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arXiv:1106.0278 · Physical Review B

Rabi-vibronic resonance with large number of vibrational quanta

Rachel Glenn, M. É. Raǐkh

Published Nov 23, 2011• 4 citations
arXivHTMLPDF

Abstract

We study theoretically the Rabi oscillations of a resonantly driven two-level system linearly coupled to a harmonic oscillator (vibrational mode) with frequency ${\ensuremath{\omega}}_{0}$. We show that for weak coupling, ${\ensuremath{\omega}}_{p}\ensuremath{\ll}{\ensuremath{\omega}}_{0}$, where ${\ensuremath{\omega}}_{p}$ is the polaronic shift, Rabi oscillations are strongly modified in the vicinity of the Rabi-vibronic resonance ${\ensuremath{\Omega}}_{R}={\ensuremath{\omega}}_{0}$, where ${\ensuremath{\Omega}}_{R}$ is the Rabi frequency. The width of the resonance is $({\ensuremath{\Omega}}_{R}\ensuremath{-}{\ensuremath{\omega}}_{0})\ensuremath{\sim}{\ensuremath{\omega}}_{p}^{2/3}{\ensuremath{\omega}}_{0}^{1/3}\ensuremath{\gg}{\ensuremath{\omega}}_{p}$. Within this domain of ${\ensuremath{\Omega}}_{R}$ the actual frequency of the Rabi oscillations exhibits a bistable behavior as a function of ${\ensuremath{\Omega}}_{R}$. Importantly, within the resonant domain, the oscillator is highly excited, which allows us to treat it classically.

DOI
10.1103/physrevb.84.195454

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We study theoretically the Rabi oscillations of a resonantly driven two-level system linearly coupled to a harmonic oscillator (vibrational mode) with frequency \ensuremathω0{\ensuremath{\omega}}_{0}\ensuremathω0​. We show that for weak coupling, \ensuremathωp\ensuremath≪\ensuremathω0{\ensuremath{\omega}}_{p}\ensuremath{\ll}{\ensuremath{\omega}}_{0}\ensuremathωp​\ensuremath≪\ensuremathω0​, where \ensuremathωp{\ensuremath{\omega}}_{p}\ensuremathωp​ is the polaronic shift, Rabi oscillations are strongly modified in the vicinity of the Rabi-vibronic resonance \ensuremathΩR=\ensuremathω0{\ensuremath{\Omega}}_{R}={\ensuremath{\omega}}_{0}\ensuremathΩR​=\ensuremathω0​, where \ensuremathΩR{\ensuremath{\Omega}}_{R}\ensuremathΩR​ is the Rabi frequency. The width of the resonance is (\ensuremathΩR\ensuremath−\ensuremathω0)\ensuremath∼\ensuremathωp2/3\ensuremathω01/3\ensuremath≫\ensuremathωp({\ensuremath{\Omega}}_{R}\ensuremath{-}{\ensuremath{\omega}}_{0})\ensuremath{\sim}{\ensuremath{\omega}}_{p}^{2/3}{\ensuremath{\omega}}_{0}^{1/3}\ensuremath{\gg}{\ensuremath{\omega}}_{p}(\ensuremathΩR​\ensuremath−\ensuremathω0​)\ensuremath∼\ensuremathωp2/3​\ensuremathω01/3​\ensuremath≫\ensuremathωp​. Within this domain of \ensuremathΩR{\ensuremath{\Omega}}_{R}\ensuremathΩR​ the actual frequency of the Rabi oscillations exhibits a bistable behavior as a function of \ensuremathΩR{\ensuremath{\Omega}}_{R}\ensuremathΩR​. Importantly, within the resonant domain, the oscillator is highly excited, which allows us to treat it classically.
The resonance fluorescence from a vibronic system with displaced potential-energy surfaces is studied. Because of the equal vibrational frequencies in the two electronic quantum states, a large number of vibronic transitions can be excited by a strong laser field. Even in the case of weaker driving fields, nonperturbative effects may be observed provided that the vibrational relaxation is slow enough. If the vibronic coupling is not extremely strong, the Rabi oscillations will arise mainly from the excitation of the vibrationless transition. Furthermore, the damping of the Rabi oscillations may be accompanied by a substantial decrease in intensity.
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The sensitivity of the Rabi oscillations of a resonantly driven spin-12\frac{1}{2}21​ system to a weak and slow modulation of the static longitudinal magnetic field B0{B}_{0}B0​ is studied theoretically. We establish the mapping of a weakly driven two-level system with modulation onto a strongly driven system without modulation. The mapping suggests that different regimes of spin dynamics, known for a strongly driven system, can be realized under common experimental conditions of weak driving (driving field ${B}_{1}\ensuremath{\ll}{B}_{0}$) upon proper choice of the domains of modulation frequency ${\ensuremath{\omega}}_{m}$ and amplitude B2{B}_{2}B2​. Fast modulation ${\ensuremath{\omega}}_{m}\ensuremath{\gg}{\ensuremath{\Omega}}_{R}$, where ${\ensuremath{\Omega}}_{R}$ is the Rabi frequency, emulates the regime of driving frequency much bigger than the resonant frequency. Strong modulation ${B}_{2}\ensuremath{\gg}{B}_{1}$ emulates the regime ${B}_{1}\ensuremath{\gg}{B}_{0}$. Resonant modulation ${\ensuremath{\omega}}_{m}\ensuremath{\approx}{\ensuremath{\Omega}}_{R}$ gives rise to an envelope of the Rabi oscillations. The shape of this envelope is highly sensitive to the detuning of the driving frequency from the resonance. Theoretical predictions for different domains of B2{B}_{2}B2​ and ${\ensuremath{\omega}}_{m}$ were tested experimentally using NMR of protons in water, where, without modulation, the pattern of Rabi oscillations could be observed over many periods. We present experimental results which reproduce the three predicted modulation regimes, and agree with theory quantitatively.
We consider a two-level quantum system interacting with two classical time-periodic electromagnetic fields. The frequency of one of the fields far exceeds that of the other. The effect of the high-frequency field can be averaged out of the dynamics to realize an effective transition frequency of the field-dressed two-level system. We examine the linear response, second harmonic response and Stokes and anti-Stokes Raman response of the dressed two-level system, to the weak frequency field. The vibrational resonance enhancement in each case is demonstrated for optimal strength of the high-frequency field. Our theoretical scheme is corroborated by full numerical simulation of the two-level, two-field dynamics governed by loss-free Bloch equations. We suggest that quantum optics can offer an interesting arena for the study of the vibrational resonance. This article is part of the theme issue 'Vibrational and stochastic resonance in driven nonlinear systems (part 1)'.
The multiple-linear-time-scale method is used to construct a perturbation theory for NNN-level quantum systems subjected to time-dependent perturbations. The secular and small-denominator terms which plague conventional time-dependent perturbation theory are avoided; consequently, the theory is useful for treating long-term behavior and resonant interactions. The introduction of a self-energy operator allows the shifts in energy levels to be displayed explicitly. When the perturbation is the dipole interaction with an electromagnetic field, the successive approximations yield the well-known rotating-wave approximation, corrections due to counter rotating terms, and the Bloch-Siegert frequency shift. The formalism is applicable to arbitrary pulse shapes, provided that $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}\ensuremath{\ll}\ensuremath{\hbar}\overline{\ensuremath{\omega}}$, where $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}$ represents the inter-action strength and $\overline{\ensuremath{\omega}}$ is a characteristic frequency of the field. Rabi oscillations induced by multiphoton resonances are automatically included, and this effect is demonstrated in the case of a square pulse with frequency approximately one half the resonance frequency for a transition between two vibrational levels of a molecule. These calculations are compared to an exact numerical solution in order to find the limits of validity of the approximation. Even at high intensities ($I\ensuremath{\sim}{10}^{14}$ W/cm2{\mathrm{cm}}^{2}cm2) the shifted resonance frequency is quite accurate; however, the approximate and exact solutions are slightly out of phase, so that the approximate solution can only be trusted for a few Rabi cycles. For much lower intensities ($I\ensuremath{\sim}{10}^{10}$ W/cm2{\mathrm{cm}}^{2}cm2), the approximate solution is valid for many thousands of Rabi cycles.
Rabi oscillations are coherent transitions in a quantum two-level system under the influence of a resonant drive, with a much lower frequency dependent on the perturbation amplitude. These serve as one of the signatures of quantum coherent evolution in mesoscopic systems. It was shown recently (Grønbech-Jensen N and Cirillo M 2005 Phys. Rev. Lett. 95 067001) that in phase qubits (current-biased Josephson junctions) this effect can be mimicked by classical oscillations arising due to the anharmonicity of the effective potential. Nevertheless, we find qualitative differences between the classical and quantum effects. Firstly, while the quantum Rabi oscillations can be produced by the subharmonics of the resonant frequency ω 10 (multiphoton processes), the classical effect also exists when the system is excited at the overtones, n ω 10 . Secondly, the shape of the resonance is, in the classical case, characteristically asymmetric, whereas quantum resonances are described by symmetric Lorentzians. Thirdly, the anharmonicity of the potential results in the negative shift of the resonant frequency in the classical case, in contrast to the positive Bloch–Siegert shift in the quantum case. We show that in the relevant range of parameters these features allow us to distinguish confidently the bona fide Rabi oscillations from their classical Doppelgänger.