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1.
Phys Rev Lett ; 125(4): 043603, 2020 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-32794814

RESUMO

Spectral filtering of resonance fluorescence is widely employed to improve single photon purity and indistinguishability by removing unwanted backgrounds. For filter bandwidths approaching the emitter linewidth, complex behavior is predicted due to preferential transmission of components with differing photon statistics. We probe this regime using a Purcell-enhanced quantum dot in both weak and strong excitation limits, finding excellent agreement with an extended sensor theory model. By changing only the filter width, the photon statistics can be transformed between antibunched, bunched, or Poissonian. Our results verify that strong antibunching and a subnatural linewidth cannot simultaneously be observed, providing new insight into the nature of coherent scattering.

2.
Phys Rev Lett ; 124(15): 153602, 2020 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-32357066

RESUMO

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 organic 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 localized vibrational modes of the molecule and a thermal phonon bath, which we include nonperturbatively, and is able to 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 characterization of the photon coherence of molecules, paving the way to their use in future quantum information applications.

3.
Phys Rev Lett ; 123(16): 167403, 2019 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-31702333

RESUMO

Coherent scattering of light by a single quantum emitter is a fundamental process at the heart of many proposed quantum technologies. Unlike atomic systems, solid-state emitters couple to their host lattice by phonons. Using a quantum dot in an optical nanocavity, we resolve these interactions in both time and frequency domains, going beyond the atomic picture to develop a comprehensive model of light scattering from solid-state emitters. We find that even in the presence of a low-Q cavity with high Purcell enhancement, phonon coupling leads to a sideband that is completely insensitive to excitation conditions and to a nonmonotonic relationship between laser detuning and coherent fraction, both of which are major deviations from atomlike behavior.

4.
Phys Rev Lett ; 123(9): 093601, 2019 Aug 30.
Artigo em Inglês | MEDLINE | ID: mdl-31524488

RESUMO

We show that for a quantum system coupled to both vibrational and electromagnetic environments, enforcing additivity of their combined influences results in nonequilibrium dynamics that does not respect the Franck-Condon principle. We overcome this shortcoming by employing a collective coordinate representation of the vibrational environment, which permits the derivation of a nonadditive master equation. When applied to a two-level emitter our treatment predicts decreasing photon emission rates with increasing vibrational coupling, consistent with Franck-Condon physics. In contrast, the additive approximation predicts the emission rate to be completely insensitive to vibrations. We find that nonadditivity also plays a key role in the stationary nonequilibrium model behavior, enabling two-level population inversion under incoherent electromagnetic excitation.

5.
Phys Rev Lett ; 123(2): 023603, 2019 Jul 12.
Artigo em Inglês | MEDLINE | ID: mdl-31386531

RESUMO

We show how to create maximal entanglement between spectrally distinct solid-state emitters embedded in a waveguide interferometer. By revealing the rich underlying structure of multiphoton scattering in emitters, we show that a two-photon input state can generate deterministic maximal entanglement even for emitters with significantly different transition energies and linewidths. The optimal frequency of the input is determined by two competing processes: which-path erasure and interaction strength. We find that smaller spectral overlap can be overcome with higher photon numbers, and quasimonochromatic photons are optimal for entanglement generation. Our work provides a new methodology for solid-state entanglement generation, where the requirement for perfectly matched emitters can be relaxed in favor of optical state optimization.

6.
Nat Commun ; 10(1): 3034, 2019 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-31292447

RESUMO

Vibrational environments are commonly considered to be detrimental to the optical emission properties of solid-state and molecular systems, limiting their performance within quantum information protocols. Given that such environments arise naturally it is important to ask whether they can instead be turned to our advantage. Here we show that vibrational interactions can be harnessed within resonance fluorescence to generate optical states with a higher degree of quadrature squeezing than in isolated atomic systems. Considering the example of a driven quantum dot coupled to phonons, we demonstrate that it is feasible to surpass the maximum level of squeezing theoretically obtainable in an isolated atomic system and indeed come close to saturating the fundamental upper bound on squeezing from a two-level emitter. We analyse the performance of these vibrationally-enhanced squeezed states in a phase estimation protocol, finding that for the same photon flux, they can outperform the single mode squeezed vacuum state.

7.
Nat Nanotechnol ; 14(6): 586-593, 2019 06.
Artigo em Inglês | MEDLINE | ID: mdl-31011221

RESUMO

The generation of high-quality entangled photon pairs has been a long-sought goal in modern quantum communication and computation. So far, the most widely used entangled photon pairs have been generated from spontaneous parametric down-conversion (SPDC), a process that is intrinsically probabilistic and thus relegated to a regime of low rates of pair generation. In contrast, semiconductor quantum dots can generate triggered entangled photon pairs through a cascaded radiative decay process and do not suffer from any fundamental trade-off between source brightness and multi-pair generation. However, a source featuring simultaneously high photon extraction efficiency, high degree of entanglement fidelity and photon indistinguishability has been lacking. Here, we present an entangled photon pair source with high brightness and indistinguishability by deterministically embedding GaAs quantum dots in broadband photonic nanostructures that enable Purcell-enhanced emission. Our source produces entangled photon pairs with a pair collection probability of up to 0.65(4) (single-photon extraction efficiency of 0.85(3)), entanglement fidelity of 0.88(2), and indistinguishabilities of 0.901(3) and 0.903(3) (brackets indicate uncertainty on last digit). This immediately creates opportunities for advancing quantum photonic technologies.

8.
Phys Rev Lett ; 118(23): 233602, 2017 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-28644642

RESUMO

We investigate the temperature dependence of photon coherence properties through two-photon interference (TPI) measurements from a single quantum dot (QD) under resonant excitation. We show that the loss of indistinguishability is related only to the electron-phonon coupling and is not affected by spectral diffusion. Through these measurements and a complementary microscopic theory, we identify two independent separate decoherence processes, both of which are associated with phonons. Below 10 K, we find that the relaxation of the vibrational lattice is the dominant contribution to the loss of TPI visibility. This process is non-Markovian in nature and corresponds to real phonon transitions resulting in a broad phonon sideband in the QD emission spectra. Above 10 K, virtual phonon transitions to higher lying excited states in the QD become the dominant dephasing mechanism, this leads to a broadening of the zero phonon line, and a corresponding rapid decay in the visibility. The microscopic theory we develop provides analytic expressions for the dephasing rates for both virtual phonon scattering and non-Markovian lattice relaxation.

9.
J Chem Phys ; 144(4): 044110, 2016 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-26827205

RESUMO

We explore excitonic energy transfer dynamics in a molecular dimer system coupled to both structured and unstructured oscillator environments. By extending the reaction coordinate master equation technique developed by Iles-Smith et al. [Phys. Rev. A 90, 032114 (2014)], we go beyond the commonly used Born-Markov approximations to incorporate system-environment correlations and the resultant non-Markovian dynamical effects. We obtain energy transfer dynamics for both underdamped and overdamped oscillator environments that are in perfect agreement with the numerical hierarchical equations of motion over a wide range of parameters. Furthermore, we show that the Zusman equations, which may be obtained in a semiclassical limit of the reaction coordinate model, are often incapable of describing the correct dynamical behaviour. This demonstrates the necessity of properly accounting for quantum correlations generated between the system and its environment when the Born-Markov approximations no longer hold. Finally, we apply the reaction coordinate formalism to the case of a structured environment comprising of both underdamped (i.e., sharply peaked) and overdamped (broad) components simultaneously. We find that though an enhancement of the dimer energy transfer rate can be obtained when compared to an unstructured environment, its magnitude is rather sensitive to both the dimer-peak resonance conditions and the relative strengths of the underdamped and overdamped contributions.

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