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Conference on Lasers and Electro-Optics

Single molecular phase-to-amplitude converter using femtosecond wave packet engineering

Kazuhiko Misawa, Isao Matsuda, Naoyuki T. Hashimoto, Roy Lang

Published Jan 1, 2004• 0 citations
Publisher

Abstract

We show a single molecular phase-to-amplitude converter, which converts the optical phase information of femtosecond pulses into spontaneous emission amplitude in a cyanine dye molecule through the coherent excitation of the quantum wave packet.
DOI
10.1364/iqec.2004.iwa17

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Quantum wave packet engineering is demonstrated using a phase-programmable femtosecond optical source. This paper describes development of a programmable phase modulator and coherent control of quantum wave packets. Wave packet motion in a cyanine dye molecule is observed to be dependent on the chirp direction and rate of excitation pulses. Strong reduction in excited state population is efficient for negatively chirped pulses in the cyanine dye molecule, which is explained in terms of a pump-dump process. We discuss a possibility of mutual conversion between the optical and electronic phase information by means of nonlinear light-matter interaction.
A new optical telecommunication method combining time and frequency domain multiplexing is proposed using phase-controlled femtosecond pulses. Each pulse in a pulse train can be used as a data packet with data bits in the frequency domain. We call the new principle ‘wave packet engineering’, which adjusts the amplitude and phase of the wave function in device materials arbitrarily by controlling the spectral phase of femtosecond pulses. The optical phase-to-amplitude converter is demonstrated with organic dye molecules, in which the phase information in the phase-modulated pulses can be demodulated into the luminescence intensity. The luminescence intensity from cyanine dye molecules is observed to be chirp dependent, and is explained quantum mechanically in terms of coherent population transfer. The design principle of the device using semiconductor coupled quantum nanostructures is also discussed in terms of wave packet engineering.
It is well known that the application of a pulse to a molecular electronic transition leaves the molecules vibrational modes in different electronic states in well-localized states, or wave packets[1]. One method of detecting the wave packets is via the time-dependent spectra of spontaneous emission from the excited molecule[2]. The emission consists in general of two parts, an incoherent part that depends only on the wave packet in the excited state, and a coherent part, that depends on the wave packets in both excited and ground electronic states (of a two-state molecule). This can be seen from the following simple calculation.
The quantum interference of two molecular wave packets has been precisely controlled in the B electronic state of the I2 molecule by using a pair of fs laser pulses whose relative phase is locked within the attosecond time scale and its real-time evolution has been observed by another fs laser pulse. It is clearly observed that the temporal evolution changes drastically as a function of the relative phase between the locked pulses, allowing us to read both amplitude and phase information stored in the wave functions of the molecular ensemble.