ARTICLE
Received 10 Aug 2016 | Accepted 19 Dec 2016 | Published 6 Feb 2017
Cooling a mechanical resonator mode to a sub-thermal state has been a long-standing challenge in physics. This pursuit has recently found traction in the eld of optomechanics in which a mechanical mode is coupled to an optical cavity. An alternate method is to couple the resonator to a well-controlled two-level system. Here we propose a protocol to dissipatively cool a room temperature mechanical resonator using a nitrogen-vacancy centre ensemble. The spin ensemble is coupled to the resonator through its orbitally-averaged excited state, which has a spinstrain interaction that has not been previously studied. We experimentally demonstrate that the spinstrain coupling in the excited state is 13.50.5 times stronger than the ground state spinstrain coupling. We then theoretically show that this interaction, combined with a high-density spin ensemble, enables the cooling of a mechanical resonator from room temperature to a fraction of its thermal phonon occupancy.
DOI: 10.1038/ncomms14358 OPEN
Cooling a mechanical resonator with nitrogen-vacancy centres using a room temperature excited state spinstrain interaction
E.R. MacQuarrie1, M. Otten1, S.K. Gray2 & G.D. Fuchs3
1 Department of Physics, Cornell University, Ithaca, New York 14853, USA. 2 Center for Nanoscale Materials, Argonne National Laboratory, Argonne, Illinois 60439, USA. 3 School of Applied and Engineering Physics, Cornell University, Ithaca, New York 14853, USA. Correspondence and requests for materials should be addressed to G.D.F. (email: mailto:[email protected]
Web End [email protected] ).
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Cooling a mechanical resonator to a sub-thermal phonon occupation can enhance sensing by lowering the resonators thermal noise oor and extending a sensors
linear dynamic range14. Taken to the extreme, cooling a mechanical mode to the ground state of its motion enables the exploration of quantum effects at the mesoscopic scale57. These goals have motivated researchers in the eld of optomechanics to invent methods for cooling mechanical resonators through their interactions with light. Such techniques have been able to achieve cooling to the ground state from cryogenic starting temperatures6,7 and to near the ground state from room temperature812.
A well-controlled quantum system coupled to the motion of a resonator can also be used to cool a mechanical mode13,14. Recently, nitrogen-vacancy (NV) centres in diamond have been coupled to mechanical resonators through coherent interactions with lattice strain1522. The opportunity to use these interactions has stimulated the development of single-crystal diamond mechanical resonators2326 and motivated several theoretical proposals for cooling such resonators with a single NV centre13,14,27,28. In principle, replacing the single NV centre with a many-NV ensemble can provide a collective enhancement to the strain coupling, which could increase the cooling power of these protocols. In practice, however, ensembles can shorten spin coherence times and introduce inhomogeneities that may make collective enhancement impractical, depending on the proposed mechanism. To make ensemble coupling a useful resource, it thus becomes crucial to design a cooling protocol that is insensitive to these side effects.
In this work, we study the hybrid quantum system composed of an NV centre spin ensemble collectively coupled to a mechanical resonator with the goal of developing a method for cooling the resonator from ambient temperature. Experimentally, we characterize the previously unstudied spinstrain coupling within the room temperature NV centre excited state (ES), and we nd that it is 13.50.5 times stronger than the ground state (GS) spinstrain interaction. We then propose a dissipative cooling protocol that uses this ES spinstrain interaction and theoretically show that a dense NV centre ensemble can cool a high-Q mechanical resonator from room temperature to a fraction of its thermal phonon population. The proposed protocol requires neither long spin coherence times nor strong spin-phonon coupling, and the cooling power scales directly with the NV centre density. These properties make our proposed protocol a practical approach to cooling a room temperature resonator.
ResultsNV centrestrain interactions. To achieve substantial cooling from ambient conditions, we require a room temperature NV centrestrain interaction that can be enhanced by an ensemble. We rst consider the orbital-strain coupling that exists within the NV centre ES at cryogenic temperatures. This 850130 THz per strain interaction offers a promising route towards single NV centre-mechanical resonator hybrid quantum systems21,22. For ensemble coupling, however, inevitable static strain inhomogeneities will strongly broaden the orbital transition and prohibit collective enhancement. Moreover, the orbital coherence begins to dephase above 10 K because of phonon interactions29, limiting applications of orbital-strain coupling to cryogenic operation.
A weaker (21.51.2 GHz per strain) spinstrain coupling exists at room temperature within the NV centre GS (ref. 17). The resonance condition for this interaction is determined by a static magnetic bias eld which can be very uniform across an ensemble. This GS spinstrain interaction thus offers a path towards coupling an ensemble to a mechanical resonator. As the
NV centre density grows, however, the GS spin coherence will decrease30,31, limiting the utility of the collective enhancement.
Finally, we consider spinstrain interactions in the room temperature ES, which have not been thoroughly investigated but might provide the desired compatibility with dense ensembles. For temperatures above B150 K, orbital-averaging from the dynamic JahnTeller effect erases the orbital degree of freedom from the NV centre ES Hamiltonian, resulting in an effective orbital singlet ES at room temperature29,3234. Previously, magnetic spectroscopy measured an unidentied spin splitting within the room temperature ES that is on the order of 10 times stronger than the GS spinstrain interaction. These measurements hinted that this splitting might be a spinstrain interaction in the ES (refs 35,36). Like the GS spinstrain coupling, the resonance condition for such an interaction would be determined by a static magnetic bias eld, enabling collective enhancement with an ensemble. Furthermore, the NV centre density is not expected to affect the ES coherence time, which is limited by the ES motional narrowing rate34,37. Such an ES spinstrain interaction could thus offer a promising path towards coupling a dense NV centre ensemble to a mechanical resonator. Our rst goal then becomes to understand and precisely quantify this coupling.
Assuming this ES coupling is the result of a spinstrain interaction, we can write the spin Hamiltonian for an NV centre in the presence of a magnetic eld B and non-axial strain Ex. Both the GS and room temperature ES Hamiltonians then take the form (: 1)36,38
H D0S2z gNVS B d?Ex S2x S2y
AjjSzIz 1
where De0/2p 1.42 GHz and Dg0/2p 2.87 GHz are the ES
and GS zero-eld splittings, gNV/2p 2.8 MHz/G is the NV
centre gyromagnetic ratio, Aejj=2p 40 MHz (ref. 39) and
Agjj=2p 2:166 MHz are the ES and GS hyperne couplings to
the 14N nuclear spin, S (I) is the electronic (nuclear) spin-1 Pauli vector, and the z-axis runs along the NV centre symmetry axis. Perpendicular strain Ex couples the j ms
1i and j 1i spin
states with a strength de? in the ES and dg?/2p 21.51.2 GHz
per strain in the GS (ref. 17). As shown in Fig. 1a, this interaction enables direct control of the magnetically-forbidden j 1i
2j 1i spin transition within each orbital through resonant
strain.
Device details. The combination of a large hyperne splitting in the ES and a short ES lifetime broadens the spectral features of the ES spinstrain interaction. Measuring such a spectrum then requires large magnetic eld sweeps DBz 150 G
, which in turn
require a mechanical driving eld with a high carrier frequency om=2p\420 MHz
. To this end, we fabricate a high-overtone
bulk acoustic resonator (HBAR) capable of generating large amplitude strain at gigahertz-scale frequencies. The resonator used in this work was driven at a om/2p 529 MHz mechanical
mode that has a quality factor of Q 1,79020. An antenna
fabricated on the opposite diamond face provides high-frequency magnetic elds for magnetic spin control. The nal device is pictured in Fig. 1b.
Spinstrain spectroscopy. To measure mechanical spin driving within the ES, we execute the pulse sequences shown in Fig. 2a, as a function of the magnetic bias eld Bz. In the rst sequence, a 532 nm laser initializes the NV centre ensemble into the GS level g; ms
0
j i. A magnetic adiabatic passage (AP) then moves
the spin population to g; 1
j i. At this point, we pulse the
mechanical resonator at its resonance frequency om for 3 ms.
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a b
ZnO transducer
Diamond
ZnO
Energy
AI
D
D e0
Microwave antenna
Confocal microscope objective
Pt
Magnetic bias field
Figure 1 | Energy levels and device schematic. (a) NV center ground state and excited state energy levels as a function of the magnetic bias eld. Energies have been plotted relative to the ms 0 state in each orbital, and a mechanical mode of frequency om has been drawn connecting the mI 1
hyperne sublevels. (b) Schematic of the device used in these measurements along with optical micrographs of the ZnO transducer used to generate the strain standing wave (150 mm scale bar) and the microwave antenna used to generate magnetic control elds (200 mm scale bar).
a
b
Measure S1= (Re-intialization + spin driving)
opt
t
t
1.0
0.8
0.6
0.4
0.2
0.00.0 0.1 0.2 0.3 0.4 0.5 0.6
Measure S2= Re-intialization
532 nm laser Magnetic driving
P g ,0
opt
S1 = (Re-initialization + spin driving)
Mechanical driving
Optical pulse length (s)
c
d
0.08
P +1
0.06
0.04
0.02
0.0020 93.0 93.5 94.0 94.5 95.0 95.5
40 60 80 100Bz (G) Bz (G)
120 140 160
GS transitions
0.08
0.06
0.04
0.02
0.00
ml = 1 ml = 0 ml = +1
Figure 2 | Spinstrain spectroscopy. (a) Pulse sequences used to measure excited state (ES) spin driving. (b) Population in g; 0
j i at the end of the pulse
sequences in a plotted against topt. (c) Spectrum of the spin population driven mechanically into 1
j i by the ES and ground state (GS) spinstrain
interactions. The red curve is a least squares t to the sum of six Lorentzians. (d) Zoomed in view of the GS spin transitions in c. The data in c,d were measured on one device with an NV centre ensemble, and error bars are from the s.d. in photon counting.
Just before the end of the mechanical pulse, we apply a topt
125 ns optical pulse with the 532 nm laser. This excites the ensemble to e; 1
j i and allows the spins to interact with the
mechanical driving eld in the ES. If the driving eld is resonant with the e; 1
j i2 e; 1
j i splitting, population will be driven
into e; 1
j i. The spins then follow either a spin-conserving
relaxation down to g; 1
j i or a relaxation to the singlet state S1
j i
through an intersystem crossing. The former preserves the spin state information, while relaxing to S1
j i re-initializes the state,
erases the stored signal and reduces the overall contrast of the measurement. After allowing the ensemble to relax, we apply the second magnetic AP to return the spin population in g; 1
j i to
g; 0
j i and measure the g; 0
j i population via uorescence read out.
We dene this signal as S1 and plot it as a function of topt in Fig. 2b.
In the second pulse sequence, the mechanical pulse occurs between the second AP and uorescence read out. Applying the mechanical pulse with the ensemble in g; 0
j i maintains the same
power load on the device but does not drive spin population. This sequence measures S2, the re-initialization of the ensemble from the topt optical pulse (Fig. 2b). Subtracting S2 S1 gives the
probability of nding the ensemble in 1
j i at the end of the rst
sequence. A third sequence with a single AP and a fourth with
two APs (both with topt 0) normalize the spin contrast at
each Bz.
Figure 2c shows the resulting experimental signal. The three broad, low peaks correspond to the hyperne-split e; 1
j i-
e; 1
j i transition, providing denitive evidence of a spinstrain
interaction within the room temperature ES. Population is also driven into g; 1
j i by the GS spinstrain interaction when the
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mechanical driving eld is resonant with the g; 1
j i2 g; 1
j i
splitting. Figure 2c thus contains both ES and GS spectra. We t the data to the sum of three low, broad Lorentzians describing the ES spinstrain interaction and three taller, narrower Lorentzians describing the GS interaction (see Methods). Figure 2d highlights the GS driving with a zoomed in view of Fig. 2c about the GS resonances. The GS peaks have larger amplitudes than the ES peaks because the GS interaction acts for the entire duration of the 3 ms mechanical pulse, whereas the ES interaction only acts during the B125 ns that the spin population is in the ES. Also, the reversed sign of Aejj relative to Agjj is
consistent with ab initio calculations40 and was conrmed by measurements presented in Supplementary Note 1 that were conditional on the nuclear spin state.
Quantication of de?. To quantify the strength of the ES
spinphonon interaction, we rst calibrate the strain amplitude generated by the HBAR by mechanically driving Rabi oscillations within the GS and extracting the GS mechanical Rabi eld Og as a function of the applied power (Fig. 3a). Next, we spectrally isolate the e; 1
j i2 e; 1
j i transition by xing Bz 80 G. At this eld,
the applied strain is on resonance in the ES but off resonance in the GS (Fig. 2c). We then execute a modied version of the pulse sequence described above. Here, we use B20 ns magnetic p-pulses to address the g; 0
j i2 g; 1
j i transition and measure
both S1 and S2 as a function of topt for each power level applied to the HBAR.
As Fig. 3b shows, taking S2 S1 reveals a competition between
mechanical driving into e; 1
j i and re-initialization into 0
j i via
optical pumping. For nonzero topt, the ES mechanical driving eld Oe drives spin population from e; 1
j i to e; 1
j i,
increasing P e; 1
j i, but as topt grows, optical pumping re-initializes
the ensemble into 0
j i, vacating the ms { 1, 1} subspace and
reducing P e; 1
j i to zero. A seven-level master equation model
recreates this competition and provides good ts to the data. From these ts, we extract the value of Oe. The Methods section includes a detailed description of this model, which was designed to account for inhomogeneities within the NV centre ensemble and for the polarization of the nuclear spin sublevels, among other effects. Plotting Oe against Og (Fig. 3c) shows that the transverse spinstrain coupling in the ES is 13.50.5 times stronger than the GS coupling, or de?/2p 29020 GHz
per strain.
Resonator cooling protocol. With de? quantied, we now present
a dissipative protocol for cooling a mechanical resonator with an NV centre spin ensemble. In our proposed protocol, a 532 nm
laser continuously pumps the phonon sidebands of the ensembles optical transition, and a gigahertz frequency magnetic eld continuously drives the g; 0
j i2 g; 1
j i spin transition.
This generates a steady state population surplus in e; 1
j i as
compared with e; 1
j i, enabling the net absorption of phonons
by the ensemble. Spontaneous relaxation and subsequent optical pumping continually re-initialize the system, allowing the phonon absorption cycle to continue. Figure 4a summarizes this process.
The dissipative nature of this protocol enables resonator cooling without requiring strong spin-phonon coupling. Here, we dene strong coupling as a single-spin cooperativity Z l2T 2=gnth41, where l is the single spin-single
phonon coupling strength, T 2 is the inhomogeneous spin dephasing time, g om/Q is the mechanical dissipation rate
and nth kBT= om is the thermal phonon occupancy of the
resonator mode41. A cooperativity of Z41 marks the threshold for coherent interactions between the spin and the mechanical mode. Non-idealities in spin coherence and resonator fabrication have thus far prevented the experimental realization of NV centre cooperativities approaching unity, especially at room temperature. This makes the proposed dissipative protocol a practical and attractive approach because it does not require coherent interactions for resonator cooling to occur.
To analyse the performance of the protocol we start by considering a single two-state spin system coupled to a mechanical resonator. The resulting dynamics obey the master equation (: 1) _
r i H; r
LGr Lgr 2 where H describes the coherent coupling between the spin and the resonator, LG describes the incoherent spin processes, and Lg
describes the resonator rethermalization. For resonant coupling, the quantized Hamiltonian in the JaynesCummings form is42
H om aya S S
l S S
ay a
3
where aw (a) is the creation (annihilation) operator for the mechanical mode and S are the ladder operators for the spin state. The spin relaxation term in equation (2) takes the form LGr 2T1
1D S
r 2T 2
1 SzrSz r
, where
D S
r 2S rS S S r rS S
is the Lindblad
superoperator and T1 T 2
is the transverse (longitudinal) spin coherence time. The resonator rethermalization is described by
Lgr g2 nth 1
D a
r g2 nthDaw r.
Within this two-state model, an analytic expression for the steady state phonon number nf can be found by using the matrix of second order moments (Supplementary Note 3)43.
a b c
0.04
35
25
30
25 20 15
5
0.6
Ground state Rabi oscillations Exicted state spin driving
/2 = 26 3 MHz
e/2 , (MHz)
P g ,+1 , (Arbitrary units)
0.50.40.30.20.10.0
0.0 0.5 1.0 1.5Effective Rabi interval (s) Optical pulse length (s)
P e ,+1
0.03
0.02
0.01
0.00
2.0 2.5 3.0 0.0 0.1 0.2 0.3 0.4 0.5 0.6 1.0 1.5 2.0 2.5
g/2 (MHz)
Figure 3 | Quantifying the excited state spinstrain coupling. (a) Mechanically driven Rabi oscillations within the ground state (GS) that have been t using the procedure described in Supplementary Note 2. (b) Population in e; 1
j i plotted as a function of topt. The red curves are least squares ts to a
seven-level master equation model of the measurement. The data in a,b were measured on a single device with an NV centre ensemble, and error bars are from the s.d. in photon counting. (c) The excited state mechanical driving eld plotted against the GS mechanical driving eld and t with a linear scaling. Each point corresponds to a single measurement, and error bars are standard error from the ts.
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a
opt
Orbital
Spin
c d
6,000
Final phonon number
5,000
4,000
3,000
2,000
1,000
0
1017 1018 1019 1020 1021
1.0
0.8
0.6
0.4
0.2
0.0
Fractional cooling
Aligned NV density (cm3)
Figure 4 | A dissipative protocol for cooling a mechanical resonator. (a) The seven NV centre orbital and spin states at room temperature. Fast (slow) transitions are indicated by solid (dashed) one-way arrows. Coherent couplings are indicated by two-way arrows. (b) The toy model depiction of the proposed cooling protocol. (c) Schematic of a doubly-clamped beam. (d) Final phonon number achieved by the cooling protocol as a function of the density of properly aligned NV centers. Vertical lines indicate densities that have been realized in single-crystal diamonds (7.0 1017 cm 3 (ref. 31),
1.1 1018 cm 3 (ref. 58), 2.0 1018 cm 3 (ref. 56)) and nanodiamonds (4 1020 cm 3 (ref. 57)).
a
n: 4
For an ensemble of N spins coupled to the resonator but not to one another, each spin will add an additional damping term to the resonator dynamical equation. This allows us to rewrite the last term in equation (4) as
p leff. To determine a, we solve for the 7 7 density matrix describing the steady state
of the ensemble in the absence of the mechanical resonator, calculate the population difference between e; 1
j i and e; 1
j i,
and obtain a 0.017 for optimized control elds (Supplementary
Note 4).
Elasticity theory provides a means of calculating the remaining device parameters. For a doubly-clamped beam of length l, thickness t and width w, we compute leff from the strain because of the zero-point motion of the resonator E0(y, z) with coordinates as dened in Fig. 4c (see Methods). For a uniform distribution of properly aligned NV centres at a density n, we obtain41,48
leff
Under the secular approximation and working in the limit g; l 1=T1; 1=T 2, the dynamical equation for the
phonon occupancy n hawai can be simplied to dndt g nth n
4l2 2=T 2 1=T1
1=T1;i n. If each spin within the ensemble has the same T1 and T 2, we can factorize this expression and replace the individual li with an effective
ensemble-resonator coupling leff
PNi1l2i s
PNi14l2i 2=T 2;i
. For the case of
uniform coupling, this simplies to leff
N
de?
p
Z
Z
t=2
l t=2 E20 y; z
p l, which is equivalent to the effective coupling in the TavisCummings model44,45. Solving for the steady state of the system then gives
nf
gnth
g
dydz
s : 6
Evaluating equation (6), we nd that leff is independent of w and scales as leff G0
anw
0
p =l where G0 de?
nt
p
ak0=E
,
: 5
The problem now becomes mapping the seven-level NV centre structure pictured in Fig. 4a onto this two-state spin system. We do this by distilling the seven-level landscape to a toy model that contains only the two-states that couple to the mechanical resonator, e; 1
j i and e; 1
j i, as shown in Fig. 4b. Within this
simplied landscape, we assign T 2 to be the ES coherence time (T 2e 6.0 ns (ref. 46)) and T1 to be the ES lifetime of e; 1
j i
(T1e 6.89 ns (ref. 47)). At any one moment, only a fraction a
of the spins within the ensemble will be in the proper e; 1
j i; e; 1
j i
f g subspace to participate in the cooling.
We account for this by modifying leff !
120 GHz mm, and E 1,200 GPa is the Youngs modulus
of diamond. The frequency of the resonators fundamental mode scales as om k0t/l2. As described in Supplementary Note 5,
higher order mechanical modes are spectrally isolated from the NV centre spin dynamics in the devices considered here17,41. For any thin-beam resonator in the resolved-sideband regime
om=2p41=T 2e 170 MHz, the fractional cooling nf/nth is
insensitive to the physical dimensions of the resonator because the size of the ensemble scales with the size of the resonator. This can be seen by rewriting equation (5) as nf/nth (1 w) 1, where w
4 Qna de?
k0
4l2eff 2=T
2
1=T1
2
is independent of the resonator dimensions.
For illustrative purposes, we choose to examine a resonator with a
E 2=T
2e
1=T1e
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a
Optically detected magnetic resonance Optically detected magnetic resonance
Bx frequency (GHz) Bx frequency (GHz)
b
1.000
Normalized P.L.
0.995
0.990
0.985
Normalized P.L.
1.000
0.995
0.990
0.985
Bz = 20.2 G
2.805
2.810 2.815 2.820 2.825
2.380 2.385 2.390 2.395 2.400
c
Normalized amplitude
0.6
0.5
0.4
0.3
0.2
0.1 20 40 60 80 100 120 140 160
Bz (G)
Figure 5 | Calibrating Bz-dependent nuclear polarization. (a,b) Normalized photoluminescence (P.L.) plotted as a function of the magnetic driving eld carrier frequency for (a) Bz 20.2 G and (b) Bz 171.5 G. The solid line in each plot is a least squares t to the sum of three Lorentzians. The data in a,b was
measured on a single device with an NV centre ensemble, and error bars are from the s.d. in photon counting. (c) Normalized amplitude of each mI hyperne sublevel as a function of Bz. The solid lines are least squares ts to a linear model, each point corresponds to a single measurement, and error bars are standard error from the ts.
om/2p 1 GHz fundamental mode and assume fully polarized
nuclear spins49. Potential device dimensions then become (l, t) (1.9, 0.19) mm. Finally, phononphonon interactions
limit the Q of an ideal diamond mechanical resonator at room temperature. For modes satisfying om/2p 41/T 2e, the maximum
Q 2 106 is independent of om (ref. 50), and we now have all
the parameters needed to study the performance of the protocol.
At this point, we note that distilling a seven-state model to the toy model we employ certainly requires validation. To justify our simplied model, we calculate the cooling predicted within the toy model and compare this both to an analytical LambDicke treatment of the seven-level model14,51 and to numerical simulations of a small number of seven-level NV centres coupled to a resonator. Because of the exponential growth of the Hilbert space, full seven-level numerical simulations were performed on the Titan supercomputer at Oak Ridge National Laboratory, with the most intensive simulations taking B104 core-hours. Comparing the toy model and LambDicke results to the numerical simulations, we determined that the two-level distillation outperforms the LambDicke approach in all test cases and provides an upper bound on nf (Supplementary
Note 6). This indicates that the proposed protocol cools a resonator more efciently than our toy model predicts5255.
Cooling performance. The lowest phonon occupancy that can be reached depends strongly on the density of properly aligned NV centres n. For instance, Choi, et al. reported measurements of an
NV centre ensemble with n 2.0 1018 cm 3 in single-crystal
diamond56. For this density and Q 2 106, we nd that the
proposed protocol cools a room temperature resonator to nf 0.86nth. Using the same Q and the density of n 4 1020
cm 3 reported by Baranov, et al. in nanodiamonds57, however, the protocol can cool to nf 0.03nth.
Increasing the size of the ensemble can thus dramatically increase the protocols cooling power. The magnetic eld noise from paramagnetic impurities will also grow with n, degrading the
GS coherence time. However, for large magnetic driving elds, this cooling protocol does not require a lengthy GS coherence time (Supplementary Note 4). The only coherence time that effects the protocol is T 2e, which is not expected to change with the defect density34,37. This means that large NV centre densities could in principle be used to cool a resonator with the ES spinstrain interaction. To study how increasing n affects the protocol, we plot nf against n in Fig. 4d for several different Q-values. For reference, we have included lines marking values of n that have been realized in single-crystal diamonds31,56,58 and in nanodiamonds57. The limiting density of NV centres in a single-crystal diamond nanostructure is currently unknown. Furthermore, while high defect densities have been shown to degrade the Q of om=2p 10 kHz frequency resonators59,
it remains to be seen how the gigahertz frequency resonators of interest here will be affected by the incorporation of a dense defect ensemble. These questions motivate future experimental work.
DiscussionThe insensitivity of the proposed protocol to the GS coherence time makes an ES cooling protocol an attractive and practical route to cooling a room temperature mechanical resonator with NV centres. Alternative approaches that use the GS spinstrain coupling18,19,25 are incompatible with the collective enhancement from a dense ensemble that makes the proposed protocol viable. Although the GS inhomogeneous dephasing time T 2g can be Bms long in high purity diamonds, T 2g scales roughly as 1=n in bulk
diamond and can be o100 ns for dense ensembles30,31. Within a nanostructure, effects such as exchange narrowing and the
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truncation of the spin bath mitigate this reduction in T 2g (refs 57,60) and make it difcult to predict the decrease in T 2g inside a doubly-clamped beam. Nevertheless, we can roughly compare the ES and GS spinstrain interactions by calculating Z using coherence times measured in bulk diamond (Supplementary Note 7). For a moderate NV centre density of n 2.8 1013 cm 3 (ref. 18), the single-spin cooperativity for the
ES spinstrain interaction is 2.4-times larger than in the GS, and for n 7.0 1017 cm 3 (ref. 31), Z is 19-times larger in the ES.
In both cases, the ES offers the more efcient route to cooling, and as the collective enhancement grows, the ES interaction becomes increasingly more efcient than the GS interaction. A dense ensemble coupled via the ES spinstrain interaction thus becomes the more promising route to cooling a room temperature mechanical resonator with NV centres.
It is important to note that this analysis of the proposed protocol only applies for operation at room temperature. Reducing the bath temperature will lower nth and would thus ideally lower nf. However, the ES coherence time is limited by the ES motional narrowing rate, which increases as the bath temperature decreases34,37. This is expected to lead to a reduction in T 2e at lower temperatures, followed by a complete loss of
ES spin coherence below B150 K (ref. 32). As seen from equation (5), a reduction in T 2e will lead to a loss of cooling power. For cryogenic starting temperatures, it thus becomes necessary to use either the GS spin-phonon interaction or the orbital-strain interaction to cool a mechanical resonator with NV centres.
Finally, nf could be lowered further by simultaneously implementing an optomechanical cooling protocol812 alongside the proposed protocol. Optomechanical cooling has been demonstrated to cool gigahertz frequency resonators to
nf 0:01nth (refs 6,61). The cooling rate from an optimized
realization of the proposed protocol would combine additively with the optomechanical cooling rate, allowing the two complementary techniques to operate in conjunction and enhance the total cooling.
In conclusion, we have proposed a dissipative protocol for cooling a room temperature mechanical resonator that utilizes an ensemble of NV centre spins to realize a collective enhancement in the spin-phonon coupling. After experimentally determining that the spinstrain coupling in the room temperature ES is13.50.5 times stronger than the GS spinstrain coupling, we analysed the performance of the cooling protocol. For very dense NV centre ensembles, the proposed protocol can cool a room temperature resonator to a fraction of its thermal phonon occupancy. These results shed further light on the orbitally-averaged room temperature ES of the NV centre and demonstrate a practical path towards cooling a room temperature mechanical resonator with NV centres.
Methods
Sample details. Our HBAR consists of a 2.5 mm-thick ZnO piezoelectric lm sandwiched between a 25/200 nm Ti/Pt ground plane and a 250 nm thick apodized Al top electrode, all sputtered on one face of a h100i single-crystal diamond
substrate. Applying a high-frequency voltage to this transducer launches acoustic waves into the diamond, which then serves as a FabryProt cavity to generate a comb of standing wave resonances. By apodizing the shape of the Al electrode, we mitigate the loss of power into lateral modes formed across the diameter of the HBAR. The antenna fabricated on the opposite diamond face was patterned from 25/225 nm Ti/Pt with a lift-off process.
The CVD-grown diamond used in these measurements contained NV centres at a density of B4 1014 cm 3 as purchased. Our measurements thus address an
ensemble of B70 NV centres oriented with their symmetry axis parallel to Bz. NV centres of different orientations are spectrally isolated and contribute only a constant background to the measurements.
Spectrum tting. The spectrum pictured in Fig. 2 was t to the function
P 1
j i
ce
a Bz
Table 1 | Relaxation rates used in our seven-level master equation model47.
Parameter Value (MHz) Relaxation from k42 65.31.6 ES 1
j i to GS 1
j i
k31 64.91.5 ES 0
j i to GS 0
j i
k45 79.81.6 ES 1
j i to S1
j i
k35 10.61.5 ES 0
j i to S1
j i
k52 2.610.06 S1
j i to GS 1
j i
k51 3.000.06 S1
j i to GS 0
j i
e, +1
g, +1
g, 1
g, 0
0 B
@
a0 Bz
4 G2e Bz B0 Aejj=gNV
1 2
4 G2e Bz B0
1 2
a Bz
4 G2e Bz B0 Aejj=gNV
1 2
1 C
A
0 B
@
4 G2g Bz B0 Agjj=gNV
1 2
4 G2g Bz B0
1 2
a Bz
4 G2g Bz B0 Agjj=gNV
1 2
1 C
A
7
cg a Bz
a0 Bz
where ce and cg are constant amplitudes that quantify the driven spin contrast for the ES and GS resonances, ai[Bz] are eld-dependent scaling factors that account for the dynamic nuclear polarization of the hyperne sublevels49, Ge (Gg) is the
a
b
e/2 (MHz)
35
30
25
20
15
10
5
e, 1
e, 0
31
1.0
1.5 2.0 2.5
g/2 (MHz)
Figure 6 | Transitions and rates used in the seven-level model. (a) States and transitions included in our seven-level master equation model. The kij rates are listed in Table 1. (b) Excited state mechanical driving eld Oe plotted as a function of the ground state mechanical driving eld Og with the data labelled by the optical pumping rate G0 during each measurement. Each point corresponds to a single measurement, and error bars are standard error from the ts.
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ARTICLE NATURE COMMUNICATIONS | DOI: 10.1038/ncomms14358
FWHM of the ES (GS) resonances, B0 is the resonant eld for the mI 0 hyperne
sublevel, and the other parameters are as dened above. Of these variables, ci, Gi, and B0 are free parameters in our tting procedure.
We calibrate ai[Bz] by performing hyperne-resolved magnetically-driven electron spin resonance (ESR) measurements within the NV centre GS at different values of the magnetic bias eld Bz. This is done by xing Bz and monitoring the
NV centre photoluminescence as the carrier frequency of a magnetic driving eld oriented along Bx is swept through the g; 0
j i2 g; 1
j i spin resonance. We t the
resulting curves to the function
P C
A
0
B
@
4 G2g Bz B0 Agjj
1 2
4 G2g Bz B0 Agjj
1 2
1
C
A
P0
8
A0
4 G2g Bz B0
1 2
A
j i Oe; Aejj
a 1P 1
j i Oe; 2Aejj
15
where the normalized amplitudes (
where P is the measured photoluminescence, C accounts for the driven spin contrast, Ai is the relative amplitude of each hyperne sublevel, P0 is the background photoluminescence, and we x
P
P
Ai 1. Figure 5a,b shows ESR
curves measured at Bz 20.2 G and 171 G. We have used the values of P0 returned
from the ts to normalize the photoluminescence.
Figure 5c shows the normalized amplitude of each nuclear sublevel plotted as a function of Bz. As expected, the nuclear polarization increases in the direction of the ES level anti-crossing at BLACz 507 G. In this gure, we have t each curve to a
straight line with a xed y-intercept of 13 to obtain the linear scaling functions ai[Bz] in equation (7). The sum of these scaling functions satises
P
ai 1) account for nuclear spin polarization
and have been measured separately via magnetic ESR. A least squares t of equation (15) to the data then provides Oe. Here, Oe is the only free parameter in the tting procedure.
When tting the relation between Oe and Og (Fig. 3c), we x the y-intercept of the linear tting function to be zero.
Elasticity theory. To analyse how strain couples to NV centres within a resonator, we start by assuming that the NV centres are aligned with the direction of beam deection such that the strain in an oscillating beam is entirely perpendicular to the NV centre symmetry axis. We then use elasticity theory to derive the scaling laws quoted above17,41.
The wave equation for doubly-clamped beams is
rdA @2
@t2 f t; z
EI
@4@z4 f t; z
ai[Bz] 1.
Seven-level master equation model. The master equation used to model our ES spin driving measurements is derived in the room temperature NV centre basis dened by the states g1; g0; g 1; e1; e0; e 1; S1
f g where, within the e and g
subspaces, a subscript denotes the ms value. The 7 7 density matrix evolves
according to (: 1)_
r i H; r
LGr: 9 In the rotating frame, the Hamiltonian is given by
H O2 e1
j i e 1
h j e 1
j i e1
h j
j i e1
h j 10 where Dm is the mechanical detuning. The incoherent NV centre processes are described by the superoperator
LGr GoptXi 1;0Lg ;e k42 Xi 1Le ;g k45 Xi 1Le ;S k52 Xi 1LS ;g
k31Le ;g k35Le;S k51LS ;g
1 T 2e
16
where f(t, z) is the transverse displacement in the y-direction, ^z points along the beam as indicated in Fig. 4c, A wt is the cross-sectional area of the resonator,
E 1,200 GPa is the Youngs modulus of diamond, rd 3.515 g cm 3 is the mass
density of diamond, and I wt3/12 is the resonators moment of inertia. Solutions
are of the form f(z, t) u(z)e iot where
un z an cos knz cosh knz
bn sin knz sinh knz
; 17 and the allowed k-vectors satisfy cos(knz) cosh(knz) 1. The wave vector and
amplitudes of the fundamental mode satisfy k0l 4.73 and a0/b0 1.0178.
We normalize un(z) by setting the free energy of the beam equal to the zero point energy of the mode:
W
1
2 EI
Dm e1
Xi 1;0Le ;e
11
1
2 on 18
where the eigenfrequencies of the resonator are given by on k2n
EI=rdA
where we dene
Li;f r f
j i i
h jr i
j i f
h j
1
2 i
j i i
h jr r i
j i i
h j
Z
L @2un
@z2
2
dz
0
p
: 12 Here, Gopt is the optical pumping rate of our 532 nm laser, T 2e 6.00.8 ns is the
ES coherence time46, and the relaxation rates kij are listed in Table 1. Figure 6a summarizes this landscape47.
Because optical initialization does not generate a pure state, we rst simulate the optical pumping process to obtain an initialized density matrix. To do so, we start with a thermal state rNV 13
Pi 1;0gij i gih j and apply equation (9) with Oe,
Dm 0 and Gopta0 for 10 ms. We take the resulting density matrix and apply
equation (9) for 5 ms with Oe, Dm, Gopt 0 to simulate the relaxation to g
j i.
A simulated p-pulse then swaps r22 and r33, providing the appropriate starting density matrix r0 for a given Gopt. From r0, we also extract the minimum and maximum spin contrast (smin g0
h jr0 g0
j i and smax g 1
h jr0 g 1
j i), which allow
us to properly normalize our simulations.
Next, we model the measurement of S2, the spin re-initialization. To do so, we apply equation (9) to r0 with Oe, Dm 0 and Gopta0 for a length of time topt.
Allowing the spin to relax as before gives us the measured density matrix r2. We normalize g 1
h jr2 g 1
j i using smin and smax, and repeat this simulation as a
function of topt to obtain a simulated S2 curve.
To account for spatial inhomogeneities in the optical power within the NV centre ensemble, we perform a weighted average of this simulation over the point spread function (PSF) of our microscope. We approximate the PSF by the function
Gopt z G0
sin k z0
z z0
f g
k z0
z z0
. This
expression for on can be simplied to on knt/l2, where kn knl
2
p
E=12rd
.
For the fundamental mode, k0 120 GHz mm as quoted above.
The spin-phonon coupling for a single NV centre located at (y, z) is given by l d>E0(y, z) where E0 y; z
y @@z un z
is the strain from the zero point
motion of the resonator mode. Here, the y-axis is zeroed at the neutral axis of the resonator. To compute the effective ensemble-resonator coupling, we assume a uniform distribution of properly aligned NV centres within the resonator and sum
the individual couplings in quadrature according to leff
a
PNi1 l2i s
, which gives
2
13
where G0 is the peak optical pumping rate, k[z0] denes the depth-dependent PSF width15, z is the distance below the diamond surface, and z0 7.90.9 mm is the
focus depth of the PSF. An ensemble measurement is then given by
Sens2 topt
equation (6).
Data availability. The data that support the ndings of this study are available from the corresponding author on reasonable request.
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Acknowledgements
Research support was provided by the Ofce of Naval Research (ONR) (Grant N000141410812). Device fabrication was performed in part at the Cornell NanoScale Science and Technology Facility, a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (Grant ECCS-15420819), and at the Cornell Center for Materials Research SharedFacilities which are supported through the NSF MRSEC program (DMR-1120296). Numerical simulations were performed in part at the Centre for Nanoscale Materials,a U.S. Department of Energy Ofce of Science User Facility under contractno. DE-AC02-06CH11357. This research used resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, which is supportedby the Ofce of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725.
Author contributions
E.R.M. and G.D.F. developed the concept and procedure for the experiment and the proposed cooling protocol. E.R.M. performed the experiments and analysed the data. E.R.M., M.O., S.K.G. and G.D.F. developed the toy model treatment of the proposed cooling protocol. M.O. and S.K.G. developed and performed the numerical simulations that validate the toy model treatment of the cooling protocol. E.R.M., M.O, S.K.G. and G.D.F. prepared the manuscript.
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How to cite this article: MacQuarrie, E. R. et al. Cooling a mechanical resonator with nitrogen-vacancy centres using a room temperature excited state spinstrain interaction. Nat. Commun. 8, 14358 doi: 10.1038/ncomms14358 (2017).
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Copyright Nature Publishing Group Feb 2017
Abstract
Cooling a mechanical resonator mode to a sub-thermal state has been a long-standing challenge in physics. This pursuit has recently found traction in the field of optomechanics in which a mechanical mode is coupled to an optical cavity. An alternate method is to couple the resonator to a well-controlled two-level system. Here we propose a protocol to dissipatively cool a room temperature mechanical resonator using a nitrogen-vacancy centre ensemble. The spin ensemble is coupled to the resonator through its orbitally-averaged excited state, which has a spin-strain interaction that has not been previously studied. We experimentally demonstrate that the spin-strain coupling in the excited state is 13.5±0.5 times stronger than the ground state spin-strain coupling. We then theoretically show that this interaction, combined with a high-density spin ensemble, enables the cooling of a mechanical resonator from room temperature to a fraction of its thermal phonon occupancy.
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