Physical Review Research,
Год журнала:
2025,
Номер
7(1)
Опубликована: Март 5, 2025
Despite
recent
numerical
evidence,
one
of
the
fundamental
theoretical
mysteries
polaritonic
chemistry
is
how
and
if
collective
strong
coupling
can
induce
local
changes
electronic
structure
to
modify
chemical
properties.
Here
we
present
nonperturbative
analytic
results
for
a
model
system
consisting
an
ensemble
N
harmonic
molecules
under
vibrational
(VSC)
that
alters
our
understanding
this
question.
By
applying
cavity
Born-Oppenheimer
partitioning
on
Pauli-Fierz
Hamiltonian
in
dipole
approximation,
dressed
many-molecule
problem
be
solved
nonperturbatively
analytically
dilute
limit,
i.e.,
self-consistent
solution
with
mean-field
Hartree-product
wave
function
becomes
exact.
We
discover
molecular
polarizabilities
are
modified
even
case
vanishingly
small
single-molecule
couplings.
Consequently,
polarization
mechanism
persists
large-N
limit.
In
contrast,
perturbative
calculation
based
uncoupled
leads
qualitatively
erroneous
scaling
behavior
vanishing
effects
large-N
Nevertheless,
exact
(self-consistent)
determined
from
simulations
instead.
Our
observations
demonstrate
hitherto
existing
collective-scaling
arguments
insufficient
they
pave
way
refined
single-
(or
few-)molecule
strong-coupling
systems
coupling.
Published
by
American
Physical
Society
2025
Chemical Society Reviews,
Год журнала:
2019,
Номер
48(3), С. 937 - 961
Опубликована: Янв. 1, 2019
It
is
possible
to
modify
the
chemical
and
physical
properties
of
molecules,
not
only
through
modifications
but
also
by
coupling
molecules
strongly
light.
More
intriguingly,
strong
between
light
even
without
presence
a
photon.
The
phenomenon
that
makes
this
called
vacuum
fluctuations,
which
finite
zero
point
energy
quantized
electromagnetic
field
inside
an
optical
cavity.
light-matter
coupling,
can
be
as
large
1
eV
(100
kJ
mol-1),
leads
formation
new
hybrid
states,
polaritons.
formed
states
viewed
linear
combination
(vacuum
field)
matter
(molecules),
thus
completely
changing
landscape
system.
Using
interactions
have
for
instance
been
used
change
reactivity,
charge
conductivity,
excited
state
relaxation
pathways
rates
reactions
organic
molecules.
In
review
brief
history
given,
followed
theoretical
framework,
methods
analysis,
accomplishments.
Finally,
personal
reflection
on
future
perspectives
applications
within
given.
Angewandte Chemie International Edition,
Год журнала:
2019,
Номер
58(31), С. 10635 - 10638
Опубликована: Июнь 12, 2019
Here,
we
report
the
catalytic
effect
of
vibrational
strong
coupling
(VSC)
on
solvolysis
para-nitrophenyl
acetate
(PNPA),
which
increases
reaction
rate
by
an
order
magnitude.
This
is
observed
when
microfluidic
Fabry-Perot
cavity
in
VSC
generated
tuned
to
C=O
stretching
mode
both
reactant
and
solvent
molecules.
Thermodynamic
experiments
confirm
nature
system.
The
change
follows
exponential
relation
with
respect
strength
solvent,
indicating
a
cooperative
between
molecules
reactant.
Furthermore,
study
kinetic
isotope
clearly
shows
that
overlap
bands
strongly
coupled
critical
for
catalysis
this
reaction.
combination
effects
confirms
potential
as
new
frontier
chemistry.
Nanophotonics,
Год журнала:
2018,
Номер
7(9), С. 1479 - 1501
Опубликована: Сен. 1, 2018
Abstract
In
this
article,
we
review
strong
light-matter
coupling
at
the
interface
of
materials
science,
quantum
chemistry,
and
photonics.
The
control
light
heat
thermodynamic
limits
enables
exciting
new
opportunities
for
rapidly
converging
fields
polaritonic
chemistry
optics
atomic
scale
from
a
theoretical
computational
perspective.
Our
follows
remarkable
experimental
demonstrations
that
now
routinely
achieve
limit
matter.
many
molecules
couple
collectively
to
single-photon
mode,
whereas,
in
field
nanoplasmonics,
can
be
achieved
single-molecule
limit.
Theoretical
approaches
address
these
experiments,
however,
are
more
recent
come
spectrum
merging
developments
electrodynamics
alike.
We
latest
highlight
common
features
between
two
different
limits,
maintaining
focus
on
tools
used
analyze
classes
systems.
Finally,
present
perspective
need
steps
toward
merging,
formally
computationally,
most
prominent
Nobel
Prize-winning
theories
physics
chemistry:
electronic
structure
(density
functional)
theory.
case
how
fully
description
matter
treats
electrons,
photons,
phonons
same
quantized
footing
will
unravel
effects
cavity-controlled
chemical
dynamics,
optomechanics,
nanophotonics,
other
use
phonons.
Nanophotonics,
Год журнала:
2020,
Номер
10(1), С. 549 - 577
Опубликована: Ноя. 11, 2020
Abstract
In
this
brief
review,
we
summarize
and
elaborate
on
some
of
the
nomenclature
polaritonic
phenomena
systems
as
they
appear
in
literature
quantum
materials
optics.
Our
summary
includes
at
least
70
different
types
light–matter
dressing
effects.
This
also
unravels
a
broad
panorama
physics
applications
polaritons.
A
constantly
updated
version
review
is
available
https://infrared.cni.columbia.edu
.
Nature Communications,
Год журнала:
2018,
Номер
9(1)
Опубликована: Июнь 5, 2018
Abstract
Strong
coupling
between
light
and
matter
leads
to
the
spontaneous
formation
of
hybrid
light–matter
states,
having
different
energies
than
uncoupled
states.
This
opens
up
for
new
ways
modifying
energy
landscape
molecules
without
changing
their
atoms
or
structure.
Heavy
metal-free
organic
emitting
diodes
(OLED)
use
reversed
intersystem
crossing
(RISC)
harvest
from
excited
triplet
is
a
slow
process,
thus
increasing
rate
RISC
could
potentially
enhance
OLED
performance.
Here
we
demonstrate
selective
singlet
state
Erythrosine
B
perturbing
level
nearby
state.
The
reduces
triplet–singlet
gap,
leading
four-time
enhancement
decay
rate,
most
likely
due
an
enhanced
RISC.
Furthermore,
anticipate
that
strong
can
be
used
create
energy-inverted
molecular
systems
ground
lowest
Resonance
energy
transfer
(RET),
the
transport
of
electronic
from
one
atom
or
molecule
to
another,
has
significant
importance
a
number
diverse
areas
science.
Since
pioneering
experiments
on
RET
by
Cario
and
Franck
in
1922,
theoretical
understanding
process
been
continually
refined.
This
review
presents
historical
account
post-Förster
outlook
RET,
based
quantum
electrodynamics,
up
present-day
viewpoint.
It
is
through
this
framework
that
short-range,
R–6
distance
dependence
Förster
theory
was
unified
with
long
range,
radiative
governed
inverse-square
law.
Crucial
knowledge
electric
dipole-electric
dipole
coupling
tensor;
we
outline
its
mathematical
derivation
view
explaining
some
key
physical
concepts
RET.
The
higher
order
interactions
involve
magnetic
dipoles
quadrupoles
are
also
discussed.
To
conclude,
survey
provided
latest
research,
which
includes
between
nanomaterials,
enhancement
due
surface
plasmons,
possibilities
outside
usual
ultraviolet
visible
range
within
cavity.
Proceedings of the National Academy of Sciences,
Год журнала:
2019,
Номер
116(11), С. 4883 - 4892
Опубликована: Фев. 7, 2019
Significance
Excitation
and
charge
transfer
are
fundamental
processes
in
nature,
controlling
these
is
a
major
goal
of
quantum
chemistry.
While
well
understood
for
the
usual
free-space
case,
when
electromagnetic
vacuum
changed
due
to,
e.g.,
cavity,
can
be
dramatically
different.
We
consider
changes
with
real-space
donor–acceptor
models,
where
we
put
an
emphasis
on
impact
electron–electron
correlations.
find
results
line
recent
experiments,
strong
light–matter
interaction
leads
to
enhanced
reactions,
even
corresponding
situation
no
should
possible.
highlight
that
depend
crucially
Coulomb
self-polarization
interactions.