Nonclassical States Of Light Research Articles

Plasmon Squeezing in Single-Molecule Junctions.

Scanning tunneling microscope (STM)-induced luminescence provides an ideal platform for electrical generation and the atomic-scale manipulation of nonclassical states of light. However, despite its extreme importance in quantum technologies, squeezed light emission with reduced quantum fluctuations has hitherto not been demonstrated in such a platform. Here, we theoretically predict that the emitted light from the plasmon mode can be squeezed in an STM single molecular junction subject to an external laser drive. Going beyond the traditional paradigm that generates squeezing with the quadratic interaction of photons, our prediction explores the molecular coherence involved in an anharmonic energy spectrum of a coupled plasmon-molecule-exciton system. Furthermore, we show that, by selectively exciting the energy ladder, the squeezed plasmon can show either sub- or super-Poissonian statistical properties. We also demonstrate that, following the same principle, the molecular excitonic mode can be squeezed simultaneously.

Transfer of non-classical features and quantum states of light in circularly coupled waveguide arrays

We investigate the applicability of the circular arrays of coupled single-mode optical waveguides in transferring the non-classical state of light for quantum information processing. We study the nonclassical states of light, such as a single-photon Fock state, a two-photon NOON state, a single-mode squeezed state and a two-mode squeezed state as inputs to the lattice, which are key resources for various applications in the field of quantum information science. In addition, for comparison, we also examine a coherent state. We investigate the transport of non-classical features and quantum states of light from one waveguide mode to another. For the single and two-mode squeezed states, we perform a detailed study of the evolution of the squeezing. Our work highlights the potential of the circular arrays of optical waveguides platform for the transport of non-classical features and quantum states of light. We expect our results should have applications in the physical implementation of photonic quantum technologies.

A gate-tunable graphene Josephson parametric amplifier

With a large portfolio of elemental quantum components, superconducting quantum circuits have contributed to advances in microwave quantum optics1. Of these elements, quantum-limited parametric amplifiers2-4 are essential for low noise readout of quantum systems whose energy range is intrinsically low (tens of μeV)5,6. They are also used to generate non-classical states of light that can be a resource for quantum enhanced detection7. Superconducting parametric amplifiers, such as quantum bits, typically use a Josephson junction as a source of magnetically tunable and dissipation-free non-linearity. In recent years, efforts have been made to introduce semiconductor weak links as electrically tunable non-linear elements, with demonstrations of microwave resonators and quantum bits using semiconductor nanowires8,9, a two-dimensional electron gas10, carbon nanotubes11 and graphene12,13. However, given the challenge of balancing non-linearity, dissipation, participation and energy scale, parametric amplifiers have not yet been implemented with a semiconductor weak link. Here, we demonstrate a parametric amplifier leveraging a graphene Josephson junction and show that its working frequency is widely tunable with a gate voltage. We report gain exceeding 20 dB and noise performance close to the standard quantum limit. Our results expand the toolset for electrically tunable superconducting quantum circuits. They also offer opportunities for the development of quantum technologies such as quantum computing, quantum sensing and for fundamental science14.

Optical-cavity mode squeezing by free electrons.

The generation of nonclassical light states bears a paramount importance in quantum optics and is largely relying on the interaction between intense laser pulses and nonlinear media. Recently, electron beams, such as those used in ultrafast electron microscopy to retrieve information from a specimen, have been proposed as a tool to manipulate both bright and dark confined optical excitations, inducing semiclassical states of light that range from coherent to thermal mixtures. Here, we show that the ponderomotive contribution to the electron-cavity interaction, which we argue to be significant for low-energy electrons subject to strongly confined near-fields, can actually create a more general set of optical states, including coherent and squeezed states. The postinteraction electron spectrum further reveals signatures of the nontrivial role played by A 2 terms in the light-matter coupling Hamiltonian, particularly when the cavity is previously excited by either chaotic or coherent illumination. Our work introduces a disruptive approach to the creation of nontrivial quantum cavity states for quantum information and optics applications, while it suggests unexplored possibilities for electron beam shaping.

Engineering nonclassical SU(1,1) coherent states of light by multiphoton excitation

Quantum optical systems with nonclassical features play a vital role in the physical implementation of a large variety of quantum technologies, such as quantum metrology, quantum information processing, and quantum computation protocols, and hence are important to exploit the quantum advantage. In this work, we construct a general class of nonclassical coherent states (CSs) of light and present a scheme to enhance their nonclassicality by multiphoton excitation. In particular, using various optical realizations of Lie algebra, we construct CSs of light following Barut-Girardello formalism and then perform the multiphoton discrete excitation on these continuous-variable optical CSs. We investigate the nonclassical features by analyzing the photon-counting probability distribution, Mandel parameter, quadrature squeezing, and Wigner quasi-probability distribution. Our numerical results show that, for a particular set of parametric values, these multiphoton excited states exhibit sub-Poisson photon-counting statistics, quadrature squeezing, and negativity of Wigner distribution, which are indicators of nonclassicality. Moreover, it is shown that the nonclassical nature of these states gets enhanced as the photon-excitation number increases.

Squeezed States of Light for Future Gravitational Wave Detectors at a Wavelength of 1550nm.

The generation of strongly squeezed vacuum states of light is a key technology for future ground-based gravitational wave detectors (GWDs) to reach sensitivities beyond their quantum noise limit. For some proposed observatory designs, an operating laser wavelength of 1550nm or around 2 μm is required to enable the use of cryogenically cooled silicon test masses for thermal noise reduction. Here, we present for the first time the direct measurement of up to 11.5dB squeezing at 1550nm over the complete detection bandwidth of future ground-based GWDs ranging from 10kHz down to below 1Hz. Furthermore, we directly observe a quantum shot-noise reduction of up to (13.5±0.1) dB at megahertz frequencies. This allows us to derive a precise constraint on the absolute quantum efficiency of the photodiode used for balanced homodyne detection. These results hold important insight regarding the quantum noise reduction efficiency in future GWDs, as well as for quantum information and cryptography, where low decoherence of nonclassical states of light is also of high relevance.

Efficient construction of witnesses of the stellar rank of nonclassical states of light.

The stellar hierarchy of quantum states of light classifies the states according to the Fock-state resources that are required for their generation together with unitary Gaussian operations. States with stellar rank n can be also equivalently referred to as genuinely n-photon quantum non-Gaussian states. Here we present an efficient method for construction of general witnesses of the stellar rank. The number of parameters that need to be optimized in order to determine the witness does not depend on the stellar rank and it scales quadratically with the number of modes. We illustrate the procedure by constructing stellar rank witnesses based on pairs of Fock state probabilities and also based on pairs of fidelities with superpositions of coherent states.

Beyond photon pairs—nonlinear quantum photonics in the high-gain regime: a tutorial

Integrated optical devices will play a central role in the future development of nonlinear quantum photonics. Here we consider the generation of nonclassical states of light within them with a focus on Gaussian states beyond the low-gain, single photon pair regime accurately described by perturbation theory. Starting from the solid foundation provided by Maxwell’s equations, we then move to applications by presenting a unified formulation that allows for a comparison of stimulated and spontaneous experiments in ring resonators and nanophotonic waveguides and leads directly to the calculation of the quantum states of light generated in high-gain nonlinear quantum photonic experiments.

Robust Preparation of Wigner-Negative States with Optimized SNAP-Displacement Sequences

Hosting nonclassical states of light in three-dimensional microwave cavities has emerged as a promising paradigm for continuous-variable quantum information processing. Here we experimentally demonstrate high-fidelity generation of a range of Wigner-negative states useful for quantum computation, such as Schrödinger-cat states, binomial states, Gottesman-Kitaev-Preskill states, as well as cubic phase states. The latter states have been long sought after in quantum optics and have never been achieved experimentally before. We use a sequence of interleaved selective number-dependent arbitrary phase (SNAP) gates and displacements. We optimize the state preparation in two steps. First we use a gradient-descent algorithm to optimize the parameters of the SNAP and displacement gates. Then we optimize the envelope of the pulses implementing the SNAP gates. Our results show that this way of creating highly nonclassical states in a harmonic oscillator is robust to fluctuations of the system parameters such as the qubit frequency and the dispersive shift.1 MoreReceived 10 December 2021Revised 19 April 2022Accepted 8 June 2022DOI:https://doi.org/10.1103/PRXQuantum.3.030301Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasQuantum information processing with continuous variablesQuantum Information

Molecular Optomechanics Approach to Surface-Enhanced Raman Scattering.

ConspectusMolecular vibrations constitute one of the smallest mechanical oscillators available for micro-/nanoengineering. The energy and strength of molecular oscillations depend delicately on the attached specific functional groups as well as on the chemical and physical environments. By exploiting the inelastic interaction of molecules with optical photons, Raman scattering can access the information contained in molecular vibrations. However, the low efficiency of the Raman process typically allows only for characterizing large numbers of molecules. To circumvent this limitation, plasmonic resonances supported by metallic nanostructures and nanocavities can be used because they localize and enhance light at optical frequencies, enabling surface-enhanced Raman scattering (SERS), where the Raman signal is increased by many orders of magnitude. This enhancement enables few- or even single-molecule characterization. The coupling between a single molecular vibration and a plasmonic mode constitutes an example of an optomechanical interaction, analogous to that existing between cavity photons and mechanical vibrations. Optomechanical systems have been intensely studied because of their fundamental interest as well as their application in practical implementations of quantum technology and sensing. In this context, SERS brings cavity optomechanics down to the molecular scale and gives access to larger vibrational frequencies associated with molecular motion, offering new possibilities for novel optomechanical nanodevices.The molecular optomechanics description of SERS is recent, and its implications have only started to be explored. In this Account, we describe the current understanding and progress of this new description of SERS, focusing on our own contributions to the field. We first show that the quantum description of molecular optomechanics is fully consistent with standard classical and semiclassical models often used to describe SERS. Furthermore, we note that the molecular optomechanics framework naturally accounts for a rich variety of nonlinear effects in the SERS signal with increasing laser intensity.Furthermore, the molecular optomechanics framework provides a tool particularly suited to addressing novel effects of fundamental and practical interest in SERS, such as the emergence of collective phenomena involving many molecules or the modification of the effective losses and energy of the molecular vibrations due to the plasmon–vibration interaction. As compared to standard optomechanics, the plasmonic resonance often differs from a single Lorentzian mode and thus requires a more detailed description of its optical response. This quantum description of SERS also allows us to address the statistics of the Raman photons emitted, enabling the interpretation of two-color correlations of the emerging photons, with potential use in the generation of nonclassical states of light. Current SERS experimental implementations in organic molecules and two-dimensional layers suggest the interest in further exploring intense pulsed illumination, situations of strong coupling, resonant-SERS, and atomic-scale field confinement.

Generation of nonclassical states of light via truncation of mixed states

A possible way of generating nonclassical states of light is via the truncation of a given state in the Fock basis. In recent work, we presented an alternative scheme for such quantum scissors [Phys. Rev. A 104, 033715 (2021)PLRAAN1050-294710.1103/PhysRevA.104.033715], employing a nondegenerate parametric amplifier, a beam splitter, and photodetectors. An advantage of this setup is that it does not require the generation of Fock states beforehand, as in previous proposals. Here we extend this treatment to mixed input states. We show the possibilities of generating truncated states with either a maximum Fock number N or states having a minimum Fock number N . We discuss two specific examples of states to be truncated: (i) the thermal state and (ii) the phase-diffused coherent state. In either case, the generated field states can present sub-Poissonian statistics as well as non-Gaussian character. These nonclassical properties can be adjusted by changing the parameters of the scissors, e.g., the amplifier strength and the beam-splitter transmittance.

Non-classical mechanical states guided in a phononic waveguide

The ability to create, manipulate and detect non-classical states of light has been key for many recent achievements in quantum physics and for developing quantum technologies. Achieving the same level of control over phonons, the quanta of vibrations, could have a similar impact, in particular on the fields of quantum sensing and quantum information processing. Here we present a crucial step towards this level of control and realize a single-mode waveguide for individual phonons in a suspended silicon microstructure. We use a cavity–waveguide architecture, where the cavity is used as a source and detector for the mechanical excitations while the waveguide has a free-standing end to reflect the phonons. This enables us to observe multiple round trips of phonons between the source and the reflector. The long mechanical lifetime of almost 100 μs demonstrates the possibility of nearly lossless transmission of single phonons over, in principle, tens of centimetres. Our experiment demonstrates full on-chip control over travelling single phonons strongly confined in the directions transverse to the propagation axis, potentially enabling a time-encoded multimode quantum memory at telecommunications wavelength and advanced quantum acoustics experiments. Non-classical vibrations are generated and transmitted along a mechanical waveguide, providing a platform for distributing quantum information and realizing hybrid quantum devices using phonons in a solid-state system.

Experimental Demonstration of Gaussian Boson Sampling with Displacement

Gaussian boson sampling (GBS) is a quantum sampling task in which one has to draw samples from the photon-number distribution of a large-dimensional nonclassical squeezed state of light. In an effort to make this task intractable for a classical computer, experiments building GBS machines have mainly focused on increasing the dimensionality and squeezing strength of the nonclassical light. However, no experiment has yet demonstrated the ability to displace the squeezed state in phase space, which is generally required for practical applications of GBS. In this work, we build a GBS machine that achieves the displacement by injecting a laser beam alongside a two-mode squeezed vacuum state into a 15-mode interferometer. We focus on two new capabilities. Firstly, we use the displacement to reconstruct the multimode Gaussian state at the output of the interferometer. Our reconstruction technique is in situ and requires only three measurement settings regardless of the state dimension. Secondly, we study how the addition of classical laser light in our GBS machine affects the complexity of sampling its output photon statistics. We introduce and validate approximate semiclassical models that reduce the computational cost when a significant fraction of the detected light is classical.4 MoreReceived 1 February 2022Accepted 19 April 2022DOI:https://doi.org/10.1103/PRXQuantum.3.020336Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasBoson samplingPhoton statisticsQuantum simulationQuantum states of lightQuantum tomographyQuantum InformationAtomic, Molecular & Optical

Theoretical studies on quantum imaging with time-integrated single-photon detection under realistic experimental conditions

We study a quantum-enhanced differential measurement scheme that uses quantum probes and single-photon detectors to measure a minute defect in the absorption parameter of an analyte under investigation. For the purpose, we consider two typical non-classical states of light as a probe, a twin-Fock state and a two-mode squeezed vacuum state. Their signal-to-noise ratios (SNRs) that quantifies the capability of detecting the defect are compared with a corresponding classical imaging scheme that employs a coherent state input. A quantitative comparison is made in terms of typical system imperfections such as photon loss and background noise that are common in practice. It is shown that a quantum enhancement in SNR can be described generally by the Mandel Q-parameter and the noise-reduction-factor, which characterize an input state that is incident to the analyte. We thereby identify the conditions under which the quantum enhancement remains and can be further increased. We expect our study to provide a guideline for improving the SNR in quantum imaging experiments employing a differential measurement scheme with time-integrated single-photon detectors.

High Photon Number Entangled States and Coherent State Superposition from the Extreme Ultraviolet to the Far Infrared.

We present a theoretical demonstration on the generation of entangled coherent states and of coherent state superpositions, with photon numbers and frequencies orders of magnitude higher than those provided by the current technology. This is achieved by utilizing a quantum mechanical multimode description of the single- and two-color intense laser field driven process of high harmonic generation in atoms. It is found that all field modes involved in the high harmonic generation process are entangled, and upon performing a quantum operation, lead to the generation of high photon number optical cat states spanning from the far infrared to the extreme ultraviolet spectral region. This provides direct insights into the quantum mechanical properties of the optical field in the intense laser matter interaction. Finally, these states can be considered as a new resource for fundamental tests of quantum theory, quantum information processing, or sensing with nonclassical states of light.

Entangled Photon Spectroscopy.

The enhanced interest in quantum-related phenomena has provided new opportunities for chemists to push the limits of detection and analysis of chemical processes. As some have called this the second quantum revolution, a time has come to apply the rules learned from previous research in quantum phenomena toward new methods and technologies important to chemists. While there has been great interest recently in quantum information science (QIS), the quest to understand how nonclassical states of light interact with matter has been ongoing for more than two decades. Our entry into this field started around this time with the use of materials to produce nonclassical states of light. Here, the process of multiphoton absorption led to photon-number squeezed states of light, where the photon statistics are sub-Poissonian. In addition to the great interest in generating squeezed states of light, there was also interest in the formation of entangled states of light. While much of the effort is still in foundational physics, there are numerous new avenues as to how quantum entanglement can be applied to spectroscopy, imaging, and sensing. These opportunities could have a large impact on the chemical community for a broad spectrum of applications.In this Account, we discuss the use of entangled (or quantum) light for spectroscopy as well as applications in microscopy and interferometry. The potential benefits of the use of quantum light are discussed in detail. From the first experiments in porphyrin dendrimer systems by Dr. Dong-Ik Lee in our group to the measurements of the entangled two photon absorption cross sections of biological systems such as flavoproteins, the usefulness of entangled light for spectroscopy has been illustrated. These early measurements led the way to more advanced measurements of the unique characteristics of both entangled light and the entangled photon absorption cross-section, which provides new control knobs for manipulating excited states in molecules.The first reports of fluorescence-induced entangled processes were in organic chromophores where the entangled photon cross-section was measured. These results would later have widespread impact in applications such as entangled two-photon microscopy. From our design, construction and implementation of a quantum entangled photon excited microscope, important imaging capabilities were achieved at an unprecedented low excitation intensity of 107 photons/s, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. New reports have also illustrated an advantage of nonclassical light in Raman imaging as well.From a standpoint of more precise measurements, the use of entangled photons in quantum interferometry may offer new opportunities for chemistry research. Experiments that combine molecular spectroscopy and quantum interferometry, by utilizing the correlations of entangled photons in a Hong-Ou-Mandel (HOM) interferometer, have been carried out. The initial experiment showed that the HOM signal is sensitive to the presence of a resonant organic sample placed in one arm of the interferometer. In addition, parameters such as the dephasing time have been obtained with the opportunity for even more advanced phenomenology in the future.

Extending the Hong-Ou-Mandel effect: The power of nonclassicality

We show that the parity (evenness or oddness) of a nonclassical state of light has a dominant influence on the interference effects at a balanced beam splitter, irrespective of the state initially occupying the other input mode. Specifically, the parity of the nonclassical state gives rise to destructive interference effects that result in deep valleys in the output joint number distribution of which the Hong-Ou-Mandel (HOM) effect is a limiting case. The counter-intuitive influence of even a single photon to control the output of a beam splitter illuminated by any field, be it a coherent or even a noisy thermal field, demonstrates the extraordinary power of non-classicality. The canonical example of total destructive interference of quantum amplitudes leading to the absence of coincidence counts from a 50/50 beam splitter is the celebrated HOM effect, characterized by the vanishing of the joint probability of detecting singe photons in each of the output beams. We show that this is a limiting case of more general input states upon which a 50/50 BS can create total, or near total, destructive interference of quantum amplitudes. For odd photon number input Fock states of arbitrary value n>0 we show that the joint photon number probabilities vanish when detecting identical photon numbers in each output beams. We examine the mixing of photon number states of n = 1, 2, and 3 with a CV state, such as a coherent state of arbitrary amplitude, and a thermal state. These vanishing joint probabilities form what we call a central nodal line -- a contiguous set of zeros representing complete destructive interference of quantum amplitudes. For odd or even photon number Fock states with n>1 there will be additional off-diagonal pseudo-nodal curves along which the joint photon number probabilities are either zero, or near zero, which constitute a near, but not complete, destructive interference.

Формирование неклассических многофотонных состояний света со сжатыми квантовыми флуктуациями в волокнах из модифицированного висмутом теллуритного стекла

An optical fiber with a high Kerr nonlinearity coefficient is proposed and produced from a bismuth-modified tellurite glass for creation of nonclassical multiphoton states of light. Specifically, we propose to use those fibers to squeeze the quantum fluctuations of one of the quadratures of light in the 20 W signal significantly below -10 dB compared to the standard quantum noise limit, which is important for various practical applications. Using numerical modeling based on stochastic nonlinear Schrodinger equation, we demonstrate noise squeezing stronger than -16 dB for lengths of tellurite fiber 6-14 m, while squeezing of -14 dB is expected in silica fibers for lengths of 120-300 m. Analytical formulas were used to analyse the physical factors which limit the squeezing achievable.

Nonclassical states of light in a nonlinear Michelson interferometer

Nonlinear quantum metrology schemes can lead to faster than Heisenberg-limited scalings for the measurement uncertainty. We study a Michelson interferometer embedded in a Kerr medium [Phys. Rev. A 92, 022104 (2015)] that leads to nonlinear, intensity dependent phase shifts corresponding to relative changes in the lengths of its two arms. The quantum Cram\'er-Rao bound on the minimum achievable measurement uncertainties is worked out and the requirements, in practice, to saturate the bound are investigated. The choice of input state of light into the interferometer and the readout strategy at the output end are discussed. The ideal nonclassical states of light that must be used to saturate the bound are found to be highly susceptible to photon loss noise. We identify optimal states at each noise level that are both resilient to noise and capable of giving the enhanced sensitivities and discuss practical implementations of the interferometry scheme using such states.

Vacuum-field-induced THz transport gap in a carbon nanotube quantum dot

The control of light-matter interaction at the most elementary level has become an important resource for quantum technologies. Implementing such interfaces in the THz range remains an outstanding problem. Here, we couple a single electron trapped in a carbon nanotube quantum dot to a THz resonator. The resulting light-matter interaction reaches the deep strong coupling regime that induces a THz energy gap in the carbon nanotube solely by the vacuum fluctuations of the THz resonator. This is directly confirmed by transport measurements. Such a phenomenon which is the exact counterpart of inhibition of spontaneous emission in atomic physics opens the path to the readout of non-classical states of light using electrical current. This would be a particularly useful resource and perspective for THz quantum optics.