Quantum sources of light are of paramount importance for the development of photonic quantum technologies. The growing demand for bright, efficient, and spectrally engineered photonic sources for applications in quantum sensing, spectroscopy, and imaging has motivated the development of tailored nonlinear crystals. Here, we report on the development and characterization of chirped, apodized KTP crystals specifically engineered for quantum spectroscopy. Our source exhibits an unprecedented bandwidth in a highly non-degenerate configuration, demonstrating its potential to support quantum spectroscopy protocols over broad spectral ranges while enabling significantly shorter measurement times.
Quantum sources of light are of paramount importance for the development of photonic quantum technologies. The growing demand for bright, efficient, and spectrally engineered photonic sources for applications in quantum sensing, spectroscopy, and imaging has motivated the development of tailored nonlinear crystals. Here, we report on the development and characterization of chirped, apodized KTP crystals specifically engineered for quantum spectroscopy. Our source exhibits an unprecedented bandwidth in a highly non-degenerate configuration, demonstrating its potential to support quantum spectroscopy protocols over broad spectral ranges while enabling significantly shorter measurement times.
Spectroscopy in the mid-infrared region is an indispensable tool for identifying molecular types in various fields, including physics, chemistry, and medical sciences. However, conventional infrared light sources, detectors, and noise from blackbody radiation have been the obstacles to miniaturization and higher sensitivity of infrared spectrometers. Quantum infrared spectroscopy, which uses visible and infrared photon pairs in a quantum entangled state, has attracted attention as a new sensing technology that enables infrared spectroscopy with detectors in the visible range. However, the bandwidth of conventional quantum entangled light sources is at most 1 µm or less, which hinders broadband measurements, which are important in spectroscopic applications. Here we have realized an ultra-broadband entangled state of visible–infrared photons with wavelengths from 2 to 5 µm, harnessing a specially designed nonlinear crystal with chirped poling structure inside. Furthermore, we constructed a nonlinear quantum interferometer using the ultra-broadband quantum entangled photons and realized broadband infrared spectroscopy of inorganic and organic materials using a visible detector made of silicon. Our results show that quantum infrared spectroscopy can achieve ultra-broadband spectroscopic measurements and pave the way for the highly sensitive, ultra-compact infrared spectrometers using quantum entangled photons.
Quantum light sources are essential building blocks for many quantum technologies, enabling secure communication, powerful computing, and precise sensing and imaging. Recent advancements have witnessed a significant shift toward the utilization of "flat" optics with thickness at subwavelength scales for the development of quantum light sources. This approach offers notable advantages over conventional bulky counterparts, including compactness, scalability, and improved efficiency, along with added functionalities. This review focuses on the recent advances in leveraging flat optics to generate quantum light sources. Specifically, the generation of entangled photon pairs through spontaneous parametric down-conversion in nonlinear metasurfaces, and single photon emission from quantum emitters including quantum dots and color centers in 3D and 2D materials are explored. The review covers theoretical principles, fabrication techniques, and properties of these sources, with particular emphasis on the enhanced generation and engineering of quantum light sources using optical resonances supported by nanostructures. The diverse application range of these sources is discussed and the current challenges and perspectives in the field are highlighted.
Nonlinear spectroscopy with quantum entangled photons is an emerging field of research that holds the promise to achieve superior signal-to-noise ratio and effectively isolate many-body interactions. Photon sources used for this purpose, however, lack the frequency tunability and spectral bandwidth demanded by contemporary molecular materials. Here, we present design strategies for efficient spontaneous parametric downconversion to generate biphoton states with adequate spectral bandwidth and at visible wavelengths. Importantly, we demonstrate, by suitable design of the nonlinear optical interaction, the scope to engineer the degree of spectral correlations between the photons of the pair. We also present an experimental methodology to effectively characterize such spectral correlations. Importantly, we believe that such a characterization tool can be effectively adapted as a spectroscopy platform to optically probe system-bath interactions in materials.
Entangled photon spectroscopy is a nascent field that has important implications for measurement and imaging across chemical, biology, and materials fields. Entangled photon spectroscopy potentially offers improved spatial and temporal-frequency resolutions, increased cross sections for multiphoton and nonlinear measurements, and new abilities in inducing or measuring quantum correlations. A critical step in enabling entangled photon spectroscopies is the creation of high-flux entangled sources that can use conventional detectors as well as provide redundancy for the losses in realistic samples. Here, we report a periodically poled, chirped, lithium tantalate platform that generates entangled photon pairs with ∼10−7 efficiency. For a near watt level diode laser, this results in a near μW-level flux. The single photon per mode limit that is necessary to maintain non-classical photon behavior is still satisfied by distributing this power over up to an octave-spanning bandwidth. The spectral–temporal photon correlations are observed via a Michelson-type interferometer that measures the broadband Hong–Ou–Mandel two-photon interference. A coherence time of 245 fs for a 10 nm bandwidth in the collinear case and a coherence time of 62 fs for a 125 nm bandwidth in the non-collinear case are measured using a CW pump laser and, essentially, collecting the full photon cone. We outline in detail the numerical methods used for designing and tailoring the entangled photons source, such as changing center wavelength or bandwidth, with the ultimate aim of increasing the availability of high-flux UV–Vis entangled photon sources in the optical spectroscopy community.
Abstract Shaped laser pulses have been remarkably effective in investigating various aspects of light–matter interactions spanning a broad range of research. Chirped laser pulses exhibiting a time‐varying frequency, or quadratic spectral phase, form a crucial category in the group of shaped laser pulses. This type of pulses have made a ubiquitous presence from spectroscopic applications to developments in high‐power laser technology, and from nanophotonics to quantum optical communication, ever since their introduction. In the case of quantum technologies recently, substantial efforts are being invested toward achieving a truly scalable architecture. Concurrently, it is important to develop methods to produce robust photon sources. In this context, semiconductor quantum dots hold great potential, due to their exceptional photophysical properties and on‐demand operating nature. Concerning the scalability aspect of semiconductor quantum dots, it is advantageous to develop a simple, yet robust method to generate photon states from it. Chirped pulse excitation has been widely demonstrated as a robust and efficient state preparation scheme in quantum dots, thereby boosting its applicability as a stable photon source in a real‐world scenario. Despite the rapid growth and advancements in laser technologies, the generation and control of chirped laser pulses can be demanding. Here, an overview of a selected few approaches is presented to tailor and characterize chirped pulses for the efficient excitation of a quantum dot source. By taking the chirped‐pulse‐induced adiabatic rapid passage process in quantum dot as an example, numerical design examples are presented along with experimental advantages and challenges in each method and conclude with an outlook on future perspectives.
Two important challenges in quantum photonics are to generate useful states with high fidelity, and to detect them and verify their properties. Particularly valuable states are single photons and entangled photon pairs in well-defined optical modes, as they can be used in many quantum information protocols or used to build up more complex states. For sources, we employ integrated nonlinear optics (waveguides in lithium niobite and potassium titanyl phosphate) to maximize brightness and go beyond what is possible in bulk optics, showing simultaneously high state fidelity, heralding efficiency, and spectral purity across three experiments: first we show record heralding efficiency in a fully-fibered heralded single-photon source, and use it to probe the tradeoff between spectral purity and heralding efficiency in non-engineered sources. With an engineered source, we then herald up to 50 photons in a nonclassical state. The last source is for polarization-entangled photon pairs, with brightness of 3.5 million pairs/s·mW, fidelity to a Bell state of 96%, heralding efficiency of 43%, and HOM interference visibility of 82%. Once a complex state is constructed, it must also be verified. For this we employ a time-multiplexed detector consisting of a fibre loop and a single-photon detector. Surprisingly, we are able to extract information even in the saturation regime of the detector. We use the click statistics of the time-multiplexed detector to verify the non-classicality of quantum light, and we use its extremely high dynamic range (123 dB) to measure a macroscopic power level with a single-photon detector. Eliminating calibrated attenuators with this approach will allow direct standardization of quantum and classical optical power levels.