Probing quantum geometry with two-dimensional nonlinear optical spectroscopy
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arXiv
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| Format: | Preprint |
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2025
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| _version_ | 1866911037870047232 |
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| author | Froese, Paul Hirsbrunner, Mark R. Kim, Yong Baek |
| author_facet | Froese, Paul Hirsbrunner, Mark R. Kim, Yong Baek |
| contents | Recent studies have shown that the nonlinear optical response of crystalline systems is fundamentally a quantum geometric property. In this work, we propose two-dimensional coherent spectroscopy (2DCS), which measures the nonlinear conductivity as a function of two independent frequencies using two time-delayed light pulses, as a probe of quantum geometry. We show how the two-frequency second-order nonlinear conductivity, which is naturally measured by 2DCS, decomposes into distinct quantum geometric contributions. We identify a term arising from the multi-band quantum connection that does not appear in linear response, and show that it can be measured in isolation by considering specific polarizations and enforcing time-reversal symmetry. We explore this finding via model calculations for transition metal dichalcogenides and Sr$_2$RuO$_4$. Through these examples, we demonstrate how 2DCS enables study of the quantum connection, providing a way to compare the quantum geometry of different materials. We also show that one can gain rough momentum-resolved knowledge of the quantum geometry by varying the chemical potential. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2506_05462 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Probing quantum geometry with two-dimensional nonlinear optical spectroscopy Froese, Paul Hirsbrunner, Mark R. Kim, Yong Baek Mesoscale and Nanoscale Physics Recent studies have shown that the nonlinear optical response of crystalline systems is fundamentally a quantum geometric property. In this work, we propose two-dimensional coherent spectroscopy (2DCS), which measures the nonlinear conductivity as a function of two independent frequencies using two time-delayed light pulses, as a probe of quantum geometry. We show how the two-frequency second-order nonlinear conductivity, which is naturally measured by 2DCS, decomposes into distinct quantum geometric contributions. We identify a term arising from the multi-band quantum connection that does not appear in linear response, and show that it can be measured in isolation by considering specific polarizations and enforcing time-reversal symmetry. We explore this finding via model calculations for transition metal dichalcogenides and Sr$_2$RuO$_4$. Through these examples, we demonstrate how 2DCS enables study of the quantum connection, providing a way to compare the quantum geometry of different materials. We also show that one can gain rough momentum-resolved knowledge of the quantum geometry by varying the chemical potential. |
| title | Probing quantum geometry with two-dimensional nonlinear optical spectroscopy |
| topic | Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2506.05462 |