Ilja Gerhardt

Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence

Single dye molecules at cryogenic temperatures exhibit many spectroscopic phenomena known from the study of free atoms and are thus promising candidates for experiments in fundamental quantum optics. However, the existing techniques for their detection have either sacrificed information on the coherence of the excited state or have been inefficient. Here, we show that these problems can be addressed by focusing the excitation light near to the extinction cross-section of a molecule. Our detection scheme enables us to explore resonance fluorescence over nine orders of magnitude of excitation intensity and to separate its coherent and incoherent parts. In the strong excitation regime, we demonstrate the first direct observation of the Mollow fluorescence triplet from a single solid-state emitter. Under weak excitation, we report the detection of a single molecule with an incident power as faint as 600u2009aW, paving the way for studying nonlinear effects with only a few photons.

Coherent control of single spins in silicon carbide at room temperature

Spins in solids are cornerstone elements of quantum spintronics. Leading contenders such as defects in diamond or individual phosphorus dopants in silicon have shown spectacular progress, but either lack established nanotechnology or an efficient spin/photon interface. Silicon carbide (SiC) combines the strength of both systems: it has a large bandgap with deep defects and benefits from mature fabrication techniques. Here, we report the characterization of photoluminescence and optical spin polarization from single silicon vacancies in SiC, and demonstrate that single spins can be addressed at room temperature. We show coherent control of a single defect spin and find long spin coherence times under ambient conditions. Our study provides evidence that SiC is a promising system for atomic-scale spintronics and quantum technology.

Full-field implementation of a perfect eavesdropper on a quantum cryptography system

Quantum key distribution (QKD) allows two remote parties to grow a shared secret key. Its security is founded on the principles of quantum mechanics, but in reality it significantly relies on the physical implementation. Technological imperfections of QKD systems have been previously explored, but no attack on an established QKD connection has been realized so far. Here we show the first full-field implementation of a complete attack on a running QKD connection. An installed eavesdropper obtains the entire secret key, while none of the parameters monitored by the legitimate parties indicate a security breach. This confirms that non-idealities in physical implementations of QKD can be fully practically exploitable, and must be given increased scrutiny if quantum cryptography is to become highly secure.

Strong extinction of a laser beam by a single molecule

We present an experiment where a single molecule strongly affects the amplitude and phase of a laser field emerging from a subwavelength aperture. We achieve a visibility of -6% in direct and +10% in cross-polarized detection schemes. Our analysis shows that a close to full extinction should be possible using near-field excitation.

Experimentally Faking the Violation of Bell's Inequalities

Entanglement witnesses such as Bell inequalities are frequently used to prove the nonclassicality of a light source and its suitability for further tasks. By demonstrating Bell inequality violations using classical light in common experimental arrangements, we highlight why strict locality and efficiency conditions are not optional, particularly in security-related scenarios.

Monolithic diamond optics for single photon detection.

In this work, we experimentally demonstrate a novel and simple approach that uses off-the-shelf optical elements to enhance the collection efficiency from a single emitter. The key component is a solid immersion lens made of diamond, the host material for single color centers. We improve the excitation and detection of single emitters by one order of magnitude, as predicted by theory.

Daylight operation of a free space, entanglement-based quantum key distribution system

Many quantum key distribution (QKD) implementations using a free space transmission path are restricted to operation at night time in order to distinguish the signal photons used for a secure key establishment from the background light. Here, we present a lean entanglement-based QKD system overcoming that limitation. By implementing spectral, spatial and temporal filtering techniques, we establish a secure key continuously over several days under varying light and weather conditions.

Molecular photons interfaced with alkali atoms

Future quantum communication will rely on the integration of single-photon sources, quantum memories and systems with strong single-photon nonlinearities. Two key parameters are crucial for the single-photon source: a high photon flux with a very small bandwidth, and a spectral match to other components of the system. Atoms or ions may act as single-photon sources—owing to their narrowband emission and their intrinsic spectral match to other atomic systems—and can serve as quantum nonlinear elements. Unfortunately, their emission rates are still limited, even for highly efficient cavity designs. Single solid-state emitters such as single organic dye molecules are significantly brighter and allow for narrowband photons; they have shown potential in a variety of quantum optical experiments but have yet to be interfaced with other components such as stationary memory qubits. Here we describe the optical interaction between Fourier-limited photons from a single organic molecule and atomic alkali vapours, which can constitute an efficient quantum memory. Single-photon emission rates reach up to several hundred thousand counts per second and show a high spectral brightness of 30,000 detectable photons per second per megahertz of bandwidth. The molecular emission is robust and we demonstrate perfect tuning to the spectral transitions of the sodium D line and efficient filtering, even for emitters at ambient conditions. In addition, we achieve storage of molecular photons originating from a single dibenzanthanthrene molecule in atomic sodium vapour. Given the large set of molecular emission lines matching to atomic transitions, our results enable the combination of almost ideal single-photon sources with various atomic vapours, such that experiments with giant single-photon nonlinearities, mediated, for example, by Rydberg atoms, become feasible.

Structural Attributes and Photodynamics of Visible Spectrum Quantum Emitters in Hexagonal Boron Nitride

Newly discovered van der Waals materials like MoS2, WSe2, hexagonal boron nitride (h-BN), and recently C2N have sparked intensive research to unveil the quantum behavior associated with their 2D structure. Of great interest are 2D materials that host single quantum emitters. h-BN, with a band gap of 5.95 eV, has been shown to host single quantum emitters which are stable at room temperature in the UV and visible spectral range. In this paper we investigate correlations between h-BN structural features and emitter location from bulk down to the monolayer at room temperature. We demonstrate that chemical etching and ion irradiation can generate emitters in h-BN. We analyze the emitters spectral features and show that they are dominated by the interaction of their electronic transition with a single Raman active mode of h-BN. Photodynamics analysis reveals diverse rates between the electronic states of the emitter. The emitters show excellent photo stability even under ambient conditions and in monolayers. Comparing the excitation polarization between different emitters unveils a connection between defect orientation and the h-BN hexagonal structure. The sharp spectral features, color diversity, room-temperature stability, long-lived metastable states, ease of fabrication, proximity of the emitters to the environment, outstanding chemical stability, and biocompatibility of h-BN provide a completely new class of systems that can be used for sensing and quantum photonics applications.

Microscopic diamond solid-immersion-lenses fabricated around single defect centers by focused ion beam milling

Recent efforts to define microscopic solid-immersion-lenses (SIL) by focused ion beam milling into diamond substrates that are registered to a preselected single photon emitter are summarized. We show how we determine the position of a single emitter with at least 100 nm lateral and 500 nm axial accuracy, and how the milling procedure is optimized. The characteristics of a single emitter, a Nitrogen Vacancy (NV) center in diamond, are measured before and after producing the SIL and compared with each other. A count rate of 1.0 × 10(6) counts/s is achieved with a [111] oriented NV center.