Vibrational sum frequency generation spectroscopy using inverted visible pulses

Weeraman, Champika; Mitchell, S. A.; Lausten, Rune; Johnston, Linda J.; Stolow, Albert

doi:10.1364/oe.18.011483

Cited by 26 publications

(21 citation statements)

References 16 publications

(25 reference statements)

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“…By timing the rising edge of the probe pulse to reach the sample just after the end of the pump pulse, they were able to minimise the non-resonant background while achieving strong overlap with the remainder of the FID (Figure 13). In addition, Weeraman et al [115] created probe pulses that increase exponentially with time and demonstrated that these pulses can provide high spectral resolution in VSFG while minimising the non-resonant background.…”

Section: Comparison Of Vsfg Spectra Obtained With Different Techniquesmentioning

confidence: 99%

Reexamining the interpretation of vibrational sum-frequency generation spectra

Rivera

Fourkas

2011

International Reviews in Physical Chemistry

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Vibrational sum-frequency generation (VSFG) has become a widely used technique for studying molecular orientation and intermolecular structure at interfaces. Due to the interfacial and vibrational selectivity of this technique, it can be used to probe molecular monolayers that are buried within bulk materials. Here, we present a critical review and examination of the assumptions that are generally used in the interpretation of VSFG spectra. This review focuses on three different aspects of VSFG spectroscopy. First, we examine the effect of dynamics (both reorientation and energy transfer) on the interpretation of VSFG spectra. Second, we consider whether (and under what circumstances) VSFG spectra cannot be interpreted solely in terms of the spectral properties of individual molecules. Third, we consider whether VSFG spectra obtained in different modes (frequency-domain, time-domain and broadband) should provide identical information. We conclude with a discussion of the challenges and opportunities provided by the revised viewpoint of VSFG that we present.

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Section: Comparison Of Vsfg Spectra Obtained With Different Techniquesmentioning

confidence: 99%

Reexamining the interpretation of vibrational sum-frequency generation spectra

Rivera

Fourkas

2011

International Reviews in Physical Chemistry

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“…10,14,15 While powerful, using time asymmetric pulses is not necessarily ideal for studies of insulating samples due to limited spectral/bandwidth tunability (similar to the problems with filters), and spectral artifacts that can arise in the use of time delayed or temporally asymmetric pulses. 21,22 Thus, the choice of a particular upconversion pulse waveform often predetermines the types of samples that can be optimally studied with a given spectrometer. 1 While different samples have different NIR spectral and/or temporal requirements, there was not, until recently, an avenue to change the pulse shapes in real time without substantial optical realignment.…”

Section: Articlementioning

confidence: 99%

“…To circumvent this issue, nonresonant suppression methods have been developed using an asymmetric waveform obtained from an etalon that is temporally delayed by a few 100 fs to avoid the ultrafast response of the substrate. 10,21 To create an etalon waveform using the SLM, we applied the transfer function 17…”

Section: F Temporally Asymmetric Pulse Generationmentioning

confidence: 99%

A new approach to vibrational sum frequency generation spectroscopy using near infrared pulse shaping

Chowdhury

Watson

et al. 2019

Review of Scientific Instruments

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We have developed a multipurpose vibrational sum frequency generation (vSFG) spectrometer that is uniquely capable of probing a broad range of chemical species, each requiring different experimental conditions, without optical realignment. Here, we take advantage of arbitrary near infrared (NIR) waveform generation using a 4f-pulse shaper equipped with a 2D spatial light modulator (SLM) to tailor upconversion pulses to meet sample dependent experimental requirements. This report details the experimental layout, details of the SLM calibration and implementation, and the intrinsic benefits/limitations of this new approach to vSFG spectroscopy. We have demonstrated the competency of this spectrometer by achieving an ∼3-fold increase in spectral resolution compared to conventional spectrometers by probing the model dimethyl sulfoxide/air interface. We also show the ability to suppress nonresonant background contributions from electrode interfaces using time delayed asymmetric waveforms that are generated by the NIR pulse shaper. It is expected that this advancement in instrumentation will broaden the types of samples researchers can readily study using nonlinear surface specific spectroscopies.

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“…In contrast, etalons can be used to generate time-asymmetric pulses for studies of metallic interfaces to suppress the nonresonant response of the substrate. [12, 13] In doing so, however, the asymmetric pulse shape can distort the resulting spectral line shapes, leading to limited spectral resolution – this is undesired for measuring other systems. [9, 11] Although, a significant effort has been put into understanding and eliminating the effects of the NIR pulse shape on the vSFG spectrum, there is no ‘best option’ given the diversity of samples vSFG can characterize.…”

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confidence: 99%

“…Broadband vSFG is particularly advantageous and is becoming more common, compared to the traditional point-by-point narrow band frequency scanning technique, due to the speed of data acquisition. [9, 13, 16] However, the faster data acquisition of the broadband method typically comes at the expense of spectral resolution, which is dictated by the spectral characteristics of the up-converting NIR laser pulse. In fact, all but the most specialized SFG spectrometers[11] commonly reach spectral bandwidths on the order of ~10–15 cm −1 , corresponding to laser pulses of ~1–2 ps.…”

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confidence: 99%

Flexible approach to vibrational sum-frequency generation using shaped near-infrared light

et al. 2018

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We describe a new approach that expands the utility of vibrational sum-frequency generation (vSFG) spectroscopy using shaped near-infrared (NIR) laser pulses. We demonstrate that arbitrary pulse shapes can be specified to match experimental requirements without the need for changes to the optical alignment. In this way, narrowband NIR pulses as long as 5.75 ps are readily generated, with a spectral resolution of about 2.5 cm, an improvement of approximately a factor of 3 compared to a typical vSFG system. Moreover, the utility of having complete control over the NIR pulse characteristics is demonstrated through nonresonant background suppression from a metallic substrate by generating an etalon waveform in the pulse shaper. The flexibility afforded by switching between arbitrary NIR waveforms at the sample position with the same instrument geometry expands the type of samples that can be studied without extensive modifications to existing apparatuses or large investments in specialty optics.

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Vibrational sum frequency generation spectroscopy using inverted visible pulses

Cited by 26 publications

References 16 publications

Reexamining the interpretation of vibrational sum-frequency generation spectra

Reexamining the interpretation of vibrational sum-frequency generation spectra

A new approach to vibrational sum frequency generation spectroscopy using near infrared pulse shaping

Flexible approach to vibrational sum-frequency generation using shaped near-infrared light

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