Fig. 1. (a) Schematic of the experimental setup; (b) schematic diagram of defocused wide-field imaging of single conjugated polymer molecules excited with phase-modulated ultrashort laser pulse pairs.(a)实验装置示意图; (b)利用相对相位调制的脉冲对激发的共轭聚合物单分子散焦宽场成像原理示意图

Fig. 2. Schematic of the time-domain imaging sequence and reconstructed frequency-domain imaging by Fourier transform for single conjugated polymer molecules based on defocused wide-field fluorescence imaging. The upper part of (a), (b) and (c) gives the experimental results of defocused wide-field fluorescence imaging, while the lower part shows the simulation results. (d), (e) and (f) are the reconstructed frequency-domain imaging at the same area, where red color represents positive phase and white represents negative phase, the upper part gives the results of reconstructed imaging, while the lower part shows the simulation results.共轭聚合物单分子散焦宽场荧光成像时域序列图与利用傅里叶变换频域信息重构的成像序列图 (a)—(c)上半部分为实验测得的散焦宽场荧光成像随时间变化序列, 下半部分为相应的拟合结果; (d)—(f)为与散焦宽场荧光成像同样区域分子的频域信息重构成像图, 不同颜色代表相位的差异, 其中红色代表正相位, 白色代表负相位, 上半部分为直接重构成像结果, 下半部分为拟合结果

Fig. 3. Modulated fluorescence trajectories and corresponding emission angle of single conjugated polymer molecules Ⅰ, Ⅱ and Ⅲ: (a) The sawtooth wave signal applied on EOM that used for phase modulation of pulse pairs; (b), (c), and (d) the modulated fluorescence trajectories of each molecule; (e), (f), and (g) the change of the angle for molecules Ⅰ, Ⅱ and Ⅲ, respectively.共轭聚合物单分子Ⅰ, Ⅱ和Ⅲ的荧光调制轨迹和相应发射偶极取向发射角的变化 (a)施加在EOM上的锯齿波信号; (b), (c), (d)每个分子的荧光调制轨迹; (e), (f), (g)角度的变化

Fig. 4. (a) and (b) are the snapshots of time-domain imaging based on defocused wide-field fluorescence imaging of single conjugated polymer molecules and corresponding simulation results; (c) and (d) show the reconstructed frequency-domain imaging and corresponding simulation results, where red color represents positive phase and white represents negative phase; (e) the sawtooth wave signal applied on EOM that used for phase modulation of pulse pairs; (f) and (g) show the fluorescence modulation trajectories of molecules 1 and 2, respectively; (h) and (i) show the change of emission angle of molecules 1 and 2, respectively. The absorption and emission dipole orientation of single conjugated polymer molecule 1 keep constant, while that of molecule 2 change simultaneously.(a), (b)共轭聚合物单分子散焦宽场成像时域序列图和相应模式的拟合结果; (c), (d)频域信息重构成像和相应的拟合结果, 其中红色代表正相位, 白色代表负相位; (e)施加在EOM上的锯齿波信号; (f), (g)分别显示分子1和2的荧光调制轨迹; (h), (i)分别显示分子1和2的发射角的变化; 图中展示了共轭聚合物单分子吸收和发射偶极取向均保持恒定(分子1)以及吸收和发射偶极取向同时发生变化(分子2)的情况