skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Characterization of organic crystals for second-harmonic generation
Second-harmonic generation (SHG) is a common technique with many applications. Common inorganic single-crystalline materials used to produce SHG light are effective using short IR/visible wavelengths but generally do not perform well at longer, technologically relevant IR wavelengths such as 1300, 1550, and 2000 nm. Efficient SHG materials possess many of the same key material properties as terahertz (THz) generators, and certain single-crystalline organic THz generation materials have been reported to perform at longer IR wavelengths. Consequently, this work focuses on characterizing three efficient organic THz generators for SHG, namely, DAST (trans-4-[4-(dimethylamino)-N-methylstilbazolium] p-tosylate), DSTMS (4-N,N-dimethylamino-4’-N’-methylstilbazolium 2,4,6-trimethylbenzenesulfonate), and the recently discovered generator PNPA ((E)-4-((4-nitrobenzylidene)amino)-N-phenylaniline). All three of these crystals outperform the beta-barium borate (BBO), an inorganic material commonly used for SHG, using IR pump wavelengths (1200–2000 nm).  more » « less
Award ID(s):
2104317
PAR ID:
10472393
Author(s) / Creator(s):
; ; ; ; ; ; ; ;
Publisher / Repository:
Optical Society of America
Date Published:
Journal Name:
Optics Letters
Volume:
48
Issue:
22
ISSN:
0146-9592; OPLEDP
Format(s):
Medium: X Size: Article No. 5855
Size(s):
Article No. 5855
Sponsoring Org:
National Science Foundation
More Like this
  1. N-Benzyl-2-methyl-4-nitroanaline (BNA) is currently the industry standard for terahertz generation at 800 nm using organic materials. We developed four derivatives of BNA by replacing a hydrogen atom on the benzyl substituent with either a fluorine (F-BNA), a methoxy group (MeO-BNA), a cyano group (CN-BNA), or a methyl group (Me-BNA). X-ray diffraction measurements confirmed that all derivatives were crystallized in the same space group as BNA (Pna21). The THz generation capability of F-BNA is higher than that of BNA, with the maximum Fourier amplitude increasing by an average of 14% when pumped with wavelengths of 800, 1250, and 1550 nm. The damage threshold of F-BNA was also found to be higher than that of BNA, increasing by a factor of 1.14. The phase matching of F-BNA and BNA was found to be comparable. The increased THz output is, therefore, likely due to the higher induced nonlinear polarization, molecular hyperpolarizability, and closer molecular packing of F-BNA compared to BNA. 
    more » « less
  2. Abstract Small organic molecules absorbing and emitting in the shortwave infrared (SWIR, 1000–2000 nm) region are desirable for biological imaging applications due to low auto‐fluorescence, reduce photon scattering, and good tissue penetration depth of photons which allows forin vivoimaging with high resolution and sensitivity. Si‐substituted xanthene‐based fluorophores with indolizine donors have demonstrated some of the longest wavelengths of absorption and emission from organic dyes. This work seeks to compare an indolizine heterocyclic nitrogen with dimethyl aniline nitrogen donors on otherwise identical Si‐substituted xanthene fluorophoresviaoptical spectroscopy, computational chemistry and electrochemistry. Three donors are compared including an indolizine donor, a ubiquitous dimethyl aniline donor, and a vinyl dimethyl aniline group that keeps the number of π‐bonds consistent with indolizine. Significantly higher quantum yields and molar absorptivity are observed in these studies for a dimethylamine‐based donor relative to a simple indolizine donor absorbing and emitting at similar wavelengths (~1312 nm emission). Substantially longer wavelengths are obtainable by appending aniline‐based groups to the indolizine donor (~1700 nm) indicating longer wavelengths can be accessed with indolizine donors while stronger emitters can be accessed with anilines in place of indolizine. 
    more » « less
  3. Sadwick, Laurence P; Yang, Tianxin (Ed.)
    We report on THz emission in single-crystalline SnS2 in response to above bandgap excitation. Symmetry properties of THz generation suggest that its origin is an ultrafast surface shift current, a 2nd order nonlinear effect that can occur as a result of above-gap photoexcitation of a non-centrosymmetric semiconductor. Multilayer SnS2 can exist in several polytypes that differ in the layer stacking. Of those polytypes, 2H and 18R are centrosymmetric while 4H is not. While Raman spectroscopy suggests that the single crystalline SnS2 in our experiments is 2H, its THz emission has symmetry that are fully consistent with the P3m1 phase of 4H polytype. We hypothesize that the stacking disorder, where strain-free stacking faults that interrupt regions of 2H polytype, can break inversion symmetry and result in THz emission. These results lay the foundations for application of SnS2 as an efficient, stable, flexible THz source material, and highlight the use of THz spectroscopy as a sensitive tool for establishing symmetry properties of materials. 
    more » « less
  4. We present the optical and THz properties of highly efficient organic nonlinear optical crystals PNPA and MNA. These crystals outperform industry standards in broadband THz generation through optical rectification of IR light pulses. 
    more » « less
  5. Abstract Discovery of new materials with enhanced optical properties in the visible and UV‐C range can impact applications in lasers, nonlinear optics, and quantum optics. Here, the optical floating zone growth of a family of rare earth borates,RBa3(B3O6)3(R= Nd, Sm, Tb, Dy, and Er), with promising linear and nonlinear optical (NLO) properties is reported. Although previously identified to be centrosymmetric, the X‐ray analysis combined with optical second harmonic generation (SHG) assigns the noncentrosymmetricPspace group to these crystals. Characterization of linear optical properties reveals a direct bandgap of ≈5.61–5.72 eV and strong photoluminescence in both the visible and mid‐IR regions. Anisotropic linear and nonlinear optical characterization reveals both Type‐I and Type‐II SHG phase matchability, with the highest effective phase‐matched SHG coefficient of 1.2 pm V−1at 800‐nm fundamental wavelength (for DyBa3(B3O6)3), comparable to β‐BaB2O4(phase‐matchedd22≈ 1.9 pm V−1). Laser‐induced surface damage threshold for these environmentally stable crystals is 650–900 GW cm−2, which is four to five times higher than that of β‐BaB2O4, thus providing an opportunity to pump with significantly higher power to generate about six to seven times stronger SHG light. Since the SHG arises from disorder on the Ba‐site, significantly larger SHG coefficients may be realized by “poling” the crystals to align the Ba displacements. These properties motivate further development of this crystal family for laser and wide bandgap NLO applications. 
    more » « less