Year: 2026
Type: preprint
Abstract: Advancing quantum information technologies requires qubits whose coherence can be precisely engineered. Among the qubit platforms in development, molecular spin qubits (MSQs) stand out for their atomic scale tunability and chemical specificity, making them powerful candidates for sensing, simulation, and information processing. However, integrating MSQs into solid-state architectures without degrading their coherence remains a central challenge. Here, we introduce van der Waals (vdW) confinement within two-dimensional materials as a strategy for stabilizing quantum states in MSQs by engineering their local electronic, vibrational, and symmetry environments. Using cobaltocene as a model system, we show that confinement within vdW SnS2 and CdPS3 single crystals reorganizes the single-ion energy landscape and slows spin-lattice relaxation by over two orders of magnitude relative to unconfined cobaltocene. The confined MSQs adopt deterministic orientations and self-assemble into ordered, atomically precise superlattices, establishing vdW confinement as a pathway for integrating MSQs into functional quantum devices.
Source: arXiv (Cornell University)
Authors: Champ, Anna, Mackintosh, Eleanor, Liston, André Koch, Lee, Sanghyo, Walter, Eric D., Hermann, Raphaël P., Yumnam, George, Seewald, Eric, Wu, Xuehao, Mihalyi-Koch, Willa, Braun, Augustin, van Tol, Johan, Orlando, Tomas, Ozerov, Mykhaylo, Gil, Byeongjun, Han, Myung-Geun, Zhu, Yimei, Kim, Miyoung, Pasupathy, Abhay N., Delor, Milan, Steigerwald, Michael L., Berkelbach, Timothy C., Nuckolls, Colin, Roy, Xavier, Ramanathan, Arun
Language: English
Field: Materials Science
Domain: Physical Sciences
Open Access status: green
Funders: National Science Foundation, U.S. Department of Energy, Battelle, National High Magnetic Field Laboratory, European Commission, National Research Foundation, European Synchrotron Radiation Facility, National Research Foundation of Korea, Ministry of Science and ICT, South Korea, Office of Science, Materials Research Science and Engineering Center, Harvard University, Multidisciplinary University Research Initiative, HORIZON EUROPE Framework Programme, Division of Materials Research, Division of Chemistry, Basic Energy Sciences, Biological and Environmental Research, High Magnetic Field Laboratory, Chinese Academy of Sciences, Air Force Office of Scientific Research, Oak Ridge National Laboratory, Brookhaven National Laboratory, Pacific Northwest National Laboratory, SLAC National Accelerator Laboratory
Awards: G1019936685, G1202769797, G1229526393, G125460123, G1285306620, G1286251239, G138090931, G1523888516, G1847291448, G1851334662, G1867732070, G1899721271, G2371548206, G241279073, G2506945562, G2510423872, G262532246, G2779248802, G2820049545, G2837468342, G2959246269, G2988778103, G303061748, G315621713, G3262563802, G357145406, G3648085996, G391136020, G3937223104, G4235786860, G4516885165, G4654690619, Sustainable research at micro and nano X-ray beamlines, G495301720, G498139845, G504303232, G5321382714, G5373841109, G5489601777, G5570207115, Columbia University MRSEC on Precision-Assembled Quantum Materials, G5653134238, G5726405315, G5765906131, G5936398410, G5999762652, G6002429476, G6082596627, G6089160183, G6125720754, MRI: Track 2 Acquisition of Pulsed 9/34 GHz EPR Spectrometer for Quantum Science and Biochemical Research, O.S.C.A.R.S. - Open Science Clusters’ Action for Research and Society, G6550344761, G6965541988, National High Magnetic Field Laboratory Renewal 2023-2027, G7283024673, G742574937, G7463374569, G7560550554, G7665161096, G7772403150, G8135867528, G8152425740, G821644656, G8250561942, G8382000481, G8618556185, G872144517, G8945569637, G911061179, G969889393
OpenAlex ID: W7207866865