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Title: DNA Templated Metal Nanoclusters: From Emergent Properties to Unique Applications

Abstract

Metal nanoclusters containing a few to several hundred atoms with sizes ranging from sub-nanometer to ~2 nm occupy an intermediate size regime that bridges larger plasmonic nanoparticles and smaller metal complexes. With strong quantum confinement, metal nanoclusters exhibit molecule-like properties. This paper focuses on noble metal nanoclusters that are synthesized within a single stranded DNA template. Compared to other ligand protected metal nanoclusters, DNA-templated metal nanoclusters manifest intriguing physical and chemical properties that are heavily influenced by the design of DNA templates. For example, DNA-templated silver nanoclusters can show bright fluorescence, tunable emission colors, and enhanced stability by tuning the sequence of the encapsulating DNA template. DNA-templated gold nanoclusters can also serve as excellent cocatalysts, which are integratable with other biocatalysts such as enzymes. In this Account, DNA-templated silver and gold nanoclusters are selected as paradigm systems to showcase their emergent properties and unique applications. We first discuss the DNA-templated silver nanoclusters with a focus on the creation of a complementary palette of emission colors, which has potential applications for multiplex assays. The importance of the DNA template toward enhanced stability of silver nanoclusters is also demonstrated. We then introduce a special class of activable fluorescence probes that are basedmore » on the fluorescence turn-on phenomena of DNA-templated silver nanoclusters, which are named nanocluster beacons (NCBs). NCBs have distinct advantages over molecular beacons for nucleic acid detection, and their emission mechanisms are also discussed in detail. We then discuss a universal method of creating novel DNA–silver nanocluster aptamers for protein detection with high specificity. The remainder of the Account is devoted to the DNA-templated gold nanoclusters. We demonstrate that DNA–gold nanoclusters can serve as enhancers for enzymatic reduction of oxygen, which is one of the most important reactions in biofuel cells. Although DNA-templated metal nanoclusters are still in their infancy, we anticipate they will emerge as a new type of functional nanomaterial with wide applications in biology and energy science. Future research will focus on the synthesis of size selected DNA–metal nanoclusters with atomic monodispersity, structural determination of different sized DNA–metal nanoclusters, and establishment of structure–property correlations. Some long-standing mysteries, such as the origin of fluorescence and mechanism for emission color tunability, constitute the central questions regarding the photophysical properties of DNA–metal nanoclusters. On the application side, more studies are required to understand the interaction between nanocluster and biological systems. In the foreseeable future, one can expect that new biosensors, catalysts, and functional devices will be invented based on the intriguing properties of well-designed DNA–metal nanoclusters and their composites. Altogether, DNA–metal nanoclusters can add additional spotlights into the highly vibrant field of ligand protected, quantum sized metal nanoclusters.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Univ. of Mississippi, Oxford, MS (United States). Dept. of Chemistry and Biochemistry
  3. Northern Arizona Univ., Flagstaff, AZ (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC); LANL Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1480003
Report Number(s):
LA-UR-18-25907
Journal ID: ISSN 0001-4842
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Accounts of Chemical Research
Additional Journal Information:
Journal Volume: 51; Journal Issue: 11; Journal ID: ISSN 0001-4842
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Material Science

Citation Formats

Chen, Yuxiang, Phipps, M. Lisa, Werner, James H., Chakraborty, Saumen, and Martinez, Jennifer S. DNA Templated Metal Nanoclusters: From Emergent Properties to Unique Applications. United States: N. p., 2018. Web. doi:10.1021/acs.accounts.8b00366.
Chen, Yuxiang, Phipps, M. Lisa, Werner, James H., Chakraborty, Saumen, & Martinez, Jennifer S. DNA Templated Metal Nanoclusters: From Emergent Properties to Unique Applications. United States. doi:10.1021/acs.accounts.8b00366.
Chen, Yuxiang, Phipps, M. Lisa, Werner, James H., Chakraborty, Saumen, and Martinez, Jennifer S. Fri . "DNA Templated Metal Nanoclusters: From Emergent Properties to Unique Applications". United States. doi:10.1021/acs.accounts.8b00366.
@article{osti_1480003,
title = {DNA Templated Metal Nanoclusters: From Emergent Properties to Unique Applications},
author = {Chen, Yuxiang and Phipps, M. Lisa and Werner, James H. and Chakraborty, Saumen and Martinez, Jennifer S.},
abstractNote = {Metal nanoclusters containing a few to several hundred atoms with sizes ranging from sub-nanometer to ~2 nm occupy an intermediate size regime that bridges larger plasmonic nanoparticles and smaller metal complexes. With strong quantum confinement, metal nanoclusters exhibit molecule-like properties. This paper focuses on noble metal nanoclusters that are synthesized within a single stranded DNA template. Compared to other ligand protected metal nanoclusters, DNA-templated metal nanoclusters manifest intriguing physical and chemical properties that are heavily influenced by the design of DNA templates. For example, DNA-templated silver nanoclusters can show bright fluorescence, tunable emission colors, and enhanced stability by tuning the sequence of the encapsulating DNA template. DNA-templated gold nanoclusters can also serve as excellent cocatalysts, which are integratable with other biocatalysts such as enzymes. In this Account, DNA-templated silver and gold nanoclusters are selected as paradigm systems to showcase their emergent properties and unique applications. We first discuss the DNA-templated silver nanoclusters with a focus on the creation of a complementary palette of emission colors, which has potential applications for multiplex assays. The importance of the DNA template toward enhanced stability of silver nanoclusters is also demonstrated. We then introduce a special class of activable fluorescence probes that are based on the fluorescence turn-on phenomena of DNA-templated silver nanoclusters, which are named nanocluster beacons (NCBs). NCBs have distinct advantages over molecular beacons for nucleic acid detection, and their emission mechanisms are also discussed in detail. We then discuss a universal method of creating novel DNA–silver nanocluster aptamers for protein detection with high specificity. The remainder of the Account is devoted to the DNA-templated gold nanoclusters. We demonstrate that DNA–gold nanoclusters can serve as enhancers for enzymatic reduction of oxygen, which is one of the most important reactions in biofuel cells. Although DNA-templated metal nanoclusters are still in their infancy, we anticipate they will emerge as a new type of functional nanomaterial with wide applications in biology and energy science. Future research will focus on the synthesis of size selected DNA–metal nanoclusters with atomic monodispersity, structural determination of different sized DNA–metal nanoclusters, and establishment of structure–property correlations. Some long-standing mysteries, such as the origin of fluorescence and mechanism for emission color tunability, constitute the central questions regarding the photophysical properties of DNA–metal nanoclusters. On the application side, more studies are required to understand the interaction between nanocluster and biological systems. In the foreseeable future, one can expect that new biosensors, catalysts, and functional devices will be invented based on the intriguing properties of well-designed DNA–metal nanoclusters and their composites. Altogether, DNA–metal nanoclusters can add additional spotlights into the highly vibrant field of ligand protected, quantum sized metal nanoclusters.},
doi = {10.1021/acs.accounts.8b00366},
journal = {Accounts of Chemical Research},
issn = {0001-4842},
number = 11,
volume = 51,
place = {United States},
year = {2018},
month = {10}
}

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