Laser-induced frequency tuning of Fourier-limited single-molecule emitters
Maja Colautti, Francesco S. Piccioli, Pietro Lombardi, Costanza Toninelli, Zoran ristanovic, Amin Moradi, Subhasis Adhikari, Michel Orrit, Irena Deperasinska, Boleslaw Kozankiewicz
The local interaction of charges and light in organic solids is the basis of distinct and fundamental effects. We here observe, at the single molecule scale, how a focused laser beam can locally shift by hundreds-time their natural linewidth and in a persistent way the transition frequency of organic chromophores, cooled at liquid helium temperatures in different host matrices. Supported by quantum chemistry calculations, the results are interpreted as effects of a photo-ionization cascade, leading to a stable electric field, which Stark-shifts the molecular electronic levels. The experimental method is then applied to a common challenge in quantum photonics, i.e. the independent tuning and synchronization of close-by quantum emitters, which is desirable for multi-photon experiments. Five molecules that are spatially separated by about 50 microns and originally 20 GHz apart are brought into resonance within twice their linewidth. Combining this ability with an emission linewidth that is only limited by the spontaneous decay, the system enables fabrication-free, independent tuning of multiple molecules integrated on the same photonic chip.
Single quantum emitters play a fundamental role in the development of quantum technologies such as quantum repeaters, and quantum information processing. Isolating individual molecules with stable optical emission is an essential step for these applications, specially for those molecules that present large coherence times at room temperature. Among them, vanadium-oxide phthalocyanine (VOPc) molecules stand out as promising candidates due to their large coherence times measured in ensemble. However, the optical properties of individual molecules have not yet been reported. Here we show that sin…
Directional and correlated optical emission from a waveguide-engineered molecule with local control
Center for Hybrid Quantum Networks (Hy-Q), Niels Bohr Institute, University of Copenhagen（哥本哈根大学尼尔斯·玻尔研究所混合量子网络中心）；Vienna Center for Quantum Science and Technology (VCQ) and Christian Doppler Laboratory for Photonic Quantum Computer, University of Vienna（维也纳大学维也纳量子科学与技术中心及光子量子计算机克里斯蒂安·多普勒实验室）；Experimental Physics VI, Faculty of Physics and Astronomy, Ruhr University Bochum（波鸿鲁尔大学物理与天文学系实验物理学第六研究室）
The control and manipulation of quantum-entangled non-local states is a crucial step for the development of quantum information processing. A promising route to achieve such states on a wide scale is to couple solid-state quantum emitters through their coherent dipole-dipole interactions. Entanglement in itself is challenging, as it requires both nanometric distances between emitters and nearly degenerate electronic transitions. Implementing hyperspectral imaging to identify pairs of coupled organic molecules trapped in a low temperature matrix, we reach distinctive spectral signatures of maxi…
Lattice quantum electrodynamics of a molecular emitter in a topological gap
Univ. Lille, CNRS, UMR 8523 – PhLAM – Physique des Lasers Atomes et Molécules（里尔大学）；University of Würzburg（维尔茨堡大学）；National Institute of Optics (CNR-INO)（国家光学研究所）；European Laboratory for Non-Linear Spectroscopy (LENS)（欧洲非线性光谱学实验室）；Institute of Physics, Czech Academy of Sciences（捷克科学院物理研究所）
We demonstrate the emission of photons from a single molecule into a hybrid gap plasmon waveguide (HGPW). Crystals of anthracene, doped with dibenzoterrylene (DBT), are grown on top of the waveguides. We investigate a single DBT molecule coupled to the plasmonic region of one of the guides, and determine its in-plane orientation, excited state lifetime and saturation intensity. The molecule emits light into the guide, which is remotely out-coupled by a grating. The second-order auto-correlation and cross-correlation functions show that the emitter is a single molecule and that the light emergi…
Quantum emitters in hexagonal boron nitride (hBN) are emerging as bright and robust sources of single photons for applications in quantum optics. In this work we present detailed studies on the limiting factors to achieve Fourier Transform limited spectral lines. Specifically, we study phonon dephasing and spectral diffusion of quantum emitters in hBN via resonant excitation spectroscopy at cryogenic temperatures. We show that the linewidths of hBN quantum emitters are phonon broadened, even at 5K, with typical values of the order of one GHz. While spectral diffusion dominates at increasing pu…
Extinction spectroscopy is a powerful tool for demonstrating the coupling of a single quantum emitter to a photonic structure. However, it can be challenging in all but the simplest of geometries to deduce an accurate value of the coupling efficiency from the measured spectrum. Here we develop a theoretical framework to deduce the coupling efficiency from the measured transmission and reflection spectra without precise knowledge of the photonic environment. We then consider the case of a waveguide interrupted by a transverse cut in which an emitter is placed. We apply that theory to a silicon …
Giant Purcell broadening and Lamb shift for DNA-assembled near-infrared quantum emitters
Ecole Polytechnique Fédérale de Lausanne (EPFL)（洛桑联邦理工学院）；University of Fribourg（弗里堡大学）；Materials Physics Center CSIC-UPV/EHU（CSIC-巴斯克国立自治大学材料物理中心）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）；Ikerbasque, Basque Foundation for Science（伊克拉巴斯科，巴斯克科学基金会）；University of the Basque Country (UPV/EHU)（巴斯克国立自治大学）
Quantum emitters in hexagonal Boron Nitride (hBN) were recently reported to hol a homogeneous linewidth according to the Fourier-Transform limit up to room temperature. This unusual observation was traced back to decoupling from in-plane phonon modes which can arise if the emitter is located between two planes of the hBN host material. In this work, we investigate the origins for the mechanical decoupling. Improved sample preparation enabled a reduced background and a 70-fold decrease of spectral diffusion which was so far the major drawback of defect center in hBN and allowed us to reveal a g…
The excited state population of single solid-state emitters is subjected to energy fluctuations around the equilibrium driven by the bath and relaxation through the emission of phonons or photons. Simultaneous measurement of the associated spectral dynamics requires a technique with a high spectral and temporal resolution with an additionally high temporal dynamic range. We propose a pulsed excitation-laser analog of Photon-Correlation Fourier Spectroscopy (PCFS), which extracts the lineshape and spectral diffusion dynamics along the emission lifetime trajectory of the emitter, effectively dis…
The efficient excitation of quantum sources such as quantum dots or single molecules requires high NA optics which is often a challenge in cryogenics, or in ultrafast optics. Here we propose a 3.2 um wide parabolic mirror, with a 0.8 um focal length, fabricated by direct laser writing on CdSe/CdS colloidal quantum dots, capable of focusing the excitation light to a sub-wavelength spot and to extract the generated emission by collimating it into a narrow beam. This mirror is fabricated via in-situ volumetric optical lithography, which can be aligned to individual emitters, and it can be easily …
Fundamental understanding of biological pathways requires minimally invasive nanoscopic optical resolution imaging. Many approaches to high-resolution imaging rely on localization of single emitters, such as fluorescent molecule or quantum dot. Exact determination of the number of such emitters in an imaging volume is essential for a number of applications; however, in a commonly employed intensity-based microscopy it is not possible to distinguish individual emitters without initial knowledge of system parameters. Here we explore how quantum measurements of the emitted photons using photon nu…
The successful development of future photonic quantum technologies heavily depends on the possibility of realizing robust, reliable and, crucially, scalable nanophotonic devices. In integrated networks, quantum emitters can be deployed as single-photon sources or non-linear optical elements, provided their transition linewidth is broadened only by spontaneous emission. However, conventional fabrication approaches are hardly scalable, typically detrimental for the emitter coherence properties and bear limitations in terms of geometries and materials. Here we introduce an alternative platform, b…
We theoretically demonstrate dynamically selective bidirectional emission and absorption of a single itinerant microwave photon in a waveguide. The proposed device is an artificial molecule composed of two qubits coupled to a waveguide a quarter-wavelength apart. By using simulations based on the input--output theory, we show that upon preparing an appropriate entangled state of the two qubits, a photon is emitted directionally as a result of the destructive interference occurring either at the right or left of the qubits. Moreover, we demonstrate that this artificial molecule possesses the ca…
We explore the features of an equally-spaced array of two-level quantum emitters, that can be either natural atoms (or molecules) or artificial atoms, coupled to a field with a single continuous degree of freedom (such as an electromagnetic mode propagating in a waveguide). We investigate the existence and characteristics of bound states, in which a single excitation is shared among the emitters and the field. We focus on bound states in the continuum, occurring in correspondence of excitation energies in which a single excited emitter would decay. We characterize such bound states for an arbi…
A single quantum emitter can possess a very strong intrinsic nonlinearity, but its overall promise for nonlinear effects is hampered by the challenge of efficient coupling to incident photons. Common nonlinear optical materials, on the other hand, are easy to couple to but are bulky, imposing a severe limitation on the miniaturization of photonic systems. In this work, we show that a single organic molecule acts as an extremely efficient nonlinear optical element in the strong coupling regime of cavity quantum electrodynamics. We report on single-photon sensitivity in nonlinear signal generati…
Integrated photonic circuits offer a promising route for studying coherent cooperative effects of a controlled collection of quantum emitters. However, spectral inhomogeneities, decoherence and material incompatibilities in the solid state make this a nontrivial task. Here, we demonstrate efficient coupling of a pair of organic molecules embedded in a plastic film to a TiO$_2$ microdisc resonator on a glass chip. Moreover, we tune the resonance frequencies of the molecules with respect to that of the microresonator by employing nanofabricated electrodes. For two molecules separated by a distan…
Addressing the correlation of Stokes-shifted photons emitted from two quantum emitters
Centro de Física de Materiales (CMF-MPC), CSIC-UPV/EHU（材料物理中心）；University of the Basque Country (UPV/EHU)（巴斯克大学）；Université de Bordeaux, LP2N（波尔多大学）；Institut d’Optique & CNRS, LP2N（光学研究所与法国国家科学研究中心）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）；Université de Bordeaux, CNRS, LOMA, UMR 5798（波尔多大学）；Université de Strasbourg, CNRS, Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504（斯特拉斯堡大学）；Ikerbasque, Basque Foundation for Science（伊克拉巴斯科，巴斯克科学基金会）
Dicke superradiance is an example of emergence of macroscopic quantum coherence via correlated dissipation. Starting from an initially incoherent state, a collection of excited atoms synchronizes as they decay, generating a macroscopic dipole moment and emitting a short and intense pulse of light. While well understood in cavities, superradiance remains an open problem in extended systems due to the exponential growth of complexity with atom number. Here we show that Dicke superradiance is a universal phenomenon in ordered arrays. We present a theoretical framework -- which circumvents the exp…
A ring of sub-wavelength spaced dipole-coupled quantum emitters features extraordinary optical properties when compared to a one-dimensional chain or a random collection of emitters. One finds the emergence of extremely subradiant collective eigenmodes similar to an optical resonator, which feature strong 3D sub-wavelength field confinement. Motivated by structures commonly appearing in natural light harvesting complexes, we extend these studies to stacked concentric multi-ring geometries. We predict that double rings allow to engineer significantly darker and better confined collective excita…
Generation of polarization-entangled photon pairs from two interacting quantum emitters
Centro de Física de Materiales (CMF-MPC), CSIC-UPV/EHU（材料物理中心（CMF-MPC），CSIC-巴斯克国立大学联盟）；Department of Electricity and Electronics, University of the Basque Country (UPV/EHU)（巴斯克国立大学（UPV/EHU）电力与电子工程系）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心（DIPC））；Ikerbasque, Basque Foundation for Science（伊克尔巴斯科，巴斯克科学基金会）
