Calculation of exact vibrational spectra for P2O and CH2NH using a phase space wavelet basis.
Calculation of exact vibrational spectra for P2O and CH2NH using a phase space wavelet basis.
复制标题
使用相空间小波基础计算 P2O 和 CH2NH 的精确振动光谱。
DOI：
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发表时间：
2014
影响因子：
4.4
通讯作者：
B. Poirier
中科院分区：
文献类型：
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作者：
Thomas Halverson;B. Poirier
使用动量对称高斯基，对维数广泛变化的两个分子系统（P2O 和 CH2NH）进行振动光谱的“精确”量子动力学计算。该基础先前已被证明可以克服计算成本随系统维数的指数缩放。计算是使用新的“SwitchBLADE”黑盒代码进行的，该代码利用维度无关的算法和大规模并行化来计算任何四阶力场势的大量本征态，对于这里考虑的两种分子，计算了数千个振动激发态，至少达到“中间”精度水平（数十个波数），还讨论了将精度提高到“光谱”水平的未来修改，以及新代码的其他潜在的未来改进。
'Exact" quantum dynamics calculations of vibrational spectra are performed for two molecular systems of widely varying dimensionality (P2O and CH2NH), using a momentum-symmetrized Gaussian basis. This basis has been previously shown to defeat exponential scaling of computational cost with system dimensionality. The calculations were performed using the new "SwitchBLADE" black-box code, which utilizes both dimensionally independent algorithms and massive parallelization to compute very large numbers of eigenstates for any fourth-order force field potential, in a single calculation. For both molecules considered here, many thousands of vibrationally excited states were computed, to at least an "intermediate" level of accuracy (tens of wavenumbers). Future modifications to increase the accuracy to "spectroscopic" levels, along with other potential future improvements of the new code, are also discussed.