No Arabic abstract
We report an optical technique that yields an enhancement of single-molecule photostability, by greatly suppressing photobleaching pathways which involve photoexcitation from the triplet state. This is accomplished by dynamically switching off the excitation laser when a quantum-jump of the molecule to the triplet state is optically detected. This procedure leads to a lengthened single-molecule observation time and an increased total number of detected photons. The resulting improvement in photostability unambiguously confirms the importance of photoexcitation from the triplet state in photobleaching dynamics, and may allow the investigation of new phenomena at the single-molecule level.
Strong coupling with single molecules in plasmonic picocavities has emerged as a resource for room-temperature quantum control with nanoscale light. Tip-based nanoprobes can measure the local dynamics of individual molecular picocavities, but the overhead associated with sampling an inhomogeneous picocavity distribution can be challenging for scalability. We propose a macroscopic approach in which an ensemble of molecular picocavities acts as a nonlinear plasmonic metamaterial. Using a quantum optics perspective, we study theoretical performance limits for optical cross-phase modulation in the system, taking into account realistic distributions of picocavity volumes and molecular transition frequencies. The medium nonlinearity is mediated by local strong coupling with the lowest vibronic emission sideband of individual organic chomophores. The local vacua change the refractive index of the medium at the frequency of a weak probe field $omega_p$, set to drive the bare zero-phonon absorption band. Refractive index variations $Delta n/n$ of a few percent, relative to a molecule-free scenario, are feasible with dilute ensembles. The probe phase evolution can be switched off in the presence of a signal field at a higher frequency $omega_s$, for intensities as low as 10 kW/cm$^2$. The mechanism for optical switching involves a novel ($omega_p+omega_s$) two-photon absorption channel, assisted by local vacuum fields. Our work paves the way for future studies of plasmonic metamaterials that exploit strong light-molecule interactions, for applications in optical state preparation and control.
Optical activity is the ability of chiral materials to rotate linearly-polarized (LP) electromagnetic waves. Because of their intrinsic asymmetry, traditional chiral molecules usually lack isotropic performance, or at best only possess a weak form of chirality. Here we introduce a knotted chiral meta-molecule that exhibits optical activity corresponding to a 90{deg} polarization rotation of the incident waves. More importantly, arising from the continuous multi-fold rotational symmetry of the chiral torus knot structure, the observed polarization rotation behavior is found to be independent of how the incident wave is polarized. In other words, the proposed chiral knot structure possesses two-dimensional (2-D) isotropic optical activity as illustrated in Fig. 1, which has been experimentally validated in the microwave spectrum. The proposed chiral torus knot represents the most optically active meta-molecule reported to date that is intrinsically isotropic to the incident polarization.
We realise a phase-sensitive closed-loop control scheme to engineer the fluctuations of the pump field which drives an optomechanical system, and show that the corresponding cooling dynamics can be significantly improved. In particular, operating in the counter-intuitive anti-squashing regime of positive feedback and increased field fluctuations, sideband cooling of a nanomechanical membrane within an optical cavity can be improved by 7.5~dB with respect to the case without feedback. Close to the quantum regime of reduced thermal noise, such feedback-controlled light would allow going well below the quantum backaction cooling limit.
The ability to transduce non-classical states of light from one wavelength to another is a requirement for integrating disparate quantum systems that take advantage of telecommunications-band photons for optical fiber transmission of quantum information and near-visible, stationary systems for manipulation and storage. In addition, transducing a single-photon source at 1.3 {mu}m to visible wavelengths for detection would be integral to linear optical quantum computation due to the challenges of detection in the near-infrared. Recently, transduction at single-photon power levels has been accomplished through frequency upconversion, but it has yet to be demonstrated for a true single-photon source. Here, we transduce the triggered single-photon emission of a semiconductor quantum dot at 1.3 {mu}m to 710 nm with a total detection (internal conversion) efficiency of 21% (75%). We demonstrate that the 710 nm signal maintains the quantum character of the 1.3 {mu}m signal, yielding a photon anti-bunched second-order intensity correlation, g^(2)(t), that shows the optical field is composed of single photons with g^(2)(0) = 0.165 < 0.5.
The hierarchical equations of motion (HEOM) method is a powerful numerical approach to solve the dynamics and steady-state of a quantum system coupled to a non-Markovian and non-perturbative environment. Originally developed in the context of physical chemistry, it has also been extended and applied to problems in solid-state physics, optics, single-molecule electronics, and biological physics. Here we present a numerical library in Python, integrated with the powerful QuTiP platform, which implements the HEOM for both bosonic and fermionic environments. We demonstrate its utility with a series of examples. For the bosonic case, we present examples for fitting arbitrary spectral densities, modelling a Fenna-Matthews-Olsen photosynthetic complex, and simulating dynamical decoupling of a spin from its environment. For the fermionic case, we present an integrable single-impurity example, used as a benchmark of the code, and a more complex example of an impurity strongly coupled to a single vibronic mode, with applications in single-molecule electronics.