It has been observed experimentally [H.R. Xia, C.Y. Ye, and S.Y. Zhu, Phys. Rev. Lett. {\bf 77}, 1032 (1996)] that quantum interference between two molecular transitions can lead to a suppression or enhancement of spontaneous emission. This is manifested in the fluorescent intensity as a function of the detuning of the driving field from the two-photon resonance condition. Here we present a theory which explains the observed variation of the number of peaks with the mutual polarization of the molecular transition dipole moments. Using master equation techniques we calculate analytically as well as numerically the steady-state fluorescence, and find that the number of peaks depends on the excitation process. If the molecule is driven to the upper levels by a two-photon process, the fluorescent intensity consists of two peaks regardless of the mutual polarization of the transition dipole moments. If the excitation process is composed of both a two-step one-photon process and a one-step, two-photon process, then there are two peaks on transitions with parallel dipole moments and three peaks on transitions with antiparallel dipole moments. This latter case is in excellent agreement with the experiment.
The fluorescence light emitted by a 4-level system in $J=1/2$ to $J=1/2$ configuration driven by a monochromatic laser field and in an external magnetic field is studied. We show that the spectrum of resonance fluorescence emitted on the $π$ transitions shows a signature of spontaneously generated interference effects. The degree of interference in the fluorescence spectrum can be controlled by means of the external magnetic field, provided that the Landé g-factors of the excited and the ground state doublet are different. For a suitably chosen magnetic field strength, the relative weight of t…
The squeezing spectrum of the resonance fluorescence is studied for a coherently driven four-level atom in the Y-type configuration. It is found that the squeezing properties of the fluorescence radiation are modified significantly when quantum interference of the spontaneous decays channels is included. We show a considerable enhancement of steady-state squeezing in spectral components for strong and off-resonant driving fields. The squeezing may be increased in both the inner and outer sidebands of the spectrum depending upon the choice of parameters. We also show that the interference can d…
Photon correlations are investigated for a single laser-excited ion trapped in front of a mirror. Varying the relative distance between the ion and the mirror, photon correlation statistics can be tuned smoothly from an antibunching minimum to a bunching-like maximum. Our analysis concerns the non-Markovian regime of the ion-mirror interaction and reveals the field establishment in a half-cavity interferometer.
We discuss the spontaneous emission from a coherently prepared and microwave driven doublet of potentially closely spaced excited states to a common ground level. Multiple interference mechanisms are identified which may lead to fluorescence inhibition in well-separated regions of the spectrum or act jointly in cancelling the spontaneous emission. In addition to phase independent quantum interferences due to combined absorptions and emissions of driving field photons, we distinguish two competing phase dependent interference mechanisms as means of controlling the fluorescence. The indistinguis…
We study the resonance fluorescence from a coherently driven four-level atom in the Y-type configuration. The effects of quantum interference induced by spontaneous emission on the fluorescence properties of the atom are investigated. It is found that the quantum interference resulting from cascade emission decays of the atom leads to a splitting of resonances in the excited level populations calculated as a function of light detuning. For some parameters, interference assisted enhancement of inner sidebands and narrowing of central peaks may also occur in the fluorescence spectrum. We present…
In quantum physics, measurement results are random but their statistics can be predicted assuming some knowledge about the system in the past. Additional knowledge from a future measurement deeply changes the statistics in the present and leads to purely quantum features. In particular conditioned average outcomes of a weak measurement, so-called weak values, were shown to go beyond the conventional range, give a way to directly measure complex quantities, and can be used to enhance the sensitivity of quantum meters. Recently, these concepts have been considered in the general case of open qua…
We report the phase control of spatial interference of resonance fluorescence from two duplicated two-level atoms, driving by two orthogonally polarized fields. In this closed-loop system, the relative phase is of crucial importance to the recovery of the interference patten in the fluorescence light even with strong driving.In order to improve the experimental realizability, we propose a scheme to recover the visibility with fixed relative phase by adjusting the relative intensities between the two driving fields or alternatively by using a standing-wave field.
Resonance fluorescence from a quantum emitter is an ideal source to extract indistinguishable photons. By using the cross polarization to suppress the laser scattering, we observed resonance fluorescence from GeV color centers in diamond at cryogenic temperature. The Fourier-transform-limited linewidth emission with $T_2/2T_1\sim0.86$ allows for two-photon interference based on single GeV color center. Under pulsed excitation, the 24 ns separated photons exhibit a Hong-Ou-Mandel visibility of $0.604\pm0.022$, while the continuous-wave excitation leads to a coalescence time window of 1.05 radia…
Stochastic perturbation of two-level atoms strongly driven by a coherent light field is analyzed by the quantum trajectory method. A new method is developed for calculating the resonance fluorescence spectra from numerical simulations. It is shown that in the case of dominant incoherent perturbation, the stochastic noise can unexpectedly create phase correlation between the neighboring atomic dressed states. This phase correlation is responsible for quantum interference between the related transitions resulting in anomalous modifications of the resonance fluorescence spectra.
Crossovers between Time-Bin and Energy-Time Entanglement in Homodyned Resonance Fluorescence
Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）；Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所凝聚态物理国家实验室）；University of Chinese Academy of Sciences（中国科学院大学）
We report measurements of an intensity-field correlation function of the resonance fluorescence of a single trapped Ba+ ion. Detection of a photon prepares the atom in its ground state and we observe its subsequent evolution under interaction with a laser field of well defined phase. We record the regression of the resonance fluorescence source field. This provides a direct measurement of the field of the radiating dipole of a single atom and exhibits its strong non-classical behavior. In the experimental setup an interference measurement is conditioned on a fluorescence photon detection. The …
We observe quantum interference of photons emitted by two continuously laser-excited single ions, independently trapped in distinct vacuum vessels. High contrast two-photon interference is observed in two experiments with different ion species, calcium and barium. Our experimental findings are quantitatively reproduced by Bloch equation calculations. In particular, we show that the coherence of the individual resonance fluorescence light field is determined from the observed interference.
We report the first experimental demonstration of interference-induced spectral line elimination predicted by Zhu and Scully [Phys. Rev. Lett. 76, 388 (1996)] and Ficek and Rudolph [Phys. Rev. A 60, 4245 (1999)]. We drive an exciton transition of a self-assembled quantum dot in order to realize a two-level system exposed to bichromatic laser field and observe nearly complete elimination of the resonance fluorescence spectral line at the driving laser frequency. This is caused by quantum interference between coupled transitions among the doubly dressed excitonic states, without population trapp…
We present a general input-output formalism for the few-photon transport in multiple waveguide channels coupled to a local cavity. Using this formalism, we study the effect of Fano interference in two-photon quantum transport. We show that the physics of Fano interference can manifest as an asymmetric spectral line shape in the frequency dependence of the two-photon correlation function. The two-photon fluorescence spectrum, on the other hand, does not exhibit the physics of Fano interference.
This review presents the Laser-Induced Fluorescence Spectroscopy (LIFS) of trapped gas-phase molecular ions. A brief description of the theory and experimental approaches involved in fluorescence spectroscopy, together with state-of-the-art LIFS experiments employing ion traps, is presented. Quadrupole ion traps are commonly used for spatial confinement of ions. One of the main challenges involved in such experiments is poor Signal-to-Noise Ratio (SNR) arising due to weak gas-phase fluorescence emission, high background noise, and small solid angle for the fluorescence collection optics. The e…
We demonstrate how the anisotropy of the vacuum of the electromagnetic field can lead to quantum interferences among the decay channels of close lying states. Our key result is that interferences are given by the {\em scalar} formed from the antinormally ordered electric field correlation tensor for the anisotropic vacuum and the dipole matirx elements for the two transitions. We present results for emission between two conducting plates as well as for a two photon process involving fluorescence produced under coherent cw excitation
We demonstrate an optical method for detecting the mechanical oscillations of an atom with single-phonon sensitivity. The measurement signal results from the interference between the light scattered by a single trapped atomic ion and that of its mirror image. The motion of the atom modulates the interference path length and hence the photon detection rate. We detect the oscillations of the atom in the Doppler cooling limit and reconstruct average trajectories in phase space. We demonstrate single-phonon sensitivity near the ground state of motion after EIT cooling. These results could be appli…
We collect the fluorescence from two trapped atomic ions, and measure quantum interference between photons emitted from the ions. The interference of two photons is a crucial component of schemes to entangle atomic qubits based on a photonic coupling. The ability to preserve the generated entanglement and to repeat the experiment with the same ions is necessary to implement entangling quantum gates between atomic qubits, and allows the implementation of protocols to efficiently scale to larger numbers of atomic qubits.
We describe in this Letter how inhomogeneous line broadening affects the Autler-Townes (AT) splitting in a three level open molecular cascade system. For moderate Rabi frequencies in the range of 300 to 500 MHz the fluorescence line shape from the uppermost level |3> in this system depends strongly on the frequency ratio of the two laser fields. However, the fluorescence spectrum of the intermediate level |2> appears as expected. We provide a description of the conditions for optimally resolved AT splitting in terms of the probe laser/coupling field frequency ratio and laser propagation geomet…
The effect of the laser linewidth on the resonance fluorescence spectrum of a two-level atom is revisited. The novel spectral features, such as hole-burning and dispersive profiles at line centre of the fluorescence spectrum are predicted when the laser linewidth is much greater than its intensity. The unique features result from quantum interference between different dressed-state transition channels.
We discuss quantum interference effects in a three-level atom in lambda-configuration, where both transitions from the upper state to the lower states are driven by a single monochromatic laser field. Although the system has two lower states, quantum interference is possible because there are interfering pathways to each of the two lower states. The additional interference terms allow for interesting effects such as the suppression of a dark state which is present without the interference. Finally we examine a narrow spectral feature in the resonance fluorescence of the atom with quantum inter…
The wave-particle duality of massive objects is a cornerstone of quantum physics and a key property of many modern tools such as electron microscopy, neutron diffraction or atom interferometry. Here we report on the first experimental demonstration of quantum interference lithography with complex molecules. Molecular matter-wave interference patterns are deposited onto a reconstructed Si(111) 7x7 surface and imaged using scanning tunneling microscopy. Thereby both the particle and the quantum wave character of the molecules can be visualized in one and the same image. This new approach to nano…
We discuss the connection between quantum interference effects in optical beams and radiation fields emitted from atomic systems. We illustrate this connection by a study of the first- and second-order correlation functions of optical fields and atomic dipole moments. We explore the role of correlations between the emitting systems and present examples of practical methods to implement two systems with non-orthogonal dipole moments. We also derive general conditions for quantum interference in a two-atom system and for a control of spontaneous emission. The relation between population trapping…
The interference pattern of the resonance fluorescence from a J=1/2 to J=1/2 transition of two identical atoms confined in a three-dimensional harmonic potential is calculated. Thermal motion of the atoms is included. Agreement is obtained with experiments [Eichmann et al., Phys. Rev. Lett. 70, 2359 (1993)]. Contrary to some theoretical predictions, but in agreement with the present calculations, a fringe visibility greater than 50% can be observed with polarization-selective detection. The dependence of the fringe visibility on polarization has a simple interpretation, based on whether or not…
We calculate the second-order correlation function for the atomic fluorescence in the two-photon resonance operation of a driven dissipative Jaynes-Cummings oscillator. We employ a minimal four-level model comprising the driven two-photon transition alongside two intermediate states visited in the dissipative cascaded process, in the spirit of [S. S. Shamailov et al., Opt. Commun. 283, 766 (2010)]. We point to the difference between the output of a JC oscillator exhibiting two-photon blockade and the scattered field of ordinary resonance fluorescence, and discuss the quantum interference effec…
We present an optical scheme to detect the oscillations of a two-ion string confined in a linear Paul trap. The motion is detected by analyzing the intensity correlations in the fluorescence light emitted by one or two ions in the string. We present measurements performed under continuous Doppler cooling and under pulsed illumination. We foresee several direct applications of this detection method, including motional analysis of multi-ion species or coupled mechanical oscillators, and sensing of mechanical correlations.
We demonstrate a superconducting artificial atom with strong unidirectional coupling to a microwave photonic waveguide. Our artificial atom is realized by coupling a transmon qubit to the waveguide at two spatially separated points with time-modulated interactions. Direction-sensitive interference arising from the parametric couplings in our scheme results in a non-reciprocal response, where we measure a forward/backward ratio of spontaneous emission exceeding 100. We verify the quantum nonlinear behavior of this artificial chiral atom by measuring the resonance fluorescence spectrum under a s…
The dispersion cancellation observed in Hong-Ou-Mandel (HOM) interference between frequency-entangled photon pairs has been the basis of quantum optical coherence tomography and quantum clock synchronization. Here we explore the effect of phase dispersion on ultranarrow HOM dips. We show that the higher-order dispersion, the line width of the pump laser, and the spectral shape of the parametric fluorescence have a strong effect on the dispersion cancellation in the high-resolution regime with several experimental verifications. Perfect dispersion cancellation with a linewidth of 3μm is also de…
Cavity polaritonics is capturing the imagination of the chemistry community because of the novel opportunities it creates to direct chemistry. Electron transfer (ET) reactions are among the simplest reactions, and they also underpin bioenergetics. As such, new conceptual strategies to manipulate and direct electron flow at the nanoscale are of wide-ranging interest in biochemistry, energy science, bio-inspired materials science, and chemistry. We show that optical cavities can modulate electron transfer pathway interferences and ET rates in donor-bridge-acceptor (DBA) systems. We derive the ra…
We investigate interference and correlation effects when several detuned emitters are placed along a one-dimensional photonic waveguide. Such a setup allows multiple interactions between the photons and the strongly coupled emitters, and underlies proposed devices for quantum information processing. We show, first, that a pair of detuned two-level systems (2LS) separated by a half wavelength mimic a driven Λ-type three-level system (3LS) in both the single- and two- photon sectors. There is an interference-induced transparency peak at which the fluorescence is quenched, leaving the transmitted…
High spin magnetic molecules are promising candidates for quantum information processing because they intrinsically have multiple sublevels for information storage and computational operations. However, due to their susceptibility to the environment and limitation from the selection rule, the arbitrary control of the quantum state of a multilevel system on a molecular and electron spin basis has not been realized. Here we exploit the photoexcited triplet of C70 as a molecular electron spin qutrit. After the system was initialized by photoexcitation, we prepared it into representative three-lev…
