Few-photon coherent nonlinear optics with a single molecule

Maser, A.; Gmeiner, Björn; Utikal, Tobias; Götzinger, Stephan; Sandoghdar, Vahid

doi:10.1038/nphoton.2016.63

Cited by 85 publications

(76 citation statements)

References 141 publications

(251 reference statements)

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“…46 Our findings and methodology provide interesting possibilities for new experiments that require stable single molecules in the vicinity of nanoscopic boundaries such as plasmonic antennas 47,48 and subwavelength waveguides 20 and for quantum nano-optical measurements that benefit from tight focusing. 49 Furthermore, we believe that the agglomeration of dye molecules at crystal domain boundaries in microscopic and nanoscopic samples facilitates finding dipole-coupled molecules. 50 …”

Section: Discussionmentioning

confidence: 98%

Spectroscopy and microscopy of single molecules in nanoscopic channels: spectral behavior vs. confinement depth

Gmeiner

Maser

Utikal

et al. 2016

Phys. Chem. Chem. Phys.

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We perform high-resolution spectroscopy and localization microscopy to study single dye molecules confined to nanoscopic dimensions in one direction. We provide the fabrication details of our nanoscopic glass channels and the procedure for filling them with organic matrices. Optical data on hundreds of molecules in different channel depths show a clear trend from narrow stable lines in deep channels to broader linewidths in ultrathin matrices. In addition, we observe a steady blue shift of the center of the inhomogeneous band as the channels become thinner. Furthermore, we use super-resolution localization microscopy to correlate the positions and orientations of the individual dye molecules with the lateral landscape of the organic matrix, including cracks and strain-induced dislocations. Our results and methodology are useful for a number of studies in various fields such as physical chemistry, solid-state spectroscopy, and quantum nano-optics.

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Section: Discussionmentioning

confidence: 98%

Spectroscopy and microscopy of single molecules in nanoscopic channels: spectral behavior vs. confinement depth

Gmeiner

Maser

Utikal

et al. 2016

Phys. Chem. Chem. Phys.

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“…This relation (37) has important physical consequences to single-photon scattering experiments in waveguide QED, as it demonstrates that applying a Fourier transformation on the usual transmittance data [3,5,11,59,60,73,74], one can characterize noise correlations without requiring direct access and timedependent control of the emitter. Moreover, equation (37) is particularly convenient in the case of power 6 Inverting equation (24) in the general case leads to C t t t 2 e 1…”

Section: Results Of the Protocolmentioning

confidence: 99%

“…This section introduces a simple experimental protocol to measure the average single-photon transmittance and reflectance, and to recover the correlated dephasing noise from those quantities. This protocol only requires attenuated coherent states and either homodyne or power measurements at the output-the choice of which depends mainly on whether the experiment is performed with microwave [3,5] or optical photons [60,73,74] -. In section 5.1 we summarize and discuss the most important results to apply the protocol, while section 5.2 contains details on the derivation.…”

Section: Spectroscopic Characterization Of Correlated Dephasing Noisementioning

confidence: 99%

Correlated dephasing noise in single-photon scattering

Ramos

García-Ripoll

2018

New J. Phys.

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We develop a theoretical framework to describe the scattering of photons against a two-level quantum emitter with arbitrary correlated dephasing noise. This is particularly relevant to waveguide-QED setups with solid-state emitters, such as superconducting qubits or quantum dots, which couple to complex dephasing environments in addition to the propagating photons along the waveguide. Combining input-output theory and stochastic methods, we predict the effect of correlated dephasing in single-photon transmission experiments with weak coherent inputs. We discuss homodyne detection and photon counting of the scattered photons and show that both measurements give the modulus and phase of the single-photon transmittance despite the presence of noise and dissipation. In addition, we demonstrate that these spectroscopic measurements contain the same information as standard time-resolved Ramsey interferometry, and thus they can be used to fully characterize the noise correlations without direct access to the emitter. The method is exemplified with paradigmatic correlated dephasing models such as colored Gaussian noise, white noise, telegraph noise, and 1/fnoise, as typically encountered in solid-state environments.quantum emitter in addition to the dissipative dynamics due to the coupling to photons in the waveguide. We then relate the correlations in that noise to the average scattering matrix of individual photons and coherent wavepackets, and develop strategies to extract those correlations from actual experiments, in conjunction with earlier approaches to scattering tomography [49].The paper and our main results are organized as follows. In section 2 we introduce the model for a noisy twolevel emitter in a waveguide. We describe dephasing noise as a stationary stochastic process Δ(t) and derive the stochastic input-output equations. In section 3, we review the standard procedure of Ramsey interferometry and show how to quantify the noise correlations via the Ramsey envelope C f (t). We also introduce paradigmatic correlated noise models, which will be essential to understand the scattering results in the next sections. In particular, section 4 shows that the same information provided by Ramsey spectroscopy can be obtained from single-photon scattering experiments, where we only manipulate the qubit through the scattered photons. We solve the stochastic input-output equations for a qubit that interacts with a single propagating photon, and show that the averaged single-photon scattering matrix can be related one-to-one to the Ramsey envelope. We also discuss analytical predictions for scattering under realistic dephasing models such as colored Gaussian noise and 1/f noise. We show how the noise correlations modify the spectral lineshapes on each case, recovering simple limits such as the Lorentzian profiles that are fitted in most waveguide-QED experiments. Section 5 generalizes these ideas, showing how to measure the averaged scattering matrix using weak coherent state inputs together with homodyne or photon countin...

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“…To this end, we introduce a second laser field which couples the two ground states. As expected for several waves interacting with a nonlinear medium, this gives rise to a new radiation field via an optical wave mixing process [17][18][19][20][21]. Not expected, however, is that if the laser field coupling the atomic ground states is weak enough, the fragile dark states of the cavity EIT system are not destroyed, even when all fields are on resonance with the respective atomic transitions.…”

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confidence: 95%

Continuous Generation of Quantum Light from a Single Ground-State Atom in an Optical Cavity

et al. 2020

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We show an optical wave-mixing scheme that generates quantum light by means of a single three-level atom. The atom couples to an optical cavity and two laser fields that together drive a cycling current within the atom. Weak driving in combination with strong atom-cavity coupling induces transitions between the dark states of the system, accompanied by single-photon emission and suppression of atomic excitation by quantum interference. For strong driving, the system can generate coherent or Schrödinger cat-like fields with frequencies distinct from those of the applied lasers.Many scientific and technological advances during the last decades, across diverse areas of human knowledge, can be associated to the manipulation of light-matter interaction and the generation of light fields in particular. One such achievement is the laser [1]. Here a photon stimulates an atom to decay into the ground state at the expense of the emission of another photon. To amplify this process, the emitting medium (atoms) is placed inside an optical resonator where the repeated reflection of the light allows for a sufficiently strong coupling between the atoms and the field [2]. By decreasing the volume of the optical resonator it is possible to reach a regime where a single atom and a single photon interact strongly, forming an atom-photon molecule. This establishes the research field known as cavity quantum electrodynamics (cavity QED) [3][4][5][6][7][8][9] where the atom-light interaction is controlled at its most fundamental level. Integrating the phenomenon of electromagnetically induced transparency (EIT) [10-12] adds additional capabilities such as allowing an opaque cavity QED system to become transparent [13][14][15][16]. The origin of this effect lies in the destructive interference of different absorption paths, preventing light from being absorbed by the system. We exploit this situation with a three-level atom in a Λ-type level configuration (one excited and two ground states) where one branch is strongly coupled to a mode of an optical resonator and the other to an external laser. In the EIT regime, the system remains in a state known as a dark state, since the atom does not absorb light from the fields.Here we show that this scheme can be used to continuously generate light that is genuinely quantum in nature. To this end, we introduce a second laser field which couples the two ground states. As expected for several waves interacting with a nonlinear medium, this gives rise to a new radiation field via an optical wave mixing process [17][18][19][20][21]. Not expected, however, is that if the laser field coupling the atomic ground states is weak enough, the fragile dark states of the cavity EIT system are not destroyed, even when all fields are on resonance with the respective atomic transitions. We then find that the two lasers in combination with the cavity drive transitions between dark states that differ by one photon in the cavity. Thus, the atomic excitation is suppressed due to the destructive interference of the EI...

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Few-photon coherent nonlinear optics with a single molecule

Cited by 85 publications

References 141 publications

Spectroscopy and microscopy of single molecules in nanoscopic channels: spectral behavior vs. confinement depth

Spectroscopy and microscopy of single molecules in nanoscopic channels: spectral behavior vs. confinement depth

Correlated dephasing noise in single-photon scattering

Continuous Generation of Quantum Light from a Single Ground-State Atom in an Optical Cavity

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