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Scholes, Gregory (Ed.)Vibrational fingerprints and combination bands are a direct measure of couplings that control molecular properties. However, most combination bands possess small transition dipoles. Here we use multiple, ultrafast coherent infrared pulses to resolve vibrational coupling between CH3CN fingerprint modes at 918 and 1039 cm(-1) and combination bands in the 2750-6100 cm(-1 )region via doubly vibrationally enhanced (DOVE) coherent multidimensional spectroscopy (CMDS). This approach provides a direct probe of vibrational coupling between fingerprint modes and near-infrared combination bands of large and small transition dipoles in a molecular system over a large frequency range.more » « less
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Floquet state spectroscopy is an optical analogue of multiple quantum coherence nuclear magnetic resonance (MQC-NMR). Tunable ultrafast excitation pulses resonantly excite multiple states in a sample to form the Floquet state. The Floquet state emits multiple coherent beams at frequencies and in directions that conserve energy and momenta. The different output beams differ in the time ordering and coherences created by the excitation beams. They correspond to the different methodologies in the NMR family. Isolating a specific beam and monitoring the output intensity as a function of excitation frequencies creates multidimensional spectra containing cross-peaks between coupled states. The frequency range of the multidimensional spectra is limited by phase matching constraints. This paper presents a new, to the best of our knowledge, active phase matching strategy that increases the versatility of multidimensional Floquet state spectroscopy through both longer sample path lengths and larger spectral ranges.more » « less
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Modern instrumentation development often involves the incorporation of many dissimilar hardware peripherals into a single unified instrument. The increasing availability of modular hardware has brought greater instrument complexity to small research groups. This complexity stretches the capability of traditional, monolithic orchestration software. In many cases, a lack of software flexibility leads creative researchers to feel frustrated, unable to perform experiments they envision. Herein, we describe Yet Another acQuisition (yaq), a software project defining a new standardized way of communicating with diverse hardware peripherals. yaq encourages a highly modular approach to experimental software development that is well suited to address the experimental flexibility needs of complex instruments. yaq is designed to overcome hardware communication barriers that challenge typical experimental software. A large number of hardware peripherals are already supported, with tooling available to expand support. The yaq standard enables collaboration among multiple research groups, increasing code quality while lowering development effort.more » « less