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Coherent two-dimensional electronic spectroscopy (2DES) offers a subpicosecond temporal resolution but its spatial resolution is restricted by the diffraction limit. Atomic force microscopy (AFM) overcomes the diffraction limit and routinely attains a sub-10 nm spatial resolution. In this Letter we establish a theoretical framework for the AFM-detected 2DES spectroscopy\u2500a technique that is yet to be experimentally realized but promises to deliver high temporal and spatial resolutions simultaneously. AFM-2DES would measure thermal expansion of the sample in response to interactions with multiple time-delayed laser pulses which interrogate electronic states of the system. We illustrate that the information contained in AFM-2DES spectra is complementary to other far-field action 2D spectroscopies, thus establishing AFM-2DES spectroscopy as a valuable addition to the arsenal of ultrafast spectroscopy techniques.<\/jats:p>","DOI":"10.1021\/acs.jpclett.6c02045","type":"journal-article","created":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T07:03:23Z","timestamp":1786345403000},"page":"9627-9640","source":"Crossref","is-referenced-by-count":2,"title":["Theory and Simulations\nof Atomic Force Microscopy-Based\nTwo-dimensional Electronic Spectroscopy"],"prefix":"10.1021","volume":"17","author":[{"given":"Kennet J.","family":"Rueda Espinosa","sequence":"first","affiliation":[{"name":"University of Delaware , , , ,","place":["Newark, Delaware, United States, 19716"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0847-5871","authenticated-orcid":true,"given":"Xiaoji G.","family":"Xu","sequence":"additional","affiliation":[{"name":"Stony Brook University , , , ,","place":["Stony Brook, New York, United States, 11794"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9422-7203","authenticated-orcid":true,"given":"Alexei A.","family":"Kananenka","sequence":"additional","affiliation":[{"name":"University of Delaware , , , ,","place":["Newark, Delaware, United States, 19716"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,10]]},"reference":[{"key":"2026082008265955700_cit1","doi-asserted-by":"publisher","first-page":"21","DOI":"10.1038\/s43586-026-00474-7","article-title":"Ultrafast nano-imaging and nano-spectroscopy","volume":"6","author":"Esses","year":"2026","journal-title":"Nature Reviews Methods Primers"},{"key":"2026082008265955700_cit2","doi-asserted-by":"publisher","first-page":"573","DOI":"10.1038\/s41578-019-0125-0","article-title":"Heterogeneity at\nmultiple length\nscales in halide perovskite semiconductors","volume":"4","author":"Tennyson","year":"2019","journal-title":"Nature Reviews Materials"},{"key":"2026082008265955700_cit3","doi-asserted-by":"publisher","first-page":"945","DOI":"10.1126\/science.281.5379.945","article-title":"Defects in Semiconductors: Some Fatal,\nSome Vital","volume":"281","author":"Queisser","year":"1998","journal-title":"Science"},{"key":"2026082008265955700_cit4","doi-asserted-by":"publisher","first-page":"471","DOI":"10.1021\/acsenergylett.1c02338","article-title":"Mixing Matters: Nanoscale\nHeterogeneity and\nStability in Metal Halide Perovskite Solar Cells","volume":"7","author":"Mundt","year":"2022","journal-title":"ACS Energy Letters"},{"key":"2026082008265955700_cit5","doi-asserted-by":"publisher","first-page":"66","DOI":"10.1038\/s41560-024-01660-1","article-title":"The\nimpact of interfacial quality and nanoscale\nperformance disorder on the stability of alloyed perovskite solar\ncells","volume":"10","author":"Frohna","year":"2025","journal-title":"Nature Energy"},{"key":"2026082008265955700_cit6","doi-asserted-by":"publisher","first-page":"683","DOI":"10.1126\/science.aaa5333","article-title":"Impact\nof microstructure on local carrier lifetime in perovskite solar cells","volume":"348","author":"de Quilettes","year":"2015","journal-title":"Science"},{"key":"2026082008265955700_cit7","doi-asserted-by":"publisher","first-page":"190","DOI":"10.1038\/s41565-021-01019-7","article-title":"Nanoscale chemical heterogeneity dominates\nthe optoelectronic response of alloyed perovskite solar cells","volume":"17","author":"Frohna","year":"2022","journal-title":"Nat. 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