Indistinguishable Photons from a Single Molecule

Kiraz, Alper; Ehrl, M.; Hellerer, Th; Müstecaplıoğlu, Özgür E.; Bräuchle, Christoph; Zumbusch, Andreas

doi:10.1103/physrevlett.94.223602

Cited by 81 publications

(62 citation statements)

References 26 publications

(50 reference statements)

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“…Under continuous-wave (CW) laser excitation, a high degree of indistinguishability for continuously generated RF photons has been demonstrated through post-selective HOM interference [25]. However, in the CW regime, as the emission time of the RF photons is uncontrolled, the HOM interference relies on the finite single-photon detection time resolution to discriminate and post-select a small fraction of photons that overlapped on the beam-splitter at the same time [25][26][27]. Therefore, the obtained interference visibility needs to be convoluted with-and is thus limited by-the realistic detection time response.…”

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confidence: 99%

On-demand semiconductor single-photon source with near-unity indistinguishability

et al. 2013

Nature Nanotech

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Single photon sources based on semiconductor quantum dots offer distinct advantages for quantum information, including a scalable solid-state platform, ultrabrightness, and interconnectivity with matter qubits. A key prerequisite for their use in optical quantum computing and solid-state networks is a high level of efficiency and indistinguishability. Pulsed resonance fluorescence (RF) has been anticipated as the optimum condition for the deterministic generation of high-quality photons with vanishing effects of dephasing. Here, we generate pulsed RF single photons on demand from a single, microcavity-embedded quantum dot under s-shell excitation with 3-ps laser pulses. The π-pulse excited RF photons have less than 0.3% background contributions and a vanishing two-photon emission probability. Non-postselective Hong-Ou-Mandel interference between two successively emitted photons is observed with a visibility of 0.97(2), comparable to trapped atoms and ions. Two single photons are further used to implement a high-fidelity quantum controlled-NOT gate.Single photons have been proposed as promising quantum bits (qubits) for quantum communication [1], linear optical quantum computing [2, 3] and as messengers in quantum networks [4]. These proposals primarily rely upon a high degree of indistinguishability between individual photons to obtain the Hong-Ou-Mandel (HOM) type interference [5] which is at the heart of photonic controlled logic gates and photon-interference-mediated quantum networking [1][2][3][4].Among different types of single-photon emitters [6, 7], quantum dots (QDs) are attractive solid-state devices since they can be embedded in high-quality nanostructure cavities and waveguides to generate ultra-bright sources of single and entangled photons [7][8][9][10]. QDs also provide a light-matter interface [11][12][13] and can in principle be scaled to large quantum networks [14]. Two-photon HOM interference experiments using photons from a single QD [5,15,17], as well as from independent sources [18,19], have not only demonstrated the potential of QDs as single-photon sources, but also revealed the level of dephasing arising from incoherent excitation. The method of incoherent pumping (via above band-gap or p-shell excitation) typically causes reduced photon coherence times due to homogeneous broadening of the excited state [5] and uncontrolled emission time jitter from the nonradiative high-level to s-shell relaxation [6], leading to a decrease of photon indistinguishability.To eliminate these dephasings, an increasing effort has been devoted to s-shell resonant optical excitation of QDs. The Mollow triplet spectra and photon correlations of the resonance fluorescence (RF) have been measured [1][2][3]21]. Under continuous-wave (CW) laser excitation, a high degree of indistinguishability for continuously generated RF photons has been demonstrated through post-selective HOM interference [25]. However, in the CW regime, as the emission time of the RF photons is uncontrolled, the HOM interference relies on th...

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confidence: 99%

On-demand semiconductor single-photon source with near-unity indistinguishability

et al. 2013

Nature Nanotech

501

351

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“…Indistinguishable photons are usually generated either using parametric down conversion [10], or alternatively directly from a single two-level quantum emitter such as atoms, color centers, quantum dots or organic molecules [11][12][13][14][15][16][17][18][19][20]. Parametric down conversion is presently the most mature technology available, but the usual low efficiency of the nonlinear processes is a severe limitation to the scalability of such sources.…”

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confidence: 99%

Cavity-Funneled Generation of Indistinguishable Single Photons from Strongly Dissipative Quantum Emitters

et al. 2015

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We investigate theoretically the generation of indistinguishable single photons from a strongly dissipative quantum system placed inside an optical cavity. The degree of indistinguishability of photons emitted by the cavity is calculated as a function of the emitter-cavity coupling strength and the cavity linewidth. For a quantum emitter subject to strong pure dephasing, our calculations reveal that an unconventional regime of high indistinguishability can be reached for moderate emittercavity coupling strengths and high quality factor cavities. In this regime, the broad spectrum of the dissipative quantum system is funneled into the narrow lineshape of the cavity. The associated efficiency is found to greatly surpass spectral filtering effects. Our findings open the path towards on-chip scalable indistinguishable-photon emitting devices operating at room temperature.Indistinguishable single photons are the building blocks of various optically-based quantum information applications such as linear optical quantum computing [1, 2], boson sampling [3][4][5][6][7], quantum teleportation [8] or quantum networks [9]. Indistinguishable photons are usually generated either using parametric down conversion [10], or alternatively directly from a single two-level quantum emitter such as atoms, color centers, quantum dots or organic molecules [11][12][13][14][15][16][17][18][19][20]. Parametric down conversion is presently the most mature technology available, but the usual low efficiency of the nonlinear processes is a severe limitation to the scalability of such sources. On the other hand, sources based on single solid-state quantum systems have been greatly developped in the last decade, as they hold the promise to combine indistinguishable, on-demand, energy-efficient, electrically drivable and scalable characteristics. However, except at cryogenics temperature, solid-state systems emitting single-photons are subject to strong pure dephasing processes [21][22][23][24][25][26][27][28][29], making them at first view inappropriate for quantum applications requiring photon indistinguishability.A two-level quantum emitter (QE) coupled only to vacuum fluctuations should emit perfectly indistinguishable photons. However, as soon as pure dephasing of the QE occurs, the degree of indistinguishability of the emitted photons is reduced to [30]where γ = 1/T 1 is the population decay rate, γ * /2 = 1/T * 2 the pure dephasing rate, and 1/T 2 = 2/T 1 + 1/T 2 * the total dephasing rate. For solid-state QE emitting photons at room temperature such as color centers, quantum dots or organic molecules, pure dephasing rates are typically several orders of magnitude larger than the population decay rate (typically ranging from 3 to 6 orders of magnitude) [12,14,21,22,24,[26][27][28][29]31]. Hence the intrinsic indistinguishability given by Eq. 1 is almost zero. A possible way to enhance the indistinguishability is to spectrally filter the emitted photons a posteriori. However, this linear-filter strategy leads to a very low efficiency. Engin...

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“…Recent efforts [1][2][3] have shown that organic dye molecules might offer a superior alternative if one could suppress the incoherent decay of the excited state. In this work, we present a versatile microcavity architecture that can enhance the Fourier-limited transition between the v=0 vibrational levels of the electronic excited and ground states (labeled γ 0−0 in Fig.…”

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confidence: 99%

“…Combined with a modest radius of curvature of 100 µm, such mirrors would allow Purcell factors up to 1000. Accounting for the reduction of this effect due to the finite modal solid angle, such a cavity would enhance the 0-0 spontaneous emission by about 20 times and improve the fraction of the emission in this channel from 30% [20] to about 85% if one operates at liquid helium temperatures, where 0-0 linewidths under 1 GHz are common [1][2][3]. Further reduction of the radius of curvature of the fiber mirror would lower the mode volume and allow branching ratios as large as 98%.…”

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A scanning microcavity for in situ control of single-molecule emission

Toninelli

Delley

Stöferle

et al. 2010

Applied Physics Letters

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We report on the fabrication and characterization of a scannable Fabry-Perot microcavity, consisting of a curved micromirror at the end of an optical fiber and a planar distributed Bragg reflector. Furthermore, we demonstrate the coupling of single organic molecules embedded in a thin film to well-defined resonator modes. We discuss the choice of cavity parameters that will allow sufficiently high Purcell factors for enhancing the zero-phonon transition between the vibrational ground levels of the electronic excited and ground states.

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Indistinguishable Photons from a Single Molecule

Cited by 81 publications

References 26 publications

On-demand semiconductor single-photon source with near-unity indistinguishability

On-demand semiconductor single-photon source with near-unity indistinguishability

Cavity-Funneled Generation of Indistinguishable Single Photons from Strongly Dissipative Quantum Emitters

A scanning microcavity for in situ control of single-molecule emission

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