Gil Triginer Garces, Helen M. Chrzanowski, Shakib Daryanoosh, Valerian Thiel, Anna L. Marchant, Raj B. Patel, Peter C. Humphreys, Animesh Datta, Ian A. Walmsley
备注：
The following article has been submitted to Applied Physics Letters
Nonlinear optical microscopy techniques have emerged as a set of successful tools for biological imaging. Stimulated emission microscopy belongs to a small subset of pump-probe techniques which can image non-fluorescent samples without requiring fluorescent labelling. However, its sensitivity has been shown to be ultimately limited by the quantum fluctuations in the probe beam. We propose and experimentally implement sub-shot-noise limited stimulated emission microscopy by preparing the probe pulse in an intensity-squeezed state. This technique paves the way for imaging delicate biological samples that have no detectable fluorescence with sensitivity beyond standard quantum fluctuations.
The spatial resolution and fluorescence signal amplitude in stimulated emission depletion (STED) microscopy is limited by the photostability of available fluorophores. Here, we show that negatively-charged silicon vacancy (SiV) centers in diamond are promising fluorophores for STED microscopy, owing to their photostable, near-infrared emission and favorable photophysical properties. A home-built pulsed STED microscope was used to image shallow implanted SiV centers in bulk diamond at room temperature. The SiV stimulated emission cross section for 765-800 nm light is found to be (4.0 +/- 0.3) x…
Inspired by laser operation, we address the question of whether stimulated emission into polarization entangled modes can be achieved. We describe a state produced by stimulated emission of the singlet Bell state and propose a setup for creating it. As a first important step towards an entangled-photon laser we demonstrate experimentally interference-enhanced polarization entanglement.
Stimulated Raman spectroscopy has become a powerful tool to study the spatiodynamics of molecular bonds with high sensitivity, resolution and speed. However, sensitivity and speed of state-of-the-art stimulated Raman spectroscopy are currently limited by the shot-noise of the light beam probing the Raman process. Here, we demonstrate an enhancement of the sensitivity of continuous-wave stimulated Raman spectroscopy by reducing the quantum noise of the probing light below the shot-noise limit by means of amplitude squeezed states of light. Probing polymer samples with Raman shifts around 2950 $…
We investigate surface plasmon amplification in a silver nanoparticle coupled to an externally driven three-level gain medium, and show that quantum coherence significantly enhances the generation of surface plasmons. Surface plasmon amplification by stimulated emission of radiation is achieved in the absence of population inversion on the spasing transition, which reduces the pump requirements. The coherent drive allows us to control the dynamics, and holds promise for quantum control of nanoplasmonic devices.
We studied the dynamics of an initially inverted atom in a semi-infinite waveguide, in the presence of a single propagating photon. We show that atomic relaxation is enhanced by a factor of 2, leading to maximal bunching in the output field. This optimal irreversible stimulated emission is a novel phenomenon that can be observed with state-of-the-art solid-state atoms and waveguides. When the atom interacts with two one-dimensional electromagnetic environments, the preferential emission in the stimulated field can be exploited to efficiently amplify a classical or a quantum state.
We propose a novel femtosecond stimulated Raman spectroscopy (FSRS) technique that combines entangled photons with interference detection to select matter pathways and enhance the resolution. Following photo excitation by an actinic pump, the measurement uses a pair of broadband entangled photons, one (signal) interacts with the molecule together with a third narrowband pulse induces the Raman process. The other (idler) photon provides a reference for the coincidence measurement. This interferometric photon-coincidence counting detection allows to separately measure Raman gain and loss signals…
Polarized light microscopy using path-entangled $N$-photon states (i.e., the N00N states) has been demonstrated to surpass the shot-noise limit at very low light illumination. However, the microscopy images suffer from divergence of phase sensitivity, which inevitably reduces the image quality. Here, we show that due to experimental imperfections, such a singularity also takes place in the microscopy that uses twin-Fock states of light for illumination. We propose two schemes to completely eliminate this singularity: (i) locking the phase shift sensed by the beams at the optimal working point,…
Nonlinear interferometers that replace beamsplitters in Mach-Zehnder interferometers with nonlinear amplifiers for quantum-enhanced phase measurements have drawn increasing interest in recent years, but practical quantum sensors based on nonlinear interferometry remain an outstanding challenge. Here, we demonstrate the first practical application of nonlinear interferometry by measuring the displacement of an atomic force microscope microcantilever with quantum noise reduction of up to 3~dB below the standard quantum limit, corresponding to a quantum-enhanced measurement of beam displacement o…
Quantum enhanced microscopy allows for measurements at high sensitivities and low damage. Recently, multi-pass microscopy was introduced as such a scheme, exploiting the sensitivity enhancement offered by multiple photon-sample interactions. Here we theoretically and numerically compare three different contrast enhancing techniques that are all based on self-imaging cavities: CW cavity enhanced microscopy, cavity ring-down microscopy and multi-pass microscopy. We show that all three schemes can lead to sensitivities beyond the standard quantum limit.
We show that the two-photon transition rates of quantum dots coupled to nanocavities are enhanced by up to 8 orders of magnitude relative to quantum dots in bulk host. We then propose how to take advantage of this enhancement to implement coherent quantum dot excitation by two-photon absorption, entangled photon pair generation by two-photon spontaneous emission, and single-photon generation at telecommunication wavelengths by two-photon stimulated and spontaneous emission.
Stimulated Raman adiabatic passage (STIRAP) is a widely-used technique of coherent state-to-state manipulation for many applications in physics, chemistry, and beyond. The adiabatic evolution of the state involved in STIRAP, called adiabatic passage, guarantees its robustness against control errors, but also leads to problems of low efficiency and decoherence. Here we propose and experimentally demonstrate an alternative approach, termed stimulated Raman "user-defined" passage (STIRUP), where a parameterized state is employed for constructing desired evolutions to replace the adiabatic passage…
By harnessing the quantum states of light for illumination, precise phase and absorption estimations can be achieved with precision beyond the standard quantum limit. Despite their significance for precision measurements, quantum states are fragile in noisy environments which leads to difficulties in revealing the quantum advantage. In this work, we propose a scheme to improve optical absorption estimation precision by using the correlated photon pairs from spontaneous parametric down-conversion as the illumination. This scheme performs better than clasical illumination when the loss is below …
We propose the use of the subwavelength localization via adiabatic passage technique for fluorescence microscopy with nanoscale resolution in the far field. This technique uses a Λ-type medium coherently coupled to two laser pulses: the pump, with a node in its spatial profile, and the Stokes. The population of the Λ system is adiabatically transferred from one ground state to the other except at the node position, yielding a narrow population peak. This coherent localization allows fluorescence imaging with nanometer lateral resolution. We derive an analytical expression to asses the resoluti…
Broadly tunable quantum-enhanced Raman microscopy for advancing bioimaging
Technical University of Denmark（丹麦技术大学）；Max Planck Institute for the Science of Light（马克斯·普朗克光科学研究所）；Danish Fundamental Metrology（丹麦基础计量）；University of Southern Denmark（南丹麦大学）；Friedrich-Alexander Universität Erlangen-Nürnberg（埃尔朗根-纽伦堡大学）
The interaction between light and an atom proceeds via three paradigmatic mechanisms: spontaneous emission, stimulated emission, and absorption. All three are resonant processes in the sense that they require that the radiation field be resonant with the atomic transition. The non-resonant counterparts of these effects, while necessary to maintain locality of the interaction in principle, are usually negligible because their effects tend to average out over multiple cycles of the radiation field. This state of affairs does not hold if the atom is accelerated. We show that, when accelerated, th…
We experimentally demonstrate quantum enhanced resolution in confocal fluorescence microscopy exploiting the non-classical photon statistics of single nitrogen-vacancy colour centres in diamond. By developing a general model of super-resolution based on the direct sampling of the kth-order autocorrelation function of the photoluminescence signal, we show the possibility, in some cases, to resolve in principle arbitrarily close emitting centers.
Solid state quantum emitters have shown strong potential for applications in quantum information, but spectral inhomogeneity of these emitters poses a significant challenge. We address this issue in a cavity-quantum dot system by demonstrating cavity-stimulated Raman spin flip emission. This process avoids populating the excited state of the emitter and generates a photon that is Raman shifted from the laser and enhanced by the cavity. The emission is spectrally narrow and tunable over a range of at least 125 GHz, which is two orders of magnitude greater than the natural linewidth. We obtain t…
We introduce a scheme of single photon emission based on four-wave mixing in a three mode system with weak Kerr-type nonlinearity. A highly populated lower energy mode results in strong stimulated scattering of particle pairs out of the central mode, which consequently limits the central mode occupation. Thus, the system can be reduced to a $χ^{(2)}$ nonlinear medium with greatly enhanced interaction constant. As a model setup we consider dipolaritons in semiconductor microcavities. Using the master equation approach we show strong antibunching under continuous wave pump, which largely exceeds…
Despite advances in low-light level detection, single-photon methods such as photon correlation have rarely been used in the context of imaging. The few demonstrations, for example of sub-diffraction limited imaging utilizing quantum statistics of photons, have remained in the realm of proof-of-principle demonstrations. This is primarily due to a combination of low values of fill factors, quantum efficiencies, frame rates and signal-to-noise characteristic of most available single-photon sensitive imaging detectors. Here we describe an imaging device based on a fiber bundle coupled to single-p…
The coherent interaction of electromagnetic fields with solid-state two-level systems can yield deterministic quantum light sources for photonic quantum technologies. To date, the performance of semiconductor single-photon sources based on three-level systems is limited mainly due to a lack of high photon indistinguishability. Here, we tailor the cavity-enhanced spontaneous emission from a ladder-type three-level system in a single epitaxial quantum dot (QD) through stimulated emission. After populating the biexciton (XX) of the QD through two-photon resonant excitation (TPE), we use another l…
Plasmon-enhanced Raman scattering (PERS) becomes nonlinear when phonon pumping and phonon-stimulated scattering come into play. It is fundamental to the understanding of PERS and its photobleaching behavior. By quantization of the molecular vibration coherent state into phonon number states, we theoretically predict a stepwise dependence of PERS intensity on laser power. Experimental evidence is presented by measuring a monolayer of malachite green isothiocyanate molecules sandwiched in individual gold nanosphere-plane antennas, under radially polarized laser excitation of sub-microWatt powers…
We discuss the possible role of quantum horizon fluctuations on black hole radiance, especially whether they can invalidate Hawking's analysis based upon transplanckian modes. We are particularly concerned with ``enhanced'' fluctuations produced by gravitons or matter fields in squeezed vacuum states sent into the black hole after the collapse process. This allows for the possibility of increasing the fluctuations well above the vacuum level. We find that these enhanced fluctuations could significantly alter stimulated emission but have little effect upon the spontaneous emission. Thus the the…
As charged particles surpass the speed of light in an optical medium they produce radiation - analogously to the way jet planes surpass the speed of sound and produce a sonic boom. This radiation emission, known as the Cherenkov effect, is among the most fundamental processes in electrodynamics. As such, it is used in numerous applications of particle detectors, particle accelerators, light sources, and medical imaging. Surprisingly, all Cherenkov-based applications and experiments thus far were fully described by classical electrodynamics even though theoretical work predicts new Cherenkov ph…
Two-photon excited fluorescence (TPEF) is a standard technique in modern microscopy but still affected by photo-damage of the probe. It was proposed that TPEF can be enhanced by using entangled photons, but has proven to be challenging. Recently it was shown that some features of entangled photons can be mimicked with thermal light, which finds application in ghost imaging, sub-wavelength lithography and metrology. Here, we utilize true thermal light from a super-luminescence diode to demonstrate enhanced TPEF compared to coherent light using two common fluorophores and luminescent quantum dot…
