scholarly journals Assessing the Molecular Specificity and Orientation Sensitivity of Infrared, Raman, and Vibrational Sum-Frequency Spectra

Symmetry ◽  
2020 ◽  
Vol 13 (1) ◽  
pp. 42
Author(s):  
Fei Chen ◽  
Lea Gozdzialski ◽  
Kuo-Kai Hung ◽  
Ulrike Stege ◽  
Dennis K. Hore

Linear programming was used to assess the ability of polarized infrared absorption, Raman scattering, and visible–infrared sum-frequency generation to correctly identify the composition of a mixture of molecules adsorbed onto a surface in four scenarios. The first two scenarios consisted of a distribution of species where the polarity of the orientation distribution is known, both with and without consideration of an arbitrary scaling factor between candidate spectra and the observed spectra of the mixture. The final two scenarios have repeated the tests, but assuming that the polarity of the orientation is unknown, so the symmetry-breaking attributes of the second-order nonlinear technique are required. The results indicate that polarized Raman spectra are more sensitive to orientation and molecular identity than the other techniques. However, further analysis reveals that this sensitivity is not due to the high-order angle dependence of Raman, but is instead attributed to the number of unique projections that can be measured in a polarized Raman experiment.

2012 ◽  
Vol 61 ◽  
pp. 17-24 ◽  
Author(s):  
Arthur D. Quast ◽  
Nathan C. Wilde ◽  
Sam S. Matthews ◽  
Scott T. Maughan ◽  
Steven L. Castle ◽  
...  

2005 ◽  
Vol 23 (1) ◽  
pp. 55-74 ◽  
Author(s):  
◽  
Yu. Yurik ◽  
La Hoz ◽  
◽  
◽  
...  

Abstract. When the Earth's ionosphere is irradiated by a radiofrequency (RF) electromagnetic wave of sufficiently high power density and tuned to match a natural E- or F-region plasma frequency, ionospheric magnetoionic wave modes may be excited and may generate RF electromagnetic sideband waves via nonlinear interactions. These secondary emissions, which may then escape from the ionosphere, have been termed stimulated electromagnetic emission or SEE. The frequency spectra of this radiation has been studied extensively, and a number of characteristic spectral features have been identified and in some cases related to particular plasma processes. The separation in frequency between the RF pump and the harmonics of the local electron gyrofrequency is critical in determining the amount of anomalous absorption suffered by the pump wave and the spectral properties of the stimulated sidebands. The pump can excite electrostatic waves which do not propagate away but can in some cases be observed via radio-wave scattering from the electron density fluctuations associated with them. These enhanced density fluctuations are created by processes commonly referred to as upper-hybrid and Langmuir turbulence. Langmuir turbulence has been the subject of 930-MHz scattering observations with antenna scanning through several pre-selected angles between the geographic and geomagnetic zenith directions, and a preference for pointing angles between the Spitze angle and geomagnetic field-aligned was identified. Other phenomena, such as the generation of enhanced electron temperatures and artificial aurora, have more recently been shown to have special behavior at similar angles, near but apparently not quite at field-aligned. In view of this evidence for angular structure in several pump-induced effects, in light of the rich variety of SEE phenomena strongly dependent on the geomagnetic field via the frequency interval between the pump and the gyrofrequency harmonics, and in view of the not yet understood but complex relationship between electrostatic fluctuations and SEE, it is of interest to investigate experimentally whether a similar angular structure is present in the various spectral features of the SEE signals and to compare the results with radar and other observations of RF-pump-induced effects. To this end we describe a simple two-element radio interferometer designed to search for aspect angle dependence of SEE features. We present an example of the initial data produced by this system, and draw preliminary conclusions based on the example data.


2016 ◽  
Vol 7 (11) ◽  
pp. 1945-1949 ◽  
Author(s):  
Jing Wang ◽  
Patrick J. Bisson ◽  
Joam M. Marmolejos ◽  
Mary Jane Shultz

2012 ◽  
Vol 3 (23) ◽  
pp. 3493-3497 ◽  
Author(s):  
Fadel Y. Shalhout ◽  
Sergey Malyk ◽  
Alexander V. Benderskii

2002 ◽  
Vol 106 (21) ◽  
pp. 5461-5469 ◽  
Author(s):  
Alex G. Lambert ◽  
David J. Neivandt ◽  
Adam M. Briggs ◽  
Eric W. Usadi ◽  
Paul B. Davies

2019 ◽  
Author(s):  
Tobias Garling ◽  
Kramer Campen ◽  
Martin Wolf ◽  
Martin Thaemer

<div> <div> <p>Recent years have seen a huge progress in the development of phase sensitive second order laser spectroscopy which has proven to be a very powerful tool for the investigation of interfaces. These interferometric techniques involve the nonlinear interaction between three short laser pulses with the sample. In order to obtain accurate phase information, the relative phases between the pulses must be stabilized and their timings precisely controlled. Despite much progress made, fulfilling both requirements remains a formidable experimental challenge. The two common approaches employ different beam geometries which each yields its particular advantages and deficiencies. While non-collinear spectrometers allow for a relatively simple timing control they typically yield poor phase stability and require a challenging alignment. Collinear approaches in contrast come with a simplified alignment and improved phase stability but typically suffer from a highly limited timing control. In this contribution we present a general experimental solution which allows for combining the advantages of both approaches while being compatible with most of the common spectrometer types. Based on a collinear geometry we exploit different selected polarization states of the light pulses in well- defined places in the spectrometer to achieve a precise timing control. The combination of this technique with a balanced detection scheme al- lows for the acquisition of highly accurate phase resolved nonlinear spectra without any loss in experimental flexibility. In fact, we show that the implementation of this technique allows us to employ advanced pulse timing schemes inside the spectrometer, which can be used to sup- press nonlinear background signals and extend the capabilities of our spectrometer to measure phase resolved sum frequency spectra of inter- faces in a liquid cell.</p> </div> </div>


2010 ◽  
Vol 114 (21) ◽  
pp. 7245-7249 ◽  
Author(s):  
Marcel Baer ◽  
Christopher J. Mundy ◽  
Tsun-Mei Chang ◽  
Fu-Ming Tao ◽  
Liem X. Dang

2008 ◽  
Vol 452 (1-3) ◽  
pp. 215-219
Author(s):  
Hai-Long Wang ◽  
Ming He ◽  
Dong-Ming Chen ◽  
Tian-Jing He ◽  
Fan-Chen Liu

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