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1. 1-GHz mid-infrared frequency comb spanning 3 to 13 μm

   https://doi.org/10.48550/arXiv.2201.07134  

   Hoghooghi, N.; Xing, S.; Chang, P.; Lesko, D.; Lind, A.; Rieker, G.; Diddams, S (July 2022, ArXivorg)

   Mid-infrared (MIR) spectrometers are invaluable tools for molecular fingerprinting and hyper-spectral imaging. Among the available spectroscopic approaches, GHz MIR dual-comb absorption spectrometers have the potential to simultaneously combine the high-speed, high spectral resolution, and broad optical bandwidth needed to accurately study complex, transient events in chemistry, combustion, and microscopy. However, such a spectrometer has not yet been demonstrated due to the lack of GHz MIR frequency combs with broad and full spectral coverage. Here, we introduce the first broadband MIR frequency comb laser platform at 1 GHz repetition rate that achieves spectral coverage from 3 to 13 {\mu}m. This frequency comb is based on a commercially available 1.56 {\mu}m mode-locked laser, robust all-fiber Er amplifiers and intra-pulse difference frequency generation (IP-DFG) of few-cycle pulses in \c{hi}(2) nonlinear crystals. When used in a dual comb spectroscopy (DCS) configuration, this source will simultaneously enable measurements with {\mu}s time resolution, 1 GHz (0.03 cm-1) spectral point spacing and a full bandwidth of >5 THz (>166 cm-1) anywhere within the MIR atmospheric windows. This represents a unique spectroscopic resource for characterizing fast and non-repetitive events that are currently inaccessible with other sources. 

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2. Broadband 1-GHz mid-infrared frequency comb

   https://doi.org/10.1038/s41377-022-00947-w  

   Hoghooghi, Nazanin; Xing, Sida; Chang, Peter; Lesko, Daniel; Lind, Alexander; Rieker, Greg; Diddams, Scott (September 2022, Light: Science & Applications)

   Abstract Mid-infrared (MIR) spectrometers are invaluable tools for molecular fingerprinting and hyper-spectral imaging. Among the available spectroscopic approaches, GHz MIR dual-comb absorption spectrometers have the potential to simultaneously combine the high-speed, high spectral resolution, and broad optical bandwidth needed to accurately study complex, transient events in chemistry, combustion, and microscopy. However, such a spectrometer has not yet been demonstrated due to the lack of GHz MIR frequency combs with broad and full spectral coverage. Here, we introduce the first broadband MIR frequency comb laser platform at 1 GHz repetition rate that achieves spectral coverage from 3 to 13 µm. This frequency comb is based on a commercially available 1.56 µm mode-locked laser, robust all-fiber Er amplifiers and intra-pulse difference frequency generation (IP-DFG) of few-cycle pulses inχ⁽²⁾nonlinear crystals. When used in a dual comb spectroscopy (DCS) configuration, this source will simultaneously enable measurements with μs time resolution, 1 GHz (0.03 cm⁻¹) spectral point spacing and a full bandwidth of >5 THz (>166 cm⁻¹) anywhere within the MIR atmospheric windows. This represents a unique spectroscopic resource for characterizing fast and non-repetitive events that are currently inaccessible with other sources. 

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3. Optimizing the sensitivity of high repetition rate broadband transient optical spectroscopy with modified shot-to-shot detection

   https://doi.org/10.1063/5.0143355  

   Hall, Siedah J.; Budden, Peter J.; Zats, Anne; Sfeir, Matthew Y. (April 2023, Review of Scientific Instruments)

   A major limitation of transient optical spectroscopy is that relatively high laser fluences are required to enable broadband, multichannel detection with acceptable signal-to-noise levels. Under typical experimental conditions, many condensed phase and nanoscale materials exhibit fluence-dependent dynamics, including higher order effects such as carrier–carrier annihilation. With the proliferation of commercial laser systems, offering both high repetition rates and high pulse energies, have come new opportunities for high sensitivity pump-probe measurements at low pump fluences. However, experimental considerations needed to fully leverage the statistical advantage of these laser systems have not been fully described. Here, we demonstrate a high repetition rate, broadband transient spectrometer capable of multichannel shot-to-shot detection at 90 kHz. Importantly, we find that several high-speed cameras exhibit a time-domain fixed pattern noise resulting from interleaved analog-to-digital converters, which is particularly detrimental to the conventional “ON/OFF” modulation scheme used in pump-probe spectroscopy. Using a modified modulation and data processing scheme, we achieve a noise level of 10−5 in 4 s for differential transmission, an order of magnitude lower than for commercial 1 kHz transient spectrometers for the same acquisition time. We leverage the high sensitivity of this system to measure the differential transmission of monolayer graphene at low pump fluence. We show that signals on the order of 10−6 OD can be measured, enabling a new data acquisition regime for low-dimensional materials. 

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4. In operando optical characterization of organic mixed ionic–electronic conductors for unraveling charge transport and doping dynamics—A perspective

   https://doi.org/10.1063/5.0274369  

   Chen, Linqi; Ma, Yingying; Guo, Peijun (July 2025, The Journal of Chemical Physics)

   Organic mixed ionic–electronic conductors (OMIECs) are a unique class of soft, conjugated polymeric materials. The simultaneous electronic and ionic transport of OMIECs enables a new type of device, namely, organic electrochemical transistors, among other emerging technologies. However, the dynamic nature—where charge transport, doping kinetics, and morphological changes occur concurrently—poses significant challenges in the characterization and understanding of OMIECs. Recent advances in in situ optical techniques, including ultraviolet–visible–near-infrared spectroscopy, Raman spectroscopy, and microscopy imaging, have provided valuable insights into the charge transport mechanisms and ionic doping dynamics spanning from the microscopic to the device scale. In this perspective, based on several archetypal OMIECs, we survey how spectroscopic signatures were used to reveal key physical processes in these materials. Looking forward, we propose that ultrafast spectroscopy and microscopy techniques—such as transient absorption spectroscopy, terahertz time-domain spectroscopy, pump–probe microscopy, and photothermal microscopy—hold great potential for uncovering more fundamental mechanisms of OMIEC operation, including quasiparticle dynamics, intrinsic electrical conductivity, and carrier mobility, which remain under-explored. Integrating optical characterization with electrochemical measurements will enable in operando studies on state-of-the-art devices, with results further refined by parallel advancements in theoretical modeling. Altogether, we envision in operando optical characterization with spatial, spectral, and temporal resolution across multiple scales as a powerful pathway to advance the understanding of OMIEC mechanisms and their structure–property relationships. 

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5. Ultrafast temporal phase-resolved nonlinear optical spectroscopy in the molecular frame

   https://doi.org/10.1364/OPTICA.515959  

   Pandey, Siddhant; Tan, Liang_Z; Walz, Francis; Makhija, Varun; Shivaram, Niranjan (May 2024, Optica)

   In an ultrafast nonlinear optical interaction, the electric field of the emitted nonlinear signal provides direct access to the induced nonlinear transient polarization or transient currents and thus carries signatures of ultrafast dynamics in a medium. Measurement of the electric field of such signals offers sensitive observables to track ultrafast electron dynamics in various systems. In this work, we resolve the real-time phase of the electric field of a femtosecond third-order nonlinear optical signal in the molecular frame. The electric field emitted from impulsively pre-aligned gas-phase molecules at room temperature, in a degenerate four-wave mixing scheme, is measured using a spectral interferometry technique. The nonlinear signal is measured around a rotational revival to extract its molecular-frame angle dependence from pump-probe time-delay scans. By comparing these measurements for two linear molecules, carbon dioxide and nitrogen, we show that the measured second-order phase parameter (temporal chirp) of the signal is sensitive to the valence electronic symmetry of the molecules, whereas the amplitude of the signal does not show such sensitivity. We compare measurements to theoretical calculations of the chirp observable in the molecular frame. This work is an important step towards using electric field measurements in nonlinear optical spectroscopy to study ultrafast dynamics of electronically excited molecules in the molecular frame. 

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