Organic molecules have recently gained attention as novel sources of single photons. We present a joint experiment--theory analysis of the temperature-dependent emission spectra, zero-phonon linewidth, and second-order correlation function of light emitted from a single molecule. We observe spectra with a zero-phonon-line together with several additional sharp peaks, broad phonon sidebands, and a strongly temperature dependent homogeneous broadening. Our model includes both localised vibrational modes of the molecule and a thermal phonon bath, which we include non-perturbatively, and is able capture all observed features. For resonant driving we measure Rabi oscillations that become increasingly damped with temperature, which our model naturally reproduces. Our results constitute an essential characterisation of the photon coherence of these promising molecules, paving the way towards their use in future quantum information applications.
We show that singlet-triplet superpositions of two-electron spin states in a double quantum dot undergo a phonon-induced pure dephasing which relies only on the tunnel coupling between the dots and on the Pauli exclusion principle. As such, this dephasing process is independent of spin-orbit coupling or hyperfine interactions. The physical mechanism behind the dephasing is elastic phonon scattering, which persists to much lower temperatures than real phonon-induced transitions. Quantitative calculations performed for a lateral GaAs/AlGaAs gate-defined double quantum dot yield micro-second deph…
The coupling between single-photon emitters and phonons opens many possibilities to store and transmit quantum properties. In this paper we apply the independent boson model to describe the coupling between an optically driven two-level system and a discrete phonon mode. Tailored optical driving allows not only to generate coherent phonon states, but also to generate coherent superpositions in the form of Schrödinger cat states in the phonon system. We analyze the influence of decay and dephasing of the two-level system on these phonon preparation protocols. We find that the decay transforms t…
We predict a spin pure dephasing channel in electron relaxation between states with unequal Zeeman splittings, exemplified by a spin-preserving electron tunneling between quantum dots in a magnetic field. The dephasing is caused by a mismatch in electron $g$-factors in the dots leading to distinguishability of phonons emitted during tunneling with opposite spins. Combining multiband $\boldsymbol{k}{\cdot}\boldsymbol{p}$ modeling and dynamical simulations via a Master equation we show that this fundamental effect of spin measurement effected by the phonon bath may be widely controlled by the si…
We report on the coherence properties of single photons from chromium-based colour centres in diamond. We use field-correlation and spectral lineshape measurements to reveal the interplay between slow spectral wandering and fast dephasing mechanisms as a function of temperature. We show that the zero-phonon transition frequency and its linewidth follow a power-law dependence on temperature indicating that the dominant fast dephasing mechanisms for these centres are direct electron-phonon coupling and phonon-modulated Coulomb coupling to nearby impurities. Further, the observed reduction in the…
We study electron-phonon interaction induced decoherence between two-electron singlet and triplet states in a semiconductor double quantum dot using a spin-boson model. We investigate the onset and time evolution of this dephasing, and study its dependence on quantum dot parameters such as dot size and double dot separations, as well as the host materials (GaAs and Si). At the short time limit, electron-phonon interaction only causes an incomplete initial Gaussian decay of the off-diagonal density matrix element in the singlet-triplet Hilbert space. A complete long-time exponential decay due t…
Pure dephasing is widely used in the literature to explain experimental observations on quantum dots in cavities. In many cases, its use is not enough and extra terms need to be "fictitiously" added to accomplish with the observed data as it is the case of cavity pumping of an unknown source. Here we controvert the validity of the pure dephasing mechanism as a source of decoherence and present a theoretical study based on the phonon-mediated coupling that can explain the emission spectrum and photon auto- and cross-correlation results in recent experiments without the need of any artificial as…
Reliable single photon sources constitute the basis of schemes for quantum communication and measurement based quantum computing. Solid state single photon sources based on quantum dots are convenient and versatile but the electronic transitions that generate the photons are subject to interactions with lattice vibrations. Using a microscopic model of electron-phonon interactions and a quantum master equation, we here examine phonon-induced decoherence and assess its impact on the rate of production, and indistinguishability, of single photons emitted from an optically driven quantum dot syste…
We have presented a consistent electronic transport framework for the two-dimensional extended Holstein's organic molecular-crystal based upon complete quantum-mechanical treatment through the non-equilibrium Green's function (NEGF) formalism and corresponding one-to-one semi-classical framework based upon Boltzmann transport theory for the narrow-bandwidth electronic energy organic semiconductor crystal material and device. In this process, we have formulated electronic self-energy interaction with acoustic and polar optical phonon mode with one phonon and two phonon interactions through Feyn…
We theoretically propose a biphoton entanglement-enhanced multidimensional spectroscopic technique as a probe for the dissipative polariton dynamics in the ultrafast regime. It is applied to the cavity-confined monomeric photosynthetic complex that represents a prototypical multi-site excitonic quantum aggregate. The proposed technique is shown to be particularly sensitive to inter-manifold polariton coherence between the two and one-excitation subspaces. It is demonstrated to be able to monitor the dynamical role of cavity-mediated excitonic correlations, and dephasing in the presence of phon…
We study the dephasing of two-electron states in a single quantum dot in both GaAs and Si. We investigate dephasing induced by electron-phonon coupling and by charge noise analytically for pure orbital excitations in GaAs and Si, as well as for pure valley excitations in Si. In GaAs, polar optical phonons give rise to the most important contribution, leading to a typical dephasing rate of ~5.9 GHz. For Si, intervalley optical phonons lead to a typical dephasing rate of ~140 kHz for orbital excitations and ~1.1 MHz for valley excitations. For harmonic, disorder-free quantum dots, charge noise i…
Spin qubits with long dephasing times are an essential requirement for the development of new quantum technologies and have many potential applications ranging from quantum information processing to quantum memories and quantum networking. Here we report a theoretical study and the calculation of the spin dephasing time of defect color centers for the negatively charged nitrogen vacancy center in diamond. We employ ab initio density functional theory to compute the electronic structure, and extract the dephasing time using a cumulant expansion approach. We find that phonon-induced dephasing is…
Recent studies reveal that a double-quantum-dot system hosting more than two electrons may be superior in certain aspects as compared to the traditional case in which only two electrons are confined (a singlet-triplet qubit). We study the electron-phonon dephasing occurring in a GaAs multi-electron double-quantum-dot system, in a biased case in which the singlet state is hybridized, as well as in an unbiased case in which the hybridization is absent. We have found that while the electron-phonon dephasing rate increases with the number of electrons confined in the unbiased case, this does not h…
We employ detuning-dependent decay-rate measurements of a quantum dot in a photonic-crystal cavity to study the influence of phonon dephasing in a solid-state quantum-electrodynamics experiment. The experimental data agree with a microscopic non-Markovian model accounting for dephasing from longitudinal acoustic phonons, and identifies the reason for the hitherto unexplained difference between non-resonant cavity feeding in different nanocavities. From the comparison between experiment and theory we extract the effective phonon density of states experienced by the quantum dot. This quantity de…
Design and Optimization of Spin Dynamics in Ge Quantum Dots: g-Factor Modulation, Geometry-Induced Dephasing Sweet Spots, and Phonon-Induced Relaxation
Engineering the impact of phonon dephasing on the coherence of a WSe$_{2}$ single-photon source via cavity quantum electrodynamics
Carl von Ossietzky University of Oldenburg（奥尔登堡卡尔·冯·奥西茨基大学）；University of Bremen（不来梅大学）；University of Michigan（密歇根大学）；Friedrich Schiller University Jena（耶拿弗里德里希·席勒大学）；Arizona State University（亚利桑那州立大学）；National Institute for Materials Science（日本国立材料研究所）
By using the zero-phonon line emission of an individual organic molecule, we realized a source of indistinguishable single photons in the near infrared. A Hong-Ou-Mandel interference experiment is performed and a two-photon coalescence probability of higher than 50% at 2 K is obtained. The contribution of the temperature-dependent dephasing processes to the two-photon interference contrast is studied. We show that the molecule delivers nearly ideal indistinguishable single photons at the lowest temperatures when the dephasing is nearly lifetime limited. This source is used to generate post-sel…
We have developed a full quantum microscopic theory to analyze the time evolution of transversal and longitudinal components of an exciton-single photon system coupled to bulk acoustic phonons. These components are subjected to two decay processes. One is radiative relaxation and the other is pure-dephasing due to exciton-phonon interaction. The former results in a decay with an exponent linear to time, while the latter causes a faster initial decay than the radiative decay. We analyzed the dependence of the components on the duration of the input one-photon pulse, temperature, and radiative r…
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…
We study the robustness and fragility of entanglement of open quantum systems in some exactly solvable models in which the decoherence is caused by a pure dephasing process. In particular, for the toy models presented in this paper, we identify two different time scales, one is responsible for local dephasing, while the other is for entanglement decay. For a class of fragile entangled states defined in this paper, we find that the entanglement of two qubits, as measured by concurrence, decays faster asymptotically than the quantum dephasing of an individual qubit.
Solid-state emitters are excellent candidates for developing integrated sources of single photons. Yet, phonons degrade the photon indistinguishability both through pure dephasing of the zero-phonon line and through phonon-assisted emission. Here, we study theoretically and experimentally the indistinguishability of photons emitted by a semiconductor quantum dot in a microcavity as a function of temperature. We show that a large coupling to a high quality factor cavity can simultaneously reduce the effect of both phonon-induced sources of decoherence. It first limits the effect of pure dephasi…
We investigate the temperature dependence of photon coherence properties through two photon interference (TPI) measurements from a single QD under resonant excitation. We show that the loss of indistinguishability is only related to the electron-phonon coupling without being affected by spectral diffusion. Through these measurements, and a complementary microscopic theory, we identify two independent separate decoherence processes each associated to phonons. Below 10K, we find that the relaxation of the vibrational lattice is the dominant contribution to the loss of TPI visibility. This proces…
A general formalism to describe the dynamics of quantum emitters in structured reservoirs is introduced. As an application, we investigate the optical coherence of an atom-like emitter diagonally coupled via a link-boson to a structured bosonic reservoir and obtain unconventional dephasing dynamics due to non-Markovian quantum feedback for different temperatures. For a two-level emitter embedded in a phonon cavity preservation of finite coherence is predicted up to room temperature.
We demonstrate that an optically driven spin of a carrier in a quantum dot undergoes indirect dephasing via conditional optically induced charge evolution even in the absence of any direct interaction between the spin and its environment. A generic model for the indirect dephasing with a three-component system with spin, charge, and reservoir is proposed. This indirect decoherence channel is studied for the optical spin manipulation in a quantum dot with a microscopic description of the charge-phonon interaction taking into account its non-Markovian nature.
In the field of quantum technology, nanomechanical oscillators offer a host of useful properties given their compact size, long lifetimes, and ability to detect force and motion. Their integration with superconducting quantum circuits shows promise for hardware-efficient computation architectures and error-correction protocols based on superpositions of mechanical coherent states. One limitation of this approach is decoherence processes affecting the mechanical oscillator. Of particular interest are two-level system (TLS) defects in the resonator host material, which have been widely studied i…
We theoretically demonstrate the enhanced and dephasing immune squeezing in the resonance fluorescence of a single quantum dot (QD) confined to a pillar-microcavity and driven by a continuous wave laser. We employ a formalism based on Polaron master equation theory for incorporating the influence of exciton-phonon coupling quite accurately in the dot-cavity system. We show a significant enhancement of squeezing due to cavity coupling of the QD as compared to that of an ideal single two-level system in free space. Particularly, we show a four-fold enhancement in squeezing as compared to that of…
We develop a general microscopic theory describing the phonon decoherence of quantum dots and indistinguishability of the emitted photons in photonic structures. The coherence is found to depend fundamentally on the dimensionality of the structure resulting in vastly different performance for quantum dots embedded in a nano-cavity (0D), waveguide (1D), slab (2D), or bulk medium (3D). In bulk, we find a striking temperature dependence of the dephasing rate scaling as $T^{11}$ implying that phonons are effectively 'frozen out' for $T \lesssim 4 \mathrm{K}$. The phonon density of states is strong…
A technique to measure the decoherence time of optical phonons in a solid is presented. Phonons are excited with a pair of time delayed 80 fs, near infrared pulses via spontaneous, transient Raman scattering. The fringe visibility of the resulting Stokes pulse pair, as a function of time delay, is used to measure the phonon dephasing time. The method avoids the need to use either narrow band or few femtosecond pulses and is useful for low phonon excitations. The dephasing time of phonons created in bulk diamond is measured to be tau = 6.8ps (1.56cm-1).
We theoretically investigate an exciton transfer process in a donor domain of organic photovoltaic cells focusing on the roles of local and nonlocal electron-phonon interactions. Our model consists of a three-level system described by the Holstein-Peierls Hamiltonian coupled to multiple heat baths for local and nonlocal molecular modes characterized by Brownian spectral distribution functions. We chose tetracene as a reference donor molecule, where the spectral distribution functions of the local and nonlocal modes exist. We then employ the reduced hierarchy equations of motion (HEOM) approach…
We study the generation of quantum correlations between two excitonic quantum dot qubits due to their interaction with the same phonon environment. Such generation results from the fact that during the pure dephasing process at finite temperatures, each exciton becomes entangled with the phonon environment. We find that for a wide range of temperatures quantum correlations are created due to the interaction. The temperature-dependence of the amount of correlations created displays a trade-off type behaviour; for small temperatures the phonon-induced distrubance of the qubit states is too small…
The optomechanical character of molecules was discovered by Raman about one century ago. Today, molecules are promising contenders for high-performance quantum optomechanical platforms because their small size and large energy-level separations make them intrinsically robust against thermal agitations. Moreover, the precision and throughput of chemical synthesis can ensure a viable route to quantum technological applications. The challenge, however, is that the coupling of molecular vibrations to environmental phonons limits their coherence to picosecond time scales. Here, we improve the optom…
The molecular photo cell, i.e., a single molecule donor-acceptor complex, beside being technologically important, is a paradigmatic example of a many-body system operating in strong non-equilibrium. The quantum transport and the photo-voltaic energy conversion efficiency of the photocell, attached to two external leads, are investigated within the open quantum system approach by solving the Lindblad master equation. The interplay of the vibrational degrees of freedom corresponding to the molecules (via the electron-phonon interaction) and the environment (via dephasing) shows its signature in …
Organic solar cells must separate strongly bound electron-hole pairs into free charges. This is achieved at interfaces between electron donor and acceptor organic semiconductors. The most popular electron acceptor is the fullerene derivative PCBM. Electron-hole separation has been observed on femtosecond timescales, which is incompatible with conventional Marcus theories of organic transport. In this work we show that ultrafast charge transport in PCBM arises from its broad range of electronic eigenstates, provided by the presence of three closely spaced delocalised bands near the LUMO level. …
Using the zero-phonon line (ZPL) emission of a single molecule, we realized a triggered source of near-infra-red (lambda=785 nm) single photons at a high repetition rate. A Weierstrass solid immersion lens is used to image single molecules with an optical resolution of 300 nm (~0.4*lambda) and a high collection efficiency. Because dephasing of the transition dipole due to phonons vanishes at liquid helium temperatures, our source is attractive for the efficient generation of single indistinguishable photons.
