使用 FMO 方案进行 VQE-UCCSD 计算时发现的尺寸一致性和轨道不变性问题。

IF 3.4 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Journal of Computational Chemistry Pub Date : 2024-05-25 DOI:10.1002/jcc.27438

Kenji Sugisaki, Tatsuya Nakano, Yuji Mochizuki

{"title":"使用 FMO 方案进行 VQE-UCCSD 计算时发现的尺寸一致性和轨道不变性问题。","authors":"Kenji Sugisaki, Tatsuya Nakano, Yuji Mochizuki","doi":"10.1002/jcc.27438","DOIUrl":null,"url":null,"abstract":"The fragment molecular orbital (FMO) scheme is one of the popular fragmentation-based methods and has the potential advantage of making the circuit shallow for quantum chemical calculations on quantum computers. In this study, we used a GPU-accelerated quantum simulator (cuQuantum) to perform the electron correlation part of the FMO calculation as unitary coupled-cluster singles and doubles (UCCSD) with the variational quantum eigensolver (VQE) for hydrogen-bonded (FH)<math>\n <mrow>\n <msub>\n <mo> </mo>\n <mrow>\n <mn>3</mn>\n </mrow>\n </msub>\n </mrow></math> and (FH)<math>\n <mrow>\n <msub>\n <mo> </mo>\n <mrow>\n <mn>2</mn>\n </mrow>\n </msub>\n </mrow></math>-H<math>\n <mrow>\n <msub>\n <mo> </mo>\n <mrow>\n <mn>2</mn>\n </mrow>\n </msub>\n </mrow></math>O systems with the STO-3G basis set. VQE-UCCSD calculations were performed using both canonical and localized MO sets, and the results were examined from the point of view of size-consistency and orbital-invariance affected by the Trotter error. It was found that the use of localized MO leads to better results, especially for (FH)<math>\n <mrow>\n <msub>\n <mo> </mo>\n <mrow>\n <mn>2</mn>\n </mrow>\n </msub>\n </mrow></math>-H<math>\n <mrow>\n <msub>\n <mo> </mo>\n <mrow>\n <mn>2</mn>\n </mrow>\n </msub>\n </mrow></math>O. The GPU acceleration was substantial for the simulations with larger numbers of qubits, and was about a factor of 6.7–7.7 for 18 qubit systems.","PeriodicalId":188,"journal":{"name":"Journal of Computational Chemistry","volume":"45 26","pages":"2204-2213"},"PeriodicalIF":3.4000,"publicationDate":"2024-05-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/jcc.27438","citationCount":"0","resultStr":"{\"title\":\"Size-consistency and orbital-invariance issues revealed by VQE-UCCSD calculations with the FMO scheme\",\"authors\":\"Kenji Sugisaki, Tatsuya Nakano, Yuji Mochizuki\",\"doi\":\"10.1002/jcc.27438\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The fragment molecular orbital (FMO) scheme is one of the popular fragmentation-based methods and has the potential advantage of making the circuit shallow for quantum chemical calculations on quantum computers. In this study, we used a GPU-accelerated quantum simulator (cuQuantum) to perform the electron correlation part of the FMO calculation as unitary coupled-cluster singles and doubles (UCCSD) with the variational quantum eigensolver (VQE) for hydrogen-bonded (FH)<math>\\n <mrow>\\n <msub>\\n <mo> </mo>\\n <mrow>\\n <mn>3</mn>\\n </mrow>\\n </msub>\\n </mrow></math> and (FH)<math>\\n <mrow>\\n <msub>\\n <mo> </mo>\\n <mrow>\\n <mn>2</mn>\\n </mrow>\\n </msub>\\n </mrow></math>-H<math>\\n <mrow>\\n <msub>\\n <mo> </mo>\\n <mrow>\\n <mn>2</mn>\\n </mrow>\\n </msub>\\n </mrow></math>O systems with the STO-3G basis set. VQE-UCCSD calculations were performed using both canonical and localized MO sets, and the results were examined from the point of view of size-consistency and orbital-invariance affected by the Trotter error. It was found that the use of localized MO leads to better results, especially for (FH)<math>\\n <mrow>\\n <msub>\\n <mo> </mo>\\n <mrow>\\n <mn>2</mn>\\n </mrow>\\n </msub>\\n </mrow></math>-H<math>\\n <mrow>\\n <msub>\\n <mo> </mo>\\n <mrow>\\n <mn>2</mn>\\n </mrow>\\n </msub>\\n </mrow></math>O. The GPU acceleration was substantial for the simulations with larger numbers of qubits, and was about a factor of 6.7–7.7 for 18 qubit systems.\",\"PeriodicalId\":188,\"journal\":{\"name\":\"Journal of Computational Chemistry\",\"volume\":\"45 26\",\"pages\":\"2204-2213\"},\"PeriodicalIF\":3.4000,\"publicationDate\":\"2024-05-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://onlinelibrary.wiley.com/doi/epdf/10.1002/jcc.27438\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Computational Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/jcc.27438\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Computational Chemistry","FirstCategoryId":"92","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/jcc.27438","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

摘要

片段分子轨道（FMO）方案是流行的基于片段的方法之一，其潜在优势是使量子计算机上的量子化学计算电路变得浅显。在本研究中，我们使用 GPU 加速量子模拟器（cuQuantum），以单元耦合簇单倍和双倍（UCCSD）与变异量子优解器（VQE）对氢键（FH）3 $$ {}_3 $$ 和（FH）2 $$ {}_2 $$ -H 2 $$ {}_2 $$ O 系统进行 FMO 计算的电子相关部分，并使用 STO-3G 基集。使用规范和局部 MO 集进行了 VQE-UCCSD 计算，并从尺寸一致性和轨道不变性的角度考察了受 Trotter 误差影响的结果。结果发现，使用局部MO能得到更好的结果，特别是对于(FH) 2 $$ {}_2 $$ -H 2 $$ {}_2 $$ O。对于量子比特数较多的模拟，GPU的加速效果非常明显，对于18量子比特系统，加速效果约为6.7-7.7倍。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

摘要图片

查看原文

微信好友朋友圈 QQ好友复制链接

本刊更多论文

Size-consistency and orbital-invariance issues revealed by VQE-UCCSD calculations with the FMO scheme

The fragment molecular orbital (FMO) scheme is one of the popular fragmentation-based methods and has the potential advantage of making the circuit shallow for quantum chemical calculations on quantum computers. In this study, we used a GPU-accelerated quantum simulator (cuQuantum) to perform the electron correlation part of the FMO calculation as unitary coupled-cluster singles and doubles (UCCSD) with the variational quantum eigensolver (VQE) for hydrogen-bonded (FH) $_{3}$ and (FH) $_{2}$ -H $_{2}$ O systems with the STO-3G basis set. VQE-UCCSD calculations were performed using both canonical and localized MO sets, and the results were examined from the point of view of size-consistency and orbital-invariance affected by the Trotter error. It was found that the use of localized MO leads to better results, especially for (FH) $_{2}$ -H $_{2}$ O. The GPU acceleration was substantial for the simulations with larger numbers of qubits, and was about a factor of 6.7–7.7 for 18 qubit systems.

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

来源期刊

Journal of Computational Chemistry 化学-化学综合

CiteScore

6.60

自引率

3.30%

发文量

247

审稿时长

1.7 months

期刊介绍： This distinguished journal publishes articles concerned with all aspects of computational chemistry: analytical, biological, inorganic, organic, physical, and materials. The Journal of Computational Chemistry presents original research, contemporary developments in theory and methodology, and state-of-the-art applications. Computational areas that are featured in the journal include ab initio and semiempirical quantum mechanics, density functional theory, molecular mechanics, molecular dynamics, statistical mechanics, cheminformatics, biomolecular structure prediction, molecular design, and bioinformatics.

期刊最新文献

Issue Information DC24: A new density coherence functional for multiconfiguration density‐coherence functional theory Excited state relaxation mechanisms of paracetamol and acetanilide. Stable, aromatic, and electrophilic azepinium ions: Design using quantum chemical methods Assessing small molecule conformational sampling methods in molecular docking