Tai Hyun Yoon

We realize a hardware-native time--frequency Gottesman--Kitaev--Preskill (GKP) logical qubit encoded in the continuous phase space of single photons, establishing a propagating photonic implementation of bosonic grid encoding. Finite-energy grid states are generated deterministically using coherently driven entangled nonlinear biphoton sources that produce single-photon frequency-comb supermodes. An optical-frequency-comb reference anchors the time--frequency phase space and enforces commuting displacement stabilizers directly at the hardware level, continuously defining the logical subspace. Timing jitter, spectral drift, and phase noise map naturally onto Gaussian displacement errors within this lattice, yielding intrinsic correctability inside a stabilizer cell. Logical operations correspond to experimentally accessible phase and delay controls, enabling deterministic state preparation and manipulation. Building on the modal time--frequency GKP framework, we identify a concrete pathway toward active syndrome extraction and deterministic displacement recovery using ancillary grid states and interferometric time--frequency measurements. These primitives establish a hardware-compatible route for integrating the time--frequency GKP logical layer into erasure-aware and fusion-based fault-tolerant photonic architectures.

Asynchronous and interferometric transient absorption (AI-TA) spectroscopy is a powerful technique for probing ultrafast dynamics, offering both time-resolved insights and frequency-domain information with a single-point detector. In this study, we successfully measured the transient absorption signal of rod-shaped tellurium microcrystals under low pump fluence using a mid-infrared (MIR) AI-TA setup. By leveraging exceptionally stable frequency combs for both the pump and probe beams, coherent averaging in the MIR AI-TA enabled the clear observation of transient absorption signals, even in heterogeneous samples under low pump fluence. The standard deviation of the TA signal decreases with averaging time (τavg) following a 1/τavg dependence, confirming the ergodicity of the TA measurement over extended averaging periods. These results highlight the significant potential of MIR AI-TA spectroscopy for advancing our understanding of ultrafast carrier dynamics in MIR-active materials.

By employing two synchronized mode-locked femtosecond lasers and interferometric detection of the pump-probe spectra—referred to as asynchronous and interferometric transient absorption—we have developed a method for broad dynamic range and rapid data acquisition. Using asynchronous and interferometric transient absorption, we examined photochemical changes during femtosecond pump-probe experiments on all-inorganic cesium lead halide nanomaterials. The laser pulse train facilitates photoreactions while allowing real-time observation of charge carrier dynamics. In perovskite nanocrystals undergoing photo-substitution of halide anions, transient absorption spectra showed increasing bandgap energy and faster relaxation dynamics as the Cl/Br ratio increased. For colloidal perovskite nanoplatelets, continuous observation revealed both spectral and kinetic changes during the light-induced coalescence of nanoplatelets, by analyzing temporal segments. This integrated technique not only deepens understanding of exciton dynamics and environmental influences in perovskite nanomaterials but also establishes asynchronous and interferometric transient absorption as a transformative tool for real-time observation of photochemical dynamics.

Mid‐infrared (MIR) spectroscopy has emerged as a pivotal tool for studying molecular dynamics with ultrafast time resolution, allowing precise investigations into structural changes, chemical reactions, and energy transfer processes. This review explores the transformative capabilities of femtosecond MIR spectroscopy techniques such as pump‐probe (PP) and two‐dimensional infrared (2DIR) spectroscopy, which offer unparalleled specificity in probing molecular vibrations and exploring complicated energy landscapes across diverse scientific fields. Advanced laser technologies, including pulse shapers and asynchronous optical sampling (ASOPS), have significantly enhanced the precision and efficiency of MIR spectroscopic methods. ASOPS, in particular, has revolutionized time‐resolved studies by mitigating traditional mechanical delay stage limitations, enabling robust femtosecond‐to‐nanosecond dynamics investigations with enhanced noise reduction and long‐term stability. This review provides a comprehensive overview of the evolution and strengths of MIR‐based PP and 2DIR spectroscopy, emphasizing the pivotal role of ASOPS in overcoming technical challenges. By delineating current methodologies, this review aims to guide researchers in selecting and optimizing experimental configurations tailored to their scientific inquiries.

We demonstrate continuous loading and strong collective coupling of atoms to a high finesse ring cavity. A series of spatially separated laser cooling stages delivers a continuous flux of 2.1(3)×10^{7} ^{88}Sr atoms/s into an intracavity magic wavelength lattice where the atoms are deterministically transported inside the ring cavity. We observe a continuous atom-cavity vacuum Rabi splitting, demonstrating the first steady-state strong collective coupling on a narrow linewidth atomic transition. This Letter opens the path to future continuous cold atom devices, such as a continuous wave superradiant laser with millihertz linewidth and low vibration sensitivity, enabling searches for new physics and technologies.

The photoacoustic (PA) effect has been widely used in various applications, including highly sensitive spectroscopy and label-free, non-invasive imaging. In this work, we demonstrate a fast and precise measurement of PA parameters for light-absorbing liquids using mid-infrared asynchronous sampling pump-probe measurements. To simulate the observed PA oscillation signals and extract various PA parameters as a function of pump power, we derived analytical solutions of the PA wave equation driven by a train of ultrashort Gaussian pump pulses. By fitting the analytical solution to the measured PA signals using a nonlinear curve fitting method, we could measure the PA parameters, including damping rate, viscosity, and natural frequency. Furthermore, the dynamic response of thermophysical properties of the chloroform solution is also investigated by measuring the variation of the Grüneisen parameter with pump power. We anticipate that this work will open new possibilities for precise in situ measurements of the thermal properties of light-absorbing liquids.

Current optical atomic clocks do not utilize their resources optimally. In particular, an exponential gain in sensitivity could be achieved if multiple atomic ensembles were to be controlled or read out individually, even without entanglement. However, controlling optical transitions locally remains an outstanding challenge for neutral-atom-based clocks and quantum computing platforms. Here we show arbitrary, single-site addressing for an optical transition via sub-wavelength controlled moves of atoms trapped in tweezers. The scheme is highly robust as it relies only on the relative position changes of tweezers and requires no additional addressing beams. Using this technique, we implement single-shot, dual-quadrature readout of Ramsey interferometry using two atomic ensembles simultaneously, and show an enhancement of the usable interrogation time at a given phase-slip error probability. Finally, we program a sequence that performs local dynamical decoupling during Ramsey evolution to evolve three ensembles with variable phase sensitivities, a key ingredient of optimal clock interrogation. Our results demonstrate the potential of fully programmable quantum optical clocks even without entanglement and could be combined with metrologically useful entangled states in the future.

We discuss nonclassicality of nondegenerate optical parametric oscillator operating far below-threshold with weak seed fields. We show nonclassical measure that depends on the seeding amplitude ratio has the same values for intra- and extra-cavity fields.

Time-resolved multidimensional spectroscopy is an advanced spectroscopic technique that can be used to study the molecular structure and dynamics of chromophores in condensed phases by probing multiple resonances of chemical and biophysical systems. To achieve such a multidimensional measurement, the nonlinear optical response of materials should be measured for varying time delays between multiple optical pulses. Inevitably, the data acquisition time dramatically increases with the number of dimensions and the length of each time-delay scan. Therefore, technical breakthroughs toward improved data acquisition rates and time resolutions have long been sought for more versatile and extensive use of coherent multidimensional spectroscopy. Here, we present a tutorial description of the concepts and methods of coherent multidimensional spectroscopy with multiple repetition-frequency-stabilized lasers. Pulse trains from two lasers with slightly different repetition frequencies enable an asynchronous optical sampling (ASOPS), i.e., an automatic scan of the time delay between the pulses. By combining mechanical delay lines for interferometric pulse-pair generation and signal field detection with an incoherent ASOPS scheme for probing slow population dynamics of chromophores in condensed phases, we show that the dynamic range of time-delay scan and data acquisition speed for coherent multidimensional spectroscopy could be dramatically enhanced. In this tutorial paper, we summarize the current developments in this and related research areas, and provide perspectives on all optically controlled multidimensional spectroscopy with multiple synchronized lasers.