First principles crystal engineering of nonlinear optical materials. I. Prototypical case of urea

Masunov, Artëm E.; Tannu, Arman; Dyakov, Alexander A.; Matveeva, Anastasia D.; Freidzon, Alexandra Ya.; Odinokov, Alexey V.; Bagaturyants, Alexander A.

doi:10.1063/1.4986793

Title: First principles crystal engineering of nonlinear optical materials. I. Prototypical case of urea

Journal Article · Mon Jun 26 00:00:00 EDT 2017 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4986793· OSTI ID:1497849

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^[3]; Matveeva, Anastasia D. ^[4];

^[4]; Odinokov, Alexey V. ^[5];

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Univ. of Central Florida, Orlando, FL (United States); South Ural State Univ., Chelyabinsk (Russian Federation); Moscow Engineering Physics Inst., Moscow (Russian Federation); Russian Academy of Sciences (RAS), Moscow (Russian Federation)
Univ. of Central Florida, Orlando, FL (United States)
South Ural State Univ., Chelyabinsk (Russian Federation)
Moscow Engineering Physics Inst., Moscow (Russian Federation); Russian Academy of Sciences (RAS), Moscow (Russian Federation)
Russian Academy of Sciences (RAS), Moscow (Russian Federation)

The crystalline materials with nonlinear optical (NLO) properties are critically important for several technological applications, including nanophotonic and second harmonic generation devices. Urea is often considered to be a standard NLO material, due to the combination of non-centrosymmetric crystal packing and capacity for intramolecular charge transfer. Various approaches to crystal engineering of non-centrosymmetric molecular materials were reported in the literature. Here we propose using global lattice energy minimization to predict the crystal packing from the first principles. We developed a methodology that includes the following: (1) parameter derivation for polarizable force field AMOEBA; (2) local minimizations of crystal structures with these parameters, combined with the evolutionary algorithm for a global minimum search, implemented in program USPEX; (3) filtering out duplicate polymorphs produced; (4) reoptimization and final ranking based on density functional theory (DFT) with many-body dispersion (MBD) correction; and (5) prediction of the second-order susceptibility tensor by finite field approach. This methodology was applied to predict virtual urea polymorphs. After filtering based on packing similarity, only two distinct packing modes were predicted: one experimental and one hypothetical. DFT + MBD ranking established non-centrosymmetric crystal packing as the global minimum, in agreement with the experiment. Finite field approach was used to predict nonlinear susceptibility, and H-bonding was found to account for a 2.5-fold increase in molecular hyperpolarizability to the bulk value.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE

OSTI ID:: 1497849

Journal Information:: Journal of Chemical Physics, Vol. 146, Issue 24; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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