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arXiv:2008.06435 · Physical Review A

Observation of the high-order Mollow triplet by quantum mode control with concatenated continuous driving

Guoqing Wang, Yi-Xiang Liu, Paola Cappellaro

Published Feb 12, 2021• 26 citations
arXivHTMLPDF

Abstract

The Mollow triplet is a fundamental signature of quantum optics and has been observed in numerous quantum systems. Although it arises in the ``strong driving'' regime of the quantized field, where the atoms undergo coherent oscillations, it can be typically analyzed within the rotating wave approximation. Here we report the first observation of high-order effects in the Mollow triplet structure due to strong driving. In experiments, we explore the regime beyond the rotating wave approximation using concatenated continuous driving that has less stringent requirements on the driving field power. We are then able to reveal additional transition frequencies, shifts in energy levels, and corrections to the transition amplitudes. In particular, we find that these amplitudes are more sensitive to high-order effects than the frequency shifts and that they still require an accurate determination in order to achieve high-fidelity quantum control. The experimental results are validated by Floquet theory, which enables the precise numerical simulation of the evolution and further provides an analytical form for an effective Hamiltonian that approximately predicts the spin dynamics beyond the rotating wave approximation.

DOI
10.1103/physreva.103.022415

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The Mollow triplet is a fundamental signature of quantum optics and has been observed in numerous quantum systems. Although it arises in the ``strong driving'' regime of the quantized field, where the atoms undergo coherent oscillations, it can be typically analyzed within the rotating wave approximation. Here we report the first observation of high-order effects in the Mollow triplet structure due to strong driving. In experiments, we explore the regime beyond the rotating wave approximation using concatenated continuous driving that has less stringent requirements on the driving field power. We are then able to reveal additional transition frequencies, shifts in energy levels, and corrections to the transition amplitudes. In particular, we find that these amplitudes are more sensitive to high-order effects than the frequency shifts and that they still require an accurate determination in order to achieve high-fidelity quantum control. The experimental results are validated by Floquet theory, which enables the precise numerical simulation of the evolution and further provides an analytical form for an effective Hamiltonian that approximately predicts the spin dynamics beyond the rotating wave approximation.
In the framework of the nonsecular perturbation theory based on the Bogoliubov averaging method, the coherent dynamics of multiphoton Raman transitions in a two-level spin system driven by an amplitude-modulated microwave field is studied. Closed-form expressions for the Rabi frequencies of these transitions are obtained beyond the rotating-wave approximation for the low-frequency driving component. It is shown that spin states dressed by the high-frequency component of the driving field are shifted due to the Bloch-Siegert-like effect caused by antiresonant interactions with the strong low-frequency driving. We predict that with increasing the order of the Raman transition, the Rabi frequency decreases and the contribution of the Bloch-Siegert shift to this frequency becomes dominant. It is found that the amplitude and phase of the Rabi oscillations strongly depend on the initial phase of the low-frequency field as well as on detuning from multiphoton resonance. The recent experimental data for the second- and third-order Raman transitions observed for the nitrogen-vacancy center in diamond (Z. Shu et al., arXiv:1804.10492) are well described in the frame of our approach. Our results may provide new possibilities for coherent control of quantum systems.
The Mollow triplet is the definitive spectral signature of an optically dressed quantum emitter. We predict that for emitters coupled to localized phonons, this signature is not confined to the zero-phonon line. Under a strong resonant drive, we show that Mollow triplets are strikingly replicated on the associated phonon sidebands -a surprising result, given that phonon sidebands are typically viewed as incoherent, inelastic scattering pathways. These vibronic Mollow triplets are a direct fingerprint of dynamically generated dressed states that hybridize the emitter's electronic, photonic, and vibrational degrees of freedom. We develop a scalable analytical formalism to model this effect in complex, multi-mode molecular systems, such as dibenzoterrylene. Our work provides the precise driving conditions for observing these novel spectral features, establishing a new signature of coherence in vibronically coupled systems.
We reinvestigate the famous Mollow triplet and show that most of the well-known quantum characteristics of the Mollow triplet-including incoherent emission and a nonstandard dependence of the sidebands on detuning-can be recovered quantitatively using semiclassical dynamics with a classical light field. In fact, by not relying on the rotating wave approximation, a semiclassical model predicts some quantum effects beyond the quantum optical Bloch equation, including higher-order scattering and asymmetric sideband features. This Letter highlights the fact that, with strong intensities, many putatively quantum features of light-matter interactions arise from a simple balance of mean-field electrodynamics and elementary spontaneous emission, which requires minimal computational cost. Our results suggest that the application of semiclassical electrodynamics to problems with strong light-matter coupling in the fields of nanophotonics and superradiance are likely to yield a plethora of new information.
Monochromatically driven two-level systems (i.e., Rabi models) are ubiquitous in various fields of physics. Though they have been exactly solved, the physical pictures in these exact solutions are not clear. Recently, approximate analytical solutions with neat physics have been obtained by using the counter-rotating hybridized rotating wave (CHRW) method, which has been proven to be effective over a wider range of parameters than the previous analytical solutions. However, the CHRW depends on a parameter $\ensuremath{\xi}$, which has no solution in some regimes. Here, we combine the double-unitary-transformation approach with the generalized Van Vleck nearly degenerate perturbation theory, and present approximate analytical results with clear physics for almost all parameter regimes, which agree well with the numerical solutions and the previous experimental results. Moreover, the dynamic frequencies of the Rabi model are regular, and the frequency with the highest Fourier amplitude changes from the Rabi frequency to $2n\ensuremath{\omega}$ with driving frequency $\ensuremath{\omega}$ and integer nnn, as the driving intensity increases from weak to deep-strong. In addition, we further explore the Floquet dynamics of the dissipative open Rabi model. Remarkably, the dissipations are tunable in the rotating frame, and the approximate analytical results obtained by our method are in good agreement with the numerical results in the strong driving regime. These results pave the way to quantum control using strong and deep-strong driving with applications in quantum technologies.
Abstract Dense ensembles of spin qubits are valuable for quantum applications, even though their coherence protection remains challenging. Continuous dynamical decoupling can protect ensemble qubits from noise while allowing gate operations, but it is hindered by the additional noise introduced by the driving. Concatenated continuous driving (CCD) techniques can, in principle, mitigate this problem. Here we provide deeper insights into the dynamics under CCD, based on Floquet theory, that lead to optimized state protection by adjusting driving parameters in the CCD scheme to induce mode evolution control. We experimentally demonstrate the improved control by simultaneously addressing a dense nitrogen-vacancy (NV) ensemble with 1010 spins. We achieve an experimental 15-fold improvement in coherence time for an arbitrary, unknown state, and a 500-fold improvement for an arbitrary, known state, corresponding to driving the sidebands and the center band of the resulting Mollow triplet, respectively. We can achieve such coherence time gains by optimizing the driving parameters to take into account the noise affecting our system. By extending the generalized Bloch equation approach to the CCD scenario, we identify the noise sources that dominate the decay mechanisms in NV ensembles, confirm our model by experimental results, and identify the driving strengths yielding optimal coherence. Our results can be directly used to optimize qubit coherence protection under continuous driving and bath driving, and enable applications in robust pulse design and quantum sensing.
The Jaynes–Cummings model with or without rotating-wave approximation plays a major role to study the interaction between atom and light. We investigate the Jaynes–Cummings model beyond the rotating-wave approximation. Treating the counter-rotating terms as periodic drivings, we solve the model in the extended Floquet space. It is found that the full energy spectrum folded in the quasi-energy bands can be described by an effective Hamiltonian derived in the high-frequency regime. In contrast to the Z 2 symmetry of the original model, the effective Hamiltonian bears an enlarged U(1) symmetry with a unique photon-dependent atom-light detuning and coupling strength. We further analyze the energy spectrum, eigenstate fidelity and mean photon number of the resultant polaritons, which are shown to be in accordance with the numerical simulations in the extended Floquet space up to an ultra-strong coupling regime and are not altered significantly for a finite atom-light detuning. Our results suggest that the effective model provides a good starting point to investigate the rich physics brought by counter-rotating terms in the frame of Floquet theory.