TY - JOUR
T1 - New nonlinear optical crystal of rhodamine 590 acid phthalate
AU - Nariyangadu, Sesha Bamini
AU - Choedak, Tenzin
AU - Malar, Ezekiel Joy Padma
AU - Chen, Junsheng
AU - Thyrhaug, Erling
AU - Kumar, Pushpendra
AU - Zhou, Jinming
AU - Yechuri, Vidyalakshmi
AU - Pal, Suman Kalyan
AU - Lidin, Sven
AU - Thangadhorai, Kejalakshmy Namassivayane
AU - Karki, Khadga J.
AU - Pullerits, Tönu
N1 - Publisher Copyright:
Copyright © 2020 American Chemical Society.
PY - 2020/8/25
Y1 - 2020/8/25
N2 - The synthesis and crystal structure of rhodamine 590 acid phthalate (RhAP) have been reported. This novel solid-state rhodamine derivative not only has a longer fluorescence lifetime compared to rhodamine solid-state matrixes where emission is quenched but also possesses strong nonlinear optical characteristics. The static and dynamic first- and second-order hyperpolarizabilities were calculated using the time-dependent density functional theory at the B3LYP/6-31+G∗ level. The computed static values of β and γof RhAP by the X-ray diffraction (XRD) structure were 31.9 × 10-30 and 199.0 × 10-36 esu, respectively. These values were about 62 times larger than the corresponding values in urea, an already well-known nonlinear optical material. The second-order hyperpolarizability of the compound was determined experimentally by measuring the two-photon absorption cross section using intensity-modulated light fields. The reported compound, excitable at near-infrared, exhibited frequency upconversion with the two-photon absorption coefficient enhanced by two orders of magnitude compared to that of the dye solution. Hosting the dye in the solid, at high concentrations, exploits the nonlinearity of the dye itself as well as results in significant excitonic effects including formation of broad exciton band and superradiance.
AB - The synthesis and crystal structure of rhodamine 590 acid phthalate (RhAP) have been reported. This novel solid-state rhodamine derivative not only has a longer fluorescence lifetime compared to rhodamine solid-state matrixes where emission is quenched but also possesses strong nonlinear optical characteristics. The static and dynamic first- and second-order hyperpolarizabilities were calculated using the time-dependent density functional theory at the B3LYP/6-31+G∗ level. The computed static values of β and γof RhAP by the X-ray diffraction (XRD) structure were 31.9 × 10-30 and 199.0 × 10-36 esu, respectively. These values were about 62 times larger than the corresponding values in urea, an already well-known nonlinear optical material. The second-order hyperpolarizability of the compound was determined experimentally by measuring the two-photon absorption cross section using intensity-modulated light fields. The reported compound, excitable at near-infrared, exhibited frequency upconversion with the two-photon absorption coefficient enhanced by two orders of magnitude compared to that of the dye solution. Hosting the dye in the solid, at high concentrations, exploits the nonlinearity of the dye itself as well as results in significant excitonic effects including formation of broad exciton band and superradiance.
UR - http://www.scopus.com/inward/record.url?scp=85090980893&partnerID=8YFLogxK
U2 - 10.1021/acsomega.0c02303
DO - 10.1021/acsomega.0c02303
M3 - 文章
AN - SCOPUS:85090980893
SN - 2470-1343
VL - 5
SP - 20863
EP - 20873
JO - ACS Omega
JF - ACS Omega
IS - 33
ER -