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Quantum Information Perspective on Many-Body Dispersive Forces
Phys. Rev. Lett. 135, 110403 – Published 11 September, 2025
DOI: https://doi.org/10.1103/f7yf-mxd5
Abstract
Despite its ubiquity, the quantum many-body properties of dispersion remain poorly understood. Here, we investigate the entanglement distribution in assemblies of quantum Drude oscillators, minimal models for dispersion-bound systems. We establish an analytic relationship between entanglement and correlation energy and show how entanglement monogamy determines whether many-body corrections to the pair potential are attractive, repulsive, or zero. These findings, demonstrated in trimers and extended lattices, apply in more general chemical environments where dispersion coexists with other cohesive forces.
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References (119)
- A. Stone, The Theory of Intermolecular Forces (Oxford University Press, New York, 2013).
- J. O. Hirschfelder, Intermolecular Forces (John Wiley & Sons, New York, 2009), Vol. 12.
- F. London, Z. Phys. 63, 245 (1930).
- J. Hermann, R. A. DiStasio, Jr., and A. Tkatchenko, Chem. Rev. 117, 4714 (2017).
- S. Grimme, Comput. Mol. Sci. 1, 211 (2011).
- R. A. DiStasio, V. V. Gobre, and A. Tkatchenko, J. Phys. Condens. Matter 26, 213202 (2014).
- E. Pastorczak, J. Shen, M. Hapka, P. Piecuch, and K. Pernal, J. Chem. Theory Comput. 13, 5404 (2017).
- O. A. von Lilienfeld, I. Tavernelli, U. Rothlisberger, and D. Sebastiani, Phys. Rev. Lett. 93, 153004 (2004).
- R. H. French, V. A. Parsegian, R. Podgornik, R. F. Rajter, A. Jagota, J. Luo, D. Asthagiri, M. K. Chaudhury, Y.-m. Chiang, S. Granick et al., Rev. Mod. Phys. 82, 1887 (2010).
- I. E. Dzyaloshinskii, E. M. Lifshitz, and L. P. Pitaevskii, Sov. Phys. Usp. 4, 153 (1961).
- F. H. Stillinger and T. A. Weber, Phys. Rev. B 31, 5262 (1985).
- B. Axilrod, J. Chem. Phys. 19, 724 (1951).
- L. Jansen, Phys. Rev. 135, A1292 (1964).
- S. Rsel, H. Quanz, C. Logemann, J. Becker, E. Mossou, L. Cañadillas-Delgado, E. Caldeweyher, S. Grimme, and P. R. Schreiner, J. Am. Chem. Soc. 139, 7428 (2017).
- L. Kronik and A. Tkatchenko, Acc. Chem. Res. 47, 3208 (2014).
- J. P. Wagner and P. R. Schreiner, Angew. Chem., Int. Ed. Engl. 54, 12274 (2015).
- R. A. DiStasio, Jr., O. A. von Lilienfeld, and A. Tkatchenko, Proc. Natl. Acad. Sci. U.S.A. 109, 14791 (2012).
- M. Stöhr and A. Tkatchenko, Sci. Adv. 5, eaax0024 (2019).
- A. Tkatchenko, M. Rossi, V. Blum, J. Ireta, and M. Scheffler, Phys. Rev. Lett. 106, 118102 (2011).
- K. Autumn, M. Sitti, Y. A. Liang, A. M. Peattie, W. R. Hansen, S. Sponberg, T. W. Kenny, R. Fearing, J. N. Israelachvili, and R. J. Full, Proc. Natl. Acad. Sci. U.S.A. 99, 12252 (2002).
- S. Singla, D. Jain, C. M. Zoltowski, S. Voleti, A. Y. Stark, P. H. Niewiarowski, and A. Dhinojwala, Sci. Adv. 7, eabd9410 (2021).
- A. Ambrosetti, D. Alf, R. A. DiStasio, Jr., and A. Tkatchenko, J. Phys. Chem. Lett. 5, 849 (2014).
- A. Tkatchenko, R. A. DiStasio, Jr., R. Car, and M. Scheffler, Phys. Rev. Lett. 108, 236402 (2012).
- A. J. Misquitta, R. Maezono, N. D. Drummond, A. J. Stone, and R. J. Needs, Phys. Rev. B 89, 045140 (2014).
- Y. V. Shtogun and L. M. Woods, J. Phys. Chem. Lett. 1, 1356 (2010).
- J. Hermann, D. Alfe, and A. Tkatchenko, Nat. Commun. 8, 14052 (2017).
- V. L. Deringer and G. Csanyi, J. Phys. Chem. C 120, 21552 (2016).
- W. J. Kim, M. Kim, E. K. Lee, S. Lebegue, and H. Kim, J. Phys. Chem. Lett. 7, 3278 (2016).
- N. Marom, R. A. DiStasio, Jr., V. Atalla, S. Levchenko, A. M. Reilly, J. R. Chelikowsky, L. Leiserowitz, and A. Tkatchenko, Angew. Chem., Int. Ed. Engl. 52, 6629 (2013).
- A. M. Reilly and A. Tkatchenko, Phys. Rev. Lett. 113, 055701 (2014).
- A. M. Reilly and A. Tkatchenko, J. Phys. Chem. Lett. 4, 1028 (2013).
- K. Rościszewski, B. Paulus, P. Fulde, and H. Stoll, Phys. Rev. B 62, 5482 (2000).
- T. Maaravi, I. Leven, I. Azuri, L. Kronik, and O. Hod, J. Phys. Chem. C 121, 22826 (2017).
- B. M. Terhal, IBM J. Res. Dev. 48, 71 (2004).
- G. Adesso and F. Illuminati, Int. J. Quantum. Inform. 04, 383 (2006).
- R. Horodecki, P. Horodecki, M. Horodecki, and K. Horodecki, Rev. Mod. Phys. 81, 865 (2009).
- V. Coffman, J. Kundu, and W. K. Wootters, Phys. Rev. A 61, 052306 (2000).
- T. J. Osborne and F. Verstraete, Phys. Rev. Lett. 96, 220503 (2006).
- T. Hiroshima, G. Adesso, and F. Illuminati, Phys. Rev. Lett. 98, 050503 (2007).
- M. M. Wolf, F. Verstraete, and J. I. Cirac, Int. J. Quantum. Inform. 01, 465 (2003).
- M. Pawłowski, Phys. Rev. A 82, 032313 (2010).
- S. Lloyd and J. Preskill, J. High Energy Phys. 08 (2014) 126.
- M. P. Seevinck, Quantum Inf. Process. 9, 273 (2010).
- M. Koashi and A. Winter, Phys. Rev. A 69, 022309 (2004).
- K. M. O’Connor and W. K. Wootters, Phys. Rev. A 63, 052302 (2001).
- A. Ferraro, A. García-Saez, and A. Acín, Phys. Rev. A 76, 052321 (2007).
- G. Adesso, M. Ericsson, and F. Illuminati, Phys. Rev. A 76, 022315 (2007).
- G. Adesso and F. Illuminati, J. Phys. A 40, 7821 (2007).
- J. Cioslowski and K. Strasburger, J. Phys. Chem. Lett. 15, 1328 (2024).
- D. M. Collins, Z. Naturforsch. A 48, 68 (1993).
- F. S. Cipcigan, J. Crain, V. P Sokhan, and G. J. Martyna, Rev. Mod. Phys. 91, 025003 (2019).
- A. Jones, F. Cipcigan, V. P. Sokhan, J. Crain, and G. J. Martyna, Phys. Rev. Lett. 110, 227801 (2013).
- O. Vaccarelli, D. V. Fedorov, M. Stöhr, and A. Tkatchenko, Phys. Rev. Res. 3, 033181 (2021).
- W. Bade, J. Chem. Phys. 27, 1280 (1957).
- F. Wang and K. Jordan, J. Chem. Phys. 114, 10717 (2001).
- A. P. Jones, J. Crain, V. P. Sokhan, T. W. Whitfield, and G. J. Martyna, Phys. Rev. B 87, 144103 (2013).
- A. Donchev, J. Chem. Phys. 125, 074713 (2006).
- F. S. Cipcigan, V. P. Sokhan, J. Crain, and G. J. Martyna, J. Comput. Phys. 326, 222 (2016).
- F. London, Trans. Faraday Soc. 33, 8b (1937).
- M. Sparnaay, Physica (Utrecht) 25, 217 (1959).
- J. O. Hirschfelder, C. F. Curtiss, and R. B. Bird, Molecular theory of gases and liquids (1964).
- J. Cao and B. Berne, J. Chem. Phys. 97, 8628 (1992).
- M. Sadhukhan and F. R. Manby, Phys. Rev. B 94, 115106 (2016).
- K. R. Bryenton and E. R. Johnson, J. Chem. Phys. 158 (2023).
- P. Xu, M. Alkan, and M. S. Gordon, Chem. Rev. 120, 12343 (2020).
- A. Khabibrakhmanov, D. V. Fedorov, and A. Tkatchenko, J. Chem. Theory Comput. 19, 7895 (2023).
- S. Góger, A. Khabibrakhmanov, O. Vaccarelli, D. V. Fedorov, and A. Tkatchenko, J. Phys. Chem. Lett. 14, 6217 (2023).
- A. Ambrosetti, A. M. Reilly, R. A. DiStasio, and A. Tkatchenko, J. Chem. Phys. 140 (2014).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/f7yf-mxd5 for proofs and additional details, which includes Refs. [70–78].
- J. Hermann, M. Stöhr, S. Góger, S. Chaudhuri, B. Aradi, R. J. Maurer, and A. Tkatchenko, J. Chem. Phys. 159, 174802 (2023).
- J. P. Perdew, K. Burke, and M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996).
- X. Liu, J. Yang, and W. Guo, Phys. Rev. B 101, 045428 (2020).
- A. M. Reilly and A. Tkatchenko, Chem. Sci. 6, 3289 (2015).
- J. Hermann and A. Tkatchenko, Phys. Rev. Lett. 124, 146401 (2020).
- R. A. Horn and C. R. Johnson, Matrix Analysis (Cambridge University Press, Cambridge, England, 2012).
- F. Hansen and G. K. Pedersen, Bull. London Math. Soc. 35, 553 (2003).
- J. Williamson, Am. J. Math. 58, 141 (1936).
- L. W. Anderson, M. Kiffner, P. K. Barkoutsos, I. Tavernelli, J. Crain, and D. Jaksch, Phys. Rev. A 105, 062409 (2022).
- D. C. Langreth and J. P. Perdew, Phys. Rev. B 15, 2884 (1977).
- O. Gunnarsson and B. I. Lundqvist, Phys. Rev. B 13, 4274 (1976).
- B. Jeziorski, R. Moszynski, and K. Szalewicz, Chem. Rev. 94, 1887 (1994).
- H.-Y. Kim, J. O. Sofo, D. Velegol, M. W. Cole, and A. A. Lucas, J. Chem. Phys. 124, 074504 (2006).
- D. Langbein, J. Phys. Chem. Solids 32, 133 (1971).
- M. Renne and B. Nijboer, Chem. Phys. Lett. 1, 317 (1967).
- B. Axilrod and E. Teller, J. Chem. Phys. 11, 299 (1943).
- C. Weedbrook, S. Pirandola, R. García-Patrón, N. J. Cerf, T. C. Ralph, J. H. Shapiro, and S. Lloyd, Rev. Mod. Phys. 84, 621 (2012).
- N. Schuch, J. I. Cirac, and M. M. Wolf, Commun. Math. Phys. 267, 65 (2006).
- M. M. Wolf, F. Verstraete, and J. I. Cirac, Phys. Rev. Lett. 92, 087903 (2004).
- A. Serafini, Quantum Continuous Variables: A Primer of Theoretical Methods (CRC Press, Boca Raton, 2017).
- J. Dereziński, J. Math. Phys. (N.Y.) 58, 121101 (2017).
- J. Colpa, Physica (Amsterdam) 93A, 327 (1978).
- J. Van Hemmen, Z. Phys. B 38, 271 (1980).
- O. Maldonado, J. Math. Phys. (N.Y.) 34, 5016 (1993).
- M. B. Plenio, J. Eisert, J. Dreissig, and M. Cramer, Phys. Rev. Lett. 94, 060503 (2005).
- M. Cramer, J. Eisert, M. B. Plenio, and J. Dreissig, Phys. Rev. A 73, 012309 (2006).
- G. Giedke, M. M. Wolf, O. Krüger, R. F. Werner, and J. I. Cirac, Phys. Rev. Lett. 91, 107901 (2003).
- G. Giedke, B. Kraus, M. Lewenstein, and J. I Cirac, Phys. Rev. Lett. 87, 167904 (2001).
- G. Adesso, S. Ragy, and A. R. Lee, Open Syst. Inf. Dyn. 21, 1440001 (2014).
- J. Manuceau and A. Verbeure, Commun. Math. Phys. 9, 293 (1968).
- A. S. Holevo, Theor. Math. Phys. 6, 1 (1971).
- K. Audenaert, J. Eisert, M. B. Plenio, and R. F. Werner, Phys. Rev. A 66, 042327 (2002).
- L. Amico, R. Fazio, A. Osterloh, and V. Vedral, Rev. Mod. Phys. 80, 517 (2008).
- G. Vidal and R. F. Werner, Phys. Rev. A 65, 032314 (2002).
- M. M. Wolf, G. Giedke, O. Krüger, R. F. Werner, and J. I. Cirac, Phys. Rev. A 69, 052320 (2004).
- G. Adesso and F. Illuminati, Phys. Rev. A 72, 032334 (2005).
- R. Simon, Phys. Rev. Lett. 84, 2726 (2000).
- G. Adesso, A. Serafini, and F. Illuminati, Phys. Rev. A 70, 022318 (2004).
- A. Ibrahim and P.-N. Roy, J. Chem. Phys. 156 (2022).
- R. J. Hinde, Chem. Phys. Lett. 460, 141 (2008).
- P. Wind and I. Røeggen, Chem. Phys. 211, 179 (1996).
- A. Ibrahim and P.-N. Roy, J. Chem. Phys. 157 (2022).
- M. Gori, P. Kurian, and A. Tkatchenko, Nat. Commun. 14, 8218 (2023).
- S. Lee, J. Lee, H. Zhai, Y. Tong, A. M. Dalzell, A. Kumar, P. Helms, J. Gray, Z.-H. Cui, W. Liu et al., Nat. Commun. 14, 1952 (2023).
- L. Ding, S. Mardazad, S. Das, S. Szalay, U. Schollwock, Z. Zimborás, and C. Schilling, J. Chem. Theory Comput. 17, 79 (2020).
- L. Ding and C. Schilling, J. Chem. Theory Comput. 16, 4159 (2020).
- M. Molina-Espíritu, R. Esquivel, S. López-Rosa, and J. Dehesa, J. Chem. Theory Comput. 11, 5144 (2015).
- K. Boguslawski, P. Tecmer, G. Barcza, Ö. Legeza, and M. Reiher, J. Chem. Theory Comput. 9, 2959 (2013).
- K. Boguslawski, P. Tecmer, O. Legeza, and M. Reiher, J. Phys. Chem. Lett. 3, 3129 (2012).
- L. Ding, S. Knecht, Z. Zimborás, and C. Schilling, Quantum Sci. Technol. 8, 015015 (2022).