Deniz Bozyigit

Observation of resonant photon blockade at microwave frequencies using correlation function measurements.

Creating a train of single photons and monitoring its propagation and interaction is challenging in most physical systems, as photons generally interact very weakly with other systems. However, when confining microwave frequency photons in a transmission line resonator, effective photon-photon interactions can be mediated by qubits embedded in the resonator. Here, we observe the phenomenon of photon blockade through second-order correlation function measurements. The experiments clearly demonstrate antibunching in a continuously pumped source of single microwave photons measured by using microwave beam splitters, linear amplifiers, and quadrature amplitude detectors. We also investigate resonance fluorescence and Rayleigh scattering in Mollow-triplet-like spectra.

Observation of Two-Mode Squeezing in the Microwave Frequency Domain

Continuous variable entanglement between two modes of a radiation field is usually studied at optical frequencies. As an important step towards the observation of entanglement between propagating microwave photons we demonstrate the experimental state reconstruction of two field modes in the microwave domain. In particular, we generate two-mode correlated states with a Josephson parametric amplifier and detect all four quadrature components simultaneously in a two-channel heterodyne setup using amplitude detectors. Analyzing two-dimensional phase space histograms for all possible pairs of quadratures allows us to determine the full covariance matrix and reconstruct the four-dimensional Wigner function. We demonstrate strong correlations between the quadrature amplitude noise in the two modes. Under ideal conditions two-mode squeezing below the standard quantum limit should be observable in future experiments.

Experimental State Tomography of Itinerant Single Microwave Photons

A wide range of experiments studying microwave photons localized in superconducting cavities have made important contributions to our understanding of the quantum properties of radiation. Propagating microwave photons, however, have so far been studied much less intensely. Here we present measurements in which we reconstruct the Wigner function of itinerant single photon Fock states and their superposition with the vacuum using linear amplifiers and quadrature amplitude detectors. We have developed efficient methods to separate the detected single photon signal from the noise added by the amplifier by analyzing the moments of the measured amplitude distribution up to 4th order. This work is expected to enable studies of propagating microwaves in the context of linear quantum optics.

Quantification of deep traps in nanocrystal solids, their electronic properties, and their influence on device behavior.

We implement three complementary techniques to quantify the number, energy, and electronic properties of trap states in nanocrystal (NC)-based devices. We demonstrate that, for a given technique, the ability to observe traps depends on the Fermi level position, highlighting the importance of a multitechnique approach that probes trap coupling to both the conduction and the valence bands. We then apply our protocol for characterizing traps to quantitatively explain the measured performances of PbS NC-based solar cells.

A quantitative model for charge carrier transport, trapping and recombination in nanocrystal-based solar cells

Improving devices incorporating solution-processed nanocrystal-based semiconductors requires a better understanding of charge transport in these complex, inorganic–organic materials. Here we perform a systematic study on PbS nanocrystal-based diodes using temperature-dependent current–voltage characterization and thermal admittance spectroscopy to develop a model for charge transport that is applicable to different nanocrystal-solids and device architectures. Our analysis confirms that charge transport occurs in states that derive from the quantum-confined electronic levels of the individual nanocrystals and is governed by diffusion-controlled trap-assisted recombination. The current is limited not by the Schottky effect, but by Fermi-level pinning because of trap states that is independent of the electrode–nanocrystal interface. Our model successfully explains the non-trivial trends in charge transport as a function of nanocrystal size and the origins of the trade-offs facing the optimization of nanocrystal-based solar cells. We use the insights from our charge transport model to formulate design guidelines for engineering higher-performance nanocrystal-based devices.

Highly Luminescent, Size- and Shape-Tunable Copper Indium Selenide Based Colloidal Nanocrystals

We report a simple, high-yield colloidal synthesis of copper indium selenide nanocrystals (CISe NCs) based on a silylamide-promoted approach. The silylamide anions increase the nucleation rate, which results in small-sized NCs exhibiting high luminescence and constant NC stoichiometry and crystal structure regardless of the NC size and shape. In particular, by systematically varying synthesis time and temperature, we show that the size of the CISe NCs can be precisely controlled to be between 2.7 and 7.9 nm with size distributions down to 9–10%. By introducing a specific concentration of silylamide-anions in the reaction mixture, the shape of CISe NCs can be preselected to be either spherical or tetrahedral. Optical properties of these CISe NCs span from the visible to near-infrared region with peak luminescence wavelengths of 700 to 1200 nm. The luminescence efficiency improves from 10 to 15% to record values of 50–60% by overcoating as-prepared CISe NCs with ZnSe or ZnS shells, highlighting their potential for applications such as biolabeling and solid state lighting.

Soft surfaces of nanomaterials enable strong phonon interactions

Phonons and their interactions with other phonons, electrons or photons drive energy gain, loss and transport in materials. Although the phonon density of states has been measured and calculated in bulk crystalline semiconductors, phonons remain poorly understood in nanomaterials, despite the increasing prevalence of bottom-up fabrication of semiconductors from nanomaterials and the integration of nanometre-sized components into devices. Here we quantify the phononic properties of bottom-up fabricated semiconductors as a function of crystallite size using inelastic neutron scattering measurements and ab initio molecular dynamics simulations. We show that, unlike in microcrystalline semiconductors, the phonon modes of semiconductors with nanocrystalline domains exhibit both reduced symmetry and low energy owing to mechanical softness at the surface of those domains. These properties become important when phonons couple to electrons in semiconductor devices. Although it was initially believed that the coupling between electrons and phonons is suppressed in nanocrystalline materials owing to the scarcity of electronic states and their large energy separation, it has since been shown that the electron–phonon coupling is large and allows high energy-dissipation rates exceeding one electronvolt per picosecond (refs 10, 11, 12, 13). Despite detailed investigations into the role of phonons in exciton dynamics, leading to a variety of suggestions as to the origins of these fast transition rates and including attempts to numerically calculate them, fundamental questions surrounding electron–phonon interactions in nanomaterials remain unresolved. By combining the microscopic and thermodynamic theories of phonons and our findings on the phononic properties of nanomaterials, we are able to explain and then experimentally confirm the strong electron–phonon coupling and fast multi-phonon transition rates of charge carriers to trap states. This improved understanding of phonon processes permits the rational selection of nanomaterials, their surface treatments, and the design of devices incorporating them.

Characterizing quantum microwave radiation and its entanglement with superconducting qubits using linear detectors

Recent progress in the development of superconducting circuits has allowed for realizing interesting sources of nonclassical radiation at microwave frequencies. Here, we discuss field quadrature detection schemes for the experimental characterization of itinerant microwave photon fields and their entanglement correlations with stationary qubits. In particular, we present joint state tomography methods of a radiation field mode and a two-level system. Including the case of finite quantum detection efficiency, we relate measured photon field statistics to generalized quasi-probability distributions and statistical moments. We also present maximum-likelihood methods to reconstruct density matrices from measured field quadrature histograms.

Deep Level Transient Spectroscopy (DLTS) on Colloidal-Synthesized Nanocrystal Solids

We demonstrate current-based, deep level transient spectroscopy (DLTS) on semiconductor nanocrystal solids to obtain quantitative information on deep-lying trap states, which play an important role in the electronic transport properties of these novel solids and impact optoelectronic device performance. Here, we apply this purely electrical measurement to an ethanedithiol-treated, PbS nanocrystal solid and find a deep trap with an activation energy of 0.40 eV and a density of NT = 1.7 × 10(17) cm(-3). We use these findings to draw and interpret band structure models to gain insight into charge transport in PbS nanocrystal solids and the operation of PbS nanocrystal-based solar cells.

Electroluminescence from Nanoscale Materials via Field-Driven Ionization

The high degree of morphological and energetic disorder inherent to many nanosized materials places limitations on charge injection into and transport rates through thin films of these materials. We demonstrate electroluminescence achieved by local generation of charge that eliminates the need for injection of charge carriers from the device electrodes. We show electroluminescence from thin films of nanoscale materials that do not support direct current excitation and suggest a mechanism for the charge generation and electroluminescence that is consistent with our time-averaged and time-resolved observations.