Amplification of the linear and nonlinear optical response of a chiral molecular crystal

Abstract

General rightsIt is not permitted to download or to forward/distribute the text or part of it without the consent of the author(s) and/or copyright holder(s), other than for strictly personal, individual use, unless the work is under an open content license (like Creative Commons). Disclaimer/Complaints regulationsIf you believe that digital publication of certain material infringes any of your rights or (privacy) interests, please let the Library know, stating your reasons. In case of a legitimate complaint, the Library will make the material inaccessible and/or remove it from the website. Please Ask the Library: http://uba.uva.nl/en/contact, or a letter to: Library of the University of Amsterdam, Secretariat, Singel 425, 1012 WP Amsterdam, The Netherlands. You will be contacted as soon as possible. We have observed large second-order nonlinear optical and vibrational circular dichroism (VCD) responses in a charge-transfer-type L-Histidinium salt. Using X-ray Diffraction, VCD spectroscopy, and time-dependent density functional theory to characterize the compound, we employ a two-level model to explain and quantify the strongly enhanced optical signals. We find that both linear and nonlinear optical responses are greatly enhanced by a single low-lying charge-transfer state.

Ultrafast Tuning of Various Photochemical Pathways in Perylene–TCNQ Charge-Transfer Crystals

“…Organic charge-transfer (CT) complexes provide another possibility of tuning photochemical pathways due to the presence of two or more molecules in molecular compounds and by adjustment of stoichiometry. CT complexes have attracted substantial attention through their technological applications for optoelectronic devices such as light-emitting diodes, , field-effect transistors, , and photovoltaic and nonlinear optical systems. − Multicomponent molecular crystals made from charge-transfer compounds are highly advantageous materials due to few imperfections in stacking structure and overall low impurity, which greatly enhance the performance of optoelectronic devices. − Binary CT crystals are composed of two constituents via noncovalent intermolecular interaction, one with higher electron affinity acting as an electron acceptor and the other with lower ionization potential acting as an electron donor. Various studies were performed on the growth, charge-transfer, and optical/electronic properties of crystals such as perylene–F x TCNQ, , tetrathiofulvalene–7,7,8,8-tetracyanoquinodimethane (TTF–TCNQ), − and metal dithiolate–perylene crystals .…”

On the Performance of Hybrid Functionals for Non‐linear Optical Properties and Electronic Excitations in Chiral Molecular Crystals: The Case of Butterfly‐Shaped Dicinnamalacetone

“…The critical step of crystallisation in ac hiral group may be ensured by using co-formers with chiral centres, together with dipolar,o ctupolar or mixed-character molecules. [4,5] Another strategyi st oc hoose molecules that adopt ap ropeller-like Purely organic chiralm olecular assemblies in the solid state hold great potential for non-linear opticala pplications. Herein, an ewly synthesised molecular system is reported, namely,d icinnamalacetone, an otherwise planarm olecule that crystallises in ad isordered non-centrosymmetric form with four different conformationsh aving an overall predominance of ap articular helicity.Acombined experimental and theoretical ap-proach,i ncluding single-crystal X-ray diffraction, Kurtz-Perry and ab initio methods, is employed to characterise the system and benchmark the performance of hybrid functionals for the prediction of non-linear opticalp roperties and electronic excitations.C omparisono fe xperiment and theory points to ap articular set of hybrid functionals that provides an optimal descriptionoft his molecular system.…”

Bulk growth and physical properties of diguanidinium phosphate monohydrate (G2HP) as a multi-functional crystal

“…[9][10][11][12][13] The salts of protonated amino acids have become an interesting class of hydrogen bonded compounds following the discovery of the outstanding nonlinear optical (NLO) properties of L-arginine phosphate monohydrate (LAP) by our group. [14][15][16][17][18][19][20][21] Besides high NLO coefficients, short ultraviolet (UV) transparency cutoff and low level of hygroscopicity, the most attractive feature of this material is the high laser-induced damage threshold with a value of 63 GW cm −2 (1 ns pulses at 1053 nm). 22 Its deuterated analog (DLAP) exhibits an even higher damage threshold.…”