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International Conference on Ultrafast Phenomena

Phase-locked femtosecond photon echo: A new dimension in ultrafast spectroscopy

Douwe A. Wiersma, Wim P. de Boeij, Maxim S. Pshenichnikov

Published Jan 1, 1996• 0 citations

Abstract

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.

DOI: 10.1364/up.1996.wd.1

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Phase-Locked Photon Echoes at 10-fs Time Scale

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Phase-locked optical coherence experiments were performed on the 10 fs time scale. A 13 fs cavity-dumped Ti:sapphire laser was considered as an ideal source to extend these experiments to the 10 fs time scale due to extremely high amplitude and spectral stability. Femtosecond phase-locked heterodyne detected femtosecond stimulated photon echo (PL-HSPE) proved to be very useful for exploring the details of the optical dynamics of the optical system. The PL-HSPE involves a six-dimensional experiment governed by three times between four fs pulses, two relative phases between paired pulses, and signal amplitude.

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This Week in Science

Mixing light waves of different frequencies is a routine technique for synthesizing waveforms of arbitrary shape and spectral composition. For applications in coherent quantum control, ultrafast optical pulses over a range of wavelengths may be required. Shelton et al. (p. 1286; see the Perspective by Brown et al. ), building on recent advances involving phase-locking of femtosecond optical pulses, generation of a comb of optical frequencies, and precision measurement of optical frequencies, now show that two waveforms can be coherently stitched together from separate femtosecond lasers to form a coherent pulse train.

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Summary form only given.We report on a general approach to coherent control in semiconductors, based on optical waveforms with synthesized intensity and phase versus time. This technique is limited only by the bandwidth of the initial laser pulses and the spectral resolution of the pulse-shaping apparatus. It is therefore especially suitable to investigate effects such as off-resonant Rabi oscillations and polaritons in multiple quantum wells. Experiments were performed in four-wave mixing (FWM) and differential reflection geometry based on a mode-locked Ti:sapphire laser emitting 100-fs pulses.

Conference on Lasers and Electro-Optics•Nov 27, 2002•0 citations

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.

Phase-locked optical coherence experiments were performed on the 10 fs time scale. A 13 fs cavity-dumped Ti:sapphire laser was considered as an ideal source to extend these experiments to the 10 fs time scale due to extremely high amplitude and spectral stability. Femtosecond phase-locked heterodyne detected femtosecond stimulated photon echo (PL-HSPE) proved to be very useful for exploring the details of the optical dynamics of the optical system. The PL-HSPE involves a six-dimensional experiment governed by three times between four fs pulses, two relative phases between paired pulses, and signal amplitude.

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.

Mixing light waves of different frequencies is a routine technique for synthesizing waveforms of arbitrary shape and spectral composition. For applications in coherent quantum control, ultrafast optical pulses over a range of wavelengths may be required. Shelton et al. (p. 1286; see the Perspective by Brown et al. ), building on recent advances involving phase-locking of femtosecond optical pulses, generation of a comb of optical frequencies, and precision measurement of optical frequencies, now show that two waveforms can be coherently stitched together from separate femtosecond lasers to form a coherent pulse train.

Summary form only given.We report on a general approach to coherent control in semiconductors, based on optical waveforms with synthesized intensity and phase versus time. This technique is limited only by the bandwidth of the initial laser pulses and the spectral resolution of the pulse-shaping apparatus. It is therefore especially suitable to investigate effects such as off-resonant Rabi oscillations and polaritons in multiple quantum wells. Experiments were performed in four-wave mixing (FWM) and differential reflection geometry based on a mode-locked Ti:sapphire laser emitting 100-fs pulses.