switches the laser frequency from ω_0 (the peak frequency of the transition resonance) into another frequency ω. This switching procedure introduced by Brewer et al. for the observation of transients in the forward direction of the laser allows one to observe coherent transients in gases,[1,2] solids[3-5] and molecular beams.[6] Typically, the dispersion of the nonlinear EO crystal (e.g., AD*P) gives a 60 MHz frequency shift within the inhomogeneous resonance of the optical transition (width ~GHz or larger). Therefore, to switch the laser frequency further, one must use high-voltage signals that are usually hard to obtain especially for multiple-pulse experiments. Secondly, there is a limit on the frequency shift which is conditioned by the mode spacing of the cavity. Thirdly, because the laser is switched into a new group of molecules some complications may arise in interpreting the transient spectra especially in large molecules. This is because in large molecules the density of excited states is high and thus the buildup of transients of w molecules (which could be complex) will be superimposed on the decay of ω_0 molecules. Finally, off-resonance effects (e.g., beats) between the molecules at frequency ω and ω_0 cannot be avoided.
We report on phase-locked optical coherence experiments on the 10 fs timescale. While optical-phase sensitive experiments have been contemplated [1] and performed in the past on a 100 fs timescale [2], exploration of their true potential had to wait for the right fs laser to appear on the scene. It turns out that the almost ideal laser to perform these very subtle phase-locked experiments is the (cavity-dumped) mode-locked Ti:sapphire laser. This laser is capable not only of generating pulses of 10 fs or less [3], but exhibits also little amplitude noise, which is an important characteristics for stabilisation schemes based on an feedback loop. In our group we have gone one step further: our 13-fs cavity-dumped laser [4] and experimental set-up now functions under complete control of a PC computer such that fs photon echo experiments can be done uninterrupted for days if not weeks.