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 $5.2~\mathrm{dB}$ 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 $3100~\mathrm{cm}^{-1}$. Applied to quantum imaging of metabolites in biological tissue (pork muscle), our quantum-enhanced Raman microscope achieves an average noise suppression of $3.6~\mathrm{dB}$ 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.

Abstract Multimode squeezed light is a key resource for high-dimensional quantum technologies, enhancing metrological sensitivity, boosting communication security, and enabling parallel processing in computation. Its practical potential, however, remains constrained by the inherent single-mode operation of homodyne detection, necessitating post-processing for multimode characterization. Here, we overcome this long-standing challenge by employing multimode optical parametric amplification, enabling loss-tolerant direct detection of squeezing in each mode, which in turn permits mode sorting after amplification. As a result, we demonstrate, for the first time to the best of our knowledge, the real-time monitoring of multimode squeezing. With a spatial light modulator sorting the modes, we simultaneously measure squeezing in nine spatial modes co-propagating within one beam. Although mode sorting and filtering reduce the detection efficiency to less than 0.3%, we observe high-purity squeezing of up to − 7.9 ± 0.6 dB – to the best of our knowledge, the highest squeezing recorded for pulsed light. Furthermore, we demonstrate real-time, loss-tolerant characterization of continuous-variable entanglement and extend it to the detection of cluster states. Similar methods can be applied in the frequency domain, facilitating a crucial capability for scalable quantum technologies.

Characterizing macroscopic quantum states of light is a frontier challenge at the interface of quantum optics and high-intensity photonics. Here, we demonstrate the first, to our knowledge, direct phase-space tomography of a bright, ultrafast quantum state. We adapt a single-shot f-2f interferometer to sample the Husimi Q-function of a 25 fs bright squeezed vacuum (BSV) pulse (mean photon number N ∼10 12 ) subject to Kerr nonlinearity. Our measurement reveals a clear transformation from a Gaussian distribution with pronounced quadrature antisqueezing to a characteristic "S"-shaped profile as the intensity-dependent nonlinear phase increases. Crucially, we show theoretically that despite optical loss, the state does not degrade into classically modulated light but is rigorously described as a statistical mixture of squeezed coherent states. While global Wigner negativity is masked by technical noise, our results show theoretically that the constituent states individually retain strong Wigner-negative features. This work bridges quantum optics and high-intensity photonics, establishing a platform for diagnosing bright quantum resources.

Spontaneous parametric down-conversion (SPDC) in subwavelength nonlinear nanostructures is emerging as a promising source of quantum light, owing to its intrinsic multifunctionality and ability to generate versatile and complex quantum states. Despite this growing interest, the physical mechanisms governing photon-pair generation in nanostructures remain only partially understood. In particular, experimental investigations of key emission properties in individual resonators, such as spatial directionality and spectral characteristics, are still lacking, and predictive theoretical frameworks with direct experimental validation have not yet been established. Here we measure, for the first time, the spatial and spectral properties of photon pairs generated via SPDC in a lithium-niobate bullseye nanostructured resonator. Both spatial and spectral properties show a resonant behavior, which we describe within an extended quasi-normal-mode theoretical framework. This comparison with the theory is enabled by photon-pair count rates reaching up to 0.45 Hz/mW, to our knowledge, the highest reported to date for a nanostructured resonator. Our results provide new physical insight into SPDC in nanostructures and represent an important step toward predictive design strategies for efficient nanoscale sources of quantum light.

We adapt the Jaynes-Cummings model to study the interface of cavity quantum electrodynamics with strong field and attosecond physics. We show how multi-photon resonances in the Jaynes- Cummings system driven by a strong low-frequency classical light field lead to the generation of highly non-classical, quantum-correlated harmonics of the classical driver. Our treatment assumes no approximations, apart from the typical Jaynes-Cummings model assumption of only a few discrete quantum modes of light. The paper is dedicated to Joseph Henry Eberly, whose remarkable research has left indelible mark on both strong field physics and quantum optics.

Pairs of entangled photons are crucial for photonic quantum technologies. The demand for integrability and multi-functionality suggests 'flat' platforms - ultrathin layers and metasurfaces - as sources of photon pairs. With the success in demonstrating spontaneous parametric down-conversion (SPDC) from such sources, an alternative process to generate photon pairs, spontaneous four-wave mixing (SFWM), also starts to attract interest. In materials with nonzero second-order nonlinear susceptibility χ^(2), SFWM can generate photon pairs both directly, through the third-order nonlinear susceptibility χ^(3), and in a cascaded way, through second harmonic generation (SHG) followed by SPDC. Usually, the cascaded process is more efficient. Here, we show that in a thin layer, direct SFWM dominates, because the wavevector mismatch for SFWM is much smaller than for SHG or SPDC. To demonstrate it, we implement the photon pair generation via SFWM in a second-order nonlinear material - a thin layer of lithium niobate (LN). The existence of both second- and third-order nonlinear processes offers broader opportunities for quantum state engineering.

We introduce an ultrafast, bright, entangled twin-beam source generated by type-0 parametric down-conversion in periodically-poled lithium niobate at MHz repetition rate, with continuously tunable Schmidt number K set by the pump pulse duration. Photon-number statistics characterization via g(2)(0) and singular-value decomposition of the signal spectral density matrix yield K ~ 1.05 and K ~ 1.03, respectively, maintained over multiple orders of magnitude in brightness. Group-delay dispersion of the pump drives a continuous transition from single-mode operation to a controlled multimode regime, consistent with the temporal gain window departing from the inverse phase-matching bandwidth. Strong non-degeneracy of the source (signal at 1.37 µm, idler at 4.0 µm, ~ 100 fs duration) decouples a mid-infrared interaction wavelength, which overlaps with molecular vibrational resonances, from a near-infrared detection band, establishing a practical platform for quantum-enhanced metrology, nonlinear interferometry, and mid-infrared spectroscopic sensing. We show that in the bright few-mode limit, the total entanglement resource is clearly separated between modal and occupational degrees of freedom, and that our source allocates up to 95-97% of that resource to the occupational sector.

Non-Gaussian states of light are essential for numerous quantum information protocols; thus, certifying non-Gaussianity is crucial. Full quantum state tomography achieves this, but it implies observing the Wigner function negativity, which requires efficient detection. Certifying non-Gaussianity through directly measurable parameters is a simpler alternative, typically achieved by measuring photon-number probabilities - either directly using photon-number resolving detectors or through Hanbury Brown-Twiss type measurements with single-photon detectors. Here, we demonstrate theoretically and experimentally that optical parametric amplification combined with conventional intensity detectors can effectively replace this approach without the need for photon-number resolution. In our method, we measure the mean photon number and the second-order correlation function for the amplified state. Using it, we successfully certify the non-Gaussianity of a heralded quasi-single-photon state. Since optical parametric amplification is a multimode process, our method provides a foundation for developing high-dimensional quantum technologies utilizing multimode non-Gaussian states.

Flat-optics platforms offer new opportunities for the generation of entangled photons by relaxing traditional phase-matching constraints, enabling the use of a broader range of nonlinear materials. Among these, gallium arsenide and aluminum gallium arsenide stand out for their exceptionally high second-order nonlinearities, but their conventional orientation (001) has limited their applicability for photon-pair generation. By transitioning to crystals with (111) surface orientation, we overcome these limitations. We demonstrate a flat-optics-based telecom-range SPDC source using Al 0.30 Ga 0.70 As that achieves a high photon-pair generation rate per pump power and bandwidth of up to 0.24 Hz/mW/nm. The choice of 30% aluminum concentration allowed us to reduce pump absorption and photoluminescence background for photon pairs generation at telecom wavelengths by at least an order of magnitude compared to that of GaAs. The specific layer orientation facilitates the generation of orthogonally polarized entangled photons, a prerequisite for polarization-entangled states. Rather than directly probing entanglement, we observe the effect of hidden polarization. Our results highlight AlGaAs (111) as a promising platform for scalable quantum photonic sources and shed light on nonclassical polarization effects accessible through flat-optics engineering.

Die Starkfeldphysik untersucht die Interaktion von intensivem Licht mit Materie. Während für entsprechende Experimente bisher praktisch ausschließlich klassisches Laserlicht verwendet wurde, haben wir mit Hilfe von Wolframspitzen untersucht, wie sich Starkfeld‐Phänomene verhalten, wenn stattdessen intensives Quantenlicht als Treiber verwendet wird.

Multimode squeezed light is a key resource for high-dimensional photonic quantum technologies, enabling applications in quantum-enhanced sensing, quantum communication, and quantum computing. Efficient detection of such a multimode squeezed state is essential for unlocking its full potential. Optical parametric amplification (OPA) has recently gained attention as a powerful technique offering loss-tolerant, direct broadband detection, and multimode operation. While OPA has been used to characterize spatially multimode squeezing, its application to spectrally multimode squeezing has not yet been demonstrated. Here, we report on the first experimental demonstration of spectrally multimode squeezing detection using OPA. We achieve simultaneous detection of squeezing across more than 60 spectral modes of a broadband squeezed vacuum state. The observed squeezing is nearly uniform, ranging from -6.5 to -7 dB, which makes the source particularly suitable for constructing continuous-variable cluster states, and indicates the multimode capability of the OPA. The results extend the capabilities of OPA detection into the spectral domain, advancing spectral-mode-based high-dimensional photonic quantum technologies.

Until recently, attosecond optical spectroscopy and quantum optics evolved along non-overlapping directions. In attosecond science, attosecond pulses have been regarded as classical waves, applied to probe electron dynamics on their natural time scale. Here, we transfer fundamental concepts of quantum optics into attosecond physics, enabling control of both the properties of the XUV attosecond pulses and the quantum fluctuations of matter on attosecond time scales. By combining bright squeezed vacuum (BSV) with a strong laser field to drive high-harmonic generation, we transfer the quantum properties of the BSV onto the resulting XUV attosecond pulses. Applying advanced attosecond interferometry, we reconstruct the quantum state of the XUV high harmonics and their associated attosecond pulses with attosecond precision. Finally, we resolve the squeezing of the electron's wavepacket during one of the most fundamental strong-field phenomena - field induced tunneling. The ability to measure and control quantum correlations in both electrons and XUV attosecond pulses establishes a foundation for attosecond quantum electrodynamics, manipulating the quantum state of electrons and photons with sub-cycle precision.

Attosecond science relies on driving electrons after photoemission with the strong optical field of a laser pulse, representing an intense classical coherent state of light. Bright squeezed vacuum (BSV) is a quantum state of light intense enough to drive strong-field physics. However, its mean optical electric field is zero, suggesting that, in a semiclassical view, electrons should not experience strong driving. The question arises if and how this quantum state of light can generate attosecond science signatures in strong-field photoemission. Here we show that the key signatures of strong-field physics - the high energy plateau and the 10-U_p-cut-off - also appear under BSV driving of a needle tip, but only when we post-select electron energy spectra on the individual photon number of each BSV pulse. When averaging over many BSV shots, we observe broad energy spectra featuring no plateau. This suggests that BSV-driven electrons behave as if driven by an ensemble of coherent states of light. Our findings bridge strong-field physics and quantum optics, offering insights into BSV and other quantum light states. Our work paves the way for electron quantum state engineering and the use of strongly driven electrons as quantum light sensors.

The ability to engineer pairs of entangled photons is essential to quantum information science, and generating these states using spontaneous parametric down-conversion (SPDC) in nano- and micrometer-scale materials offers numerous advantages. To properly engineer such sources, a reliable model describing nano- and micrometer-scale SPDC is necessary; however, such a theoretical description remains a challenge. Here, we propose and derive a simplified model to describe SPDC in resonant structures, which considers the generation of photon pairs and the resonant enhancement of spectral bands to be separate processes, even though they actually occur simultaneously. We compare our simplified model to both the rigorous theory of SPDC in an etalon – a simple example of a resonant structure – and our experiments on SPDC in etalons and find agreement for low-gain SPDC. By simplifying the calculations required to generate photon pairs, our model promises to make designing complex resonant structures easier, and it promises to hasten the iteration of designs across the field of quantum state engineering.

The extreme light-matter interaction has brought unique tools for the subfemtosecond control of electron dynamics [1] and ultra-fast spectroscopy [2]. Until recently, the strong-field regime was accessible only with coherent states of light, which can be well described by classical electric fields when many photons are present (Fig. 1a). With the use of intense states of non-classical light, this situation has changed. New opportunities emerge with bright squeezed vacuum (BSV), which can be generated from optical parametric amplification of quantum vacuum fluctuations. Unlike classical light, BSV is a quantum superposition of coherent states with an amplitudes spanning a range from zero to very high values, up to ~1 TW/cm2 [3]. BSV has a zero mean electric field and the variance of the electric field oscillates at the double carrier frequency (Fig. 1a). How such a non-classical electric field can affect the dynamics of photoemitted electrons was theoretically demonstrated recently [4]. Furthermore, the photon-number distribution of BSV has a very long tail in contrast to coherent light. These photon-number distributions can be imprinted onto the photon statistics of optical harmonics [3] and the statistics of electrons [5].

Pairs of entangled photons are crucial for photonic quantum technologies. The demand for integrability and multi-functionality suggests "flat" platforms-ultrathin layers and metasurfaces-as sources of photon pairs. Despite the success in the demonstration of spontaneous parametric downconversion (SPDC) from such sources, there are almost no works on spontaneous four-wave mixing (SFWM)-an alternative process to generate photon pairs. Meanwhile, SFWM can be implemented in any nanostructures, including ones made of isotropic materials, which are easier to fabricate than crystalline SPDC sources. Here, we investigate photon pair generation through SFWM in subwavelength films of amorphous silicon nitride (SiN) with varying nitrogen content. For all samples, we demonstrate two-photon quantum correlations, indicated by the normalized second-order correlation function g(2)(0): it exceeds 2 and decays as the pump power increases. By observing two-photon interference between SFWM from the SiN films and the fused silica (FS) substrate, we find the third-order susceptibilities of films with different nitrogen content.

Strong optical nonlinearities are key to a range of technologies, particularly in the generation of photonic quantum states. The strongest nonlinearity in hot atomic vapors originates from electromagnetically induced transparency (EIT), which, while effective, often lacks tunability and suffers from significant losses due to atomic absorption. We propose and demonstrate an N-level EIT scheme, created by an optical frequency comb that excites a warm rubidium vapor. The massive number of comb lines simultaneously drive numerous transitions that interfere constructively to induce a giant and highly tunable cross-Kerr optical nonlinearity. The obtained third-order nonlinearity values range from 1.2 × 10^-7 to 7.7 × 10^-7 m^2 V^-2. Above and beyond that, the collective N-level interference can be optimized by phase shaping the comb lines using a spectral phase mask. Each nonlinearity value can then be tuned over a wide range, from 40% to 250% of the initial strength. We utilize the nonlinearity to demonstrate squeezing by self polarization rotation of CW signals that co-propagate with the pump and are tuned to one of the EIT transparent regions. Homodyne measurements reveal a quadrature squeezing level of 3.5 dB at a detuning of 640 MHz. When tuned closer to an atomic resonance, the nonlinearity is significantly enhanced while maintaining low losses, resulting in the generation of non-Gaussian cubic phase states. These states exhibit negative regions in their Wigner functions, a hallmark of quantum behavior. Consequently, N-level EIT enables the direct generation of photonic quantum states without requiring postselection.

Two-photon interference, a quantum phenomenon arising from the principle of indistinguishability, is a powerful tool for quantum state engineering and plays a fundamental role in various quantum technologies. These technologies demand robust and efficient sources of quantum light, as well as scalable, integrable and multifunctional platforms. In this regard, quantum optical metasurfaces (QOMs) are emerging as promising platforms for quantum light generation, namely biphotons via spontaneous parametric down-conversion (SPDC), and its engineering. Due to the relaxation of phase matching, SPDC in QOMs allows different channels of biphoton generation, such as those supported by overlapping resonances, to occur simultaneously. In previously reported QOMs, however, SPDC was too weak to observe such effects. Here we develop QOMs based on [110]-oriented GaAs that provide more than an order of magnitude enhancement in SPDC rate, after accounting for the spectral bandwidth, compared to any other QOMs studied to date. This boosted efficiency allows the QOMs support the simultaneous generation of SPDC from several spectrally overlapping optical modes. Using polarization components in the interferometer analyzer, we intentionally erase the distinguishability between the biphotons from a high-Q quasi-bound-state-in-the-continuum resonance and a low-Q Mie resonance, which results in the first-time observation of two-photon interference in the spectral domain in these types of devices. This quantum interference can considerably enrich the generation of entangled photons in metasurfaces. Their advanced multifunctionality, improved nonlinear response, ease of fabrication and compact footprint of [110]-GaAs QOMs position them as promising platforms to fulfill the requirements for photonic quantum technologies.

Non-Gaussian states of light are a critical resource for fault-tolerant quantum computing and enhanced metrology, but are typically faint and often obtained via post-selection. Here, we demonstrate the deterministic generation of a bright non-Gaussian state by introducing a Kerr nonlinearity to a macroscopic state of light called bright squeezed vacuum (BSV). To characterize the resulting state, we use a single-shot f-2f interferometer to sample its Husimi function. We observe a clear transformation from a 2D Gaussian distribution to an 'S'-shaped non-Gaussian profile, which is the direct statistical evidence of the intensity-dependent nonlinear phase. The negativity of the Wigner function, which is an intrinsic property of any pure non-Gaussian state, cannot be observed because BSV is a mixed state even under minute optical loss. However, we show that BSV can be considered as a mixture of pure squeezed coherent states, for some of which Kerr-induced Wigner-function negativity is quite tolerant to loss. This work bridges the gap between quantum optics and ultrafast nonlinear optics, opening a path to quantum applications that require high photon flux.