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Supplementary Information for Hierarchical Assembly of a Dual-responsive Macroscopic Insulated Molecular Wire Bundle in a Gradient System Yujie Sheng, Qibin Chen*, Junyao Yao, Ying Wang and Honglai Liu* Key Laboratory for Advanced Materials and Department of Chemistry, East China University of Science and Technology, Shanghai 200237, China *Corresponding authors: qibinchen@ecust.edu.cn (Q. Chen) and hlliu@ecust.edu.cn (H. Liu) Table of Contents Experimental Details S3 Computational Details S5 Synthesis S6 Supplementary Figures S7 Supplementary Movies S11 References S12 Additional Spectrum S13 Experimental Details General All commercially available reagents and solvents were purchased from Adamas, General-reagent and Shanghai Lingfeng chemical reagent Co. Ltd.. The reagents used were of reagent grade, and the solvents used were of analytical grade unless otherwise stated; all reagents were directly used without further purification. 1H NMR and 1H/1H Nuclear Overhauser Effect Spectroscopy (NOESY) spectra were recorded on an Avance III 400 MHz NMR spectrometer (Bruker, Germany), and chemical shifts are reported in ppm (δ) using the signal of tetramethylsilane (TMS) as an internal standard. Electron spray ionisation (ESI) mass spectrometry was conducted using an 1100 LC/MSD SL instrument (Agilent, USA). UV-Vis spectra were measured using a UV2550 spectrometer (Shimadazu, Japan), and circular dichroism spectra were recorded using a J-815 CD spectrometer (JASCO, Japan). Solution density was measured using a DMA 4500 M density meter (Anton Paar, Australia). Solution composition was characterised using a NAR-1T refractometer (Precision Instrument Co. Ltd., China). Solute concentration was measured using an Agilent 6890-5973 gas chromatography-mass spectrometry (GC-MS) instrument (Agilent, USA). Attenuated Total Reflectance Infrared (ATR-IR) spectra were measured using a Nicolet iS10 infrared spectrometer equipped with a SMART iRT accessory (Thermo, USA). B
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