## 2 Experimental Procedure
### Surface Free Energy of Nanoimprint Resist Materials  
The surface free energy of nanoimprint resist materials is essential to prevent the generated resist based defects on the template when the template is removed from the nanoimprint resist material after pressing the template into the nanoimprint resist material. The surface free energies of TPULR9, TPULR4.5, and TPULR0 were calculated using the reported surface free energy components of water, n-hexadecane, and diiodomethane, together with the experimental contact angles of water, n-hexadecane, and diiodomethane on TPULR9, TPULR4.5, and TPULR0 layers. The following Equations (1), (2), and (3) were used, proposed by [PERSON] [10] who extended the [PERSON] concept [11].  
\[\gamma_{\mathrm{L}}(1+\cos\theta)=2\left(\gamma_{\mathrm{S}}^{\mathrm{d}}\cdot \gamma_{\mathrm{L}}^{\mathrm{d}}\right)^{1/2}+2\left(\gamma_{\mathrm{S}}^{ \mathrm{p}}\cdot\gamma_{\mathrm{L}}^{\mathrm{p}}\right)^{1/2}+2\left(\gamma_{ \mathrm{S}}^{\mathrm{h}}\cdot\gamma_{\mathrm{L}}^{\mathrm{h}}\right)^{1/2} \tag{1}\]  
\[\gamma_{\mathrm{S}}=\gamma_{\mathrm{S}}^{\mathrm{d}}+\gamma_{\mathrm{S}}^{ \mathrm{p}}+\gamma_{\mathrm{S}}^{\mathrm{h}} \tag{2}\]  
\[\gamma_{\mathrm{L}}=\gamma_{\mathrm{L}}^{\mathrm{d}}+\gamma_{\mathrm{L}}^{ \mathrm{p}}+\gamma_{\mathrm{L}}^{\mathrm{h}} \tag{3}\]  
\begin{table}
\begin{tabular}{l c c c c} \hline \hline
**Resist** & \begin{tabular}{c} **Heptadecafluoro-** \\ **2-hydroxyundecyl** \\ **acrylate** \\ \end{tabular} & \begin{tabular}{c} **Tricylodecane** \\ **dimethanol** \\ **diacrylate** \\ \end{tabular} & \
\begin{tabular}{c} **Di-pentaerythnitol** \\ **polyacrylate** \\ \end{tabular} &
\begin{tabular}{c} **2-Hydroxy-2-** \\ **methyl-1-phenyl-** \\ **propane-1-one** \\ \end{tabular} \\ \hline TPULR0 & 0 wt\% & 47 wt\% & 47 wt\% & 6.0 wt\% \\ TPULR4.5 & 4.5 & 45 & 45 & 5.5 \\ TPULR9 & 9 & 43 & 43 & 5 \\ \hline \hline \end{tabular}
\end{table}
Table 1: Formulation of the developed nanoimprint resist materials TPULR9, TPULR4.5, and TPULR0.  
In the criterion, \(\gamma_{\rm L}\) is surface free energy, \(\gamma_{\rm L}^{\rm d}\) is the dispersive component, \(\gamma_{\rm L}^{\rm p}\) is the polar component, and \(\gamma_{\rm L}^{\rm h}\) is the hydrogen-bonded component of the liquid solvent. \(\gamma_{\rm S}\) is surface free energy of the solid nanoimprint resist materials, \(\gamma_{\rm S}^{\rm d}\) is the dispersive component, \(\gamma_{\rm S}^{\rm p}\) is the polar component, and \(\gamma_{\rm S}^{\rm h}\) is the hydrogen-bonded component.  
In the contact angle measurement process, which enables the determination of the surface free energy, three types of solvents, water, n-hexadecane, and diiodomethane, were selected, and the surface free energy components were reported as shown in Table 2[12].  
TPULR9, TPULR4.5, and TPULR0 were spin-coated onto the underlayer material TPU-UL at 2,500 rpm for 60 s and then UV-polymerized. The contact angles of water, n-hexadecane, and diiodomethane on TPULR9, TPULR4.5, and TPULR0 layers were measured using a dynamic contact angle analyzer DropMaster500Z (Kyowa Interface Science) as follows (analysis method: 0/2 method, drop amount: 1.0 \(\mu\)L, measurement time after droping: 1.0 s).