Amplification of Impulsively Excited Molecular Rotational Coherence

Bustard, Philip J.; Sussman, Benjamin J.

doi:10.1103/physrevlett.104.193902

Cited by 23 publications

(15 citation statements)

References 16 publications

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“…Chirping the pulse, therefore, should provide another degree of control 30 . This new concept, which we refer to as 'strong-laser-induced interference (SLI)', is a new resource to develop the logic gates in MEIP, and provides a new method to manipulate wave packets with strong femtosecond laser pulses in general applications of coherent control, such as chemical reaction control [16][17][18][19][20] . Importantly, SLI is not specific to the vibrational eigenstates of a molecule, but universal to the superposition of any eigenstates in a variety of quantum systems.…”

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confidence: 99%

Strong-laser-induced quantum interference

et al. 2011

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Molecules are expected to be promising information devices 1-8. Theoretical proposals have been made for logic gates with a molecular wave packet modulated by a strong femtosecond laser pulse 9-15. However, it has not yet been observed how this changes the population of each eigenstate within the wave packet. Here we demonstrate direct observation of the population beating clearly as a function of the delay of the strong laser pulse. The period is close to the recurrence period of the wave packet, even though a single eigenstate should have no information on the wave-packet motion. This unusual beat arises from quantum interference among multiple eigenstates combined on a single eigenstate. This new concept, which we refer to as 'strong-laser-induced interference', is not specific to molecular eigenstates, but universal to the superposition of any eigenstates in a variety of quantum systems, being a new tool for quantum logic gates, and providing a new method to manipulate wave packets with femtosecond laser pulses in general applications of coherent control 16-20. The wavefunctions of electrically neutral systems can replace electric charges of the present Si-based circuits, whose further downsizing will soon reach its limit where current leakage will cause heat and errors with insulators thinned to atomic levels 21. Atoms and molecules are promising candidates for these neutral systems, in which the population and phase of each eigenstate serve as carriers of information 1,2,22,23. A shaped ultrashort laser pulse can access many eigenstates simultaneously within a single atom or molecule, manipulating the amplitude and phase of each eigenstate individually to write more than one million distinct binary codes in the angstrom space 1,2. Molecules in particular are now expected to be promising components to develop scalable quantum computers 5-8. The development of I /O and logic gates with molecules should be meaningful for us to be prepared for such a future scalable system. It is therefore important to study information processing with molecular eigenstates for both high-density classical information processing and quantum information processing. This background has motivated us to propose molecular eigenstate-based information processing (MEIP), and to demonstrate the ultrafast Fourier transform based on the temporal evolution of a molecular wave packet 2-4. For more universal computing in MEIP, however, one should consider another class of logic gates with a strong femtosecond laser pulse whose broad bandwidth and high intensity allow for multiple transitions among different eigenstates within a wave packet simultaneously. This scheme has been employed in a number of theoretical studies on MEIP logic gates 9-15 , and also in a few experimental studies 24 , but it has not yet been observed experimentally how each eigenstate changes its population with those multiple transitions within a wave packet. Here, we report the direct observation of the population of each vibrational eigenstate within a wave packet mod...

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confidence: 99%

Strong-laser-induced quantum interference

et al. 2011

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“…The present study focuses on the quantum initiation of coherence in a Raman comb spontaneously created in H 2 -filled HC-PCF, and demonstrates for the first time an ultra-wide comb containing coherence between lines that are generated purely from quantum-initiated vacuum noise fields, using a single narrow-band pump pulse. This single-pump-laser technique contrasts with the above-mentioned Raman excitation configurations [7][8][9], which rely on classically exciting the medium coherence by using multiple pump lasers or ultra-short pulsed lasers. We present direct experimental confirmation of the mutual coherence of the comb spectral lines and their quantum origin.…”

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confidence: 99%

Quantum-Fluctuation-Initiated Coherence in Multioctave Raman Optical Frequency Combs

Wang

Couny

et al. 2010

Phys. Rev. Lett.

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We show experimentally and theoretically that the spectral components of a multioctave frequency comb spontaneously created by stimulated Raman scattering in a hydrogen-filled hollow-core photonic crystal fiber exhibit strong self-coherence and mutual coherence within each 12 ns driving laser pulse. This coherence arises in spite of the field's initiation being from quantum zero-point fluctuations, which causes each spectral component to show large phase and energy fluctuations. This points to the possibility of an optical frequency comb with nonclassical correlations between all comb lines.

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“…The idea is that the modulator can be used to efficiently generate sidebands on a femtosecond oscillator to produce a broad spectrum with a large number of spectral components. This scheme was first suggested by Kien et al [53], and was later experimentally demonstrated with Q-switched pulsed lasers by Marangos and colleagues [54][55][56]. Consider a broadband laser with power spectral density F (ν).…”

Section: Modulation Of a Femtosecond Ti:sapphire Oscillatormentioning

confidence: 99%

Continuous-Wave Molecular Modulation Using a High-Finesse Cavity

2014

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Abstract:We demonstrate an optical modulator at a frequency of 90 THz that has the capability to modulate any laser beam in the optical region of the spectrum. The modulator is constructed by placing deuterium molecules inside a high-finesse cavity and driving a vibrational transition with two continuous-wave laser beams. The two beams, the pump and the Stokes, are resonant with the cavity. The high intra-cavity intensities that build up drive the molecules to a coherent state. This molecular coherence can then be used to modulate an independent laser beam, to produce frequency up-shifted and down-shifted sidebands. The beam to be modulated is not resonant with the cavity and thus the sidebands are produced in a single pass.

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Amplification of Impulsively Excited Molecular Rotational Coherence

Cited by 23 publications

References 16 publications

Strong-laser-induced quantum interference

Strong-laser-induced quantum interference

Quantum-Fluctuation-Initiated Coherence in Multioctave Raman Optical Frequency Combs

Continuous-Wave Molecular Modulation Using a High-Finesse Cavity

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