Recent advances in generating light in specific quantum states facilitate new sensing applications and enhance or revitalize established measurement and sensing techniques. Stimulated Raman spectroscopy (SRS), a measurement modality based on Raman scattering, could benefit from tuning the quantum properties of the pump and the Stokes lights or the properties of quantum states of the stimulating and excitation fields. Additionally, this modality could also benefit from field enhancement accompanied by plasmon excitation in the surface regions of metal nanoparticles. We present a theoretical investigation of stimulated Raman scattering involving squeezed states of light. The concept of surface- and quantum-enhanced stimulated Raman scattering is introduced. Furthermore, expressions for the respective SRS transition rates are derived, and their dependence on the quantum states of the optical field is discussed, with particular emphasis on the squeezing parameters characterizing these states. For cases involving surface enhancements, we also employ classical computational electrodynamics to guide our exploration of atomically large systems that support plasmon excitation.
Recent advances in generating light in specific quantum states facilitate new sensing applications and enhance or revitalize established measurement and sensing techniques. Stimulated Raman spectroscopy (SRS), a measurement modality based on Raman scattering, could benefit from tuning the quantum properties of the pump and the Stokes lights or the properties of quantum states of the stimulating and excitation fields. Additionally, this modality could also benefit from field enhancement accompanied by plasmon excitation in the surface regions of metal nanoparticles. We present a theoretical investigation of stimulated Raman scattering involving squeezed states of light. The concept of surface- and quantum-enhanced stimulated Raman scattering is introduced. Furthermore, expressions for the respective SRS transition rates are derived, and their dependence on the quantum states of the optical field is discussed, with particular emphasis on the squeezing parameters characterizing these states. For cases involving surface enhancements, we also employ classical computational electrodynamics to guide our exploration of atomically large systems that support plasmon excitation.
We study the stimulated Raman scattering (SRS) of light from an atomic system embedded in a photonic crystal and coherently pumped by a laser field. In our study, the electromagnetic field is treated classically and the atomic system is described quantum mechanically. Considering a decomposition of the pump and Stokes fields into the Bloch modes of the photonic crystals and using a multiscale analysis, we derive the Maxwell-Bloch equations for SRS in photonic crystals. These equations contain effective parameters that characterize the SRS gain, the nonlinear atomic response to the electromagnetic field, and the group velocity and that can be calculated in terms of the Bloch modes of the unperturbed photonic crystal. We show that if the pump laser frequency is tuned near a photonic band edge and the atomic system is carefully chosen such that the Stokes mode matches another photonic band edge, low-threshold, enhanced Raman amplification is possible. Possible physical realizations of SRS in photonic crystals are also discussed.
Stimulated Raman scattering (SRS) microscopes are a standard technique to image cells, tissues or track the uptake of drugs [1] . The sensitivity in these devices is directly linked to the laser power. While an increase of sensitivity is desired, increasing the laser power is challenging and squeezed light offers a solution to this challenge. Recently squeezed light has been used to enhance the sensitivity of continuous-wave and pulsed SRS [2] , [3] setups and stimulated emission spectroscopy [4] .
In optical microscopy, as in any biological measurement performed with light, there is a compromise between increasing power to improve resolution and decreasing power to prevent photodamage to the biological structure. Quantum optics allows this compromise to be overcome, enabling improved precision without increased illumination intensity. This thesis demonstrates, for the first time, absolute quantum advantage in microscopy, with a specific focus on Stimulated Raman Scattering (SRS) microscopy.SRS microscopy is a powerful tool widely used in many fields, especially in biomedical sciences. It uses a two-photon process where the light is downshifted in frequency by being absorbed and subsequently inelastically scattered by the intrinsic molecular vibrations in the sample. Each element or molecule has a different response, allowing selective imaging of biological systems. SRS microscopy is particularly useful because it is label-free (no addition of dyes, beads or any implanted tracer), meaning that imaging contrast is achieved without modification of, or interference with, the specimen. Here I present our newly built state-of-the-art shot-noise limited SRS microscope. I also characterize the Raman microscope, describe the developped imaging system and show SRS spectroscopy and imaging of both polystyrene beads and living yeast cells.The quantisation of light introduces a fundamental uncertainty, or quantum noise, in both the amplitude and phase quadratures of an optical field. A squeezed state of light is a state of the optical field where the uncertainty of one of these quadratures is reduced below the quantum noise. Therefore, it provides an approach to reduce the noise level below this quantum noise limit and consequently increases measured signal-to-noise ratio. Here I describe the concepts involved in this technique and present our newly built light squeezer. I characterize the squeezing and show up to -1.3 dB of noise floor reduction for a 6 picosecond pulsed laser, which is the pulse duration that maximises the Raman interaction.In this thesis we apply squeezed states of light in SRS, developping a quantum-enhanced micro- scope. Our SRS Raman intensity noise is ∆I/I ≈ 10^(−7) and the measured quantum efficiency of the built photodiode is η = 72%. In this proof of principle we show a reduction of the noise floor of at least 13% below the quantum noise limit for Raman imaging of polystyrene beads and living yeast cells. This enhancement allowed us to resolve the cell membrane where with conventional microscope would be unresolvable. It also allowed sub-micron spatial resolution. The improved image contrast and reduced imaging time, while avoiding photodamage in the sample, surpasses the current state-of-the-art Raman microscopes and opens opportunities for new discoveries in biophysics.
Squeezed light has been applied in stimulated Raman scattering (SRS) spectroscopy [1] and microscopy [2] to break the shot-noise-limited sensitivity. The sub-shot-noise sensitivity achieved in quantum-enhanced SRS (QE-SRS) systems is advantageous for uncovering weak signals and achieving faster imaging speed, which attract the attention of biomedical scientists. To break the sensitivity of state-of-the-art SRS microscopes, the applied squeezed light power in QE-SRS systems should be high enough (>10mW). Recently, high-power picosecond-pulsed QE-SRS spectroscopy [3] based on balanced detection scheme [4] was reported, and a sensitivity that is comparable to state-of-the-art SRS microscopes was firstly demonstrated in QE-SRS microscopy based on the same scheme [5]. An important issue of QE-SRS based on balanced detection is the 3-dB additional noise, so >3-dB squeezing level is required to demonstrate an absolute sensitivity improvement compared with state-of-the-art SRS microscopes in single-photodiode detection scheme. However, it's hard to generate highly squeezed pulsed light because of the difficulty in temporal and spatial mode matching between squeezed vacuum (SQV) and local oscillator (LO). Here, we introduce QE-SRS in dual-polarization scheme, which can be implemented in high-power regime but is free from the 3-dB signal-to-noise ratio drawback.
Stimulated Raman scattering (SRS) microscopy has emerged as a powerful technique for probing the spatiotemporal dynamics of molecular bonds with exceptional sensitivity, resolution, and speed. However, classically, its performance remains fundamentally constrained by optical shot noise, which imposes a strict limit on detection sensitivity and speed. Here, we demonstrate a quantum-enhanced SRS microscopy platform that circumvents this barrier by harnessing amplitude-squeezed light. Specifically, we generate a Stokes beam with 5.2dB of amplitude squeezing using traveling-wave optical parametric amplification in second-order nonlinear waveguides, and combine it with a tunable coherent pump to access vibrational modes spanning from 1000 to 3100cm−1. Applied to quantum imaging of metabolites in biological tissue (pork muscle), our quantum-enhanced Raman microscope achieves an average noise suppression of 3.6dB and a 51% enhancement in signal-to-noise ratio (SNR) -- to the best of our knowledge, the largest improvement reported to date in quantum-enhanced SRS microscopy of biological samples.
Quantum-enhanced stimulated Raman scattering (QE-SRS) is a promising technique for highly sensitive molecular vibrational imaging and spectroscopy surpassing the shot noise limit. However, the previous demonstrations of QE-SRS utilized rather weak optical power which hinders from competing with the sensitivity of state-of-the-art SRS microscopy and spectroscopy using relatively high-power optical pulses. Here, we demonstrate SRS spectroscopy with quantum-enhanced balanced detection (QE-BD) scheme, which works even when using high-power optical pulses. We used 4-ps pulses to generate pulsed squeezed vacuum at a wavelength of 844 nm with a squeezing level of −3.28 ± 0.12 dB generated from a periodically-poled stoichiometric LiTaO3 waveguide. The squeezed vacuum was introduced to an SRS spectrometer employing a high-speed spectral scanner to acquire QE-SRS spectrum in the wavenumber range of 2000–2280 cm-1 within 50 ms. Using SRS pump pulses with an average power of 11.3 mW, we successfully obtained QE-SRS spectrum whose SNR was better than classical SRS with balanced-detection by 2.27 dB.