Going for Gold(-Standard): Attaining Coupled Cluster Accuracy in Oxide-Supported Nanoclusters
Fuente:
arXiv
Saved in:
| Main Authors: | , , , |
|---|---|
| Format: | Preprint |
| Published: |
2023
|
| Subjects: | |
| Online Access: | |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1866911882898571264 |
|---|---|
| author | Shi, Benjamin X. Wales, David J. Michaelides, Angelos Myung, Chang Woo |
| author_facet | Shi, Benjamin X. Wales, David J. Michaelides, Angelos Myung, Chang Woo |
| contents | The structure of oxide-supported metal nanoclusters plays an essential role in their sharply enhanced catalytic activity over bulk metals. Simulations provide the atomic-scale resolution needed to understand these systems. However, the sensitive mix of metal-metal and metal-support interactions which govern their structure puts stringent requirements on the method used, requiring going beyond standard density functional theory (DFT). The method of choice is coupled cluster theory [specifically CCSD(T)], but its computational cost has so far prevented applications. In this work, we showcase two approaches to make CCSD(T) accuracy readily achievable in oxide-supported nanoclusters. First, we leverage the SKZCAM protocol to provide the first benchmarks of oxide-supported nanoclusters, revealing that it is specifically metal-metal interactions that are challenging to capture with DFT. Second, we propose a CCSD(T) correction ($Δ$CC) to the metal-metal interaction errors in DFT, reaching comparable accuracy to the SKZCAM protocol at significantly lower cost. This forges a path towards studying larger systems at reliable accuracy, which we highlight by identifying a ground state structure in agreement with experiments for Au$_{20}$ on MgO; a challenging system where DFT models have yielded conflicting predictions. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2311_01426 |
| institution | arXiv |
| publishDate | 2023 |
| record_format | arxiv |
| spellingShingle | Going for Gold(-Standard): Attaining Coupled Cluster Accuracy in Oxide-Supported Nanoclusters Shi, Benjamin X. Wales, David J. Michaelides, Angelos Myung, Chang Woo Materials Science Chemical Physics The structure of oxide-supported metal nanoclusters plays an essential role in their sharply enhanced catalytic activity over bulk metals. Simulations provide the atomic-scale resolution needed to understand these systems. However, the sensitive mix of metal-metal and metal-support interactions which govern their structure puts stringent requirements on the method used, requiring going beyond standard density functional theory (DFT). The method of choice is coupled cluster theory [specifically CCSD(T)], but its computational cost has so far prevented applications. In this work, we showcase two approaches to make CCSD(T) accuracy readily achievable in oxide-supported nanoclusters. First, we leverage the SKZCAM protocol to provide the first benchmarks of oxide-supported nanoclusters, revealing that it is specifically metal-metal interactions that are challenging to capture with DFT. Second, we propose a CCSD(T) correction ($Δ$CC) to the metal-metal interaction errors in DFT, reaching comparable accuracy to the SKZCAM protocol at significantly lower cost. This forges a path towards studying larger systems at reliable accuracy, which we highlight by identifying a ground state structure in agreement with experiments for Au$_{20}$ on MgO; a challenging system where DFT models have yielded conflicting predictions. |
| title | Going for Gold(-Standard): Attaining Coupled Cluster Accuracy in Oxide-Supported Nanoclusters |
| topic | Materials Science Chemical Physics |
| url | https://arxiv.org/abs/2311.01426 |