Publications

Coherent control of quantum transitionsindispensable in quantum technologygenerally relies on the interaction of quantum systems with electromagnetic radiation. Here, we theoretically demonstrate that the nonradiative electromagnetic near field of a temporally modulated free-space electron beam can be utilized for coherent control of quantum systems. We show that such manipulation can be performed with only classical control over the electron beam itself and is readily realizable with current technology. This approach may provide a pathway toward spectrally selective quantum control with nanoscale spatial resolution, harnessing the small de Broglie wavelength of electrons.

Transmission electron microscopy (TEM) of vitrified biological macromolecules (cryo-EM) is limited by the weak phase contrast signal that is available from such samples. Using a phase plate would thus substantially improve the signal-to-noise ratio. We have previously demonstrated the use of a high-power Fabry-Perot cavity as a phase plate for TEM. We now report improvements to our laser cavity that allow us to achieve record continuous wave intensities of over 450 GW/cm2, sufficient to produce the optimal 90° phase shift for 300 keV electrons. In addition, we have performed the first cryo-EM reconstruction using a laser phase plate, demonstrating that the stability of this laser phase plate is sufficient for use during standard cryo-EM data collection.

Transmission electron microscopy (TEM) of rapidly frozen biological specimens, or cryo-EM, would benefit from the development of a phase plate for in-focus phase contrast imaging. Several types of phase plates have been investigated, but rapid electrostatic charging of all such devices has hindered these efforts. Here, we demonstrate electron phase manipulation with a high-intensity continuous-wave laser beam, and use it as a phase plate for TEM. We demonstrate the laser phase plate by imaging an amorphous carbon film. The laser phase plate provides a stable and tunable phase shift without electrostatic charging or unwanted electron scattering. These results suggest the possibility for dose-efficient imaging of unstained biological macromolecules and cells.

Objects at finite temperature emit thermal radiation with an outward energymomentum flow, which exerts an outward radiation pressure. At room temperature, a caesium atom scatters on average less than one of these blackbody radiation photons every 108 years. Thus, it is generally assumed that any scattering force exerted on atoms by such radiation is negligible. However, atoms also interact coherently with the thermal electromagnetic field. In this work, we measure an attractive force induced by blackbody radiation between a caesium atom and a heated, centimetre-sized cylinder, which is orders of magnitude stronger than the outward-directed radiation pressure. Using atom interferometry, we find that this force scales with the fourth power of the cylinders temperature. The force is in good agreement with that predicted from an a.c. Stark shift gradient of the atomic ground state in the thermal radiation field1. This observed force dominates over both gravity and radiation pressure, and does so for a large temperature range.

Abstract: Manipulating free-space electron wave functions with laser fields can bring about new electron-optical elements for transmission electron microscopy (TEM). In particular, a Zernike phase plate would enable high-contrast TEM imaging of soft matter, leading to new opportunities in structural biology and materials science. A Zernike phase plate can be implemented using a tight, intense continuous laser focus that shifts the phase of the electron wave by the ponderomotive potential. Here, we use a near-concentric cavity to focus 7.5 kW of continuous-wave circulating laser power at 1064 nm into a 7 µm mode waist, achieving a record continuous laser intensity of 40 GW/cm². Such parameters are su cient to impart a phase shift of 1 rad to a 10 keV electron beam, or 0.16 rad to a 300 keV beam. Our numerical simulations confirm that the standing-wave phase shift profile imprinted on the electron wave by the intra-cavity field can serve as a nearly ideal Zernike phase plate.

According to quantum electrodynamics, the exchange of virtual photons in a system of identical quantum emitters causes a shift of its energy levels. Such shifts, known as cooperative Lamb shifts, have been studied mostly in the near-field regime. However, the resonant electromagnetic interaction persists also at large distances, providing coherent coupling between distant atoms. Here, we report a direct spectroscopic observation of the cooperative Lamb shift of an optical electric-dipole transition in an array of Sr+ ions suspended in a Paul trap at inter-ion separations much larger than the resonance wavelength. By controlling the precise positions of the ions, we studied the far-field resonant coupling in chains of up to eight ions, extending to a length of 40 mu m. This method provides a novel tool for experimental exploration of cooperative emission phenomena in extended mesoscopic atomic arrays.

The optical diffraction limit imposes a bound on imaging resolution in classical optics. Over the last twenty years, many theoretical schemes have been presented for overcoming the diffraction barrier in optical imaging using quantum properties of light. Here, we demonstrate a quantum superresolution imaging method taking advantage of nonclassical light naturally produced in fluorescence microscopy due to photon antibunching, a fundamentally quantum phenomenon inhibiting simultaneous emission of multiple photons. Using a photon counting digital camera, we detect antibunching-induced second and third order intensity correlations and perform subdiffraction limited quantum imaging in a standard wide-field fluorescence microscope.

Stochastic distortion of light beams in scattering samples makes in-depth photoexcitation in brain tissue a major challenge. A common solution for overcoming scattering involves adaptive pre-compensation of the unknown distortion^1-3. However, this requires long iterative searches for sample-specific optimized corrections, which is a problem when applied to optical neurostimulation where typical timescales in the system are in the millisecond range. Thus, photoexcitation in scattering media that is independent of the properties of a specific sample would be an ideal solution. Here, we show that temporally focused two-photon excitation⁴with generalized phase contrast⁵ enables photoexcitation of arbitrary spatial patterns within turbid tissues with remarkable robustness to scattering. We demonstrate three-dimensional confinement of tailored photoexcitation patterns >200 μm in depth, both in numerical simulations and through brain slices combined with patch-clamp recording of photoactivated channelrhodopsin-2.

Luminescence intermittency, also termed 'blinking', refers to spontaneous changes in the brightness of a luminescent fluorophore under continuous optical excitation. Blinking was first observed in colloidal semiconductor nanocrystals over fifteen years ago, shortly after synthetic protocols became advanced enough to produce brightly luminescent nanocrystals. The underlying physical mechanism was initially associated with long-lived photo-induced charging of the nanocrystals. In recent years, however, significant evidence has accumulated to point at a more complex physical picture of the process, which involves several distinct mechanisms and is mediated by surface charge trapping. In parallel, efforts to synthesize highly luminescent semiconductor nanocrystals that do not exhibit blinking have recently borne fruit. We review the recent progress in understanding of blinking and potential applications in bioimaging using inorganic fluorescent tags.

Although colloidal quantum dots (QDs) exhibit excellent photostability under mild excitation, intense illumination makes their emission increasingly intermittent, eventually leading to photobleaching. We study fluorescence of two commonly used types of QDs under pulsed excitation with varying power and repetition rate. The photostability of QDs is found to improve dramatically at low repetition rates, allowing for prolonged optical saturation of QDs without apparent photodamage. This observation suggests that QD blinking is facilitated by absorption of light in a transient state with a microsecond decay time. Enhanced photostability of generic quantum dots under intense illumination opens up new prospects for fluorescence microscopy and spectroscopy.

Photon antibunching is ubiquitously observed in light emitted from quantum systems but is usually associated only with the lowest excited state of the emitter. Here, we devise a fluorophore that upon photoexcitation emits in either one of two distinct colors but exhibits strong antibunching between the two. This work demonstrates the possibility of creating room-temperature quantum emitters with higher complexity than effective two level systems via colloidal synthesis.

A synthetic route for preparation of inorganic WS ₂ nanotube (INT)-colloidal semiconductor quantum dot (QD) hybrid structures is developed, and transient carrier dynamics on these hybrids are studied via transient photoluminescence spectroscopy utilizing several different types of QDs. Measurements reveal efficient resonant energy transfer from the QDs to the INT upon photoexcitation, provided that the QD emission is at a higher energy than the INT direct gap. Charge transfer in the hybrid system, characterized using QDs with band gaps below the INT direct gap, is found to be absent. This is attributed to the presence of an organic barrier layer due to the relatively long-chain organic ligands of the QDs under study. This system, analogous to carbon nanotube-QD hybrids, holds potential for a variety of applications, including photovoltaics, luminescence tagging and optoelectronics. This journal is

Breaking the diffraction limit in microscopy by utilizing the quantum properties of light has been the goal of intense research in recent years. We propose a super-resolution technique based on nonclassical emission statistics of fluorescent markers, routinely used as contrast labels for bioimaging. The technique can be readily implemented with current technology.

Utilizing quantum properties of light to break the diffraction limit has been the goal of intense research in the recent years. This paper is a progress report on a study aimed at experimentally demonstrating a superresolution microscopy technique enabled by photon antibunching, a non-classical emission statistics feature exhibited by most emitters used as fluorescent markers. We find that photon antibunching gives rise to correlations that encode high spatial frequency information on the distribution of fluorescent emitters. Detecting these correlations using photon counting instrumentation in a standard fluorescence microscope setting allows for three-dimensional superresolution imaging of fluorophore stained samples. The technique provides a quantum alternative to the established superresolution tools.

The waveforms of attosecond pulses produced by high-harmonic generation carry information on the electronic structure and dynamics in atomic and molecular systems. Current methods for the temporal characterization of such pulses have limited sensitivity and impose significant experimental complexity. We propose a new linear and all-optical method inspired by widely used multidimensional phase retrieval algorithms. Our new scheme is based on the spectral measurement of two attosecond sources and their interference. As an example, we focus on the case of spectral polarization measurements of attosecond pulses, relying on their most fundamental property-being well confined in time. We demonstrate this method numerically by reconstructing the temporal profiles of attosecond pulses generated from aligned CO₂ molecules.

Ultrafast science is inherently, due to the lack of fast enough detectors and electronics, based on nonlinear interactions. Typically, however, nonlinear measurements require significant powers and often operate in a limited spectral range. Here we overcome the difficulties of ultraweak ultrafast measurements by precision time-domain localization of spectral components. We utilize this for linear self-referenced characterization of pulse trains having ∼ 1 photon per pulse, a regime in which nonlinear techniques are impractical, at a temporal resolution of ∼ 10 fs. This technique does not only set a new scale of sensitivity in ultrashort pulse characterization, but is also applicable in any spectral range from the near-infrared to the deep UV.

A linear self-referenced technique for temporal characterization of ultraweak pulse trains is presented. Shot-noise limited time-resolved single photon detection enables temporal resolution down to 10fs for pulse trains with ∼ 1 photon per pulse.

We propose a new linear and all-optical method for attosecond pulses characteri-zation. Our scheme is based only on spectral and polarization measurements. We demonstrate this method numerically on attosecond pulses generated from aligned CO₂ molecules.

The observed intermittent light emission from colloidal semiconductor nanocrystals has long been associated with Auger recombination assisted quenching. We test this view by observing transient emission dynamics of CdSe/CdS/ZnS semiconductor nanocrystals using time-resolved photon counting. The size and intensity dependence of the observed decay dynamics seem inconsistent with those expected from Auger processes. Rather, the data suggest that in the "off" state the quantum dot cycles in a three-step process: photoexcitation, rapid trapping, and subsequent slow nonradiative decay.

Biological photonic systems composed of anhydrous guanine crystals evolved separately in several taxonomie groups. Here, two such systems found in fish and spiders, both of which make use of anhydrous guanine crystal plates to produce structural colors, are examined. Measurements of the photoniccrystal structures using cryo-SEM show that the crystal plates in both fish skin and spider integument are ∼20-nm thick. The reflective unit in the fish comprises stacks of single plates alternating with ∼ 230-nm-thick cytoplasm layers. In the spiders the plates are formed as doublet crystals, cemented by 30-nm layers of amorphous guanine, and are stacked with ∼200nm of cytoplasm between crystal doublets. They achieve light reflective properties through the control of crystal morphology and stack dimensions, reaching similar efficiencies of light reflectivity in both fish skin and spider integument. The structure of guanine plates in spiders are compared with the more common situation in which guanine occurs in the form of relatively unorganized prismatic crystals, yielding a matt white coloration.

Blinking in colloidal nanocrystals is studied through photon counting from single nanocrystals. Size independent 'off' state dynamics are observed in contrast to predictions by prevailing models which attribute 'dark' states to Auger recombination assisted quenching.

We demonstrate an optical nonlinearity free ultrashort pulse characterization technique relying on spectral component localization in time domain. Ultraweak pulses in NIR to XUV range can be characterized with resolution depending only on integration time.

Surface plasmon resonance exhibited by noble metal nanoparticles makes them attractive agents for advanced microscopic imaging applications. In this work we study third harmonic generation in gold nanorods under conditions of resonance of the laser frequency with the longitudinal plasmon mode. Large resonant enhancement and the symmetry properties of third harmonic generation allow for background-free, orientation sensitive optical imaging of individual nanoparticles.

Pupil filters are widely used to improve the resolution of confocal microscopes. We analyze the possibilities of applying them to N-photon microscopy. We find that taking a linear combination of images obtained with several pupil filters can improve the resolution by a factor of N (compared to a conventional microscope). When applied to saturable fluorescence, this technique allows one to observe fluorescent objects with, in principle, unlimited spatial resolution.

We overview our recent developments in the theory of dispersion-managed (DM) solitons within the context of optical applications. First, we present a class of localized solutions with a period multiple to that of the standard DM soliton in the nonlinear Schrdinger equation with periodic variations of the dispersion. In the framework of a reduced ordinary differential equation-based model, we discuss the key features of these structures, such as a smaller energy compared to traditional DM solitons with the same temporal width. Next, we present new results on dissipative DM solitons, which occur in the context of mode-locked lasers. By means of numerical simulations and a reduced variational model of the complex Ginzburg-Landau equation, we analyze the influence of the different dissipative processes that take place in a laser.

We present a class of solutions with a period multiple to that one of the standard dispersion-managed soliton in the nonlinear Schrödinger equation with periodic variations of dispersion.

Solution of many problems of gas kinetics, transport phenomena, and spectroscopy can be significantly simplified using the linearized Boltzmann equation within so called one-dimensional approximation, in which the collision kernel is averaged over the transverse velocities. The error introduced by this approximation is usually considered to be small, however, no quantitative analysis of its value has been done so far. We study the accuracy of the one-dimensional approximation in a particular problem of calculating spectral line shapes in gases. The inaccuracy is shown to be small in the wings of line, in the cases of light buffer molecules or low collision frequency. For arbitrary parameters the error is calculated numerically within the rigid-sphere model. These results outline the area of applicability of computationally economic one-dimensional approach.

We examine the problem of fiber Bragg grating reconstruction from its reflection coefficient. A direct numerical method of solving the GelfandLevitanMarchenko integral equations for the problem is developed. The method is based on a bordering procedure, Cholesky decomposition, and piecewise-linear approximation. It is tested using high-reflectance homogeneous and hyperbolic secant profiles. The proposed method is shown to concede the popular discrete layer peeling technique in efficiency but surpasses it in accuracy and stability at high reflectance.

The Coulomb corrections (CC) to the processes of bremsstrahlung and pair production are investigated. The next-to-leading term in the high-energy asymptotics is found. This term becomes very essential in the region of intermediate energies. The influence of screening for CC is small for differential cross section, spectrum, and the total cross section of pair production. The same is true for the spectrum of bremsstrahlung, but not for the differential cross section, where the influence of screening can be very large. The corresponding screening corrections as well as the modification of the differential cross section of bremsstrahlung are found. A comparison of our results for the total cross section of pair production with the experimental data available is performed. This comparison has justified our analytical results and allowed to elaborate a simple ansatz for the next-to-leading correction. The influence of the electron beam shape on CC for bremsstrahlung is investigated. It turns out that the differential cross section is very sensitive to this shape.

We consider the differential and partially integrated cross sections for bremsstrahlung from high-energy electrons in an atomic field, with this field taken into account exactly. We use the semiclassical electron Green function and wavefunctions in an external electric field. It is shown that the Coulomb corrections to the differential cross section are very susceptible to screening. Nevertheless, the Coulomb corrections to the cross section summed over the final-electron states are independent of screening in the leading approximation in the small parameter 1/mr scr (r scr is the screening radius and m is the electron mass, ℏ = c = 1). We also consider bremsstrahlung from a finite-size electron beam on a heavy nucleus. The Coulomb corrections to the differential probability are also very susceptible to the beam shape, while the corrections to the probability integrated over momentum transfer are independent of it, apart from the trivial factor, which is the electron-beam density at zero impact parameter. For the Coulomb corrections to the bremsstrahlung spectrum, the next-to-leading terms with respect to the parameters mε (ε is the electron energy) and 1/mr scr are obtained.