TY - JOUR
T1 - A Self-Assembled Rhombohedral DNA Crystal Scaffold with Tunable Cavity Sizes and High-Resolution Structural Detail
AU - Simmons, Chad R.
AU - MacCulloch, Tara
AU - Zhang, Fei
AU - Liu, Yan
AU - Stephanopoulos, Nicholas
AU - Yan, Hao
N1 - Funding Information:
The Berkeley Center for Structural Biology is supported in part by the Howard Hughes Medical Institute. The Advanced Light Source is a Department of Energy Office of Science User Facility under Contract No. DE-AC02-05CH11231. Results derived from work performed at Argonne National Laboratory ANL, Structural Biology Center (SBC) at the Advanced Photon Source (APS), were supported under U.S. Department of Energy, Office of Biological and Environmental Research contract DE-AC02-06CH11357. Results from beamlines AMX (17-ID) and FMX (17-BM) at the National Synchrotron Light Source II, which is a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. The Life Science Biomedical Technology Research resource is primarily supported by the National Institute of Health, National Institute of General Medical Sciences (NIGMS) through a Biomedical Technology Research Resource P41 grant (P41GM111244). N.S. acknowledges startup funds from Arizona State University. This material is based upon work supported by the Air Force Office of Scientific Research under award number FA9550-17-1-0053. H.Y. and N.S. gratefully acknowledge support from the National Science Foundation Division of Materials Research (NSF2004250). H.Y. was additionally supported by the DOE Office of Biological and Environmental Research (KP1605010) and the Presidential Strategic Initiative Fund from Arizona State University.
Funding Information:
The Berkeley Center for Structural Biology is supported in part by the Howard Hughes Medical Institute. The Advanced Light Source is a Department of Energy Office of Science User Facility under Contract No. DE‐AC02‐05CH11231. Results derived from work performed at Argonne National Laboratory ANL, Structural Biology Center (SBC) at the Advanced Photon Source (APS), were supported under U.S. Department of Energy, Office of Biological and Environmental Research contract DE‐AC02‐06CH11357. Results from beamlines AMX (17‐ID) and FMX (17‐BM) at the National Synchrotron Light Source II, which is a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE‐SC0012704. The Life Science Biomedical Technology Research resource is primarily supported by the National Institute of Health, National Institute of General Medical Sciences (NIGMS) through a Biomedical Technology Research Resource P41 grant (P41GM111244). N.S. acknowledges startup funds from Arizona State University. This material is based upon work supported by the Air Force Office of Scientific Research under award number FA9550‐17‐1‐0053. H.Y. and N.S. gratefully acknowledge support from the National Science Foundation Division of Materials Research (NSF2004250). H.Y. was additionally supported by the DOE Office of Biological and Environmental Research (KP1605010) and the Presidential Strategic Initiative Fund from Arizona State University.
Publisher Copyright:
© 2020 Wiley-VCH GmbH
PY - 2020/10/12
Y1 - 2020/10/12
N2 - DNA is an ideal molecule for the construction of 3D crystals with tunable properties owing to its high programmability based on canonical Watson–Crick base pairing, with crystal assembly in all three dimensions facilitated by immobile Holliday junctions and sticky end cohesion. Despite the promise of these systems, only a handful of unique crystal scaffolds have been reported. Herein, we describe a new crystal system with a repeating sequence that mediates the assembly of a 3D scaffold via a series of Holliday junctions linked together with complementary sticky ends. By using an optimized junction sequence, we could determine a high-resolution (2.7 Å) structure containing R3 crystal symmetry, with a slight subsequent improvement (2.6 Å) using a modified sticky-end sequence. The immobile Holliday junction sequence allowed us to produce crystals that provided unprecedented atomic detail. In addition, we expanded the crystal cavities by 50 % by adding an additional helical turn between junctions, and we solved the structure to 4.5 Å resolution by molecular replacement.
AB - DNA is an ideal molecule for the construction of 3D crystals with tunable properties owing to its high programmability based on canonical Watson–Crick base pairing, with crystal assembly in all three dimensions facilitated by immobile Holliday junctions and sticky end cohesion. Despite the promise of these systems, only a handful of unique crystal scaffolds have been reported. Herein, we describe a new crystal system with a repeating sequence that mediates the assembly of a 3D scaffold via a series of Holliday junctions linked together with complementary sticky ends. By using an optimized junction sequence, we could determine a high-resolution (2.7 Å) structure containing R3 crystal symmetry, with a slight subsequent improvement (2.6 Å) using a modified sticky-end sequence. The immobile Holliday junction sequence allowed us to produce crystals that provided unprecedented atomic detail. In addition, we expanded the crystal cavities by 50 % by adding an additional helical turn between junctions, and we solved the structure to 4.5 Å resolution by molecular replacement.
KW - DNA lattices
KW - Holliday junctions
KW - host–guest scaffolds
KW - self-assembly
KW - structural DNA nanotechnology
UR - http://www.scopus.com/inward/record.url?scp=85089550406&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85089550406&partnerID=8YFLogxK
U2 - 10.1002/anie.202005505
DO - 10.1002/anie.202005505
M3 - Article
C2 - 32533629
AN - SCOPUS:85089550406
SN - 1433-7851
VL - 59
SP - 18619
EP - 18626
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 42
ER -