Photon Correlation Experiments Research Articles

(Invited) Quantum Light Emission from Coupled Defect-States in DNA-Functionalized Carbon Nanotubes

Solid-state single-photon sources are the essential building block for quantum photonics and quantum information technologies. The report here illustrates an advanced perspective of implanting coupled fluorescent quantum defects in single-wall carbon nanotubes (SWCNTs) through chemical reactions between the nanotube sidewall and the guanine nucleotides in single-stranded DNA (ssDNA) that coats the nanotube. Through low-temperature photoluminescence spectroscopy and photon correlation experiments, we have revealed that multiple guanine defects within a single ssDNA strand couple together to form a cumulative deep trapping potential supporting a localized quantum state that is capable of room-temperature single-photon emission. Helical wrapping of multiple ssDNA strands in single nanotubes allows a series of exciton localization sites to be created along the length of the SWCNTs. Such unique exciton trapping potential landscape gives rise to previously inaccessible intrinsic emission characteristics including coupling of multiple spatially separated quantum emitters. Our joint experimental and computational studies together reveal quantum emission properties from multiple spatially patterned covalent defects in SWCNTs, identify capture of the band-edge exciton as the underlying cause of the cross-correlated photon emission and open a distinctive prospect for tailoring chemically altered nanotubes as quantum light emitters.

Exciton generation and recombination dynamics of quantum dots embedded in GaNAsP nanowires

Semiconductor quantum dots (QDs) acting as single-photon-emitters are potential building blocks for various applications in future quantum information technology. For such applications, a thorough understanding and precise control of charge states and capture/recombination dynamics of the QDs are vital. In this work, we study the dynamics of QDs spontaneously formed in GaNAsP nanowires, belonging to the dilute nitride material system. By using a random population model modified for these highly mismatched materials, we analyze the results from photoluminescence and photon correlation experiments and show a general trend of disparity in positive and negative trion populations and also a strong dependence of the capture/recombination dynamics and QD charge states on its surroundings. Specifically, we show that the presence of hole-trap defects in the proximity to some QDs facilitates formation of negative trions, which also causes a dramatic reduction of the neutral exciton lifetime. These findings underline the importance of proper understanding of the QD capture and recombination processes and demonstrate the possibility to use highly mismatched materials and defects for charge engineering of QDs.

Efficient Single-Photon Detection with 7.7 ps Time Resolution for Photon-Correlation Measurements

A broad range of scientific and industrial disciplines require precise optical measurements at very low light levels. Single-photon detectors combining high efficiency and high time resolution are pivotal in such experiments. By using relatively thick films of NbTiN (8-11 nm) and improving the pattern fidelity of the nanostructure of the superconducting nanowire single-photon detectors (SNSPD), we fabricated devices demonstrating superior performance over all previously reported detectors in the combination of efficiency and time resolution. Our findings prove that small variations in the nanowire width, in the order of a few nanometers, can lead to a significant penalty on their temporal response. Addressing these issues, we consistently achieved high time resolution (best device 7.7 ps, other devices a10-16 ps) simultaneously with high system detection efficiencies (80-90%) in the wavelength range of 780-1000 nm, as well as in the telecom bands (1310-1550 nm). The use of thicker films allowed us to fabricate large-area multipixel devices with homogeneous pixel performance. We first fabricated and characterized a 100 × 100 μm2 16-pixel detector and showed there was little variation among individual pixels. Additionally, to showcase the power of our platform, we fabricated and characterized 4-pixel multimode fiber-coupled detectors and carried out photon-correlation experiments on a nanowire quantum dot resulting in g2(0) values lower than 0.04. The multipixel detectors alleviate the need for beamsplitters and can be used for higher order correlations with promising prospects not only in the field of quantum optics, but also in bioimaging applications, such as fluorescence microscopy and positron emission tomography.

Cyclic (Amino)(aryl)carbenes Enter the Field of Chromophore Ligands: Expanded π System Leads to Unusually Deep Red Emitting CuI Compounds.

A series of copper(I) complexes bearing a cyclic (amino)(aryl)carbene (CAArC) ligand with various complex geometries have been investigated in great detail with regard to their structural, electronic, and photophysical properties. Comparison of [CuX(CAArC)] (X = Br (1), Cbz (2), acac (3), Ph2acac (4), Cp (5), and Cp* (6)) with known CuI complexes bearing cyclic (amino)(alkyl), monoamido, or diamido carbenes (CAAC, MAC, or DAC, respectively) as chromophore ligands reveals that the expanded π-system of the CAArC leads to relatively low energy absorption maxima between 350 and 550 nm in THF with high absorption coefficients of 5-15 × 103 M-1 cm-1 for 1-6. Furthermore, 1-5 show intense deep red to near-IR emission involving their triplet excited states in the solid state and in PMMA films with λemmax = 621-784 nm. Linear [Cu(Cbz)(DippCAArC)] (2) has been found to be an exceptional deep red (λmax = 621 nm, ϕ = 0.32, τav = 366 ns) thermally activated delayed fluorescence (TADF) emitter with a radiative rate constant kr of ca. 9 × 105 s-1, exceeding those of commercially employed IrIII- or PtII-based emitters. Time-resolved transient absorption and fluorescence upconversion experiments complemented by quantum chemical calculations employing Kohn-Sham density functional theory and multireference configuration interaction methods as well as temperature-dependent steady-state and time-resolved luminescence studies provide a detailed picture of the excited-state dynamics of 2. To demonstrate the potential applicability of this new class of low-energy emitters in future photonic applications, such as nonclassical light sources for quantum communication or quantum cryptography, we have successfully conducted single-molecule photon-correlation experiments of 2, showing distinct antibunching as required for single-photon emitters.

Conditional spectroscopy via nonstationary optical homodyne quantum state tomography

Continuous variable quantum state tomography is one of the most powerful techniques to study the properties of light fields in quantum optics. However, the need for a fixed phase reference has so far prevented widespread usage in other fields such as semiconductor spectroscopy. Here, we introduce non-stationary quantum state tomography, which adapts the technique to the special requirements of ultrafast spectroscopy. In detail, we gain access to the amplitude and phase of light fields with a temporal resolution of about 100\,fs without the need for a fixed phase reference. Further, we show how our technique allows us to perform conditional studies of stochastic dynamics that are inaccessible experimentally by conventional means, and demonstrate the capabilities experimentally by monitoring the stochastic dynamics of a thermal light field on the sub-ps scale. Finally, we discuss differences and similarities to more standard Hanbury Brown-Twiss photon correlation experiments, which may be considered as the discrete variable analogues of our technique.

Surface acoustic wave modulation of single photon emission from GaN/InGaN nanowire quantum dots

On-chip quantum information processing requires controllable quantum light sources that can be operated on-demand at high-speeds and with the possibility of in-situ control of the photon emission wavelength and its optical polarization properties. Here, we report on the dynamic control of the optical emission from core-shell GaN/InGaN nanowire (NW) heterostructures using radio frequency surface acoustic waves (SAWs). The SAWs are excited on the surface of a piezoelectric lithium niobate crystal equipped with a SAW delay line onto which the NWs were mechanically transferred. Luminescent quantum dot (QD)-like exciton localization centers induced by compositional fluctuations within the InGaN nanoshell were identified using stroboscopic micro-photoluminescence (micro-PL) spectroscopy. They exhibit narrow and almost fully linearly polarized emission lines in the micro-PL spectra and a pronounced anti-bunching signature of single photon emission in the photon correlation experiments. When the nanowire is perturbed by the propagating SAW, the embedded QD is periodically strained and its excitonic transitions are modulated by the acousto-mechanical coupling, giving rise to a spectral fine-tuning within a ~1.5 meV bandwidth at the acoustic frequency of ~330 MHz. This outcome can be further combined with spectral detection filtering for temporal control of the emitted photons. The effect of the SAW piezoelectric field on the QD charge population and on the optical polarization degree is also observed. The advantage of the acousto-optoelectric over other control schemes is that it allows in-situ manipulation of the optical emission properties over a wide frequency range (up to GHz frequencies).

Development of a hard X-ray split-and-delay line and performance simulations for two-color pump-probe experiments at the European XFEL.

A hard X-ray Split-and-Delay Line (SDL) under construction for the Materials Imaging and Dynamics station at the European X-Ray Free-Electron Laser (XFEL) is presented. This device aims at providing pairs of X-ray pulses with a variable time delay ranging from -10 ps to 800 ps in a photon energy range from 5 to 10 keV for photon correlation and X-ray pump-probe experiments. A custom designed mechanical motion system including active feedback control ensures that the high demands for stability and accuracy can be met and the design goals achieved. Using special radiation configurations of the European XFEL's SASE-2 undulator (SASE: Self-Amplified Spontaneous Emission), two-color hard x-ray pump-probe schemes with varying photon energy separations have been proposed. Simulations indicate that more than 109 photons on the sample per pulse-pair and up to about 10% photon energy separation can be achieved in the hard X-ray region using the SDL.

Probing dynamical symmetry breaking using quantum-entangled photons

We present an input/output analysis of photon-correlation experiments whereby a quantum mechanically entangled bi-photon state interacts with a material sample placed in one arm of a Hong–Ou–Mandel apparatus. We show that the output signal contains detailed information about subsequent entanglement with the microscopic quantum states in the sample. In particular, we apply the method to an ensemble of emitters interacting with a common photon mode within the open-system Dicke model. Our results indicate considerable dynamical information concerning spontaneous symmetry breaking can be revealed with such an experimental system.

Debye Process and β-Relaxation in 1-Propanol Probed by Dielectric Spectroscopy and Depolarized Dynamic Light Scattering.

We revisit the reorientational dynamics of 1-propanol as a prototype of a monohydroxy alcohol and H-bonding system by dielectric spectroscopy (DS) and depolarized dynamic light scattering (DDLS). In particular, we address the question of whether the Debye relaxation, which is seen as a dominant process in DS, is visible in light scattering and discuss how the Johari-Goldstein (JG) β-process, which is also a prominent feature of the dielectric spectrum, appears in photon correlation spectroscopy. For that purpose we performed depolarized photon correlation experiments with an improved setup and performed additional time domain dielectric experiments which gives us the possibility to compare dielectric and light scattering data in a broad temperature range. It turns out that the improved setup allows to unambiguously identify the JG β-process, which shows almost identical properties in DDLS as in the dielectric spectra, but a Debye relaxation is not present in the DDLS data and can be excluded down to a level of 2.5% of the α-process amplitude.

On the use of two-time correlation functions for X-ray photon correlation spectroscopy data analysis.

Multi-time correlation functions are especially well suited to study non-equilibrium processes. In particular, two-time correlation functions are widely used in X-ray photon correlation experiments on systems out of equilibrium. One-time correlations are often extracted from two-time correlation functions at different sample ages. However, this way of analysing two-time correlation functions is not unique. Here, two methods to analyse two-time correlation functions are scrutinized, and three illustrative examples are used to discuss the implications for the evaluation of the correlation times and functional shape of the correlations.

Multi-exciton emission from solitary dopant states of carbon nanotubes.

By separating the photons from slow and fast decays of single and multi-exciton states in a time gated 2nd order photon correlation experiment, we show that solitary oxygen dopant states of single-walled carbon nanotubes (SWCNTs) allow emission of photon pairs with efficiencies as high as 44% of single exciton emission. Our pump dependent time resolved photoluminescence (PL) studies further reveal diffusion-limited exciton-exciton annihilation as the key process that limits the emission of multi-excitons at high pump fluences. We further postulate that creation of additional permanent exciton quenching sites occurring under intense laser irradiation leads to permanent PL quenching. With this work, we bring out multi-excitonic processes of solitary dopant states as a new area to be explored for potential applications in lasing and entangled photon generation.

Quantum Dot-Like Behavior of Compositional Fluctuations in AlGaN Nanowires.

We report on the structural and optical properties of AlxGa(1-x)N nanowire sections grown by plasma-assisted molecular beam epitaxy on GaN nanowire bases used as a template. Based on a combination of scanning electron microscopy, microphotoluminescence, time-resolved microphotoluminescence, and photon correlation experiments, it is shown that compositional fluctuations in AlxGa(1-x)N sections associated with carrier localization optically behave as quantum dots. Moreover, most of the micro-optical properties of such fluctuations are demonstrated to be very little dependent on kinetic growth parameters such as AlxGa(1-x)N growth temperature and AlN molar fraction in the alloy, which govern the macrostructural properties of AlxGa(1-x)N sections.

Single-Nanocrystal Photoluminescence Spectroscopy Studies of Plasmon-Multiexciton Interactions at Low Temperature.

Using thick-shell or "giant" CdSe/CdS nanocrystal quantum dots (g-NQDs), characterized by strongly suppressed Auger recombination, we studied the influence of plasmonic interactions on multiexciton emission. Specifically, we assessed the separate effects of plasmonic absorption and plasmonic emission enhancement by a systematic analysis of the pump fluence dependence of low-temperature photoluminescence (low-T PL) derived from individual CdSe/CdS g-NQDs deposited on nanoroughened silver films. Our study reveals that (1) the multiexciton (MX) emissions in g-NQD coupled to silver films were enhanced not only through the creation of more excitons via enhancement of absorption but also through the direct modification of the competition between the radiative and nonradiative recombination processes of MXs; (2) strong enhancement in absorption is not necessary for strong multiexciton emission; and (3) the emission of MXs can become stronger with the increase of multiexciton order. We also exploited the strong enhancement of MX emission to perform second-order photon correlation and cross-correlation experiments using very low pump fluences and observed a strong photon bunching that decays with increasing pump fluence.

Disentangling the effects of clustering and multi-exciton emission in second-order photon correlation experiments

In single particle spectroscopy, the degree of observed fluorescence anti-bunching in a second-order cross correlation experiment is indicative of its bi-exciton quantum yield and whether or not a particle is well isolated. Advances in quantum dot synthesis have produced single particles with bi-exciton quantum yields approaching unity. Consequently, this creates uncertainty as to whether a particle has a high bi-exciton quantum yield or if it exists as a cluster. We report on a time-gated anti-bunching technique capable of determining the relative contributions of both multi-exciton emission and clustering effects. In this way, we can now unambiguously determine if a particle is single. Additionally, this time-gated anti-bunching approach provides an accurate way for the determination of bi-exciton lifetime with minimal contribution from higher order multi-exciton states.

Single photon emission in the red spectral range from a GaAs-based self-assembled quantum dot

Low temperature micro-photoluminecence and second-order single photon correlation experiments were performed on individual self-assembled In0.47Al0.34Ga0.19As/Al0.3Ga0.7As/GaAs quantum dots emitting in the range of 680–780 nm. Emission lines originating from exciton, biexciton, and charge exciton confined in the same dot could be identified. The derived exciton fine structure splitting is ∼125 μeV, whereas the biexciton and charge exciton binding energies are ∼4 and ∼9 meV, respectively. The photon correlation statistics measured for the exciton emission exhibited a clear antibunching with the value of gX−X2(0)=0.30±0.05, confirming unambiguously that such quantum dots act as true single photon quantum emitters.

Single Photon Counting from Individual Nanocrystals in the Infrared

Experimental restrictions imposed on the collection and detection of shortwave-infrared photons (SWIR) have impeded single molecule work on a large class of materials whose optical activity lies in the SWIR. Here we report the successful observation of room-temperature single nanocrystal photoluminescence at SWIR wavelengths using a highly efficient multielement superconducting nanowire single photon detector. We confirm that the photoluminescence from single lead sulfide nanocrystals is strongly antibunched, demonstrating the feasibility of performing sophisticated photon correlation experiments on individual weak SWIR emitters, and, more broadly, paving the way for sensitive measurements of spectral observables on infrared quantum systems that are incompatible with current detection techniques.

Optical Manipulation of a Single Mn Spin in a CdTe-Based Quantum Dot

Two coupled CdTe quantum dots, selected from a self-assembled system, one of them containing a single Mn ion, were studied by continuous wave and modulated photoluminescence, photoluminescence excitation, and photon correlation experiments. Optical writing of information on the spin state of the Mn ion has been demonstrated, using the orientation of the Mn spin by spin-polarized carriers transferred from the neighboring quantum dot. Mn spin orientation time values from 20 to 100 ns were measured, depending on the excitation power. Storage time of the information on the Mn spin was found to be enhanced by application of a static magnetic field of 1 T, reaching hundreds of microseconds in the dark. Simple rate equation models were found to describe correctly the static and dynamical properties of the system.

Single Photon Emission from Site-Controlled InAs Quantum Dots Grown on GaAs(001) Patterned Substrates

We present a fabrication method to produce site-controlled and regularly spaced InAs/GaAs quantum dots for applications in quantum optical information devices. The high selectivity of our epitaxial regrowth procedure can be used to allocate the quantum dots only in positions predefined by ex-situ local oxidation atomic force nanolithography. The quantum dots obtained following this fabrication process present a high optical quality which we have evaluated by microphotoluminescence and photon correlation experiments.

Two-Photon Gateway in One-Atom Cavity Quantum Electrodynamics

Single atoms absorb and emit light from a resonant laser beam photon by photon. We show that a single atom strongly coupled to an optical cavity can absorb and emit resonant photons in pairs. The effect is observed in a photon correlation experiment on the light transmitted through the cavity. We find that the atom-cavity system transforms a random stream of input photons into a correlated stream of output photons, thereby acting as a two-photon gateway. The phenomenon has its origin in the quantum anharmonicity of the energy structure of the atom-cavity system. Future applications could include the controlled interaction of two photons by means of one atom.

Single-photon emitter using excitation energy transfer between quantum dots

We demonstrated a high-quality single-photon emitter based on excitation energy transfer between two different-sized CuCl quantum dots (QDs). It is operated under triple blockade mechanisms. The mechanisms are tuning the incident light to the smaller QD and using an electric dipole forbidden excitation energy level in the larger QD, using the optical near-field interaction to transfer energy from the smaller QD to the electric dipole forbidden level of the larger QD, and using a single exciton emission level in the larger QD. These mechanisms are supported by the large binding energy of the exciton molecule. A 99.3% plausibility of single-photon emission was confirmed with 99.98% accuracy based on a photon correlation experiment with 80-MHz repetition frequency using an optical fiber probe.