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Pulsed squeezed light: characterization and applications

Triginer Garcés, Gil

Published Jan 1, 2019• 0 citations
Publisher

Abstract

Squeezed light is expected to enable new quantum metrology and quantum computation applications, but the very high degree of experimental control required in practice places severe demands on the physical devices used to generate it. As ultrafast squeezed light sources are reaching an unprecedented degree of brightness and modal control, there is a strong interest in developing methods for their experimental characterization and theoretical understanding. In this thesis, we demonstrate both a new application and a new characterization technique for pulsed squeezed light. In the first part of the thesis, we present a new metrological application of pulsed squeezed light: quantum-enhanced label-free nonlinear microscopy. Stimulated emission microscopy (SEM) is a state-of-the-art pump-probe microscopy technique whose sensitivity is ultimately limited by shot noise in the probe beam. We propose to overcome this fundamental limitation by using a sub-Poissonian probe generated via optical parametric amplification. We demonstrate an intensity-squeezed sub-picosecond pulsed probe, and a simple stimulated emission microscope. Using this squeezed probe, sub-Poissonian statistics are observed in the SEM signal. After this proof-of-principle experiment, we aim to provide an improved design for a source of intensity-squeezed light. First, we develop a theoretical framework to simulate the photon statistics of a general sub-Poissonian source, considering pulsed and focused pump and seed fields in a unified spatio-temporal description. Next, we use this framework to suggest possible improvements to our previous squeezed probe. In the second part of this thesis, we provide new theoretical and experimental tools to analyze the high gain regime of pulsed spontaneous parametric down-conversion (SPDC). We study a waveguided source capable of generating twin-beams with tens of photons in a single spatio-temporal mode. We develop a framework to efficiently simulate SPDC for an arbitrary nonlinear gain, including the effect of parasitic nonlinearities such as self-phase modulation (SPM) of the pump and cross-phase modulation (XPM) between pump and twin-beams. We experimentally characterize our source using a new technique based on stimulated difference-frequency generation (DFG). In a type-II down-conversion process, we measure the frequency generation produced not only in the orthogonal polarization to the seeding beam, but also in its same polarization, which we interpret as cascaded difference-frequency generation. We argue that the additional information obtained in this measurement allows for a self-referenced estimation of the squeezing gain. Using these measurements, we accurately fit our theoretical model, revealing that, in the high gain regime, parasitic nonlinearities strongly affect the spectral structure of the twin-beams. We propose a simple strategy to reduce the impact of these nonlinearities on the modal structure of SPDC.

DOI
10.5287/ora-koryqj7vn

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Squeezed light is expected to enable new quantum metrology and quantum computation applications, but the very high degree of experimental control required in practice places severe demands on the physical devices used to generate it. As ultrafast squeezed light sources are reaching an unprecedented degree of brightness and modal control, there is a strong interest in developing methods for their experimental characterization and theoretical understanding. In this thesis, we demonstrate both a new application and a new characterization technique for pulsed squeezed light. In the first part of the thesis, we present a new metrological application of pulsed squeezed light: quantum-enhanced label-free nonlinear microscopy. Stimulated emission microscopy (SEM) is a state-of-the-art pump-probe microscopy technique whose sensitivity is ultimately limited by shot noise in the probe beam. We propose to overcome this fundamental limitation by using a sub-Poissonian probe generated via optical parametric amplification. We demonstrate an intensity-squeezed sub-picosecond pulsed probe, and a simple stimulated emission microscope. Using this squeezed probe, sub-Poissonian statistics are observed in the SEM signal. After this proof-of-principle experiment, we aim to provide an improved design for a source of intensity-squeezed light. First, we develop a theoretical framework to simulate the photon statistics of a general sub-Poissonian source, considering pulsed and focused pump and seed fields in a unified spatio-temporal description. Next, we use this framework to suggest possible improvements to our previous squeezed probe. In the second part of this thesis, we provide new theoretical and experimental tools to analyze the high gain regime of pulsed spontaneous parametric down-conversion (SPDC). We study a waveguided source capable of generating twin-beams with tens of photons in a single spatio-temporal mode. We develop a framework to efficiently simulate SPDC for an arbitrary nonlinear gain, including the effect of parasitic nonlinearities such as self-phase modulation (SPM) of the pump and cross-phase modulation (XPM) between pump and twin-beams. We experimentally characterize our source using a new technique based on stimulated difference-frequency generation (DFG). In a type-II down-conversion process, we measure the frequency generation produced not only in the orthogonal polarization to the seeding beam, but also in its same polarization, which we interpret as cascaded difference-frequency generation. We argue that the additional information obtained in this measurement allows for a self-referenced estimation of the squeezing gain. Using these measurements, we accurately fit our theoretical model, revealing that, in the high gain regime, parasitic nonlinearities strongly affect the spectral structure of the twin-beams. We propose a simple strategy to reduce the impact of these nonlinearities on the modal structure of SPDC.
In this thesis we study three aspects of squeezed light. First, we investigate the generation of pulsed, near‑pure, degenerate, single‑temporal‑mode squeezed light produced by dual‑pump spontaneous four wave mixing in integrated silicon‑nitride coupled‑ring resonators. We show that parasitic spontaneous four wave mixing processes inherent to the dual‑pump configuration can substantially degrade the amount of generated squeezing and state purity. To mitigate these effects we explore pump detuning, engineered dispersion, and an auxiliary‑ring structure as suppression strategies. We then optimize the incident pump amplitude and phase, demonstrating that longer pump pulses can yield highly squeezed, temporally separable states and that an appropriate pre‑chirp tracks the effects of self‑ and cross‑phase modulation, increasing intracavity pump amplitudes and the amount of generated squeezing. Next, we analyze the spectral–temporal structure and photon statistics of strongly correlated squeezed light. We develop a general formalism based on the Whittaker–Shannon interpolation of the joint‑temporal amplitude that is particularly useful in the long‑pulse and continuous‑wave limits, where the instantaneous photon density is low but the total photon number may be large. This packet‑based description provides a local, physically transparent account of the state and its photon statistics that complements the Schmidt decomposition, and extends to nonclassical states for which a Schmidt decomposition is not available. Finally, we examine whether or not squeezed illumination can enhance two‑photon excitation relative to classical light, and whether any enhancement is experimentally detectable. We construct a model including radiative and nonradiative broadening to compute scattered and absorbed energy, and apply it to fluorescence from cesium atoms in a magneto‑optical trap driven by classical and squeezed light in both continuous‑wave and pulsed regimes. Under ideal conditions squeezed light can produce a measurable enhancement in both limits, but the gains are moderate and smaller than some recent molecular reports; additional broadening or loss would further reduce detectability.
The fields of quantum and nonlinear optics have given rise to a variety of nonclassical states of light that have been proven to surpass certain limitations set by classical physics. Namely, certain squeezed and entangled states have been shown to beat the shot-noise limit when making precision phase measurements in interferometry, as well as write lithographic patterns that are smaller than classically allowed by the Rayleigh diffraction limit. Additionally, single-photon sources and entangled photon pairs have given rise to provably secure quantum key distribution for cryptography. Producing these quantum states of light has proven a difficult task. Nonlinear crystals, when pumped by a laser, produce pairs of single photons via the process of spontaneous parametric down conversion (SPDC). This process is mediated by the second order nonlinear susceptibility of the material. When pumped in a high gain regime, these crystals give rise to optical parametric amplification, which is a viable source of squeezed light. The vast majority of research in this area has focused on crystals that are seeded by vacuum in their two modes. This dissertation concerns the field of quantum nonlinear optics. It is an investigation into the processes that occur when nonlinear materials interact with the electromagnetic field on the single photon level. I have focused on seeding nonlinear crystals with quantum states of light, including single photons and entangled states. This process results in various states directly applicable to interferometry, imaging, and cryptography. Another application investigated is an absolute radiance measurement via stimulated parametric down conversion resulting from non-vacuum seeding of a nonlinear crystal. Additionally, other nonlinear processes, including four-wave mixing, nonlinear magneto-optical effects and coherent population trapping in warm atomic vapor involving quantum states of light are investigated. The process of seeding third-order nonlinear interactions, such as in atomic vapors, gives rise to a variety of interesting, nonclassical phenomena such as entangled image transfer and nonlocal imaging. Strong analogies between SPDC and four-wave mixing are drawn. I also experimentally show an all optical pi-only phase shift of one light beam via another in warm Cesium vapor.
Nonlinear optical microscopy techniques have emerged as a set of successful tools for biological imaging. Stimulated emission microscopy belongs to a small subset of pump-probe techniques which can image non-fluorescent samples without requiring fluorescent labelling. However, its sensitivity has been shown to be ultimately limited by the quantum fluctuations in the probe beam. We propose and experimentally implement sub-shot-noise limited stimulated emission microscopy by preparing the probe pulse in an intensity-squeezed state. This technique paves the way for imaging delicate biological samples that have no detectable fluorescence with sensitivity beyond standard quantum fluctuations.
Squeezed states of light enable enhanced measurement precision by reducing noise below the standard quantum limit. A key application of squeezed light is nonlinear microscopy, where state-of-the-art performance is limited by photodamage and quantum-limited noise. Such microscopes require bright, pulsed light for optimal operation, yet generating and detecting bright pulsed squeezing at high levels remains challenging. In this work, we present an efficient technique to generate high levels of bright picosecond pulsed squeezed light using a χ2χ^2χ2 optical parametric amplification process in a waveguide. We measure −3.2 dB-3.2~\mathrm{dB}−3.2 dB of bright squeezing with optical power compatible with nonlinear microscopy, as well as −3.6 dB-3.6~\mathrm{dB}−3.6 dB of vacuum squeezing. Corrected for losses, these squeezing levels correspond to −15.4−8.7+2.7 dB-15.4^{+2.7}_{-8.7}~\mathrm{dB}−15.4−8.7+2.7​ dB of squeezing generated in the waveguide. The measured level of bright amplitude pulsed squeezing is to our knowledge the highest reported to date, and will contribute to the broader adoption of quantum-enhanced nonlinear microscopy in biological studies.
Nonlinear optical microscopy techniques have emerged as a set of successful tools for biological imaging. Stimulated emission microscopy belongs to a small subset of pump–probe techniques, which can image non-fluorescent samples without requiring fluorescent labeling. However, its sensitivity has been shown to be ultimately limited by the quantum fluctuations in the probe beam. We propose and experimentally implement sub-shot-noise limited stimulated emission microscopy by preparing the probe pulse in an intensity-squeezed state. This technique paves the way for imaging delicate biological samples that have no detectable fluorescence with sensitivity beyond standard quantum fluctuations.
Ultrafast quantum light pulses with durations of 1ps and below show great promise as information carriers in quantum communication and computation. In future they may also be used to probe physical processes at ultrashort timescales with a resolution beyond the limits of Heisenberg uncertainty. This thesis focuses on the creation and manipulation of quantum light pulses with second order nonlinear optical processes in optical waveguides. In chapter 1. Introduction, we lead the reader towards this work's topic by giving a brief qualitative overview over the EPR paradox, quantum entanglement, three-wave-mixing and quantum light pulses. Chapter 2. Basic concepts familiarizes the reader with the physical concepts and mathematical tools underlying this thesis. In chapter 3. Spectral engineering, we discuss the requirements to produce separable photon pair states with group velocity matching and examine several nonlinear materials widely used for optical waveguide inscription for their suitability to group velocity matching in the telecom wavelength regime. In chapter 4. A PP-KTP waveguide as parametric downconversion source, we give the basic spontaneous parametric downconversion source setup, as well as some initial measurements to characterize the single photon detectors, to demonstrate the production of correlated photons, and to determine the phasematching properties of the PP-KTP source. In the following chapter, 5. Fiber spectrometer, we present the single-photon fiber spectrometer. We discuss the experimental setup and calibration of the device, and measure the joint spectrum of photon pairs from our PP-KTP source. Finally, we investigate the behavior of a joint spectrum measurement of a high mean photon number source with binary detectors. In 6. Two-mode squeezed vacuum source, we characterize spectral correlations of an ultrafast SPDC source with the second order correlation function g². We present the g² measurement results and show that we can control the spectral correlations to produce a two-mode squeezed vacuum state of light. We then determine the mean photon number and gain of the source. 7. Quantum pulse gate: While the previous chapters focus on the creation and characterization of ultrafast quantum pulses of light, we now propose a way to manipulate the mode structure of a given quantum light state. We discuss the concept of an active optical filter sensitive to spectral/temporal pulse shape: The quantum pulse gate. In the final chapter 8. Conclusion and outlook, we recapitulate the main results of this thesis and provide a few pointers towards possibilities for future research building on it.