Synthesis of Organic Salts with Large Second-Order Optical Nonlinearities

Marder, Seth R.; Perry, Joseph W.; Schaefer, William P.

doi:10.1126/science.245.4918.626

Cited by 659 publications

(424 citation statements)

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“…In general these materials exhibit Peierls or spin-Peierls transitions that strongly affect the optical, magnetic, and electrical properties of such systems (1,2). Recently, these materials were examined for large optical nonlinearities (3).…”

Section: Introductionmentioning

confidence: 99%

A study of the phase transition in semiconducting 1:2 tetracyanoquinodimethane charge transfer complexes with dipropylamine derivatives: X-ray structure and polarized reflection spectra

Truong¹,

Pépin²,

Bandrauk³

et al. 1991

Can. J. Chem.

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Chem. 69, 1804 (1991).The donors dipropylamine (DPA), methyldipropylamine (MDPA), and ethyldipropylamine (EDPA) from 1:2 charge transfer complexes with the acceptor tetracyanoquinodimethane (TCNQ). All crystals in the above series are semiconductors and undergo a first-order phase transition at the temperature around 210 K as obtained from conductivity measurements. The X-ray structure of DPA-(TCNQ)? was obtained as a function of temperature, and shows a distinct order-disorder transition in the hydrogen-bond network between donors and acceptors. Polarized reflection spectra on single crystals of these compounds were measured as a function of temperature in the frequency range from 400 to 4000 crn-'. A detailed study of the e N modes of TCNQ indicates this mode is strongly influenced by the transition due to it being hydrogen bonded to the donors. The reflection coefficients of the IR active Ag modes of TCNQ also undergo a sharp discontinuity at the transition temperature. These results are interpreted as due to a cooperative order-disorder and electronic spin -Peierls transition.Key words: organic semiconductors, X-ray structure, polarized reflection spectra, phase transition, cooperative orderdisorder transition, spin-Peierls transition. La dipropylamine (DPA), la mCthyldipropylamine (MDPA) et l'ithyldipropylamine (EDPA) agissent comme donneurs pour former des complexes de transfert de charge 1 : 2 avec le titracyanoquinornithane (TCNQ) qui agit comme accepteur. Tous les cristaux des series sus-mentionnies sont des semi-conducteurs et, d'aprks les mesures de conductiviti, ils subissent une transition de phase du premier ordre B une tempirature d'environ 210 K. Faisant appel B la diffraction des rayons-X, on a dCterminC la structure du complexe DPA-(TCNQ)? en fonction de la tempirature; on observe une transition distincte ordreldCsordre dans le riseau des liaisons hydrogknes entre donneurs et accepteurs. On a mesuri le spectre de riflexion polarisie de cristaux uniques en fonction de la tempirature entre 400 et 4000 cm-' . Une Ctude dttaillCe des modes C=N du TCNQ indique que ce mode est fortement influencC par la transition; cet effet est dfi au fait que cette liaison est impliquie dans une liaison hydrogkne avec les donneurs. Les coefficients de riflexion des modes Ag du TCNQ actifs en infrarouge subissent aussi une discontinuiti importante au niveau de la temperature de transition. On interprkte ces risultats en fonction d'une transition coopirative ordreldksordre et spin ClectroniquelPeierls.

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Section: Introductionmentioning

confidence: 99%

A study of the phase transition in semiconducting 1:2 tetracyanoquinodimethane charge transfer complexes with dipropylamine derivatives: X-ray structure and polarized reflection spectra

Truong¹,

Pépin²,

Bandrauk³

et al. 1991

Can. J. Chem.

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“…Compared to inorganic crystals, the DAST provides very large nonlinear optical susceptibility 19 for optical rectification (v ð2Þ 111 ¼ 480 pm=V at k p ¼ 1.5 lm) paired with a low absorption for both the THz and the pump laser. THz radiation in DAST is emitted in forward direction collinear with the pump and carries the same linear polarization as the pump pulse.…”

mentioning

confidence: 99%

Strong-field single-cycle THz pulses generated in an organic crystal

Hauri

Ruchert

Vicario

et al. 2011

Applied Physics Letters

199

133

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We present high-power single-cycle carrier-envelope phase locked THz pulses at a central frequency of 2.1 THz with MV/cm electric field strengths and magnetic field strengths beyond 0.3 T. The THz radiation is generated by optical rectification in an organic salt crystal 4-N,N-dimethylamino-4′-N′-methyl stilbazolium tosylate called DAST pumped with the signal wavelength of a powerful optical parametric amplifier. Conversion efficiencies of more than 2% are reported.

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“…Some of the advantages offered by the organic materials are the high values of electronic susceptibility [3,4], fast response times and much greater versatility in molecular design, compared with their inorganic counterparts. However, purely organic compounds lack mechanical strength for practical uses and it is difficult to grow single crystals of sufficient quality.…”

Section: Introductionmentioning

confidence: 99%

Experimental and theoretical studies of the second- and third-order NLO properties of a semi-organic compound: 6-Aminoquinolinium iodide monohydrate

et al. 2014

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Experimental and Theoretical Studies of the Second-and Third-Order NLO Properties of a semi-organic compound: 6-Aminoquinolinium Iodide Monohydrate, Chemical Physics (2013), doi: http:// dx.doi.org/10. 1016/j.chemphys.2013.11.001 This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. AbstractA new semi-organic compound, 6-aminoquinolinium iodide monohydrate (I), has been synthesized and characterized by single crystal X-ray diffraction, UV-Vis absorption and fluorescence spectroscopy and nonlinear optical (NLO) measurements. The second-and third-order NLO responses were investigated with the second-and third-harmonic Maker fringes techniques, carried out on thin films at a fundamental wavelength of 1064 nm. From the molecular structure, the molecular hyperpolarizability tensors were determined with density functional theory and second-order Møller-Plesset perturbation method. The second-and third-order susceptibility tensors of the reported crystal were evaluated using the oriented gas model with the Lorenz-Lorentz and the Wortmann-Bishop local-field corrections. The calculations using the Wortmann-Bishop local-field were able to reproduce the correct order of magnitude of the experimental third-order susceptibilities. The value of χobtained by summing the effective third-order polarizability calculated for the asymmetric unit surrounded by ESP-derived charges have also the same order of magnitude of the experimental.

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Synthesis of Organic Salts with Large Second-Order Optical Nonlinearities

Cited by 659 publications

References 14 publications

A study of the phase transition in semiconducting 1:2 tetracyanoquinodimethane charge transfer complexes with dipropylamine derivatives: X-ray structure and polarized reflection spectra

A study of the phase transition in semiconducting 1:2 tetracyanoquinodimethane charge transfer complexes with dipropylamine derivatives: X-ray structure and polarized reflection spectra

Strong-field single-cycle THz pulses generated in an organic crystal

Experimental and theoretical studies of the second- and third-order NLO properties of a semi-organic compound: 6-Aminoquinolinium iodide monohydrate

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