Electronic Supplementary Information (ESI)
Shape-Engineering of Self-Assembled Organic Single Microcrystal as Optical
Microresonator for laser Applications
Xuedong Wang1,2, Qing Liao3, Xiaomei Lu3, Hui Li1,2, Zhenzhen Xu3, and Hongbing Fu*,1,3
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.
3
Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital
Normal University, Beijing 100048, P. R. China.
S1
Contents
1. Figure S1. AFM images and corresponding height profiles of 1D microwires and
2D microplates.
2. Figure S2. X-ray diffraction patterns of HDMAC 1D microwires (blue), 2D
microplates (red) and simulated powder pattern from single crystal data (black)
using Mercury software.
3. Figure S3. Optimized the structure of HDMAC-C2H5OH complex.
4. Figure S4. Schematic illustration of the near-field scanning optical microscopy.
5. Figure S5. The plot of FWHM versus the optical pump density.
6. Figure S6. The lasing behaviors for the three microwires with different sizes.
7. Figure S7. The calculated quality factor Q for the three microwires with different
sizes.
8. Figure S8. The calculated quality factor Q for the three microplates with different
sizes.
9. Figure S9. TE and TM mode in 2D-MD resonator.
10. Figure S10. The simulated electric energy density in 1D-MW and 2D-MD
microcavity.
11. Table S1. The calculated attachment energy for various faces of HDMAC growth
morphology without solvent effect.
S2
Supplementary Figure S1 - (a) and (b) The AFM images of one sample microwire and one sample
microdisk. (c) and (d) The height profiles of the corresponding sample 1D microwire and the
corresponding sample 2D microdisk.
S3
Supplementary Figure S2 - X-ray diffraction patterns of HDMAC 1D microwires (blue line), 2D
microdisks (red line) and simulated powder pattern from single crystal data (black line) using Mercury
software is also included.
Supplementary Figure S3 - Optimized the structure of HDMAC-C2H5OH complex by DFT calculation
at MP2/6-31G** level. The calculation result indicates that hydrogen-bonding is formed between the
HDMAC molecule and the protic solvent molecules.
S4
Supplementary Figure S4 - Schematic illustration of (a) the near-field scanning optical microscopy and
(b) the transmittance optical path for the spatially resolved PL measurements.
Single 1D microwire or 2D microdisk was investigated at room temperature in air by a home-made
optical microscopy equipped with a 50 × 0.9NA excitation objective. The second harmonic (400 nm, 150
fs, 1 kHz) of a regenerative amplifier (Spitfire, Spectra Physics) seeded with a mode-locked Ti:sapphire
laser (Tsunami, Spectra Physics) was focused to a 50-μm-diameter spot to excite the selected individual
microwire or microdisk. Then PL spectra were collected underneath by using a 50 × 0.9NA objective that
was mounted a 3D movable stage. A 420-nm long-wave pass dielectric filter was used to block any
scattered excitation light. Finally the collected PL was coupled to an optical fiber and detected using a
liquid-nitrogen-cooled CCD (SPEC-10-400B/LbN, Roper Scientific) attached to a polychromator
(Spectropro-550i, Acton). The spectral resolution is 0.1 nm. Figure S1 is a representative of our setup.
S5
Supplementary Figure S5 - The FWHM (blue squares) has a nearly constant value of about 10 nm at
low power, and abruptly narrows to the small value of 0.5 nm at high pump density. Solid symbols
correspond to experimental data and lines are guides to the eye.
S6
Supplementary Figure S6 - (a) The lasing spectra for the three microwires with different sizes. (b)-(d)
The SEM image of the three sample microwires. The length of these microwires is denoted with yellow
arrow in their individual SEM image. (e)-(g) Simulated 2D normalized electric field (λ = 650 nm, n =
1.80) in the cross-section along the length of these three corresponding microwires in Figure S3b-d. Red
corresponds to the highest field density and blue is the lowest field density.
S7
Supplementary Figure S7 - (a)-(c) The calculated quality factor Q for the three microwires with
different sizes with length l = 16.9 μm, l = 23.9 μm, and l = 36.1 μm for the emission range from 640 nm
to 680 nm.
S8
Supplementary Figure S8 - (a)-(c) The calculated quality factor Q for the three microdisks with different
sizes with w1 = 8.8 μm, w2 = 6.8 μm; w1 = 11.8 μm, w2 = 7.6 μm; and w1 = 20.0 μm, w2 = 16.7 μm.
S9
Supplementary Figure S9 - (a) Unpolarized (black curve), TE polarized (green curve) and TM-polarized
(red curve) PL spectra obtained from one sample rectangular, whose SEM image is shown in the inset. (b)
The calculated quality factor Q of this microdisk microresonator versus the wavelength of the emission
range (from 645 to 670 nm). This simulated results shows that there exists two high-Q modeS, which is
constituent with the observed resonance peaks in experiment. (c) and (d) Simulated 2D normalized
electric field (λ = 650 nm, n = 1.80) of the TE-mode and TM-mode within this square microdisk resonator.
Red corresponds to the highest field density and blue is the lowest field density.
S10
Supplementary Figure S10 - (a) Simulated 2D electric energy density time average (J/m3, λ = 650 nm, n
= 1.80) of the 2D-disk resonator. The edge lengths of this typical 2D-disk are 4.4 µm and 3.8 µm. (b)
Simulated 2D electric energy density time average (J/m3, λ = 650 nm, n = 1.80) of the square 1D-wire
resonator. The length of this typical 1D-wire is 16.9 µm. The 2D-WGM resonator has higher electric
energy density than that of 1D-FP resonator.
S11
Supplementary Table S1 - The calculated attachment energy for the various faces of HDMAC
growth morphology.
Face
Attachment energy (kcal/mol)
{ 1 0 0}
-40.039
{ 0 1 1}
-57.040
{ 1 1 0}
-58.977
{ 0 1 0}
-71.097
{ 0 0 2}
-73.288
S12