Coupled Quantum Emitters Research Articles

(Invited) Coupled Quantum Emitters in Carbon Nanotubes

The development of covalent diazonium functionalization of carbon nanotubes brings unique opportunities in terms of original quantum sources of light. In particular, it should be possible to create a linear ensemble of closely packed single-photon sources along the carbon nanotube backbone. The physical proximity of several dopants would make it possible to couple them simultaneous to a resonant cavity mode and to induce original dynamics and light emission properties. Here, we investigate experimentally the case of a series of four quantum emitters attached to the same carbon nanotube coupled to a high finesse fiber cavity. We explore their properties through PLE, polarization and super-localization measurements and their light emission properties using time-correlation techniques and photo-luminescence decay measurements. We show that two pairs show qualitatively different behaviors in terms of spectral diffusion and luminescence saturation, which we interpret using two models of electronically coupled or uncoupled two-level systems.

N-photon correlations from non-identical strongly coupled quantum emitters

N-photon correlations from non-identical strongly coupled quantum emitters

Tailoring the superradiant and subradiant nature of two coherently coupled quantum emitters

The control and manipulation of quantum-entangled states is crucial for the development of quantum technologies. A promising route is to couple solid-state quantum emitters through their optical dipole-dipole interactions. Entanglement in itself is challenging, as it requires both nanometric distances between emitters and nearly degenerate electronic transitions. Here we implement hyperspectral imaging to identify pairs of coupled dibenzanthanthrene molecules, and find distinctive spectral signatures of maximally entangled superradiant and subradiant electronic states by tuning the molecular optical resonances with Stark effect. We demonstrate far-field selective excitation of the long-lived subradiant delocalized state with a laser field tailored in amplitude and phase. Optical nanoscopy of the coupled molecules unveils spatial signatures that result from quantum interferences in their excitation pathways and reveal the location of each emitter. Controlled electronic-states superposition will help deciphering more complex physical or biological mechanisms governed by the coherent coupling and developing quantum information schemes.

Long-distance coupling and energy transfer between exciton states in magnetically controlled microcavities

Coupling of quantum emitters in a semiconductor relies, generally, on short-range dipole-dipole or electronic exchange type interactions. Consistently, energy transfer between exciton states, that is, electron-hole pairs bound by Coulomb interaction, is limited to distances of the order of 10 nm. Here, we demonstrate polariton-mediated coupling and energy transfer between excitonic states over a distance exceeding 2 μm. We accomplish this by coupling quantum well-confined excitons through the delocalized mode of two coupled optical microcavities. Use of magnetically doped quantum wells enables us to tune the confined exciton energy by the magnetic field and in this way to control the spatial direction of the transfer. Such controlled, long-distance interaction between coherently coupled quantum emitters opens possibilities of a scalable implementation of quantum networks and quantum simulators based on solid-state, multi-cavity systems.

Coherent photon coincidence spectroscopy of single quantum systems

Non-equilibrium photon correlations of coherently excited single quantum systems can reveal their internal quantum dynamics and provide spectroscopic access. Here we propose and discuss the fundamentals of a coherent photon coincidence spectroscopy based on the application of laser pulses with variable delay and the detection of an time-averaged two-photon coincidence rate. For demonstration, two simple but important cases, i.e., an exciton - biexciton in a quantum dot and two coupled quantum emitters, are investigated based on quantum dynamics simulations demonstrating that this nonlinear spectroscopy reveals information specific to the particular single quantum system.

Disorder-assisted excitation localization in chirally coupled quantum emitters

One-dimensional quantum emitters with chiral couplings can exhibit nonreciprocal decay channels, along with light-induced dipole-dipole interactions mediated via an atom-waveguide interface. When the position disorders are introduced to such atomic array, we are able to identify the dynamical phase transition from excitation delocalization to localization, with an interplay between the directionality of decay rates and the strength of light-induced dipole-dipole interactions. Deep in the localization phase, its characteristic length decreases and saturates toward a reciprocal coupling regime, leading to a system dynamics whose ergodicity is strongly broken. We also find an interaction-driven re-entrant behavior of the localization phase and a reduction of level repulsion under strong disorder. The former coincides with a drop in the exponent of power-law decaying von Neumann entropy, which gives insights to a close relation between the preservation of entanglement and nonequilibrium dynamics in open quantum systems, while the latter presents a distinct narrow distribution of gap ratios in this particular disordered system.

Excitation of Hybrid Plasmonic Waveguide Modes by Colloidal Quantum Dots

Quantum information technologies will greatly benefit from efficiently coupled quantum emitter–waveguide systems. Hybrid plasmonic waveguide modes are relatively low-loss confined modes, which prov...

Enhanced collective Purcell effect of coupled quantum emitter systems

Cavity-embedded quantum emitters show strong modifications of free space radiation properties such as an enhanced decay known as the Purcell effect. The central parameter is the cooperativity $C$, the ratio of the square of the coherent cavity coupling strength over the product of cavity and emitter decay rates. For a single emitter, $C$ is independent of the transition dipole moment and dictated by geometric cavity properties such as finesse and mode waist. In a recent work [Phys. Rev. Lett. 119, 093601 (2017)] we have shown that collective excitations in ensembles of dipole-dipole coupled quantum emitters show a disentanglement between the coherent coupling to the cavity mode and spontaneous free space decay. This leads to a strong enhancement of the cavity cooperativity around certain collective subradiant antiresonances. Here, we present a quantum Langevin equations approach aimed at providing results beyond the classical coupled dipoles model. We show that the subradiantly enhanced cooperativity imprints its effects onto the cavity output field quantum correlations while also strongly increasing the cavity-emitter system's collective Kerr nonlinear effect.

Probing the State of a Mechanical Oscillator with an Ultrastrongly Coupled Quantum Emitter.

Performing accurate position measurements of a mechanical resonator by coupling it to some optically driven quantum emitter is an important challenge for quantum sensing and metrology. We fully characterize the quantum noise associated with this measurement process, by deriving master equations for the coupled emitter and the resonator valid in the ultrastrong coupling regime. At short timescales, we show that this noise sets a fundamental limit to the readout sensitivity and that the standard quantum limit can be recovered for realistic experimental conditions. At long timescales, the scattering of the mechanical quadratures leads to the decoupling of the emitter from the driving light, switching off the noise source. This method can be used to describe the interaction of any quantum system strongly coupled to a finite size reservoir.

Cavity Antiresonance Spectroscopy of Dipole Coupled Subradiant Arrays.

An array of N closely spaced dipole coupled quantum emitters exhibits super- and subradiance with characteristic tailorable spatial radiation patterns. Optimizing the emitter geometry and distance with respect to the spatial profile of a near resonant optical cavity mode allows us to increase the ratio between light scattering into the cavity mode and free space emission by several orders of magnitude. This leads to distinct scaling of the collective coherent emitter-field coupling vs the free space decay as a function of the emitter number. In particular, for subradiant states, the effective cooperativity increases much faster than the typical linear ∝N scaling for independent emitters. This extraordinary collective enhancement is manifested both in the amplitude and the phase profile of narrow collective antiresonances appearing at the cavity output port in transmission spectroscopy.

Reconstruction of exciton wave functions of coupled quantum emitters including spin with ultrafast spectroscopy using localized nanooptical fields

Coulomb-induced resonance energy transfer mechanisms between coupled nanostructures lead to the formation of new, delocalized exciton states. Their hybrid wave functions can be decomposed into the basis of local states of the uncoupled system by the use of coherent, spatially resolved spectroscopy. The suggested quantum state tomography protocol combines nanooptical fields with a four-wave mixing technique: At least one pulse of the pulse sequence is spatially localized at a specific quantum emitter. It was suggested to use nanoplasmonic structures together with pulse-shaped fields for the localization. In this paper, the method is applied to a system of two coupled semiconductor quantum dots. The basic reconstruction concept first proposed in Richter et al. (Phys Rev B 86:085308, 2012) and Schlosser et al. (New J Phys 15:025004, 2013) is extended to the case of including different spin states of the excitons in the quantum dots. For this purpose, the theoretical scheme has to be modified and the localized fields need the ability to change their polarization. We show that the application of the developed reconstruction scheme to two-dimensional spectra gives full access to the internal structure of the interacting quantum states.

Collective effects in subwavelength hybrid systems: a numerical analysis

Optical properties of ensembles of coupled three-level quantum emitters are investigated in linear and non-linear regimes. The model of the Maxwell–Liouville von Neumann equations is implemented to explore the reflection, transmission, and absorption of a thin layer of atom-like emitters at low and high densities. The stimulated Raman adiabatic passage is analysed in systems of coupled quantum emitters of various densities. It is shown that coupling via local electromagnetic fields shifts the energy levels and modifies propagating fields leading to a mixed final population distribution and appearance of new absorption resonances. Strong femtosecond pulses induce population inversion in emitters leading to optical gain.

Using localized double-quantum-coherence spectroscopy to reconstruct the two-exciton wave function of coupled quantum emitters

Coherent multidimensional spectroscopy allows us to inspect the energies and the coupling of quantum systems. Coupled quantum systems—such as a coupled semiconductor quantum dot or pigments in photosynthesis—form delocalized exciton and two-exciton states. A technique is presented to decompose these delocalized wave functions into the basis of individual quantum emitters. This quantum state tomography protocol is illustrated for three coupled InAs quantum dots. To achieve the decomposition of the wavefunction, we combine the double-quantum-coherence spectroscopy with spatiotemporal control, which allows us to localize optical excitations at a specific quantum dot. Recently, a protocol was proposed for single exciton states (Richter et al 2012 Phys. Rev. B 86 085308). In this paper, we extend the method presented by Richter et al with respect to: the reconstruction of two-exciton states, a detailed analysis process of reconstruction and the effect of filtering to enhance the quality of the reconstructed wave function.

Stimulated Raman adiabatic passage as a route to achieving optical control in plasmonics

Optical properties of ensembles of three-level quantum emitters coupled to plasmonic systems are investigated employing a self-consistent model. It is shown that the stimulated Raman adiabatic passage (STIRAP) technique can be successfully adopted to control optical properties of hybrid materials with collective effects present and playing an important role in light-matter interactions. We consider a core-shell nanowire composed of a silver core and a shell of coupled quantum emitters and utilize a STIRAP scheme to control the scattering efficiency of such a system in a frequency and spatially dependent manner. After the STIRAP-induced population transfer to the final state takes place, the core-shell nanowire exhibits two sets of Rabi splittings with Fano line shapes, indicating strong interactions between two different atomic transitions driven by plasmon near-fields.

Deterministic nanoassembly of a coupled quantum emitter–photonic crystal cavity system

Controlling the interaction of a single quantum emitter with its environment is a key challenge in quantum optics. Here, we demonstrate deterministic coupling of single nitrogen-vacancy (NV) centers to high-quality photonic crystal cavities. We preselect single NV centers and position their 50-nm-sized host nanocrystals into the mode maximum of photonic crystal S1 cavities with few-nanometer accuracy. The coupling results in a strong enhancement of NV center emission at the cavity wavelength.