Scholarlink

<p>Electron-nuclear coupling plays a crucial role in strong laser induced molecular dissociation dynamics. The interplay between electronic and nuclear degrees of freedom determines the pathways and outcomes of molecular fragmentation. However, a full quantum mechanical treatment of electron-nuclear dynamics is computationally intensive. In this work, we have developed a Strong Laser Induced non-adiabatic Multi-Ionic-Multi-Electric States (SLIMIMES) approach, which contains the electron-laser and electron-nuclear couplings. We validate our model using a showcase example: water dissociation under strong infrared (IR) laser pulses. Our investigation reveals the predominant role of a non-vertical dissociation pathway in the photo-ionization dissociation (PID) process of <InlineEquation ID="IEq3"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="41598_2024_83209_Article_IEq3.gif" Format="GIF" Height="18" Rendition="HTML" Resolution="72" Type="Linedraw" Width="48" /> </InlineMediaObject> <EquationSource Format="TEX">\(\mathrm {D_{2}O^{2+}}\)</EquationSource> </InlineEquation>. This pathway originates from neutral <InlineEquation ID="IEq4"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="41598_2024_83209_Article_IEq4.gif" Format="GIF" Height="16" Rendition="HTML" Resolution="72" Type="Linedraw" Width="33" /> </InlineMediaObject> <EquationSource Format="TEX">\(\mathrm {D_{2}O}\)</EquationSource> </InlineEquation>, which undergoes vertical multi-photon-single-ionization, reaching the intermediate dissociation states of <InlineEquation ID="IEq5"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="41598_2024_83209_Article_IEq5.gif" Format="GIF" Height="21" Rendition="HTML" Resolution="72" Type="Linedraw" Width="111" /> </InlineMediaObject> <EquationSource Format="TEX">\(\mathrm {D_{I} + OD_{II}^{+} (2^{3}\Sigma )}\)</EquationSource> </InlineEquation> within <InlineEquation ID="IEq6"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="41598_2024_83209_Article_IEq6.gif" Format="GIF" Height="18" Rendition="HTML" Resolution="72" Type="Linedraw" Width="42" /> </InlineMediaObject> <EquationSource Format="TEX">\(\mathrm {D_{2}O^{+}}\)</EquationSource> </InlineEquation>. Subsequently, <InlineEquation ID="IEq7"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="41598_2024_83209_Article_IEq7.gif" Format="GIF" Height="21" Rendition="HTML" Resolution="72" Type="Linedraw" Width="74" /> </InlineMediaObject> <EquationSource Format="TEX">\(\mathrm {OD_{II}^{+} (2^{3}\Sigma )}\)</EquationSource> </InlineEquation> dissociates into <InlineEquation ID="IEq8"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="41598_2024_83209_Article_IEq8.gif" Format="GIF" Height="18" Rendition="HTML" Resolution="72" Type="Linedraw" Width="65" /> </InlineMediaObject> <EquationSource Format="TEX">\(\mathrm {O^{+} + D_{II}}\)</EquationSource> </InlineEquation>, with both <InlineEquation ID="IEq9"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="41598_2024_83209_Article_IEq9.gif" Format="GIF" Height="16" Rendition="HTML" Resolution="72" Type="Linedraw" Width="18" /> </InlineMediaObject> <EquationSource Format="TEX">\(\mathrm {D_{I}}\)</EquationSource> </InlineEquation> and <InlineEquation ID="IEq10"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="41598_2024_83209_Article_IEq10.gif" Format="GIF" Height="16" Rendition="HTML" Resolution="72" Type="Linedraw" Width="23" /> </InlineMediaObject> <EquationSource Format="TEX">\(\mathrm {D_{II}}\)</EquationSource> </InlineEquation> fragments potentially ionizing an electron during interaction with the IR laser. This sequential PID pathway significantly contributes to the dissociation yields of water dication. Our calculations are consistent with recent experimental data, which focus on measuring the branching ratio of water dication dissociation. We aim for our model to provide a deeper understanding and a fresh perspective on the coupling between electron and nuclear dynamics induced by a strong IR laser field.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Non vertical ionization-dissociation model for strong IR induced dissociation dynamics of \({{D}_{2}}O^{2+}\)

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年1月2日

查看全文
  • Jun Wang,
  • Shu Ning Gao,
  • Aihua Liu,
  • Lanhai He,
  • Xi Zhao

摘要

Electron-nuclear coupling plays a crucial role in strong laser induced molecular dissociation dynamics. The interplay between electronic and nuclear degrees of freedom determines the pathways and outcomes of molecular fragmentation. However, a full quantum mechanical treatment of electron-nuclear dynamics is computationally intensive. In this work, we have developed a Strong Laser Induced non-adiabatic Multi-Ionic-Multi-Electric States (SLIMIMES) approach, which contains the electron-laser and electron-nuclear couplings. We validate our model using a showcase example: water dissociation under strong infrared (IR) laser pulses. Our investigation reveals the predominant role of a non-vertical dissociation pathway in the photo-ionization dissociation (PID) process of \(\mathrm {D_{2}O^{2+}}\) . This pathway originates from neutral \(\mathrm {D_{2}O}\) , which undergoes vertical multi-photon-single-ionization, reaching the intermediate dissociation states of \(\mathrm {D_{I} + OD_{II}^{+} (2^{3}\Sigma )}\) within \(\mathrm {D_{2}O^{+}}\) . Subsequently, \(\mathrm {OD_{II}^{+} (2^{3}\Sigma )}\) dissociates into \(\mathrm {O^{+} + D_{II}}\) , with both \(\mathrm {D_{I}}\) and \(\mathrm {D_{II}}\) fragments potentially ionizing an electron during interaction with the IR laser. This sequential PID pathway significantly contributes to the dissociation yields of water dication. Our calculations are consistent with recent experimental data, which focus on measuring the branching ratio of water dication dissociation. We aim for our model to provide a deeper understanding and a fresh perspective on the coupling between electron and nuclear dynamics induced by a strong IR laser field.