Organic chemistry offers the potential to synthesize individual molecules for specific tasks in quantum information processing. One of their striking properties is the emission of single photons with nearly ideal coherence. Here, we implement Ramsey spectroscopy to measure the electronic state coherence of a single molecule. Conventionally, the emitter’s coherence is characterized by saturation or intensity auto-correlation measurements. However, both methods are under the steady influence of continuous interaction with the excitation laser. This influence can be eliminated by using a pump–probe sequence of two optical pulses to observe the decoherence. We have measured a near-transform-limited decoherence time of 17.6 ns, while the radiative lifetime is 10.1 ns. We also perform frequency-detuned excitation, gaining richer insights into the dephasing behavior of the molecule. The experiments exhibit that optical Ramsey spectroscopy is a promising tool for measuring the emitter’s coherence properties.
Organic chemistry offers the potential to synthesize individual molecules for specific tasks in quantum information processing. One of their striking properties is the emission of single photons with nearly ideal coherence. Here, we implement Ramsey spectroscopy to measure the electronic state coherence of a single molecule. Conventionally, the emitter’s coherence is characterized by saturation or intensity auto-correlation measurements. However, both methods are under the steady influence of continuous interaction with the excitation laser. This influence can be eliminated by using a pump–probe sequence of two optical pulses to observe the decoherence. We have measured a near-transform-limited decoherence time of 17.6 ns, while the radiative lifetime is 10.1 ns. We also perform frequency-detuned excitation, gaining richer insights into the dephasing behavior of the molecule. The experiments exhibit that optical Ramsey spectroscopy is a promising tool for measuring the emitter’s coherence properties.
Single molecules trapped in the solid state at liquid helium temperatures are promising quantum emitters for the development of quantum technologies owing to their remarkable photostability and their lifetime-limited optical coherence time of the order of 10 ns. The coherent preparation of their electronic state requires resonant excitation with a Rabi period much shorter than their optical coherence time. Sculpting the optical excitation with sharp edges and a high on–off intensity ratio (∼3 × 105) from a single-frequency laser beam, we demonstrate sub-nanosecond drive of a single dibenzanthanthrene molecule embedded in a naphthalene matrix at 3.2 K, over more than 17 Rabi periods. With pulses tailored for a half-Rabi period, the electronic excited state is prepared with fidelity as high as 0.97. Using single-molecule Ramsey spectroscopy, we prove up to 5 K that the optical coherence lifetime remains at its fundamental upper limit set by twice the excited-state lifetime, making single molecules suitable for quantum bit manipulations under standard cryogen-free cooling technologies.
ingle luminescent molecules provide a unique approach in the development of quantum technologies utilizing single photon sources. This includes quantum metrology by using a molecule’s sensitivity of its emission and magnetic properties to the local environment. In this thesis, we present our investigation of the optical properties of several different classes of luminescent molecules. We begin by providing some theoretical background of single quantum emitters as well as a brief description of the experimental methodologies and equipment. Next, we present an optical investigation of an ensemble of iron phthalocyanines molecules. This molecule possesses a ground state triplet, which is a desirable property for optically active spin qubits, but has a very weak optical emission. Diffraction limited spots displayed photo-instability in the form of blinking and irreversible bleaching. In ensemble form however, their optical stability allowed us to identify a possible Raman peak where we calculated the associated phonon frequency. Next, we present our single molecule study of vanadium phthalocyanine. This molecule has been documented as displaying very long spin coherence times even at room temperatures. We confirmed the presence of a single molecule by measuring the second order correlation function. Additionally, we looked at the intensity and spectral response as a function of the excitation laser polarization. The spectrum was fitted to a two Gaussian function, which may correspond to the two dipole transitions as suggested by theoretical calculations. Lastly, we looked at the optical properties of rare earth europium complexes known for having very sharp optical transitions in the emission spectrum, with each having varying levels of sensitivity to the local environment. Motivated by techniques to investigate non-radiative decay channels, we looked at the optical response of four different europium complexes under two 1 µs pulses of 515 nm laser separated by 1 µs. Each displayed a very different results and allowed us to identify the best candidates for single molecule studies. Finally, we looked at the emission spectrum as well as the optical response under a 6 µs long pulse using time-correlation single photon spectroscopy.
Even though the quantized interaction between light and matter in the photoelectric effect is considered one of the cornerstones in the development of quantum mechanics, it was long thought impossible to directly observe the quantized nature of light itself. The advent of light-intensity autocorrelation techniques in the 1950s, first developed to study the size of stars, changed little in this perception, until true single-photon correlation spectroscopy from trapped ions was proven to be possible in the late 1970s: Photons from a single quantum emitter tend to arrive in bunches, but each light quantum is spaced apart in time—it is antibunched. Initially considered only as the workhorse of atomic quantum optics, over the past two decades, photon correlation techniques have become a standard in fields as diverse as quantum-information processing, biological imaging, polymer physics, and materials science, in general. The technique is particularly useful for probing materials that are specifically designed to emit or absorb light in optoelectronic devices, such as light-emitting diodes, solar cells, or lasers. The central question in such studies is how large a mesoscopic piece of material can become and still behave as an atom-like source of single photons. What interactions may arise between multiple excitations within a material, and what sort of dark states may give rise to intermittency in the stream of photons? We review the many different classes of optoelectronic materials for which photon-correlation spectroscopy has proven to offer useful insight into excited-state dynamics, ranging from molecular, over semiconductor to metallic nanostructures. The technique is particularly suited to probing mesoscopic aggregates of organic semiconductors since each single molecule acts as a quantum emitter itself.
Ramsey interferometry is a widely used tool for precisely measuring transition frequencies between two energy levels of a quantum system, with applications in time keeping, precision spectroscopy, quantum optics, and quantum information. Often, the coherence time of the quantum system surpasses the one of the oscillator probing the system, thereby limiting the interrogation time and associated spectral resolution. Correlation spectroscopy overcomes this limitation by probing two quantum systems with the same noisy oscillator for a measurement of their transition frequency difference; this technique has enabled very precise comparisons of atomic clocks. Here, we extend correlation spectroscopy to the case of multiple quantum systems undergoing strong correlated dephasing. We model Ramsey correlation spectroscopy with N particles as a multiparameter phase estimation problem and demonstrate that multiparticle correlations can assist in reducing the measurement uncertainties even in the absence of entanglement. We derive precision limits and optimal sensing techniques for this problem and compare the performance of probe states and measurement with and without entanglement. Using one- and two-dimensional ion Coulomb crystals with up to 91 qubits, we experimentally demonstrate the advantage of measuring multiparticle correlations for reducing phase uncertainties and apply correlation spectroscopy to measure ion-ion distances, transition frequency shifts, laser-ion detunings, and path-length fluctuations. Our method can be straightforwardly implemented in experimental setups with globally coherent qubit control and qubit-resolved single-shot readout and is, thus, applicable to other physical systems such as neutral atoms in tweezer arrays. Published by the American Physical Society 2024
Experiments with single quantum systems are at the frontier of modern physics. Probing single molecules allows for very precise control of light-matter interaction and for quantum optical studies. Moreover, a single guest molecule in a solid host matrix is a very sensitive probe of local dynamics in its nano-environment. Fluorescence excitation spectroscopy on single molecules is a powerful tool for spectroscopic characterizations at highest resolution, as information can be revealed that is not accessible in experiments on ensembles of molecules. The detection of the fluorescence signal of a single absorber is achieved by exploiting the high spectral selectivity given by the ratio (10 10) of homogeneous to inhomogeneous linewidths of optical transitions at cryogenic temperatures (zero-phonon transitions). Two-photon fluorescence excitation, a fundamental nonlinear optical process, was observed on a single quantum system [1]. Single diphenyl-octatetraene molecules trapped in an n-tetradecane matrix were excited from the 1Ag ground to the lowest excited singlet state by simultaneous absorption of two photons using a single-mode cw laser. Excited molecules were observed through weak one-photon emission resulting from a symmetry breaking induced by the crystal field. The fundamental principles and the experimental technique of single molecule spectroscopy will be introduced briefly and some particular single molecule experiments presented. This work was done in collaboration with T. Plakhotnik, A. Renn and U.P. Wild