Supporting Information: Self-assembly of functionalized RNA nanoparticles demonstrating potential advancements in automated nanomedicine

Kirill A. Afonin1,2*, Wade W. Grabow1*, Faye M. Walker1,Eckart Bindewald3, Marina A. Dobrovolskaia4, Bruce A. Shapiro2#, and Luc Jaeger1#

1 Department of Chemistry and Biochemistry, Biomolecular Science and Engineering Program, University of California, Santa Barbara, CA 93106-9510, USA

2Center for Cancer Research Nanobiology Program, NCI-Frederick, Frederick, MD 21702, USA

3 Basic Science Program, SAIC-Frederick, Inc., NCI-Frederick, Frederick, MD 21702, USA

4 Nanotechnology Characterization Laboratory, Advanced Technology Program, SAIC-Frederick Inc., NCI-Frederick, Frederick, MD 21702, USA

* - these authors contributed equally to this project

# - to whom correspondence should be addressed: Luc Jaeger, phone 805-893-3628; fax 805-893-4120; e-mail: ; Bruce Shapiro, phone 301-846-5536; fax 301-846-5598; email:

RNA sequences used in this project

Non-concatenated cube and ring scaffold sequences are used from previously published works1, 2.

Sense and antisense concatenated cube sequences:

Letter sequences below the RNA strands indicate the desired interactions between different strands. Dots indicate the parts of the strands that are per design single-stranded. Sequence characters in upper case represent the cube scaffold; siRNA-related sequence regions are denoted in lower case. RNA sequences were obtained regions related to the EGFPS1 siRNAby in vitro transcription of PCR generated DNA templates.

3` antisense siRNA (EGFPS1) modifications of RNA cubes with 10 bp per side and3Us at the corners

siA

GGCAACUUUGAUCCCUCGGUUUAGCGCCGGCCUUUUCUCCCACACUUUCACGuucgguggugcagaugaacuucaggguca

MMMMMM...KKKKKKLLLL...FFFFFFGGGG...BBBBBBCCCC...NNNN..ZZZZZZZZZZZZZZZZZZZZZZZZZ..

siB

GGGAAAUUUCGUGGUAGGUUUUGUUGCCCGUGUUUCUACGAUUACUUUGGUCuucgguggugcagaugaacuucaggguca

QQQQQQ...PPPPPPPPPP...MMMMMMNNNN...EEEEEEEEEE...RRRR..ZZZZZZZZZZZZZZZZZZZZZZZZZ..

siC

GGACAUUUUCGAGACAGCAUUUUUUCCCGACCUUUGCGGAUUGUAUUUUAGGuucgguggugcagaugaacuucaggguca

IIIIII...OOOOOOOOOO...QQQQQQRRRR...DDDDDDDDDD...JJJJ..ZZZZZZZZZZZZZZZZZZZZZZZZZ..

siD

GGCGCUUUUGACCUUCUGCUUUAUGUCCCCUAUUUCUUAAUGACUUUUGGCCuucgguggugcagaugaacuucaggguca

FFFFFF...HHHHHHHHHH...IIIIIIJJJJ...AAAAAAAAAA...GGGG..ZZZZZZZZZZZZZZZZZZZZZZZZZ..

siE

GGGAGAUUUAGUCAUUAAGUUUUACAAUCCGCUUUGUAAUCGUAGUUUGUGUuucgguggugcagaugaacuucaggguca

BBBBBB...AAAAAAAAAA...DDDDDDDDDD...EEEEEEEEEE...CCCC..ZZZZZZZZZZZZZZZZZZZZZZZZZ..

siF

GGGAUCUUUACCUACCACGUUUUGCUGUCUCGUUUGCAGAAGGUCUUUCCGAuucgguggugcagaugaacuucaggguca

KKKKKK...PPPPPPPPPP...OOOOOOOOOO...HHHHHHHHHH...LLLL..ZZZZZZZZZZZZZZZZZZZZZZZZZ..

sense

acccugaaguucaucugcaccaccg

ZZZZZZZZZZZZZZZZZZZZZZZZZ

5` sense siRNA (EGFPS1) modifications of RNA cubes with 10 bp per side and3Us at the corners

siA

ggcaagcugacccugaaguucauccaaGGCAACUUUGAUCCCUCGGUUUAGCGCCGGCCUUUUCUCCCACACUUUCACG ZZZZZZZZZZZZZZZZZZZZZZZZZ..MMMMMM...KKKKKKLLLL...FFFFFFGGGG...BBBBBBCCCC...NNNN

siB

ggcaagcugacccugaaguucauccaaGGGAAAUUUCGUGGUAGGUUUUGUUGCCCGUGUUUCUACGAUUACUUUGGUC

ZZZZZZZZZZZZZZZZZZZZZZZZZ..QQQQQQ...PPPPPPPPPP...MMMMMMNNNN...EEEEEEEEEE...RRRR

siC

ggcaagcugacccugaaguucauccaaGGACAUUUUCGAGACAGCAUUUUUUCCCGACCUUUGCGGAUUGUAUUUUAGG ZZZZZZZZZZZZZZZZZZZZZZZZZ..IIIIII...OOOOOOOOOO...QQQQQQRRRR...DDDDDDDDDD...JJJJ

siD

ggcaagcugacccugaaguucauccaaGGCGCUUUUGACCUUCUGCUUUAUGUCCCCUAUUUCUUAAUGACUUUUGGCC ZZZZZZZZZZZZZZZZZZZZZZZZZ..FFFFFF...HHHHHHHHHH...IIIIIIJJJJ...AAAAAAAAAA...GGGG

siE

ggcaagcugacccugaaguucauccaaGGGAGAUUUAGUCAUUAAGUUUUACAAUCCGCUUUGUAAUCGUAGUUUGUGU ZZZZZZZZZZZZZZZZZZZZZZZZZ..BBBBBB...AAAAAAAAAA...DDDDDDDDDD...EEEEEEEEEE...CCCC

siF

ggcaagcugacccugaaguucauccaaGGGAUCUUUACCUACCACGUUUUGCUGUCUCGUUUGCAGAAGGUCUUUCCGA ZZZZZZZZZZZZZZZZZZZZZZZZZ..KKKKKK...PPPPPPPPPP...OOOOOOOOOO...HHHHHHHHHH...LLLL

antisense (As)

ggaugaacuucagggucagcuugccuu

ZZZZZZZZZZZZZZZZZZZZZZZZZ..

3` antisense siRNA (HIV-1) modifications of RNA cubes with 10 bp per side and 3Us at the corners

The names of corresponding siRNAs3, 4 are indicated for eachconcatenated cube strand.

siA_ldr
GGCAACUUUGAUCCCUCGGUUUAGCGCCGGCCUUUUCUCCCACACUUUCACGuugacggacucgcacccaucucucuccuu
MMMMMM...KKKKKKLLLL...FFFFFFGGGG...BBBBBBCCCC...NNNN..SSSSSSSSSSSSSSSSSSSSSSSSS..
siB_nef
GGGAAAUUUCGUGGUAGGUUUUGUUGCCCGUGUUUCUACGAUUACUUUGGUCuuggaggaaauuagcccuuccagucccuu
QQQQQQ...PPPPPPPPPP...MMMMMMNNNN...EEEEEEEEEE...RRRR..TTTTTTTTTTTTTTTTTTTTTTTTT..
siC_pol
GGACAUUUUCGAGACAGCAUUUUUUCCCGACCUUUGCGGAUUGUAUUUUAGGuucuaagacuguaucaucugcuccuguuu
IIIIII...OOOOOOOOOO...QQQQQQRRRR...DDDDDDDDDD...JJJJ..UUUUUUUUUUUUUUUUUUUUUUUUU..
siD_r/t
GGCGCUUUUGACCUUCUGCUUUAUGUCCCCUAUUUCUUAAUGACUUUUGGCCuucgcugacuccgcuucuuccugccauuu
FFFFFF...HHHHHHHHHH...IIIIIIJJJJ...AAAAAAAAAA...GGGG..VVVVVVVVVVVVVVVVVVVVVVVVV..
siE_gag
GGGAGAUUUAGUCAUUAAGUUUUACAAUCCGCUUUGUAAUCGUAGUUUGUGUuuccuggaaugcugucaucauuucuucuu
BBBBBB...AAAAAAAAAA...DDDDDDDDDD...EEEEEEEEEE...CCCC..WWWWWWWWWWWWWWWWWWWWWW
siF_pol47
GGGAUCUUUACCUACCACGUUUUGCUGUCUCGUUUGCAGAAGGUCUUUCCGAuuucuugaauuacuacugccccuucacuu
KKKKKK...PPPPPPPPPP...OOOOOOOOOO...HHHHHHHHHH...LLLL..XXXXXXXXXXXXXXXXXXXXXXXXX..

Corresponding siRNAsense strands

ldr
ggagagagaugggugcgaguucguc

SSSSSSSSSSSSSSSSSSSSSSSSS
nef
gggacuggaagggcuaauuuucucc

TTTTTTTTTTTTTTTTTTTTTTTTT
pol
acaggagcagaugauacaguuuuag

UUUUUUUUUUUUUUUUUUUUUUUUU
r/t
auggcaggaagaagcggaguuagug

VVVVVVVVVVVVVVVVVVVVVVVVV
gag
gaagaaaugaugacagcauuucagg

WWWWWWWWWWWWWWWWWWWWWWWWW
pol47
gugaaggggcaguaguaauuuaaga
XXXXXXXXXXXXXXXXXXXXXXXXX

Sense and antisense concatenated ring sequences:

Bold letter sequences indicate kissing loop regions. siRNA sequences used for NR modifications are identical to those in the case of cube NPs shown above. RNA sequences were obtained by in vitro transcription of PCR generated DNA templates.

3` antisense siRNA (EGFPS1) modifications of RNA rings

((((((((...... ))))))))(((((((...... )))))))......

siA

GGGAAUCCGUCCACUGGAUUCCCGUCACAGAGCCUGCCUGUGACuucgguggugcagaugaacuucaggguca

siB

GGGAAUCCGCAGGCUGGAUUCCCGUCACAGAGAACGCCUGUGACuucgguggugcagaugaacuucaggguca

siC

GGGAAUCCGCGUUCUGGAUUCCCGUCACAGACGUCUCCUGUGACuucgguggugcagaugaacuucaggguca

siD

GGGAAUCCGAGACGUGGAUUCCCGUCACAGUCGUGGUCUGUGACuucgguggugcagaugaacuucaggguca

siE

GGGAAUCCACCACGAGGAUUCCCGUCACAGAACCAUCCUGUGACuucgguggugcagaugaacuucaggguca

siF

GGGAAUCCGAUGGUUGGAUUCCCGUCACAGAGUGGACCUGUGACuucgguggugcagaugaacuucaggguca

sense

acccugaaguucaucugcaccaccg

5` sense siRNA (EGFPS1) modifications of RNA rings

...... ((((((((...... ))))))))(((((((...... )))))))

siA

ggcaagcugacccugaaguucauccaaGGGAAUCCGUCCACUGGAUUCCCGUCACAGAGCCUGCCUGUGAC

siB

ggcaagcugacccugaaguucauccaaGGGAAUCCGCAGGCUGGAUUCCCGUCACAGAGAACGCCUGUGAC

siC

ggcaagcugacccugaaguucauccaaGGGAAUCCGCGUUCUGGAUUCCCGUCACAGACGUCUCCUGUGAC

siD

ggcaagcugacccugaaguucauccaaGGGAAUCCGAGACGUGGAUUCCCGUCACAGUCGUGGUCUGUGAC

siE

ggcaagcugacccugaaguucauccaaGGGAAUCCACCACGAGGAUUCCCGUCACAGAACCAUCCUGUGAC

siF

ggcaagcugacccugaaguucauccaaGGGAAUCCGAUGGUUGGAUUCCCGUCACAGAGUGGACCUGUGAC

antisense (As)

ggaugaacuucagggucagcuugccuu

3` antisense siRNA (HIV-1) modifications of RNA rings

The names of corresponding siRNAs3, 4are indicated for eachconcatenated ring strand.

((((((((...... ))))))))(((((((...... )))))))......

siA_ldr
GGGAAUCCGUCCACUGGAUUCCCGUCACAGAGCCUGCCUGUGACuugacggacucgcacccaucucucuccuu

siB_r/t
GGGAAUCCGCAGGCUGGAUUCCCGUCACAGAGAACGCCUGUGACuucgcugacuccgcuucuuccugccauuu

siC_gag
GGGAAUCCGCGUUCUGGAUUCCCGUCACAGACGUCUCCUGUGACuuccuggaaugcugucaucauuucuucuu

siD_pol47
GGGAAUCCGAGACGUGGAUUCCCGUCACAGUCGUGGUCUGUGACuuucuugaauuacuacugccccuucacuu

siE_pol
GGGAAUCCACCACGAGGAUUCCCGUCACAGAACCAUCCUGUGACuucuaagacuguaucaucugcuccuguuu

siF_nef
GGGAAUCCGAUGGUUGGAUUCCCGUCACAGAGUGGACCUGUGACuuggaggaaauuagcccuuccagucccuu

Corresponding siRNAsense strands

ldr
ggagagagaugggugcgaguucguc
nef
gggacuggaagggcuaauuuucucc
pol
acaggagcagaugauacaguuuuag
r/t
auggcaggaagaagcggaguuagug
gag
gaagaaaugaugacagcauuucagg
pol47
gugaaggggcaguaguaauuuaaga

References

1.Afonin, K.A. et al. In vitro assembly of cubic RNA-based scaffolds designed in silico. Nat Nanotechnol5, 676-682 (2010).

2.Grabow, W.W. et al. Self-assembling RNA nanorings based on RNAI/II inverse kissing complexes. Nano letters11, 878-887 (2011).

3.Berkhout, B. & Sanders, R.W. Molecular strategies to design an escape-proof antiviral therapy. Antiviral research (2011).

4.Liu, Y.P. et al. Combinatorial RNAi against HIV-1 using extended short hairpin RNAs. Mol Ther17, 1712-1723 (2009).