Simple fully reflective method of scatter reduction in 2D-IR spectroscopy

Spector, Ivan C.; Olson, Courtney M.; Huber, Christopher; Massari, Aaron M.

doi:10.1364/ol.40.001850

Cited by 14 publications

(11 citation statements)

References 22 publications

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“…The long CN stretch vibrational lifetime (∼36 ps) permitted the observation of complete orientational relaxation and spectral diffusion in the aqueous phase of MCM41 for the first time, although not without the need for several experimental improvements. Powdered solids are challenging to study with PSPP and 2D IR experiments, as these techniques are susceptible to scattered light from the pulses that generate the signal. , The scattered light was reduced in this study using a combination of methods, ranging from the sample preparation procedure to a newly developed phase cycling scheme. In the 2D IR experiments, a previously reported method of combining mid-IR frequency-domain pulse shaping techniques , and a polarization filter was successfully employed to reveal water–anion hydrogen bond dynamics in the MCM41 pores.…”

Section: Introductionmentioning

confidence: 99%

Water Dynamics in Nanoporous Silica: Ultrafast Vibrational Spectroscopy and Molecular Dynamics Simulations

et al. 2019

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Nanoporous silica materials are important in catalysis, energy, and materials applications in which water is an essential component. System performance is intimately connected to the water dynamics occurring in the confined environment. However, the dynamics and associated structures of water in nanoporous silica have proven challenging to measure and predict. Here, confined water dynamics are examined via the ultrafast infrared spectroscopy of selenocyanate (SeCN–) dissolved in the hydrated ∼2.4 nm silica mesopores of MCM41. Polarization selective pump–probe and two-dimensional infrared measurements on the CN stretching mode of SeCN– are used to probe the effect of confinement on orientational relaxation and spectral diffusion dynamics. The dynamics of SeCN– provide information on the surrounding water hydrogen bond dynamics. The long CN stretch lifetime (∼36 ps), relative to the water hydroxyl stretch (<2 ps), significantly extends the time scales that can be accessed. Complete orientational relaxation (C 2(t), orientational correlation function) and spectral diffusion (C ω(t), frequency–frequency correlation function) dynamics are presented and compared to the simulated time correlation functions in a model silica pore of the same size. A slow decay component not present in the bulk liquid is observed in both experiments, indicating that the hydrogen bond dynamics are significantly altered by confinement. The simulations reveal a qualitative difference in the functional dependence of C 2(t;d) and C ω(t;d) on d, the distance from the interface. The former becomes exponentially faster with distance while the latter makes an abrupt transition from slower to faster dynamics midway between the surface and pore center, d ≅ 6 Å.

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Section: Introductionmentioning

confidence: 99%

Water Dynamics in Nanoporous Silica: Ultrafast Vibrational Spectroscopy and Molecular Dynamics Simulations

et al. 2019

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“…The spectral resolution of the detection system was ∼4 cm –1 . Data collection was performed with fibrillation to remove scatter from all three pump beams, as described previously . The resulting absolute value 2D-IR spectra were analyzed using peak volumes to extract kinetic information directly from the 2D-IR spectra. − …”

Section: Methodsmentioning

confidence: 99%

Measuring Dopant-Modulated Vibrational Energy Transfer over the Surface of Silicon Nanoparticles by 2D-IR Spectroscopy

et al. 2018

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2D-IR spectroscopy was used to characterize the vibrational dynamics of surface hydride modes on silicon nanoparticles (SiNPs). Energy transfer was compared between undoped (intrinsic) SiNPs and particles that were doped with boron and phosphorus. FTIR spectra reported changes in the relative proportions of Si–H, Si–H2, and Si–H3 populations when boron and phosphorus atoms were incorporated, while 2D-IR spectroscopy revealed that there was vibrational energy transfer on the tens of ps time scale between all three mode types for intrinsic SiNPs. This energy transfer was severely diminished by including just 0.05 atomic % of boron and was completely extinguished for 2.5 atomic % of phosphorus. In addition, the vibrational lifetimes of mono and polyhydride modes on intrinsic silicon particles were uniformly fast, while doped nanoparticles showed frequency dependent relaxation times reminiscent of porous and amorphous silicon films.

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“…Since the first measurements of ultrafast 2D-IR spectra, 10 many technical developments in spectrometer design have become available to improve on the speed, sensitivity and reliability of acquisition of 2D-IR data. [11][12][13][14][15][16][17][18][19][20] The other significant area where improvement is required is in the laser sources used. So far, most published 2D-IR setups have used IR light generated through nonlinear processes driven by commercial Ti:Sapphire amplifiers.…”

Section: Introductionmentioning

confidence: 99%

A 100 kHz Pulse Shaping 2D-IR Spectrometer Based on Dual Yb:KGW Amplifiers

et al. 2018

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A high-speed, high-sensitivity and compact two-dimensional infrared (2D-IR) spectrometer based on 100 kHz Yb:KGW regenerative amplifier technology is described and demonstrated. The setup is three color, using an independent pump OPA and two separately tunable probe OPAs. The spectrometer uses 100 kHz acousto-optic pulse shaping on the pump beam for rapid 2D-IR acquisitions. The shot-to-shot stability of the laser system yields excellent signal-to-noise figures (∼10 μOD noise on 5000 laser shots). We show that the reduced bandwidth of the Yb:KGW amplifiers in comparison with conventional Ti:sapphire systems does not compromise the ability of the setup to generate high-quality 2D-IR data. Instrument responses of <300 fs are demonstrated and 2D-IR data presented for several systems of interest to physical chemists, showing spectral diffusion in NaSCN, amide I and II bands of a β sheet protein and DNA base-pair-backbone couplings. Overall, the increased data acquisition speed, intrinsic stability, and robustness of the Yb:KGW lasers are a significant step forward for 2D-IR spectroscopy.

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Simple fully reflective method of scatter reduction in 2D-IR spectroscopy

Cited by 14 publications

References 22 publications

Water Dynamics in Nanoporous Silica: Ultrafast Vibrational Spectroscopy and Molecular Dynamics Simulations

Water Dynamics in Nanoporous Silica: Ultrafast Vibrational Spectroscopy and Molecular Dynamics Simulations

Measuring Dopant-Modulated Vibrational Energy Transfer over the Surface of Silicon Nanoparticles by 2D-IR Spectroscopy

A 100 kHz Pulse Shaping 2D-IR Spectrometer Based on Dual Yb:KGW Amplifiers

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