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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Femtosecond wave packet engineering in a cyanine dye molecule

Kazuhiko Misawa, Isao Matsuda, Roy Lang

Published Dec 1, 2002• 2 citations
Publisher

Abstract

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.

DOI
10.1117/12.453853

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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.
Mechanisms and optimal experimental conditions in coherent control still intensely stimulate debates. In this work, a phase-only control mechanism in an open quantum system is investigated experimentally and numerically. Several parameterizations for femtosecond pulse shaping (combination of chirp and multipulses) are exploited in transient absorption of a prototype organic molecule to control population and vibrational coherence in ground and excited states. Experimental results are further numerically simulated and corroborated with a four-level density-matrix model, which reveals a phase-only control mechanism based on the interaction between the tailored phase of the excitation pulse and the induced transient absorption. In spite of performing experiment and numerical simulations in the linear regime of excitation, the control effect amplitude depends non-linearly on the excitation energy and is explained as a pump-dump control mechanism. No evidence of single-photon control is observed with the model. Moreover, our results also show that the control effect on the population and vibrational coherence is highly dependent on the spectral detuning of the excitation spectrum. Contrary to the popular belief in coherent control experiments, spectrally resonant tailored excitation will lead to the control of the excited state only for very specific conditions.
We demonstrate the ability to coherently control ultracold atomic Rb collisions using frequency-chirped light on the nanosecond time scale. For certain center frequencies of the chirp, the rate of inelastic trap-loss collisions induced by negatively chirped light is dramatically suppressed compared to the case of a positive chirp. We attribute this to a fundamental asymmetry in the system: an excited wave packet moves inward on the attractive molecular potential. For a positive chirp, the resonance condition moves outward in time, while for a negative chirp, it moves inward, in the same direction as the excited wave packet; this allows multiple interactions between the wave packet and the light, enabling the wave packet to be returned coherently to the ground state. Classical and quantum calculations support this interpretation.
Creating and controlling well-defined single-photon states is important for many quantum enhanced technologies. Information can be encoded in any degree of freedom associated with a single-photon field excitation, for example in the polarization or transverse spatial mode structure. The ability to encode multiple qubits in these states is desirable for high data transmission rates and increased information processing capacity. The spectral-temporal domain offers a large Hilbert space for encoding information, well suited to integrated optical architectures owing to the low cross-talk between channels. Indeed, time-frequency encoding is an integral component of existing information technologies infrastructure. Thus, complete, coherent control of the spectral-temporal mode structure of light is essential to advancing optical quantum technologies. Arbitrary control of single-photon states has been demonstrated in the polarization and spatial-momentum degrees of freedom however, is yet to be established in the spectral-temporal domain. Recently it was shown that spectral-temporal pulse shaping is experimentally feasible using nonlinear optical methods. However, such techniques can introduce noise photons, are challenging to implement deterministically and require specially prepared auxiliary pump pulses. Furthermore, they are typically only possible at relatively low repetition rates to avoid damage of nonlinear optical materials. Here, we demonstrate deterministic pulse shaping of single-photon wave packets by introducing a time-varying phase. Applying linear or quadratic phase to the wave packet introduces a spectral shift or spectral broadening, respectively. Achieving significant spectral manipulation requires temporal-phase modulation on the order of π. The phase must also vary on the same time scale as the optical pulses, approximately 1 ps in duration here. This relatively rapid phase variation is achieved using a fast electro-optic phase modulator. The modulator is driven by a time-varying voltage that is synchronized with a pulse train of single-photon wave packets for accurate temporal phase control. In this thesis, we experimentally demonstrate control of the spectral-temporal state of single-photon wave packets using this method. Heralded single-photon wave packets are generated by spontaneous parametric down conversion pumped by a frequency-doubled Titanium-Sapphire laser oscillator with 80 MHz repetition rate. To achieve significant modulation of single-photon pulses a 10 V peak-to-peak radio-frequency signal of 40 GHz drives the phase modulator, which requires approximately 3.6 V to achieve a π phase shift. The signal is synchronized with the oscillator pulse train using custom designed electronics. Details of these electronics are presented, resulting in a robust phase and amplitude controllable 40 GHz voltage source, phase locked to the single-photon pulse train. To demonstrate the utility of this pulse-shaping method we experimentally show spectral shearing of almost 1 nm for single-photon wave packets with 830 nm central wavelength and 1 nm bandwidth. Measurement of the second-order intensity correlation before and after the wave-packet manipulation remains constant within uncertainty of the measurement, showing that the quantum nature of the single-photon source is not deteriorated by the modulator. Preservation of the wave-packet coherence is verified by two-photon interference between spectrally sheared and non-modulated single-photons.
Iterative vibrational wave packet squeezing by a sequence of femtosecond pulses is proposed. Analytic formulas are derived for the harmonic oscillator case, and the practical implementation of the scheme is tested on different electronic transitions in Rb2{\mathrm{Rb}}_{2}Rb2​.