Relativistic effects on inversion barriers of pyramidal group 15 hydrides

Santiago Régis T.; Haiduke Roberto L. A.

摘要

Abstract > Quantum chemistry is an important tool for determining general molecular properties, although relativistic corrections are usually required for systems containing heavy and super heavy elements. Non‐relativistic along with relativistic two‐ and four‐component electronic structure calculations done with the CCSD‐T method and the new RPF‐4Z basis set have therefore been applied for determining inversion barriers, corresponding to the change from a pyramidal (C <sub>3v</sub> ) ground‐state structure to the trigonal planar (D <sub>3h</sub> ) transition state, TS, of group 15 hydrides, XH <sub>3</sub> (X= N, P, As, Sb, and Bi). The ground‐state structure of the McH <sub>3</sub> molecule, which contains the super heavy element Moscovium, is also predicted as pyramidal (C <sub>3v</sub> ), with an atomization energy of 90.8 kcal mol ?1 . However, although non‐relativistic calculations still provided a D <sub>3h</sub> planar TS for McH <sub>3</sub> , four‐component relativistic calculations based on single‐reference wave functions are unable to elucidate the definitive TS geometry in this case. Hence, the results show that relativistic effects are crucial for this barrier determination in those hydrides containing Bi and Mc. Moreover, while the scalar relativistic effects predominate, increasing barrier heights by as much as 17.6 kcal mol ?1 (32%) in BiH <sub>3</sub> , the spin‐orbit coupling cannot be disregarded in those hydrides containing the heaviest group 15 elements, decreasing the barrier by 2.5 kcal mol ?1 (4.5%) in this same molecule. </abstract> </span> <span class="z_kbtn z_kbtnclass hoverxs" style="display: none;">展开▼</span> </div> <div class="translation abstracttxt"> <span class="zhankaihshouqi fivelineshidden" id="abstract"> <span>机译：</span><Abstract Type =“main”> <标题类型=“main”>抽象</标题> >量子化学是用于确定一般分子特性的重要工具，但通常需要含有重质和超重元素的系统所需的相对论校正。因此，使用CCSD-T方法和新的RPF-4Z基础组的相对性的两组和四组件电子结构计算的不相对论以及新的RPF-4Z基础组的计算，用于确定反转屏障，对应于金字塔的变化（C <SUB > 3V </ sub>）地态结构到三角形平面（D <sub> 3h </ sub>）过渡状态，第15组氢化物的Ts，Xh <sub> 3 </ sub>（x = n， P，AS，SB和BI）。含有超重元素培养基的MCH <sub> 3 </ sub>分子的地态结构也预测为金字塔（C <sub> 3v </ sub>），雾化能量为90.8千卡mol ？1 </ sup>。但是，尽管用于MCH <Sub> 3 </ sub>的非相对论计算仍提供D <sub> 3h </ sub>平面Ts，但基于单参考波函数的四分比相对论计算无法阐明最终在这种情况下TS几何体。因此，结果表明，相对论的效果对于含有Bi和MC的那些氢化物中的这种阻隔测定是至关重要的。此外，虽然标量相对论效果占主导地位，但在BIH <SUB> 3 </ sub>中增加了极高的屏障高度多达17.6千卡（32％），旋转轨道耦合不可能忽略在含有最重15元素的氢化物中，在该相同分子中将屏障降低2.5kcalmol 1 / sup>（4.5％）。 </ p> </ abstract> </span> <span class="z_kbtn z_kbtnclass hoverxs" style="display: none;">展开▼</span> </div> </div> <div class="record"> <h2 class="all_title" id="enpatent33" >著录项</h2> <ul> <li> <span class="lefttit">来源</span> <div style="width: 86%;vertical-align: text-top;display: inline-block;"> <a href='/journal-foreign-21753/'>《International Journal of Quantum Chemistry》</a> <b style="margin: 0 2px;">|</b><span>2018年第14期</span><b style="margin: 0 2px;">|</b><span>共8页</span> </div> </li> <li> <div class="author"> <span class="lefttit">作者</span> <p id="fAuthorthree" class="threelineshidden zhankaihshouqi"> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Santiago Régis T.&option=202" target="_blank" rel="nofollow">Santiago Régis T.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Haiduke Roberto L. A.&option=202" target="_blank" rel="nofollow">Haiduke Roberto L. A.;</a> </p> <span class="z_kbtnclass z_kbtnclassall hoverxs" id="zkzz" style="display: none;">展开▼</span> </div> </li> <li> <div style="display: flex;"> <span class="lefttit">作者单位</span> <div style="position: relative;margin-left: 3px;max-width: 639px;"> <div class="threelineshidden zhankaihshouqi" id="fOrgthree"> <p>Departamento de Química e Física MolecularInstituto de Química de S?o Carlos Universidade de S?o Paulo Av. Trabalhador S?o‐carlense 400 – CP 780 13560‐970 S?o CarlosSP Brazil;</p> <p>Departamento de Química e Física MolecularInstituto de Química de S?o Carlos Universidade de S?o Paulo Av. Trabalhador S?o‐carlense 400 – CP 780 13560‐970 S?o CarlosSP Brazil;</p> </div> <span class="z_kbtnclass z_kbtnclassall hoverxs" id="zhdw" style="display: none;">展开▼</span> </div> </div> </li> <li > <span class="lefttit">收录信息</span> <span style="width: 86%;vertical-align: text-top;display: inline-block;"></span> </li> <li> <span class="lefttit">原文格式</span> <span>PDF</span> </li> <li> <span class="lefttit">正文语种</span> <span>eng</span> </li> <li> <span class="lefttit">中图分类</span> <span><a href="https://www.zhangqiaokeyan.com/clc/1186.html" title="物理化学（理论化学）、化学物理学">物理化学（理论化学）、化学物理学;</a></span> </li> <li class="antistop"> <span class="lefttit">关键词</span> <p style="width: 86%;vertical-align: text-top;"> </p> </li> </ul> </div> </div> <div class="literature cardcommon"> <div class="similarity "> <h3 class="all_title" id="enpatent66">相似文献</h3> <div class="similaritytab clearfix"> <ul> <li class="active" >外文文献</li> <li >中文文献</li> <li >专利</li> </ul> </div> <div class="similarity_details"> <ul > <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/journal-foreign-detail/0704019755706.html">Relativistic effects on inversion barriers of pyramidal group 15 hydrides</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Santiago Régis T.&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Santiago Régis T.,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Haiduke Roberto L. 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</div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/061201136284.html">IL-15Rα sushi结构域作为通过IL-15Rβ/γ的IL-15作用的选择性和有效的增强剂以及超激动剂(IL15Rα sushi-IL15)融合蛋白</a> <b>[P]</b> . <span> 中国专利： CN101360827B </span> <span> . 2013.03.20</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120105556754.html">IL－15Rαsushi结构域作为通过IL－15Rβ/γ的IL－15作用的选择性和有效的增强剂以及超激动剂(IL15Rαsushi－IL15)融合蛋白</a> <b>[P]</b> . <span> 中国专利： CN101360827A </span> <span> . 2009-02-04</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130439044119.html">Waste bin has lid which at least in edge region slopes downwards and outwards at angle of especially at least 15 degrees to horizontal, and which is in pyramid form and at least partially curved</a> <b>[P]</b> . <span> 外国专利：  DE202004013543U1 </span> <span> . 2004-12-02</span> </div> <p class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：废物箱具有盖，该盖至少在边缘区域中向下和向外倾斜成与水平方向至少成15度角，并且呈金字塔形并且至少部分弯曲 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130473886215.html">Alarm clock emitting a heartbeat-imitation pulse sequence/H0I In an alarm clock (1) with acoustic emission of a heartbeat- imitation pulse sequence (7) it is desirable to obtain and transmit such calming effects and at the same time to improve these effects themselves. For this purpose, it is intended to derive the imitation pulse sequence (7) from the time-holding electric circuit (12) for the clock time display device (2) and to emit these sequences electroacoustically via an audio final stage (15), for example by means of a cushion loudspeaker (8) connectable via a cable (10,. The imitation pulse sequence (7) is preferably obtained directly from the sequence of the switching pulses (13) of a stepping motor drive for a seconds hand, from which a pulse shaper circuit (17) can generate the double pulses characteristic of the heartbeat. With a bipolar stepping motor drive a bridgeable diode (19) results in a simple switching means between low and high frequency of the imitation</a> <b>[P]</b> . <span> 外国专利：  DE3312795A1 </span> <span> . 1984-10-11</span> </div> <p class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：发出心跳模仿脉冲序列的闹钟</ H0I>在具有心跳模仿脉冲序列（7）的声音发射的闹钟（1）中，希望获得并传递这种镇静效果，并同时进行改进这些影响本身。为此目的，旨在从用于时钟时间显示装置（2）的保持电路（12）中导出仿制脉冲序列（7），并通过音频末级（15）电声发射这些序列，例如，通过可通过电缆（10）连接的缓冲扬声器（8）。仿制脉冲序列（7）优选直接从步进电机驱动器的秒针切换脉冲（13）的序列中获得，脉冲整形器电路（17）可以从中产生心跳的双脉冲特性，通过双极步进电机驱动，可桥接二极管（19）可以在低频和高频之间进行简单的切换 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130409662481.html">Group 13-15 interstitial metal hydride catalysts and associated processes</a> <b>[P]</b> . <span> 外国专利：  US9663728B2 </span> <span> . 2017-05-30</span> </div> <p class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：13-15组间质金属氢化物催化剂及相关工艺 </span> </p> </li> </ul> </div> </div> </div> <div class="theme cardcommon" style="overflow: auto;display:none"> <h3 class="all_title" id="enpatent55">相关主题</h3> <ul id="subject"> </ul> </div> </div> </div> </div> <div class="right rightcon"> <div class="details_img cardcommon clearfix" style="margin-bottom: 10px;display:none;" > </div> </div> </div> <div id="thesis_get_original1" class="downloadBth" style="bottom: 19px;z-index: 999;" onclick="ywcd('0704019755706','4',7,2,1,'',this,24)" class="delivery" prompt="010401" title="通过人工服务将文献原文发送至邮箱" >获取原文</div> <div class="journalsub-pop-up" style="display: none"> <div class="journal-sub"> <h2>期刊订阅</h2> <img src="https://cdn.zhangqiaokeyan.com/img/loginclose.png" alt="关闭" onclick="$('.journalsub-pop-up').hide()"> <p class="pardon">抱歉，该期刊暂不可订阅，敬请期待！</p> <p class="current">目前支持订阅全部北京大学中文核心（2020）期刊目录。</p> <div 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