Entangled photons exhibit non-classical light-matter interactions that create new opportunities in materials and molecular science. For example, in entangled two-photon absorption, the intensity-dependence scales linearly as if only one photon was present. The entangled two-photon absorption cross section approaches but does not match the one-photon absorption cross section. The entangled two photon cross section also does not follow classical two photon molecular design motifs. Questions such as these seed the rich but nascent field of entangled light-matter interactions. In this perspective, we use the experimental developments in entangled photon spectroscopy to outline the current status of the field. Now that the fundamental tools are outlined, it is time to start the exploration of how materials, molecules, and devices can control or utilize interactions with entangled photons.
We propose a novel femtosecond stimulated Raman spectroscopy (FSRS) technique that combines entangled photons with interference detection to select matter pathways and enhance the resolution. Following photo excitation by an actinic pump, the measurement uses a pair of broadband entangled photons, one (signal) interacts with the molecule together with a third narrowband pulse induces the Raman process. The other (idler) photon provides a reference for the coincidence measurement. This interferometric photon-coincidence counting detection allows to separately measure Raman gain and loss signals…
Multidimensional optical signals are commonly recorded by varying the delays between time ordered pulses. These control the evolution of the density matrix and are described by ladder diagrams. We propose a new non-time-ordered protocol based on following the time evolution of the wavefunction and described by loop diagrams. The time variables in this protocol allow to observe different types of resonances and reveal information about intraband dephasing not readily available by time ordered techniques. The time variables involved in this protocol become coupled when using entangled light, whi…
In virtual-state spectroscopy, information about the energy-level structure of an arbitrary sample is retrieved by Fourier transforming sets of measured two-photon absorption probabilities of entangled photon pairs where the degree of entanglement and the delay time between the photons have been varied. This works well for simple systems but quickly becomes rather difficult when many intermediate states are involved. We propose and discuss an extension of entangled two-photon absorption spectroscopy that solves this problem by means of repeated measurements at different pump wavelengths. Speci…
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 sampl…
Optical interferometry has been a long-standing setup for characterization of quantum states of light. Both the linear and the nonlinear interferences can provide information about the light statistics an underlying detail of the light-matter interactions. Here we demonstrate how interferometric detection of nonlinear spectroscopic signals may be used to improve the measurement accuracy of matter susceptibilities. Light-matter interactions change the photon statistics of quantum light, which are encoded in the field correlation functions. Application is made to the Hong-Ou-Mandel two-photon in…
Entangled two-photon absorption spectroscopy (TPA) has been widely recognized as a powerful tool for revealing relevant information about the structure of complex molecular systems. However, to date, the experimental implementation of this technique has remained elusive, mainly because of two major difficulties. First, the need to perform multiple experiments with two-photon states bearing different temporal correlations, which translates in the necessity to have at the experimenter's disposal tens, if not hundreds, of sources of entangled photons. Second, the need to have \emph{a priori} know…
Conventional nonlinear spectroscopy uses classical light to detect matter properties through the variation of its response with frequencies or time delays. Quantum light opens up new avenues for spectroscopy by utilizing parameters of the quantum state of light as novel control knobs and through the variation of photon statistics by coupling to matter. We present an intuitive diagrammatic approach for calculating ultrafast spectroscopy signals induced by quantum light, focusing on applications involving entangled photons with nonclassical bandwidth properties - known as "time-energy entangleme…
Interaction of light with media often occurs with a femtosecond response time. Its measurement by conventional techniques requires the use of femtosecond lasers and sophisticated time-gated optical detection1-3. Here we demonstrate that by exploiting quantum interference of entangled photons it is possible to measure the phase relaxation time of a media on the femtosecond time scale (down to 100 fs) using accessible continuous wave laser and single-photon counting. We insert the sample in the Hong-Ou-Mandel interferometer4 and infer the phase relaxation time from the modification of the two-ph…
Entangled photon pairs are predicted to linearize and increase the efficiency of two-photon absorption, allowing continuous wave laser diodes to drive ultrafast time-resolved spectroscopy and nonlinear processes. Despite a range of theoretical studies and experimental measurements, inconsistencies persist about the value of the entanglement enhanced interaction cross section. A spectrometer is constructed that can temporally and spectrally characterize the entangled photon state before, during, and after any potential two-photon excitation event. For the molecule Rhodamine 6G, which has a virt…
Recent investigations suggest that the use of non-classical states of light, such as entangled photon pairs, may open new and exciting avenues in experimental two-photon absorption spectroscopy. Despite several experimental studies of entangled two-photon absorption (eTPA), there is still a heated debate on whether eTPA has truly been observed. This interesting debate has arisen, mainly because it has been recently argued that single-photon-loss mechanisms, such as scattering or hot-band absorption may mimic the expected entangled-photon linear absorption behavior. In this work, we focus on tr…
Entangled photon pairs have been promised to deliver a substantial quantum advantage for two-photon absorption spectroscopy. However, recent work has challenged the previously reported magnitude of quantum enhancement in two-photon absorption. Here, we present an experimental comparison of sum-frequency generation and molecular absorption, each driven by isolated photon pairs. We establish an upper bound on the enhancement for entangled-two-photon absorption in Rhodamine-6G, which lies well below previously reported values.
Infrared (IR) spectroscopy is an indispensable tool for many practical applications including material analysis and sensing. Existing IR spectroscopy techniques face challenges related to the inferior performance and the high cost of IR-grade components. Here, we develop a new method, which allows studying properties of materials in the IR range using only visible light optics and detectors. It is based on the nonlinear interference of entangled photons, generated via Spontaneous Parametric Down Conversion (SPDC). In our interferometer, the phase of the signal photon in the visible range depen…
Polarization-resolved single dot spectroscopy performed on (211)B InAs/GaAs quantum dots reveals that the fine structure splitting of the excitonic levels in these dots is much lower compared to the usual (100)-grown InAs dots. Time-resolved measurements confirm the high oscillator strength of these dots, and thus their good quantum efficiency at 4 K, comparable with that of (100) InAs/GaAs dots. Last, photon correlation measurements demonstrate single photon emission out of the excitonic optical transition of these dots. All these features make this novel dot system very promising for impleme…
Nanophotonic entangled-photon sources are a critical building block of chip-scale quantum photonic architecture and have seen significant development over the past two decades. These sources generate photon pairs that typically span over a narrow frequency bandwidth. Generating entanglement over a wide spectral region has proven to be useful in a wide variety of applications including quantum metrology, spectroscopy and sensing, and optical communication. However, generation of broadband photon pairs with temporal coherence approaching an optical cycle on a chip is yet to be seen. Here we demo…
We use frequency entangled photons, generated via spontaneous parametric down conversion, to measure the broadband spectral response of an array of gold nanoparticles exhibiting Fano-type plasmon resonance. Refractive index sensing of a liquid is performed by measuring the shift of the array resonance. This method is robust in excessively noisy conditions compared with conventional broadband transmission spectroscopy. Detection of a refractive index change is demonstrated with a noise level 70 times higher than the signal, which is shown to be inaccessible with the conventional transmission sp…
The realization of a future quantum Internet requires processing and storing quantum information at local nodes, and interconnecting distant nodes using free-space and fibre-optic links. Quantum memories for light are key elements of such quantum networks. However, to date, neither an atomic quantum memory for non-classical states of light operating at a wavelength compatible with standard telecom fibre infrastructure, nor a fibre-based implementation of a quantum memory has been reported. Here we demonstrate the storage and faithful recall of the state of a 1532 nm wavelength photon, entangle…
Ultrastrong light-matter coupling in near-field coupled split-ring resonators revealed by photocurrent spectroscopy
Institute of Industrial Science, University of Tokyo（东京大学工业科学研究所）；Institute for Nano Quantum Information Electronics, University of Tokyo（东京大学纳米量子信息电子学研究所）
