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Shape-engineering of self-assembled organic single microcrystal as optical microresonator for laser applications.

Wang X, Liao Q, Lu X, Li H, Xu Z, Fu H - Sci Rep (2014)

Bottom Line: Furthermore, these as-prepared microcrystals demonstrate shape-dependent microresonator properties that 1D microwires act as Fabry-Pérot (FP) mode lasing resonator and 2D microdisks provide the whispering-gallery-mode (WGM) resonator for lasing oscillator.More significantly, through the investigation of the size-effect on the laser performance, single-mode lasing at red wavelength was successfully achieved in the self-assembled 2D organic microdisk at room temperature.These easily fabricated organic single-crystalline microcrystals with controlled shapes are the natural laser sources, which offer considerable promise for the multi-functionalities of coherent light devices integrated on the optics microchip.

View Article: PubMed Central - PubMed

Affiliation: 1] Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China [2] Graduate University of Chinese Academy of Sciences, Beijing 100049, P. R. China.

ABSTRACT
Single micro/nanocrystals based on π-conjugated organic molecules have caused tremendous interests in the optoelectronic applications in laser, optical waveguide, nonlinear optics, and field effect transistors. However, the controlled synthesis of these organic micro/nanocrystals with regular shapes is very difficult to achieve, because the weak interaction (van der Waals' force, ca. 5 kJ/mol) between organic molecules could not dominate the kinetic process of crystal growth. Herein, we develop an elaborate strategy, selective adhesion to organic crystal plane by the hydrogen-bonding interaction (ca. 40 kJ/mol), for modulating the kinetic process of the formation of microcrystal, which leads to the self-assembly of one organic molecule 3-[4-(dimethylamino)phenyl]-1-(2-hy-droxyphenyl)prop-2-en-1-on (HDMAC) into one-dimensional (1D) microwires and 2D microdisks respectively. Furthermore, these as-prepared microcrystals demonstrate shape-dependent microresonator properties that 1D microwires act as Fabry-Pérot (FP) mode lasing resonator and 2D microdisks provide the whispering-gallery-mode (WGM) resonator for lasing oscillator. More significantly, through the investigation of the size-effect on the laser performance, single-mode lasing at red wavelength was successfully achieved in the self-assembled 2D organic microdisk at room temperature. These easily fabricated organic single-crystalline microcrystals with controlled shapes are the natural laser sources, which offer considerable promise for the multi-functionalities of coherent light devices integrated on the optics microchip.

No MeSH data available.


Related in: MedlinePlus

The photophysical properties of the HDMAC microcrystals.(a) Absorption (blue line) and photoluminescence spectra (red line) of HDMAC microcrystals. (b) Photoluminescence decay, at room temperature, from the microcrystals, showing a lifetime of 1.12 ns. Right inset: The HOMO and the LUMO of HDMAC molecule simulated with DFT calculation.
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f3: The photophysical properties of the HDMAC microcrystals.(a) Absorption (blue line) and photoluminescence spectra (red line) of HDMAC microcrystals. (b) Photoluminescence decay, at room temperature, from the microcrystals, showing a lifetime of 1.12 ns. Right inset: The HOMO and the LUMO of HDMAC molecule simulated with DFT calculation.

Mentions: Note that HDMAC belongs to a typical intramolecular charge-transfer (ICT) compound, as indicated by the obvious change of electric-cloud distribution between the Highest Occupied Molecular Orbital (HOMO) and the Lowest Unoccupied Molecular Orbital (LUMO) of the HDMAC molecule by the DFT caculation (right inset of Fig. 3b). Due to the photophysical properties of the ICT excited state, the photoluminescence (PL) emission spectrum (red line in Fig. 3a) of the HDMAC crystals shows the central emission around 650 nm with no fine electronic-phonon coupling structures. Further analysis of the absorption (blue line in Fig. 3a) and the emission spectra (red line in Fig. 3a), we can find that the HDMAC crystal has a large stokes shift around 110 nm. This large shift contributes to the reduction of self-absorption effect in the optical materials42. More importantly, the HDMAC single crystal has excellent optical properties with solid quantum yield Φ of 30 ± 0.5% and the efficient radiate decay rate kf = 0.27 ± 0.1 ns−1 according to the equation, kf = Φ/τ (τ = 1.12 ± 0.03 ns, as shown in Fig. 3b)43. These outstanding optical properties hold a promise that the HDMAC could be a candidate active media for the laser action.


Shape-engineering of self-assembled organic single microcrystal as optical microresonator for laser applications.

Wang X, Liao Q, Lu X, Li H, Xu Z, Fu H - Sci Rep (2014)

The photophysical properties of the HDMAC microcrystals.(a) Absorption (blue line) and photoluminescence spectra (red line) of HDMAC microcrystals. (b) Photoluminescence decay, at room temperature, from the microcrystals, showing a lifetime of 1.12 ns. Right inset: The HOMO and the LUMO of HDMAC molecule simulated with DFT calculation.
© Copyright Policy - open-access
Related In: Results  -  Collection

License
Show All Figures
getmorefigures.php?uid=PMC4228325&req=5

f3: The photophysical properties of the HDMAC microcrystals.(a) Absorption (blue line) and photoluminescence spectra (red line) of HDMAC microcrystals. (b) Photoluminescence decay, at room temperature, from the microcrystals, showing a lifetime of 1.12 ns. Right inset: The HOMO and the LUMO of HDMAC molecule simulated with DFT calculation.
Mentions: Note that HDMAC belongs to a typical intramolecular charge-transfer (ICT) compound, as indicated by the obvious change of electric-cloud distribution between the Highest Occupied Molecular Orbital (HOMO) and the Lowest Unoccupied Molecular Orbital (LUMO) of the HDMAC molecule by the DFT caculation (right inset of Fig. 3b). Due to the photophysical properties of the ICT excited state, the photoluminescence (PL) emission spectrum (red line in Fig. 3a) of the HDMAC crystals shows the central emission around 650 nm with no fine electronic-phonon coupling structures. Further analysis of the absorption (blue line in Fig. 3a) and the emission spectra (red line in Fig. 3a), we can find that the HDMAC crystal has a large stokes shift around 110 nm. This large shift contributes to the reduction of self-absorption effect in the optical materials42. More importantly, the HDMAC single crystal has excellent optical properties with solid quantum yield Φ of 30 ± 0.5% and the efficient radiate decay rate kf = 0.27 ± 0.1 ns−1 according to the equation, kf = Φ/τ (τ = 1.12 ± 0.03 ns, as shown in Fig. 3b)43. These outstanding optical properties hold a promise that the HDMAC could be a candidate active media for the laser action.

Bottom Line: Furthermore, these as-prepared microcrystals demonstrate shape-dependent microresonator properties that 1D microwires act as Fabry-Pérot (FP) mode lasing resonator and 2D microdisks provide the whispering-gallery-mode (WGM) resonator for lasing oscillator.More significantly, through the investigation of the size-effect on the laser performance, single-mode lasing at red wavelength was successfully achieved in the self-assembled 2D organic microdisk at room temperature.These easily fabricated organic single-crystalline microcrystals with controlled shapes are the natural laser sources, which offer considerable promise for the multi-functionalities of coherent light devices integrated on the optics microchip.

View Article: PubMed Central - PubMed

Affiliation: 1] Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China [2] Graduate University of Chinese Academy of Sciences, Beijing 100049, P. R. China.

ABSTRACT
Single micro/nanocrystals based on π-conjugated organic molecules have caused tremendous interests in the optoelectronic applications in laser, optical waveguide, nonlinear optics, and field effect transistors. However, the controlled synthesis of these organic micro/nanocrystals with regular shapes is very difficult to achieve, because the weak interaction (van der Waals' force, ca. 5 kJ/mol) between organic molecules could not dominate the kinetic process of crystal growth. Herein, we develop an elaborate strategy, selective adhesion to organic crystal plane by the hydrogen-bonding interaction (ca. 40 kJ/mol), for modulating the kinetic process of the formation of microcrystal, which leads to the self-assembly of one organic molecule 3-[4-(dimethylamino)phenyl]-1-(2-hy-droxyphenyl)prop-2-en-1-on (HDMAC) into one-dimensional (1D) microwires and 2D microdisks respectively. Furthermore, these as-prepared microcrystals demonstrate shape-dependent microresonator properties that 1D microwires act as Fabry-Pérot (FP) mode lasing resonator and 2D microdisks provide the whispering-gallery-mode (WGM) resonator for lasing oscillator. More significantly, through the investigation of the size-effect on the laser performance, single-mode lasing at red wavelength was successfully achieved in the self-assembled 2D organic microdisk at room temperature. These easily fabricated organic single-crystalline microcrystals with controlled shapes are the natural laser sources, which offer considerable promise for the multi-functionalities of coherent light devices integrated on the optics microchip.

No MeSH data available.


Related in: MedlinePlus